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X-Ray Tomography

in Material Science

0 HERMES Science Publications, Paris, 2000


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While every effort has been made to check the accuracy of the information in this book, no
responsability is assumed by Author or Publisher for any damage or injury to or loss of
property or persons as a matter of product liability, negligence or otherwise, or from any
use of materials, techniques, methods, instructions, or ideas contained herein.

X-Ray Tomography
in Material Science

Jose Baruchel
Jean-Yves Buffiere
Eric Maire
Paul Merle
Gilles Peix

cience

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Authors

ANDERSON P., Department of Biophysics in Relation to Dentistry, St Bartholomew's


and The Royal London Scool of Medecine and Dentistry, Queen Mary and
Westfield College, Mile End Road, London, El 4NS, UK
BABOT D., Laboratoire CNDI, INSA, Batiment 303, 69621 Villeurbane Cedex,
France
BARUCHEL J., European Synchrotron Radiation Facility, BP 220, F-38043 Grenoble,
France
BELLET D., Laboratoire GPM2, INPG, BP 46, 38402 Saint-Martin-d'Heres
BENOUALI A.-H., Department of Metallurgy and Materials Engineering, Katholieke
Universiteit Leuven, De Croylaan 2, B-3001 Heverlee, Belgium
BERNARD D., ICMCB, CNRS, 87 avenue du docteur Albert Schweitzer, 33608
Pessac, France
BLANDIN J.-J., Genie physique et mecanique des materiaux, ENSPG-UJF, BP 46,
F-38402 Saint-Martin-d'Here Cedex, France
BOLLER E., European Synchrotron Radiation Facility, BP 220, F-38043 Grenoble,
France
BOUCHET S., Ecole des mines , ENSMP, 35 rue St Honore, 77300 Fontainebleau,
France
BRACCINI M., Genie physique et mecanique des materiaux, ENSPG-UJF, BP 46,
F-38402 Saint-Martin-d'Here Cedex, France
BUFFIERE J.-Y., GEMPPM INSA Lyon, 20 avenue Albert Einstein, 69621
Villeurbane Cedex, France
CLOETENS P., European Synchrotron Radiation Facility, BP 220, F-38043 Grenoble,
France
DAVIS G., Department of Biophysics in Relation to Dentistry, St Bartholomew's and
The Royal London Scool of Medecine and Dentistry, Queen Mary and Westfield
College, Mile End Road, London, El 4NS, UK
DEGISCHER H.P., Institute of Materials Science and Testing, Vienna University of
Technology, Karlsplatz 13, A-1040 Wien

X-ray tomography in material science

DERBY B., Manchester Materials Science Centre, UMIST and the University of
Manchester, Grosvenor Street, Manchester, Ml 7HS,UK
DUVAUCHELLE P., Laboratoire CNDI, INSA, Batiment 303, 69621 Villeurbane
Cedex, France
ELLIOTT J., Department of Biophysics in Relation to Dentistry, St Bartholomew's
and The Royal London Scool of Medecine and Dentistry, Queen Mary and
Westfield College, Mile End Road, London, El 4NS, UK
FOROUGHI B., Institute of Materials Science and Testing, Vienna University of
Technology, Karlsplatz 13, A-1040 Wien
FREUD N., Laboratoire CNDI, INSA, Batiment 303, 69621 Villeurbane Cedex,
France
FROYEN L., Department of Metallurgy and Materials Engineering, Katholieke
Universiteit Leuven, De Croylaan 2, B-3001 Heverlee, Belgium
GuiGAY J.-P., University of Antwerp, RUCA Groenenborgerlaan 171, B-2020
Antwerp, Belgium
HEINTZ J.-M., ICMCB, CNRS, 87 avenue du docteur Albert Schweitzer, 33608
Pessac, France
JOSSEROND C., Genie physique et mecanique des materiaux, ENSPG-UJF, BP 46,
F-38402 Saint-Martin-d'Here Cedex, France
JUSTICE I., Department of Materials, University of Oxford, Parks Rd, Oxford, OX1
3PH, UK
KAFTANDJIAN V., Laboratoire CNDI, INSA, Batiment 303, 69621 Villeurbane
Cedex, France
KOTTAR A., Institute of Materials Science and Testing, Vienna University of
Technology, Karlsplatz 13, A-1040 Wien
LUDWIG W., European Synchrotron Radiation Facility, BP 220, F-38043 Grenoble,
France
MAIRE E., GEMPPM INSA Lyon, 20 avenue Albert Einstein, 69621 Villeurbane
Cedex, France
MARC A., LETI-CEA/Grenoble, 17 rue des martyrs, 38054 Grenoble Cedex 9,
France
MARTIN C.F., Genie physique et mecanique des materiaux, ENSPG-UJF, BP 46,
F-38402 Saint-Martin-d'Here Cedex, France
PEK G., Laboratoire CNDI, INSA, Batiment 303, 69621 Villeurbane Cedex, France
PEYRIN F., CREATIS, INSA-Lyon, 69621 Villeurbane, France
ROBERT-COUTANT C., LETI-CEA/Grenoble, 17 rue des martyrs, 38054 Grenoble
Cedex 9, France
SALVO L., Genie physique et mecanique des materiaux, ENSPG-UJF, BP 46,
F-38402 Saint-Martin-d'Here Cedex, France
SAVELLI S., GEMPPM INSA Lyon, 20 avenue Albert Einstein, 69621 Villeurbane
Cedex, France
SCHLENKER M., CNRS, Laboratoire Louis Neel, BP 166, F-38042 Grenoble, France
SUERY M., Genie physique et mecanique des materiaux, ENSPG-UJF, BP 46,
F-38402 Saint-Martin-d'Here Cedex, France

Authors

VAN DYCK D., University of Antwerp, RUCA Groenenborgerlaan 171, B-2020


Antwerp, Belgium
VERRIER S., Genie physique et mecanique des materiaux, ENSPG-UJF, BP 46,
F-38402 Saint-Martin-d'Here Cedex, France
VIGNOLES G.-L., LCTS, CNRS-SNECMA-CEA, Universite Bordeaux 1, 3 allee La
Boetie, F-33600 Pessac, France
WEVERS M., Department of Metallurgy and Materials Engineering, Katholieke
Universiteit Leuven, De Croylaan 2, B-3001 Heverlee, Belgium

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Table of contents

Foreword

13

Chapitre 1. General principles

G. PEIX, P. DUVAUCHELLE, N. FREUD


1.1. Introduction
1.2. X and gamma-ray tomography: physical basis
1.3. Different scales, different applications
1.4. Quntitative tomography
1.5 Conclusion
1.6. References

15
15
16
20
23
26
26

Chapitre 2. Phase contrast tomography

P. CloETENS, W. LUDWIG, J.-P. GUIGAY, J. BARUCHEL, M. SCHLENKER,


D. VANDYCK
2.1. Introduction
2.2. X-ray phase modulation
2.3. Phase sensitive imaging methods
2.4. Direct imaging
2.5. Quantitative imaging
2.6. Conclusion
2.7. References

29
29
30
32
38
38
42
43

Chapitre 3. Microtomography at a third generation syncrotron


radiation facility

J. BARUCHEL, E. BOLLER, P. CLOETENS, W. LUDWIG, F. PEYRIN


3.1. Introduction
3.2. Syncrotron radiation and microtomography

45
45
46

10

X-ray tomography in material science

3.3. Improvement in the signal to noise ratio in the 3D images


3.4. Improvement in the spatial resolution
3.5. Quantitative measurement (absorption case)
3.6. Present state of "local" tomography
3.7. Sample environment in microtomography
3.8. Phase Imaging
3.9. Other new approaches in microtomography
3.10. Conclusion
3.11. References

49
50
51
53
54
55
56
57
57

Chapitre 4. Introduction to reconstruction methods


C. ROBERT-COUTANT, A. MARC

61

4.1. Introduction
4.2. Description of projection measurements
4.3. Backprojection
4.4. Projection-slice theorem
4.5. Fourier reconstruction methods
4.6. Filtering in Fourier methods
4.7. ART-type methods
4.8. Conclusion
4.9. References

61
62
65
66
67
69
70
74
74

Chapitre 5. Study of materials in the semi-solid state

S. VERREER, M. BRACCINI, C. JOSSEROND, L. SALVO, M. SUERY, W. LUDWIG,


P. CLOETENS, J. BARUCHEL
5.1.
5.2.
5.3.
5.4.
5.5.
5.6.

Introduction
Experimental device and procedure
Results on Al-Si alloys
Results on Al-Cu alloys
Conclusion and perspectives
References

,...

77
77
79
80
85
86
87

Chapitre 6. Characterisation of void and reinforcement distributions


by edge contrast

I. JUSTICE, B. DERBY, G. DAVIS, P. ANDERSON, J. ELLIOTT


6.1. Introduction
6.2. Dual energy X-ray microtomography
6.3. Experimental materials
6.4. Results and discussion
6.5. Conclusions
6.6. References

89
89
90
92
94
100
101

Table of contents

11

Chapitre 7. Characterisation of MMCp and cast Aluminium alloys

J.-Y. BUFFIERE, S. SAVELLI, E. MAIRE


7.1.
7.2.
7.3.
7.4.
7.5.

103

Introduction
Experimental methods
Results and discussion
Conclusion
References

103
104
107
112
113

Chapitre 8. X-ray tomography of Aluminium foams and Ti/SiC composites

E. MAIRE, J.-Y. BUFFIERE

115

8.1. General introduction


8.2. Aluminium foams
8.3. Titanium composites
8.4. General conclusion
8.5. References

115
116
121
124
125

Chapitre 9. Simulation tool for X-ray imaging techniques

P. DUVAUCHELLE, N. FREUD, V. KAFTANDJIAN, G. PEIX, D. BABOT


9.1.
9.2.
9.3.
9.4.
9.5.
9.6.

127

Introduction
Background
Simulation possibilities
Simulation examples in tomography
Conclusions and future directions
References

127
128
129
132
135
136

Chapitre 10. Micro focus computed tomogrgraphy of Aluminium foams


A.-H. BENAOULI, L. FROYEN, M. WEVERS
10.1.
10.2.
10.3.
10.4.
10.5.
10.6.

Introduction
Production process of Aluminium foams
Mechanics of foams
Non-destructive investigation of Aluminium foams
Conclusion
References

139
139
140
142
144
151
152

Chapitre 11. 3D observation of grain boundary penetration in Al alloys


W. LUDWIG, S. BOUCHET, D. BELLET, J.-Y. BUFFIERE

11.1. Introduction
11.2. Experimental set-up
11.3. Result
11.4. Conclusions
11.5. References

.*.

155

155
157
158
160
163

12

X-ray tomography in material science

Chapitre 12. Determination of local mass density distribution

H.P. DESISCHER, A. KOTTAR, B. FOROUGHI


12.1. Introduction
12.2. Material
12.3. X-ray radiography
12.4. Result
12.5. Application of the mean local density distribution
12.6. References

165
165
166
166
168
172
175

Chapitre 13. Modelling porous materials evolution

D. BERNARD, G.-L. VIGNOLES, J.-M. HEINTZ


13.1. Introduction
13.2. Evolution of sandstone reservoir rocks by pressure solution
13.3. C-C
13.4. Ceramics sintering
13.5. Conclusions and forthcoming works
13.6. References

177
177
179
185
187
190
191

Chapitre 14. Study of damage during superplastic deformation

C.-F. MARTIN, J.-J. BLANDIN, L. SALVO, C. JOSSEROND, P. CLOETENS,


E. BOLLER
14.1. Introduction to damage in superplasticity
14.2. Usual techniques of characterisation
14.3. Experimental procedure
14.4. X-ray microtomography results
14.5. Quantification of the coalescence process
14.6. Conclusions
14.7. References

193
193
197
198
199
200
203
204

Foreword

This book collects the texts of the lectures given during the Workshop on the
application ofX-Ray tomography in material science which was organised by the
Groupe d'Etudes de Metallurgie Physique et de Physique des Materiaux (GEMPPM)
in Villeurbanne on October 28-29 1999. Researchers from several European
universities, research centres and companies attended the lectures which were given
by experts in both materials science and X-ray tomography. The workshop was
subsidised by the INSA Lyon, the MMC Assess european network and the
Region Rhone Alpes and we would like to acknowledge their support.
The scope of this European workshop was to provide material scientists with a
detailed presentation of X-Ray tomography techniques, including the latest
developments, and to present recent applications of these techniques in the field of
structural materials.
The interest of material scientists in X ray tomography arises from two facts: 1)
most structural materials are opaque, and 2) it is of very crucial importance to
observe what occurs in the bulk of materials when they are subjected to a
mechanical loading. The apparent contradiction between these two facts has been
overcome by recent progress in X Ray tomography which has allowed 3D non
destructive images of structural materials, with a resolution around 1 micron, to be
achieved. Synchrotron radiation sources are necessary to record these very high
resolution images. Moreover, the phase contrast images, easily obtainable with X
ray sources emitting photons with a high spatial coherence, even permits the
visualisation of features with weak attenuation differences. This technique is
especially well adapted for studying metal matrix composites which are among the
most promising structural materials and for which damage development under stress
is of crucial importance.
Within this framework, the workshop was divided into two parts. The first one
included a global description of the technique itself, an introduction to the

14

X-ray tomography in material science

reconstruction algorithms, and an overview of the new possibilities offered by


synchrotron X ray sources with an emphasis on the phase contrast images. The
second part was devoted to the presentation of some examples of the application of
X-Ray tomography to investigating micro-heterogeneous structural materials. The
use of synchrotron and laboratory X-Ray sources was illustrated.
The workshop was a stimulating event which has given scientists with various
backgrounds the opportunity to discuss and exchange ideas and experiences. We do
hope that this book will bring useful information to material scientists looking for
new characterisation methods in their research fields.
The organisers,
Jose Baruchel
Staff Scientist, Group Leader ESRF
Jean-Yves Buffiere
Maitre de conferences INSA Lyon
Eric Maire
Charge de recherches INSA Lyon
Paul Merle
Professeur INSA Lyon
Gilles Peix
Maitre de conferences INSA Lyon

Chapitre 1

General principles

Among the different methods allowing to obtain, in a non-invasive way, the


image of a slice of matter within a bulky object, X-ray transmission tomography is
widely used in both the medical and the industrial fields. In the latter case, defect
detection, dimensional inspection as well as local characterization are possible.
Non destructive testing, process tomography and reverse engineering are thus
feasible. A wide range of sizes can be 1 mm small inspected, starting from a sample,
up to a whole rocket motor (several meters in diameter). The present paper describes
the physical basis and give examples of some industrial applications. The main
reconstruction artifacts are described.

1.1. Introduction
Tomography is referred to as the quantitative description of a slice of matter
within a bulky object. Several methods are available, delivering specific images,
depending on the selected physical excitation:
- ultrasonics,
- magnetic field (in the case of nuclear magnetic resonance imaging),
- X and gamma-rays (y rays),
- electric field (in the case of electrical impedance or capacitance tomography).
In the field of industrial non-destructive testing (NOT), as well as in the field of
materials characterization, X-ray or y-ray tomography is mostly used today.
Tomography is a relatively "new" technique. The very first images were obtained
in 1957 by Bartolomew and Casagrande [BAR 57]: they characterized the density of

16 X-ray tomography in material science


particles of a fluidized bed, inside a steel-walled riser. The first medical images
were performed by Hounsfield in 1972, and most industrial applications were
developed much later, in the 1980's. This slow development can be explained by the
huge amount of data to handle, and thus by the need for high speed and high
memory computers. Industrial benefits of what is called computed tomography (CT)
today are numerous. This is due to the wide range of potential applications, starting
from the small sample, 1mm in size, dedicated to the characterization of advanced
composite materials, and displayed in three dimensions with a one micrometer (urn)
voxel size, up to the single slice image, across a 1 meter diameter riser, with a five
centimeter pixel size.
1.2. X and gamma-ray tomography: physical basis
1.2.1. Different acquisition set-ups
The simplest set-up consists in detecting the photons which are transmitted
through the investigated object (Fig. 1.1): transmission tomography delivers a map
of u, the linear attenuation coefficient, quantity which is in turn a function of p (the
density) and Z (the atomic number).

Figure 1.1. X-ray transmission tomography

The clear separation between p and Z implies to perform either bi-energy


tomography or scattered photons tomography [ZHU 95, DUV 98] (Fig. 1.2). This
last technique is based on the clear differentiation between Compton and Rayleigh
scattered photons. The ratio between those two measured quantities is purely
proportional to Z and is not affected by the density.
The third possibility is to detect photons emitted by the investigated object itself.
Such is the case when gamma-ray sources are distributed inside a nuclear waste
container, for instance. Emission tomography is thus performed [THI 99] (Fig. 1.3).
An alternative is encountered when the distributed source is a positon emitter: the

General principles

17

local positon annihilation delivers pairs of 0.51 MeV annihilation photons which are
detected outside. This is the PET technique, used in the medical field.

Figure 1.2. Scattered photons tomography

Figure 1.3. Emission tomography

1.2.2. X-ray transmission tomography


The present paper will be focused on transmission tomography, which is widely
used in both industrial and medical fields. It is based on the application of equation
[1], known as the Beer-Lambert law, or attenuation law. Figure 1.4 describes the
basic experimental set-up for transmission tomography inside a single slice.

N l=

Ar0exp[-

v(x,yi)dx]

[1]

path

Measuring the number N0 of photons emitted by the source and the number N, of
photons transmitted throughout a single line across the sample allows to calculate
the integral of ja along the considered path:
[2]
N

path

The term ((x,y) represents the value of the linear attenuation coefficient at the
point (x,y). Repeating such a measurement along a sufficient number of straight
lines within the same slice delivers the Radon transform of the object. Radon
demonstrated in 1917 the possibility to find an inverse to that transform and thus to
reconstruct the n(x,y) map of the slice [KAK 87].

18 X-ray tomography in material science


As industrial tomography makes frequently use of an X-ray generator, we will
focus our discussion on that kind of experimental set-up. Nevertheless, some
comments will be made on gamma-ray tomography.

Figure 1.4. Physical basis of transmission tomography inside a slicef

1.2.3. The linear attenuation coefficient


Transmission tomography delivers a map of (x,y), the linear attenuation
coefficient, which is correlated to i) the photon energy E, ii) the density p and iii)
the atomic number Z of the investigated material. Figure 1.5 displays the
dependance between those quantities for carbon (Z=6) and iron (Z=26). It must be
noticed that the quantity displayed on Fig. 1.5 is in fact the ratio /p, the mass
attenuation coefficient.

Figure 1.5. Value of the mass attenuation coefficient for carbon and iron

Two main domains appear in Fig. 1.5. Below 200 keV, the photoelectric effect
dominates and jj/p is sharply dependant on E and Z. Equation [3] is often used to
describe this behaviour [ATT 68]:

General principles

19

[3]

where K is a constant. Such an equation implies that, for any given photon energy,
is proportional to p and to Z4. Performing images in the photoelectric domain
implies two main characteristics:
- a comparison of p between two areas of the object (or between two objects)
can be achieved only in the case when Z is constant (same atomic element or same
composition),
- a change in p between two areas can be cancelled by a change in Z in the
opposite direction.
It thus appears that a clear separation between Z and p can not be obtained, in
the photoelectric domain, unless two tomographic images are performed, using two
different energies.
Within the Compton domain, above 200 keV, u can be considered as weakly
dependant on Z and on photon energy. Tomography thus delivers an information
which is nearly proportional to p. However, due to the higher photons energy, and
hence to the lower value of u, the contrast within the object image is lower, as can
be derived from Beer-Lambert law.

1.2.4. Different experimental set-ups


In the field of industrial tomography, three different configurations are mainly
encountered. They are displayed on figure 1.6.

Figure 1.6. Different experimental set-ups in the field of industrial tomography: a) first
generation scanner, b fan-beam scanner, c) cone-beam scanner

20 X-ray tomography in material science


Figure 1.6.a corresponds to the simplest experimental set-up. A single sensitive
element is used and a rather long scanning time is needed, as the acquisition of a
single linear "projection" needs a set of elementary translations. Successive
projections are then acquired, corresponding to different value of the angle of
rotation. A half turn is sufficient to reconstruct the image of a slice. Figure 1.6.b
implies the use of a linear array. Acquisition is shorter, as a whole linear projection
is acquired at a time. A complete turn is needed since the beam diverges. Figure
1.6.c makes the best use of the X-ray cone-beam; one turn of the object is needed.
The Feldkamp algorithm [PEL 84] allows the direct 3D reconstruction of the whole
object.

1.3. Different scales, different applications


1.3.1. Industrial tomography
The main application in the field of X-ray tomography is Non-Destructive
Testing (NOT) of manufactured components, i.e. detection of internal defects.
Among other issues there are i) "reverse engineering", whose purpose is the
geometrical inspection of a component, in such a way to assist the design, ii) local
characterization of materials (density measurements, for instance) and Hi) process
tomography, able to deliver some kind of control on a continuous manufacturing
process. As industrial applications involve a broad range of sizes and a great variety
of materials to be inspected, the corresponding devices may be very different.
1.3.1.1. Different photon sources
Inspection of small components can be performed using a standard industrial Xray tube (160 kV for instance). Much attention must be paid to the stability of both
the high-voltage and the anode current, because the consecutive projections must be
acquired within constant conditions. A focus size within the range 1 to 3 mm is
acceptable. Inspecting heavier components may require a 450kV tube, or even a
linear accelerator. Two different high capacity scanners were constructed by the
french Atomic Energy Commission (CEA-LETI, Grenoble). A 420 kV X-ray
generator in the first case and an 8 MeV linear accelerator in the other case allow
the complete inspection of a whole (empty) rocket motor, up to 2.3 meters in
diametre, of a nuclear waste container or of a whole car engine.
Gamma-ray sources can be used, in spite of the very low emitted photon flux.
The Elf Research Centre (Solaize-France) uses a cesium 137 source with an activity
up to 18 GBq (gigabecquerels). The high monochromatic energy (662 keV)
delivered by the source allows to map the density of solid particles inside a fluidized

General principles

21

bed, through the steel wall of the riser (0.85 meter in diametre). A single source and
a single detector (Nal) are used, thus constituting a first generation tomograph, as
shown in Fig. 1.6a. The scan lasts 3 hours [BER 95]. The University of Bergen and
the Norsk-Hydro Company built a static device using a set of five americium 241
sources (energy: 60 keV) distributed around a pipe [JOH 96]. A linear array
comprising 17 semiconductor detectors is set opposite to each source, allowing a
near real-time (0.1 second) imaging of the slice. The purpose is to visualize the
liquid components (oil, water) apart from gas within a pipe. This application is an
example of process tomography, i.e. fast imaging dedicated to the control of a
manufacturing process.
1.3.1.2. Different families of detectors
Four main families of detectors can be found:
1. gas ionisation detectors were used in the early medical scanners. They are still
in use today in some industrial applications. Their main characteristic is their high
dynamic range. Filled with gas having a high atomic number, they can be used even
with high energies. Linear arrays are available.
2. image intensifiers (I.I.) are used in "desktop" scanners for industrial NDT of
small components. Their low dynamic range and the inherent distortion of the image
need some care. Significative 3D images can nevertheless be obtained.
3. scintillation detectors, composed of a fluorescent material (e.g. gadolinium
oxysulphide Gd2O2S, or caesium iodide Csl) are nowadays widely used. Those
detectors are of two kinds: i) the fluorescent material is directly coupled to an array
of photodiodes [KAF 96] or of photomultipliers (in some cases the coupling is
realized using tapered optic fibers), ii) the fluorescent material is spread on a screen,
which is optically coupled to a CCD camera via a lens [CEN 99].
4. arrays of semiconductors (e.g. CdTe or ZnCdTe), which allow a direct photon
detection are promising. High energy applications are possible.

1.3.2. Microtomography
Considering advanced materials characterization, the need of 3D images with a
very high resolution (a few um) obtained through a non invasive method is growing.
Figures 1.7 and 1.8 show two specific examples of 3D tomographic images
performed with two different scanners, conceived and built in our laboratory [KAF
96] [CEN 99]. Such 3D images are then used by the researchers for the modelisation
of the mechanical properties of materials, within finite elements models
computations. For such applications micro-focus X-ray tubes, with a focus size in
the range 5 - 1 0 micrometers, are used. A very low focus size allows to set the
investigated object directly at the window of the tube. A geometrical magnification

22 X-ray tomography in material science


can thus be obtained. Figure 1.9 shows that the magnification can be easily
modified.
A limit exists to the magnification: the geometrical unsharpness [HAL 92] must
be kept lower than p, the size of the sensitive element of the detector (sampling
step). In practice, this upper boundary to the magnification Gg can be computed
according to equation [4], where
represents the size of the focus:
[4]

Figure 1.7. 3D rendered view of a


tomographic image of a composite material
with 400 yon glass balls inside an organic
matrix.
(Herve
Lebail;
Laboratory
GEMPPM). The voxel size is set to 42 jjm

Figure 1.8. 3D rendered view of a


tomographic image of an aluminium foam
(density 0.06) (Eric Maire; Laboratory
GEMPPM). The voxel size is 150 pm. The
size of the sample is 3cm

Figure 1.9. According to the location of the investigated object between the focus and the
screen, different geometrical magnifications are attained

General principles

23

Designing and building such a kind of scanner implies some care in at least three
domains:
- the low photon flux delivered by the micro-focus X-ray tube results in long
exposure times; the camera must therefore deliver a very low noise,
- the choice of the photon energy is important: low energy photons deliver
images with an higher contrast, but also with an higher relative noise,
- the accuracy of the mechanical setting must be better than the expected image
resolution.
Today, the most powerful tool involves the use of synchrotron radiation. The
European Synchrotron Radiation Facility (ESRF-Grenoble) delivers a huge X-ray
flux and thus allows very short exposure times. A complete scan can be acquired
within a few minutes, with a spatial resolution down to 1 um. On beam-line ID 19,
the source is located far from the working hutch (145 meters), thus delivering
photons with a high spatial coherence. This property of the X-ray flux generates
diffraction features which underline the edges within the sample, and thus
highlighting sharp defects. Such a phenomenon, the so-called "phase contrast" [CLO
97], allows very small defects to be detected. As the beam is non-diverging, the
resolution is set by the detector itself. Transparent luminescent screens are used,
with a 5 jam sensitive layer of an yttrium-aluminium (YAG) or lutetium-aluminium
(LUAG) garnet, epitaxially grown on a YAG monocrystal, 170 jim in thickness;
they allows a high resolution (1 fim) and a 4% to 8% efficiency for 14 keV photons.

1.4. Quantitative tomography


As mentionned earlier, tomography offers many possibilities. If the goal is just
defect detection, the selected resolution must therefore be adjusted to the size of the
details to be observed. Much attention must also be paid to the noise of the camera
or, more precisely, to its dynamic range [CEN 99]. When the inspection's issue is
the determination of the accurate size of some internal feature, or the local
characterization of materials (density measurement for instance), then an increased
attention must be paid to the reconstruction artifacts. They create artificial patterns
inside the reconstructed slice (streak artifacts), or they locally modify the pixels
values (cupping effect), and hence the quantitative result [ISO 99] [SCH 90]. In the
following lines, we will describe the main physical mechanisms leading to
erroneous reconstructions, as well as the shape of the corresponding artifact in the
reconstructed image.
- Beam hardening
As an X-ray tube delivers a polychromatic spectrum, differential attenuation of
photons within the investigated object leads to the rapid attenuation of the lowest

24 X-ray tomography in material science

energy photons, and hence to the gradual increase of the mean energy along the
path. The reconstruction algorithm uses, for the reconstruction of any single point,
experimental data corresponding to individual rays impinging the point of interest,
but coming from different orientations. The corresponding information therefore
corresponds to different attenuations, and hence different energies, and different
values of ji. Two kinds of artifacts are generated by beam-hardening: i) cupping
effect and ii) streaks. Cupping effect corresponds to measured values of \JL which are
corrupted, thus preventing the measurement of the "true" density. As the measured
values, inside an homogeneous sample, are lower at the center than at the edges, the
name of cupping effect is generally used to describe this artifact. Projections can be
corrected by acquiring an image of a step-wedge, made of the same material, in such
a way to correlate the mesured attenuation to the true material thickness. Streaks
artifact correspond to abnormal values along lines which correspond, inside the
object, to high attenuation. Beam hardening artifacts can be avoided when using
some filter, i.e. a metallic foil, directly set at the window of the X-ray tube and
intended to pre-harden the spectrum [KAF 96]. Figure 1.10 displays an example of
streaks inside the tomographic image of a set of six samples surrounded by air (Fig
l.lO.a); the streaks are suppressed by the use of a copper filter, 0.1 mm in thickness
(Fig. l.lO.b).

Figure 1.10. The reconstructed slice (l.lO.a) is corrupted by streaks due to beamhardening (l.lO.a). Filtration with a foil of copper, (0.1 mm) nearly suppresses the streaks
(l.lO.b). The high voltage used for both images is 100 kV

Beam hardening is also avoided when using a monochromatic y-ray source. But
it must be kept in mind that y-ray sources deliver a very low photon flux (typically
one hundredth of the flux delivered by a tube). Tomography using synchrotron

General principles

25

radiation does not generates artifacts because a monochromator is always used,


thanks to the huge X-ray flux.
- Detector saturation
To obtain a reconstruction which is free of defect, the signal delivered by every
cell of the detector must be strictly proportional to the photon flux. Thus high values
(approaching the upper limit of the digitization range) as well as low values
(approaching the noise level) of the flux must be avoided. Streaks artifacts, similar
to those obtained in the case of beam-hardening, are generated along lines which
correspond to high attenuation.
- Aliasing
High (spatial) frequencies are encountered in the signal corresponding to every
projection. They are due to the steep edges which are eventually present in the
object. As the detector samples the signal (all along the projection) with a non-zero
step, high frequencies corrupt the data, within the Fourier domain. Streaks are
generated [KAK 87]. On figure 1.11, aliasing is visible at the corners of the objects.
- Scattered photons
Photons scattered by the sample or by its environment deliver a wrong
information which leads to cupping effect. Collimation can improve the
reconstructed image.

Figure 1.11. Aliasing at the corners

Figure 1.12. Ring artifacts

-111 corrected detector


The signal delivered by every sensitive cell of the detector must be linearly
spread between the offset level (corresponding to the absence of photons) and the
gain level (corresponding to the non-attenuated flux). A bad correction of one cell
will generate, in the reconstructed image a "ring artifact", i.e. the image of a ring,

26 X-ray tomography in material science

centered on the pixel corresponding to the location of the rotation axis. On figure
1.12 a great number of concentric rings are visible.
- Spatial distortion of the detector
Distortions of the projections, due for instance to the camera (e.g. distortions due
to the lens) deliver artifacts which can be corrected by software.
- Centering error
The reconstruction requires the knowledge of the location of the projection of
the center of rotation within the detector. Distortions are generated when the
reference to the centre is erroneous.

1.5. Conclusions
X and y-ray tomography allow a great number of potential applications. The
measured quantity is in fact the linear attenuation coefficient \i, and not directly the
density. A careful choice of the photons energy and the selection of a detector with a
high dynamic range allows to lessen the noise to a reasonable level. Coefficient \JL
can be estimated with an accuracy slightly better than 1%.

1.6. References
[ATT 68] Anrx F.H.R., ROESCH W.C., Radiation Dosimetry, Academic Press, 1968.
[BAR 57] BARTHOLOMEW R.N., CASAGRANDE, R.M., "Measuring solids
concentration in fluidized systems by gamma-ray absorption", Industrial and
Engineering Chemistry, vol. 49, n. 3, p. 428-431, 1957.
[BER 95] BERNARD J.R., Frontiers in Industrial Process Tomography, Engineering
Foundation, Ed. DM SCOTT& RA WILLIAMS, New-York, p. 197, 1995.
[CEN 99] CENDRE, E. et al., "Conception of a high resolution X-ray computed
tomography device; Application to damage initiation imaging inside materials",
Proceedings of the 1st World Congress on Industrial Process Tomography,
Umist Univ. (U.K.), p. 362-369, 1999.
[CLO 97] CLOETENS P., PATEYRON-SALOME M., BUFFIERE J.-Y., PEK G., BARUCHEL
J., PEYRIN F., SCHLENKER M., "Observation of microstructure and damage in
materials by phase sensitive radiography and tomography", J. Appl. Phys., vol.
81, n. 9, p. 5878-5886, 1997.
[DUV 98] DUVAUCHELLE P., Tomographie par diffusion Rayleigh et Compton avec
un rayonnement synchrotron: Application a la pathologic cerebrale, these de
doctoral, universite de Grenoble 1, 1998.
[PEL 84] FELDKAMP L.A., DAVIS L.C., KRESS J.W., "Practical cone-beam
algorithm", J. Opt. Soc., vol. 1, n. 6, p. 612-619, 1984.

General principles

27

[HAL 92] HALMSHAW R., "The effect of focal spot size in industrial
radiography",flrif/s/i Journal of NOT, vol. 34, n. 8, p. 389-394, 1992.
[HAR 99] HARTEVELD W.K. et al. "A fast active differencial capacitance
transducer for electrical capacitance tomography", Proceedings of the 1st World
Congress on Industrial Process Tomography, Umist Univ. (U.K.), p. 571-574,
1999.
[ISO 99] iso/TC 135/SC 5 , ISO document "NDT Radiation methods- Computed
tomography", Part I: Principles; Part II: Examination Practices, 1999.
[JOH 96] JOHANSEN G.A, FR0YSTEIN T., HJERTAKER B.T., OLSEN O., "A dual

sensor flow imaging tomographic system", Meas. Sci. Techn., vol. 7, n. 3, p.


297-307, 1996.
[KAF 96] KAFTANDJIAN V., PEDC G., BABOT D., PEYRIN F., "High resolution X-ray
computed tomography using a solid-state linear detector", Journal of X-ray
Science and Technology, vol. 6, p. 94-106, 1996.
[KAK 87] KAK A.C., SLANEY M., Principles of Computerized Tomographic Imaging,
IEEE Press, 1987.
[PIN 99] PlNHEIRO P.A.T. et al., "Developments of 3-D Reconstruction Algorithms
for ERT", Proceedings of the 1st World Congress on Industrial Process
Tomography, Umist Univ. (U.K.), p. 563-570, 1999.
[SCH 90], SCHNEBERK D.J., AZEVEDO S.G., MARTZ H.E., SKEATE M.F., "Sources of
error in industrial tomographic reconstruction", Materials Evaluation, vol. 48, p.
609-617, 1990.
[THI 99] THIERRY R. et al., "Simultaneous Compensation for Attenuation, Scatter
and Detector Response for 2D-Emission Tomography on Nuclear Waste within
Reduced Data", Proceedings of the 1st World Congress on Industrial Process
Tomography, Umist Univ. (U.K.), p. 542-551, 1999.
[ZHU 95] ZHU P., PEIX G., BABOT D., MULLER J., "In-line density measurement
system using X-ray Compton scattering", NDT & E International, vol. 28, n. 1,
p. 3-7, 1995.

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Chapitre 2

Phase contrast tomography

Hard X-ray radiography and tomography are common techniques for medical
and industrial imaging. They normally rely on absorption contrast. However, the
refractive index for X-rays is slightly different from unity and an X-ray beam is
modulated in its optical phase after passing through a sample. The coherence of third
generation synchrotron radiation beams makes a simple form of phase-contrast
imaging, based on simple propagation, possible. Phase imaging can be used either in
a qualitative way, mainly useful for edge-detection, or in a quantitative way,
involving numerical retrieval of the phase from images recorded at different
distances from the sample.

2.1. Introduction
The phase of an X-ray beam transmitted by an object is shifted due to the interaction with the electrons in the material. Imaging using phase contrast as opposed to
attenuation contrast is a powerful method for the investigation of light materials but
also to distinguish, in absorbing samples, phases with very similar X-ray attenuation
but different electron densities. Phase contrast imaging was pioneered in the early
seventies by Ando and Hosoya [AND 72], who obtained images of bone tissues and
of a slice of granite using a Bonse-Hart type interferometer [BON 65]. This technique
developed into a quantitative three-dimensional imaging technique. Because of the
limited quality of available lenses, elaborate forms of phase contrast imaging such as
Zernike phase-contrast [ZER 35] or off-axis holography [LEI 62] are presently ruled
out for hard X-rays. Three methods of phase sensitive imaging exist: the interferometric technique [MOM 95, BEC 97], the Schlieren technique [FOR 80, ING 95] and
the propagation technique [SNI 95, CLO 96]. They are compared in section 3. The
main advantages of the method used in this work, the propagation technique, are the
extreme simplicity of the set-up and the better spatial resolution.

30

X-ray tomography in material science

This technique was mostly used up to now in the so-called 'edge-detection regime'
to image directly the discontinuities in refractive index in the object. It is however possible to fully exploit the quantitative information entangled in the Fresnel
diffraction patterns towards high resolution quantitative phase tomography. The 'holotomographic' reconstruction is performed in two steps: first the optical phase of the
wave exiting the sample is retrieved numerically from images recorded at different distances from the sample. The refractive index distribution is then reconstructed from a
large number of phase maps using a classical tomographic algorithm. Results of quantitative phase tomography on samples of interest to materials science are discussed.

2.2. X-ray phase modulation


The interaction of a wave with matter affects its amplitude and phase. This can
formally be described by the complex refractive index n of the medium. Because its
value is nearly unity, it is usually written for X-rays as
n = l - < J + i/?

[1]

A plane monochromatic wave propagating along the z-axis in vacuum is of the form
exp(i^ L z) with A the X-ray wavelength. In a material with refractive index n this
becomes exp(m^ L z). The refractive index decrement 6 results in a phase variation
compared to propagation in vacuum. The imaginary part J3 determines the attenuation
of the wave. The X-ray intensity is the squared modulus of the wave and the absorption
index (3 is simply proportional to the linear absorption coefficient p.

,=

f>

[2]

The absorption index has a complex energy and composition dependence. It varies
abruptly near the characteristic edges of the elements. The refractive index decrement
6 on the other hand is primarily due to Thomson scattering and has a much simpler
dependency on the energy and the material characteristics. S is essentially proportional
to the electron density in the material. Generally, it can be expressed as

where the sum extends over all atoms p, with atomic number Zp, in the volume V,
rc = 2.8 fm is the classical electron radius, and f'p is the real part of the wavelengthdependent dispersion correction, significant near absorption edges, to the atomic scattering factor. If the composition of the material is known in terms of mass fractions
qp, the following equivalent expressions can be used

Phase contrast tomography

31

[5]

with NA Avogadro's number and Ap the mass number. 6P and pp are respectively the
refractive index decrement and mass density of the pure species.
If the dispersion correction fp can be neglected, 6 is proportional to the electron
density pe, i.e. S = r c A 2 p e /(27r). The ratios ZP/AP appearing in Equation 4 are similar for many atomic species ( 1/2), and 6 is thus to a good approximation determined
by the mass density p of the material [GUI 94]

[6]
Both 6 and ft are small, typically 10~5 - 10~6 and 10~8 - 10~9 respectively for light
materials, indicating the power of phase sensitive imaging compared to the absorption. Figure 1 shows the ratio S /ft, a figure of merit for phase effects compared to
attenuation effects, as a function of the X-ray energy E for aluminium. The energy
range includes soft X-rays and hard X-rays. In the soft X-ray range, more precisely
in the 'water window' where soft X-ray microscopes usually operate, a gain exists but
it is relatively modest. On the other hand in the hard X-ray range (energies above 6
keV) this ratio increases with energy to huge values (up to 1000). Practically, if one
selects for example an X-ray energy of 25 keV to be able to cross a thick aluminium
sample, a hole in this metal should have a diameter of at least 20 /zm to produce 1 %

Figure 2.1. Ratio S//3 of the refractive ondex decrement and the absorption index as a
function of the X-ray energy for the element aluminiu. This is a figure of merit for phase
effects compared to attenuation effects

32

X-ray tomography in material science

absorption contrast. Using the effect on the phase, the minimum detectable hole is
reduced to about 0.05 yum. X-rays are adapted for imaging of thick samples thanks
to their low absorption at high energies. If it is possible to visualise the phase of the
transmitted wave, the sensitivity and spatial resolution remain good.
For inhomogeneous samples the wave at the exit of the sample will be modulated
in both phase and attenuation. Propagation inside the sample itself can usually be
neglected and it is possible to project the object onto a single plane perpendicular to
the propagation direction. The transmission function T(x, y) gives the ratio of the
transmitted and the incident amplitudes. It can be compared to exp( f n(x, y, z)dz)
that gives the ratio of the transmitted and the incident intensities according to LambertBeer's law. This transmission function corresponds to the projection of the refractive
index distribution through
T(x,y) = A(x,y)eirtx>ri

[7]

with the amplitude


A(x,y) = e-W*'*)

and

B(x,y} - y j 0(x,y,z)dz

[8]

(p(x, y) = Y / [1 - <5(z, y, z)]dz = (?0 - -^ / 6(x, y, z}dz .

[9]

and the phase modulation

(p0 is the phase modulation that would occur in the absence of the object. In classical
absorption tomography the projection of n is determined for a large number of angular positions of the sample. The three-dimensional (3D) distribution of n(x, y, z)
or equivalently of / 3 ( x , y , z} is then reconstructed from the set of projections using a
tomographic reconstruction algorithm. Similarly if the phase map (p(x, y) is known
for a large enough number of angular positions of the object, it is straightforward to
reconstruct the distribution of the refractive index decrement 8(x, y, z).

2.3. Phase sensitive imaging methods


There are three methods of phase sensitive imaging: the interferometric technique
[MOM 95, EEC 97], the Schlieren technique [FOR 80, ING 95] and the propagation
technique [SNI 95, CLO 96]. The co-existence of the different methods shows that
they all have their advantages and disadvantages with respect to the accessible phaseinformation, the complexity of the set-up, the requirements on the beam or the spatial
frequency range covered.

Phase contrast tomography

33

2.3.1. The interferometric technique


Here contrast is due to interference of the beam transmitted through the object with
a reference beam. If the beams are coherent with each other, the intensity will be directly affected by the local phase shift. Bragg-diffraction by perfect crystal slices cut
out from a large, almost perfect monolithic silicon crystal is used to split, deviate and
recombine the two beams. A possible configuration [HAR 75] is shown in Figure 2a.
The recorded interference pattern cannot be exploited as it is because the interference
fringes cannot be directly linked to a projection of the object and because an intrinsic
fringe pattern is always present. The image treatment to quantitatively reconstruct the
phase modulation introduced by the sample is however rather straightforward. Several
images for different external phase shifts, typically 8 (including flatfield images), must
be recorded to reconstruct a single phase-map.
The possibility to perform phase tomography and to reconstruct the local distribution
of the refractive index decrement with an X-ray interferometer was demonstrated by
Momose et al and Beckmann et al in 1995 [MOM 95, BEC 95]. The interest of phase
imaging compared to absorption imaging was frequently illustrated [MOM 96]. The
complexity and stability requirements of this technique are however serious drawbacks. The sample must be immersed in a liquid that matches the refractive index of
the sample. Otherwise large phase jumps at air-sample boundaries perturb the interference fringes and the large deflection in the sample reduces the visibility of the fringes.
Some blurring is necessarily associated to the passage of the beam through the analyser crystal. This limits the resolution to about 15 /^m in the best case [BEC 97]. On
the other hand the frequency range covered is not limited towards the low frequencies
and a spatially homogeneous phase shift can be measured with respect to the reference
beam.

2.3.2. Schlieren technique


This differential phase contrast method is sensitive to the angular deviations of the
X-ray beam. Phase gradients present in the object locally deviate the beam by an angle

Forster et al [FOR 80] used a double crystal arrangement similar to the one shown in
Figure 2b. The first crystal acts as a collimator in limiting the angular and spectral
range. The angular deviations introduced by the sample change the incidence angle
with respect to the analyser that acts as an angular filter. The variety in the nomenclature for this approach can be noted: Schlieren-imaging [FOR 80, CLO 96], refraction contrast [SOM 91], phase dispersive imaging [ING 95, ING 96], phase contrast
imaging [DAV 95] and diffraction enhanced imaging [CHA 98] are the most com-

34

X-ray tomography in material science

Figure 2.2. Set-up for phase sensitive methods: (a) Interferometric technique, (b) Schlieren
technique and (c) Propagation technique

mon names. The possibility to visualise phase gradients (occuring for example at
edges) was shown by many groups, but no reconstructed (differential) phase map was
presented and the method was not extended to 3D imaging through tomographic techniques. Compared to the interferometric technique, the experimental set-up is simplified and the stability requirements are less stringent. To obtain a good sensitivity
to phase gradients, the width of the rocking curve for one of the crystals relative to
the other should be small, typically 2-10 yurad, and the angular stability should be
about 0.2 yurad [ING 96]. As the alignment is less critical, the collimator and analyser
crystal do not need to be part of a monolithic block, and the space available for the
sample and its environment increases. The samples are in general not immersed in a
liquid. The spatial resolution is again affected by the passage of the wave through the
analyser crystal. This method is less adapted than the previous one to covering the
low spatial frequency range, and very smooth variations of the phase may introduce a
phase gradient that is too small to be detected. This imaging scheme can be used on a
laboratory X-ray source. Most of the published results were obtained under these conditions, resulting in long exposure times of 15-30 minutes [ING 96] for a radiograph.
This technique corresponds to Schlieren imaging in classical optics [HEC 98].

Phase contrast tomography

35

2.3.3. The propagation technique


The spatial redistribution of the photons due to deflections or more generally Fresnel diffraction is considered a nuisance in absorption contact and projection radiography and in interferometric and Schlieren phase imaging. It is however also a unique
contrast mechanism for phase sensitive imaging, with advantages in the simplicity of
the set-up and the achievable resolution. In this case there is no distinct reference
beam as in the interferometric technique, and the beam transmitted through the object
plays this role itself. The occurrence of contrast can be understood as due to interference between parts of the wavefront that have suffered slightly different angular
deviations associated to different phase gradients. The overlap between parts of the
wavefront is only possible after propagation over a certain distance. As in previous
case, this is a differential phase imaging technique. A homogeneous phase gradient
cannot be detected because it corresponds to an overall deflection of the beam; detectable contrast requires the second derivative of the phase to be non-zero. When
the direction of the X-ray beam is tangential to the edge of structures in the sample,
such a perturbation of the wavefront is expected and contrast will appear. Possible
internal structures are holes and cracks, inclusions, reinforcing particles or fibers in a
composite material. Experimentally the sample is set in a (partially) coherent beam
and the transmitted beam is recorded at a given distance d with respect to the sample
[SNI 95, CLO 96]. The experimental set-up shown in Figure 2c is thus essentially
the same as for absorption radiography except for the increased sample to detector
distance. The crystal system upstream of the sample selects a narrow spectral range,
delivering a quasi-monochromatic beam to the sample.
The image contrast changes tremendously with the sample detector distance d.
The latter determines the defocusing distance D through [BOR 80]

with / the source sample distance. In the case of the long ESRF beamline ID 19 (d <C
/ = 145m), the defocusing distance and the sample-detector distance are practically
equal. The absorption radiograph corresponds of course to an image recorded close to
the sample (D 0). The region of the object mainly contributing to the corresponding
point of the image (the first Fresnel zone) has a radius equal to

When it is small compared to the typical transverse dimension a of the features in


the sample, a separate fringe pattern shows up for every border in the sample, and the
images are characteristic of the 'edge-detection regime' (rp <; a). Three-dimensional
reconstruction of the boundaries inside the volume is feasible with the algorithm for
absorption tomography (cf. section 4). At larger distance (rp w a) several interference fringes show up in the radiographs. These deformed images, corresponding to

36

X-ray tomography in material science

the 'holographic regime', give little direct information on the sample. However, combining such images recorded at different distances with a suitable numerical algorithm
gives access to the phase modulation (cf. section 5). For the largest distances, rarely
accessible with X-rays, one reaches the Fraunhofer limit (rp a). Figure 3 shows as
an example four radiographs of a 0.5 mm thick piece of polystyrene foam at increasing
distances D. The beam is monochromatised to 18 keV. As the distance increases, the
contrast and width of the Fresnel fringes both increase. The radiographs are recorded
with a CCD based detector involving X-ray / visible light conversion in a transparent
YAG:Ce screen [KOC 98], with an effective pixel size of 0.95 //m.
The most striking advantage of this method is the extreme simplicity of the setup. It is essentially the same as for absorption radiography. The transition between
absorption and phase radiography or between the different regimes of phase imaging is
simply obtained by changing the sample detector distance. The stability requirements
on the (few) elements downstream of the monochromator, i.e. the sample and the
detector, are easily met. The monochromator can be well upstream of the sample and
the sample detector distance can often be chosen quite large. The free space around
the sample can be used for all kinds of devices for in-situ and real-time observations.
However the optical elements of the beamline have to be carefully prepared to avoid
spurious phase images.
It can be shown that for a given defocusing distance the image is most sensitive
to a specific frequency range. The optimum distance to be sensitive to phase features
with spatial frequency / is such that

This frequency selectivity will intrinsically limit the accessibility to the low frequency
range, i.e. the smooth variations in the object's phase. The optimum distance, increasing as the square of the object size, will not be reached for these frequencies due to
physical limitations (size of the experimental hutch) or the coherence conditions. The
image is not spoiled by the passage of the modulated wave through a crystal as is the
case in the interferometric and Schlieren techniques. The resolution in the propagation technique depends on the image processing after recording. For untreated images
recorded in the edge-detection regime the resolution is limited by the fringe spacing
to about 2rp. When the fringes are disentangled in a holographic reconstruction, the
spatial resolution is limited essentially by the detector. The stringent requirements on
the beam incident on the sample explain why this technique emerged only recently
[HAR 94, SNI 95, CLO 96, NUG 96] with the appearance of partially coherent X-ray
beams delivered by third generation synchrotron radiation sources. The geometrical
resolution in the Fresnel diffraction pattern is equal to Dsa with sa f the angular source size and s the source size. The condition for observation of the spatial
frequency / is

Phase contrast tomography

37

Figure 2.3. Phase sensitive radiographs of a 0.5 mm thick piece of polystyrene foam, with the
detector at various distances dfrom the sample. X-ray energy 18 keV. (a) d= 0.03 m, (b) d =
0.2 m, (c) d = 0.5 m and (d) d = 0.9 m. The contrast and the width of the interference fringes
increase trough the series

The blurring due to source size and detector resolution explains why no interference
fringes are observed with classical laboratory sources although the propagation distances are also non-zero in projection radiography. Alternatively, the interference pattern involves the coherent superposition of laterally separated portions of the incident
beam. The interfering waves must originate from points that are mutually coherent,
and thus laterally separated by a distance smaller than the transverse coherence length
/t that can be defined as l[ = A/(2s a ). The incident beam must be coherent over the
first Fresnel zone for optimum conditions.
The conditions on the monochromaticity are less stringent. The beam is usually
monochromatised using a monochromator based on perfect silicon crystals. The en-

38

X-ray tomography in material science

ergy spread AA/A 10~4 is thus very small. The thickness of the samples that
can be investigated is not limited to the longitudinal coherence length (= A 2 /AA)
[CLO 96]. An increase in energy spread by one or even two orders of magnitude can
still correspond to quasi-monochromatic conditions. This allows to increase considerably the flux using a multi-layer monochromator with a very high substrate quality.
Using the same propagation principle but working with the polychromatic radiation
delivered by a laboratory X-ray microsource to retain some flux, deflection sensitive
images were obtained [WIL 96, POG 97]. This seems promising for work in the edge
detection regime as the main contrast, a white and black fringe, is unchanged over a
large spectral range.

2.4. Direct imaging


Most of the tomographic work performed until now using the propagation technique is based on the usual algorithm for absorption tomography. This is a workable
solution especially when the defocusing distance D is small and the sample is made
up of different (metallographic) phases with different densities [CLO 97]. This qualitative approach allows to visualise, in 3D, density discontinuities, such as reinforcing
SiC particles in an aluminium matrix composite [BUF 99]. Density jumps appear as
dark / light fringes. Another advantage is the possibility to detect and localise features
that are actually smaller than the pixel size as the interference fringes produced can be
larger than the feature itself (regime with rp > a). This makes it possible to detect
cracks with sub-micron opening. An example of a tomographic slice of an aluminiumsilicon alloy obtained using this direct approach based on a single distance is shown
on Figure 6b in the next section. However, with this approach the spatial resolution is
limited by the Fresnel fringe distribution and artefacts occur in some cases due to the
ill-suited algorithm. Binarisation of the edge-regime images is extremely tedious and
was done essentially manually. It must also be noted that the quantitative information
on density and composition is lost. For these reasons there is a need for more adapted
algorithms preserving resolution and quantitative information, at the expense of an
increased data volume and computational effort.

2.5. Quantitative imaging


A new approach, holotomography, has now been implemented to extract the quantitative distribution of the phase (and attenuation) in two-dimensional projection images, then to turn it into 3D reconstructions. It is based on images obtained at several
values of D for each angular position of the sample, in analogy with a technique
developed for electron microscopy. The reconstruction of the 3D distribution of the
refractive index is performed in two steps. In a first step (holographic reconstruction),
the phase map and if relevant the attenuation map is restored numerically for every

Phase contrast tomography

39

projection from a set of in-line holograms. In a second step (toraographic reconstruction), the Radon transform is inversed using a classical tomographic reconstruction
method, such as the filtered backprojection method. Details on the phase retrieval
method are given elsewhere [CLO 99a, CLO 99b]. Here we only give two examples:
the first is a non-absorbing polymer foam and the second an absorbing metal alloy that
introduces very large phase shifts.

2.5.1. A polymer foam

Figure 2.4. Phase map retrieved with an algorithm that combines images recorded at several
(here four) distances. The sample is a 0.5 mm thick piece of polystyrene. The X-ray energy is
18 keV.

A piece of polystyrene foam with a rather complex 3D structure was used to test
the method. It had a cross-section of 0.5 x 0.7 mm2 and negligible attenuation. Four
tomographic scans of 700 views each were automatically recorded at defocusing distances D of 0.03, 0.21, 0.51 and 0.9 m. The radiographs for a given angular position
are those of Figure 3. The corresponding reconstructed phase map is shown in Figure 4. The phase retrieval included correction for the detector response and the partial
coherence. The phase varies between about 0 and -7 rad. This phase map has a
straightforward interpretation: it is a projection along the X-ray path of the electron
density in the sample. Cells with sizes on the order of 100 ^m are clearly revealed.
The holographic reconstruction was repeated for the 700 angular positions of the
sample. The phase maps, projections of the refractive index decrement, were used to
determine the 3D distribution of 6 in the sample with a filtered backprojection algorithm. Figure 5a shows a slice of the reconstructed volume. The gray scale is linear
with respect to the index decrement 8(x, y, z), darker corresponding to a higher electron and mass density. The interpretation of the reconstructed slices is thus straightforward. The contrast of the polymer foam is excellent. This would certainly not be

40

X-ray tomography in material science

Figure 2.5. (a) A slice of the reconstructed distribution of the refractive index decrement 8 of
a polystyrene foam. S is essentially proportional to the electron and mass density in the
polymer. A phase map was determined for each of 700 angular positions using images at four
distances. From the projections the 3D distribution was determined with a filtered
backprojection algorithm. (b) Magnified portion of the reconstructed slice shown in a (a). (c)
Profile along the arrow shown in (a). E = 18 keV.

the case in absorption tomography, the ratio of the refractive index decrement and the
absorption index S/j3 being 2500. Figure 5c shows a profile of the index decrement
along a line segment shown in Figure 5b. The air/polymer transition is abrupt and from
this profile the spatial resolution is estimated to be about 2.5 jum (fwhm). In regions
that apparently contain only polymer the refractive index decrement is 6.6 10~7, corresponding to a mass density of 0.96 g/cm3, in agreement with the expected density
value for polystyrene of about 1 g/cm3. The tomographic slice of Figure 5a intersects
a cell of the foam. It is completely enclosed by a polymer wall. The thin walls were
not evident in the projection images, but they appear correctly after tomographic reconstruction. The shape of the cell is irregular and very distorted. This is probably
due to a crushing process. The magnified portion of the slice shown in Figure 5b, indicates an excellent 3D isotropic spatial resolution that can be obtained thanks to the
detector resolution, but also because the holographic reconstruction disentangled the
object information from the defocused images.

Phase contrast tomography

41

Figure 2.6. Three tomographic slices of an aluminium-silicon alloy quenched from the semisolid state, obtained (a) using absorption contrast, (b) using phase contrast and a single
propagation distance, (c) using phase contrast and holotomography based on four distances.
E = 18 keV.

42

X-ray tomography in material science

2.5.2. A metal alloy


The second sample, an aluminium-silicon alloy quenched from the semi-solid
state, represents a more tedious problem. The phase modulation must be determined
in the presence of attenuation by the matrix. The difference in attenuation between the
two metallurgic phases is however small. A severe problem is due to the large phase
modulation introduced by the cylindrical shape of the sample with a diameter of about
1.5 mm. This thickness of aluminium introduces at an X-ray energy of 18keV a phase
shift of more than 200 radians and would be very difficult to reconstruct. This large
shift was not present in the previous case because most of the foam is actually air.
It was therefore decided to reconstruct only the phase variations with respect to the
phase introduced by a homogeneous matrix. Figure 6a is a tomographic slice recorded
at D = 1 mm, sensitive only to variations in absorption. It is impossible to distinguish
the two phases, some bright spots appear corresponding to iron-rich inclusions. Figure 6b is a tomographic slice obtained for a single distance D = 0.6 m, revealing
density jumps as dark / light fringes. Binarising such an image toward quantitative
metallographic evaluation is extremely tedious. Figure 6c is a reconstructed map of
the variations in refractive index decrement 6(x, y, z), clearly showing the slight difference in density of the two (metallurgical) phases (Ap w 0.05 g/cm3). The grey
phase was the liquid in the semi-solid state and it consists of an aluminium-silicon eutectic. The dark phase was the solid in the semi-solid phase and it is essentially pure
aluminium with substitutional silicon (see L. Salvo et al, these proceedings). The data
set consisted of 4 times 800 images recorded at distances of 0.007, 0.2, 0.6 and 0.9 m
from the sample. The beam was monochromatised to 18 keV by a Ru/B4C multilayer.

2.6. Conclusion
Phase sensitive images are experimentally simple to obtain. Third generation synchrotron radiation facilities, such as ESRF, can easily produce the necessary coherent
beam. A first approach is to use the phase radiographs directly or in combination
with the algorithm for absorption tomography. In many cases this gives useful results,
for example the detection of cracks or reinforcing particles in composite materials.
A new approach, called 'holotomography' is now operational. It allows to perform
quantitative phase contrast tomography with a simple set-up. We used for the holographic reconstruction, in analogy with electron microscopy, a numerical procedure
based on images at different distances from the sample. The feasibility of this method
was demonstrated on a polystyrene foam. The results are in quantitative agreement
with the known sample composition. The study of a metal alloy, with metallographic
phases that are not distinguishable in the absorption mode, demonstrates the usefulness of this technique for materials sciences. A drastic improvement in sensitivity and
resolution is obtained compared to usual X-ray tomography.

Phase contrast tomography

43

2.7. References
[AND 72] ANDO M., HOSOYA S., "An attempt at X-ray phase-contrast microscopy", SHINODA G., KOHRA K., ICHINOKAWA T., Eds., Proc. 6th Intern. Conf. on X-ray Optics and
Microanalysis, p. 63-68, Univ. of Tokyo Press, Tokyo, 1972.

[BEC 95] BECKMANN R, BONSE U., BUSCH F., GUNNEWIG O., BIERMANN T., "A novel
system for X-ray phase-contrast microtomography", HASYLAB Annual Report II, p. 691692, 1995.
[BEC 97] B E C K M A N N F., BONSE U., BUSCH F., GUNNEWIG O., "X-ray microtomography
(//CT) using phase contrast for the investigation of organic matter", J. Computer Assist.
Tomography, vol. 21, 1997, p. 539.
[BON 65] BONSE U., HART M., "An X-ray interferometer", Appl. Phys. Lett., vol. 6, 1965,
p. 155-156.
[BOR 80] BORN M., WOLF E., Principle of Optics, 6th ed., Pergamon Press, Oxford, New
York, 1980.
[BUF 99] BUFFIERE J. Y., MAIRE E., CLOETENS P., LORMAND G., FOUGERES R., "Characterisation of internal damage in a MMCp using X-Ray synchrotron phase contrast microtomography", Acta Mater., vol. 47, 1999, p. 1613-1625.
[CHA98] CHAPMAN D., THOMLINSON W., ZHONG Z., JOHNSTON R. E., PISANO E.,
WASHBURN D., SAVERS D., SEGRE C., "Diffraction Enhanced Imaging Applied to Materials Science and Medicine", Synchrotron Radiation News, vol. 11, 1998, p. 4-11.
[CLO96] CLOETENS P., BARRETT R., BARUCHEL J., GUIGAY J. P., SCHLENKER M.,
"Phase objects in synchrotron radiation hard x-ray imaging", J. Phys. D, vol. 29, 1996,
p. 133-146.
[CLO 97] CLOETENS P., PATEYRON-SALOME M., BUFFIERE J. Y., PEIX G., BARUCHEL J.,
PEYRIN F., SCHLENKER M., "Observation of microstructure and damage in materials by
phase sensitive radiography and tomography", J. Appl. Phys., vol. 81, 1997, p. 5878-5886.
[CLO 99a] CLOETENS P., LUDWIG W., BARUCHEL J., VAN DYCK D., VAN LANDUYT J.,
GUIGAY J. P., SCHLENKER M., "Holotomography: Quantitative phase tomography with
micrometer resolution using hard synchrotron radiation x rays", Appl. Phys. Lett., vol. 75,
1999, p. 2912-2914.
[CLO99b] CLOETENS P., LUDWIG W., VAN DYCK D., GUIGAY J. P., SCHLENKER M.,
BARUCHEL J., "Quantitative phase tomography by holographic reconstruction", BONSE
U., Ed., Developments in X-Ray Tomography II, vol. 3772, 1999, p. 279-290.
[DAV 95] DAVIS T. J., GAO D., GUREYEV T. E., STEVENSON A. W., WILKINS W., "Phasecontrast imaging of weakly absorbing materials using hard X-rays", Nature, vol. 373, 1995,
p. 595-598.
[FOR 80] FORSTER E., GOETZ K., ZAUMSEIL P., "Double Crystal Diffractometry for the
Characterization of Targets for Laser Fusion Experiments", Kristall und Technik, vol. 1,
1980, p. 937-945.
[GUI 94] GUINIER A., X-Ray Diffraction In Crystals, Imperfect Crystals, and Amorphous
Bodies, Dover Publications Inc., New-York, 1994.
[HAR 75] HART M., 'Ten years of X-ray interferometry", Proc. R. Soc. Lond. A, vol. 346,
1975, p. 1.

44

X-ray tomography in material science

[HAR94] HARTMAN Y. M., SNIGIREV A., "Some examples of high energy X-rays phase
contrast", ARISTOV V. V., ERKO A. I., Eds., X-ray Microscopy IV, p. 429-432, Bogorodskii Pechatnik Publishing Company, Moscow, 1994.
[HEC 98] HECHT E., Optics, Srded., Addison-Wesley, 1998.
[ING 95] INGAL V. N., BELIAEVSKAYA E. A., "X-ray plane wave topography observation of
the phase contrast from a non-crystalline object", J. Phys. D: Appl. Phys., vol. 28, 1995,
p. 2314-2317.
[ING 96] INGAL V. N., BELIAEVSKAYA E. A., "Phase dispersion radiography of biological
objects", Physica Medico, vol. 12, 1996, p. 75-81. .
[KOC 98] KOCH A., RAVEN C., SPANNE P., SNIGIREV A., "X-ray imaging with submicrometer resolution employing transparent luminescent screens", / Opt. Soc. Am. A, vol. 15,
1998, p. 1940-1951.
[LEI 62] LEITH E. N., UPATNIEKS J., "Reconstructed Wavefronts and Communication Theory", J. Opt. Soc. Am., vol. 52, 1962, p. 1123.
[MOM 95] MOMOSE A., "Demonstration of phase-contrast X-ray computed tomography using an X-ray interferometer", Nucl. Inst. Meth. A, vol. 352, 1995, p. 622-628.
[MOM 96] MOMOSE A., TAKEDA T., ITAI Y., HIRANO K., "Phase-contrast X-ray computed
tomography for observing biological soft tissues", Nature Medicine, vol. 2, 1996, p. 473475.
[NUG96] NUGENT K. A., GUREYEV T. E., COOKSON D. F., PAGANIN D., BARNEA Z.,
"Quantitative Phase Imaging Using Hard X Rays", Phys. Rev. Lett., vol. 77, 1996, p. 29612964.
[POG 97] POGANY A., GAO D., WILKINS S. W., "Contrast and resolution in imaging with a
microfocus x-ray source", Rev. Sci. Instrum., vol. 68, 1997, p. 2774-2782.
[SNI95] SNIGIREV A., SNIGIREVA I., KOHN V., KUZNETSOV S., SCHELOKOV I., "On the
possibilities of x-ray phase contrast microimaging by coherent high-energy synchrotron
radiation", Rev. Sci. Instrum., vol. 66, 1995, p. 5486-5492.
[SOM 91] SOMENKOV V. A., TKALICH A. K., SHIL'SHTEIN S. S., "Refraction contrast in
x-ray introscopy", Zh. Tekh. Fiz., vol. 61, 1991, p. 197-201.
[WIL96] WILKINS S. W., GUREYEV T. E., GAO D., POGANY A., STEVENSON A. W.,
"Phase-contrast imaging using polychromatic hard X-rays", Nature, vol. 384, 1996, p. 335338.
[ZER 35] ZERNIKE F., Z. Tech. Phys., vol. 16, 1935, p. 454.

Chapitre 3

Microtomography at a third generation


synchrotron radiation facility

The use of the modern synchrotron radiation sources for monochromatic beam
microtomography provides several new possibilities. They include, in addition to
reduced signal-to-noise ratio and enhanced spatial resolution, the easy setup of
sample environment for in-situ experiments, the quantitative measurements, and the
rapidly increasing field of phase imaging. Other topics, such as the present state of
'local' microtomography, and some new approaches like diffraction and
fluorescence microtomography, are also briefly described.
3.1. Introduction
Since their discovery X-rays have been used to image the bulk of materials
which are non transparent for visible light, by taking advantage of their
inhomogeneous absorption. A tremendous progress was obtained, 25 years ago,
when three-dimensional (3D) visualization became available. This computerassisted tomographic approach provides the 3D information, from the many twodimensional (2D) images (radiographs) recorded at various angular positions of the
object, and via appropriate algorithms ("filtered back-projection", described for
instance in references [KAK88] and [PEY96]) and software. From the reconstructed
3D data cuts, projections, or perspective renditions of the object can be obtained at
will.
Microtomography, with spatial resolution better than 20 um, recent emerged in
years [FLA87]. Several laboratory instruments have been developed [SAS98,
RUE96], are commercially available, and produce good results. However, the best
quality images, in terms of signal-to-noise ratio and spatial resolution, are obtained

46

X-ray tomography in material science

on instruments located in synchrotron radiation facilities, which use a parallel and


monochromatic beam. The number of 2D images necessary is approximately equal
to the number of pixel columns used by the image on the detector, typically between
100 and 1000. The time needed for recording the 2D images is a function of the
source and the experimental setup.
This chapitre reports the new possibilities associated with the availability of third
generation sources of synchrotron radiation, such as the European Synchrotron
Radiation Facility (ESRF), with examples which illustrate these possibilities.
Section 3.2 comprises a brief presentation of the aspects of synchrotron radiation
which are relevant to microtomography. Section 3.3 shows how a substantial
improvement in the signal-to noise ratio is obtained when using these modern
sources. Section 3.4 shows examples where the improvement in the spatial
resolution is crucial for the observation of features of interest. Section 3.5 considers
the quantitative measurements in the absorption case. Section 3.6 shows the present
state of 'local' microtomography. Section 3.7 deals with the sample environment in
microtomography. Section 3.8 gives a brief report on all that concerns phase
imaging, which is treated extensively in a companion paper. Finally, section 3.9
introduces some new approaches such as diffraction and fluorescence
microtomography.
3.2. Synchrotron radiation and microtomography
Synchrotron radiation [RAO93] is the electromagnetic radiation produced by
ultra-relativistic electrons (energies of several GeV) in a storage ring when they are

Figure 3.1. Schematic representation of a synchrotron radiation facility, showing the linear
accelerator (LA) and the booster (B). In these two elements the electron beam energy is
raised to the wished value (6 GEV at the ESRF). Then the electron beam is introduced in the
storage ring (SR), where it produces, when accelerated by the magnetic fields which modify
its trajectory, the X-ray beams. The X-ray beams are used at the level of the beamlines (EL),
tangent to the storage ring

Microtomography at a third generation S R F

47

accelerated by a magnetic field (figure 3.1). This field is uniform over a portion of
the trajectory in the bending magnets. It oscillates spatially in the insertion devices
(wigglers and undulators) which can be set on the straight sections between two
bending magnets.

Figure 3.2. Relative brilliance (arbitrary units, logarithmic scale) of the X-ray sources from
the discovery of X-rays to 3rd generation SR facilities

The X-ray beam produced is tangent to the curved trajectory of the electrons in
the storage ring: the beamlines are thus located all around the storage ring, as
indicated on figure 3.1. Along with all synchrotron radiation sources, the ESRF
features very high intensity of the emitted beam (figure 3.2) and, when the source is
a bending magnet or a wiggler, a continuous spectrum, spanning the whole range
from the infra-red to X-rays.
The original features of third generation synchrotron radiation facilities, and
more particularly the ESRF, when considering the microtomographic applications,
are:
a) the very high intensity of the X-ray beam (fig. 3.2)
b) the high energy (6 GeV) of the electrons producing the radiation, which
implies the availability of high energy photons (beyond 100 keV)
c) the policy of providing each beam-line, through appropriate choice of the
insertion device, with the spectrum best suited to the experiment it is dedicated to,
and
d) the small size of the electron beam cross-section (< 100 um). This leads to
high brilliance, but also to a very small angular extension of the source as seen from
a point in the specimen, hence to a sizeable lateral coherence of the X-ray beam.

48

X-ray tomography in material science

These beam features make it possible to perform microtomographic experiments


that are improved and/or radically new, through the use
1) of a beam that is very intense, homogeneous, parallel, and, after passage in a
monochromator (either a perfect crystal or a multilayer), monochromatic. This is to
be compared with the relatively weak, polychromatic and divergent beam used in
laboratory tomography
2) of the coherence properties of the beam, making it possible to obtain phase
images by simply adjusting the sample-detector distance ("propagation" technique)
Two other points are not directly related to the source, but are nevertheless
crucial for this type of experiments:
3) the availability of a suitable detector, displaying at the same time a large
dynamic range, a low noise, and a transfer time shorter than the typical exposure
time. No such a detector is presently available on the market, and we use the Fast
REadout LOw Noise (FRELON) camera, developed at ESRF [LAB96], fitted with
an optical system which leads to effective pixel sizes between one and several
micrometers
4) the improvement of the reconstruction and image processing procedures,
leading to software suited to the problem, associated with the required computing
memory and calculation power.
Figure 3.3 is a scheme of the experimental setup used at the beamline ID 19 of
the ESRF, where most of the images presented as examples in the present paper
were obtained. It shows that the incoming beam can be considered as parallel, the
source being situated at 150 metres from the sample. This monochromatic parallel
beam setup exhibits many advantages. Among them let us mention that the
reconstruction algorithms are exact, free from approximations, and that quantitative
measurements are possible, avoiding all the beam hardening effects. It also shows
the main drawback of this approach: no magnification is obtained, and the spatial
resolution mainly results from the effective pixel size of the detector.

Figure 3.3. Principle of the parallel and monochromatic beam microtomography

Microtomography at a third generation S R F

49

When using the tomographic setup of the ID 19 beamline the total acquisition
time is of the order of half an hour for recording 900 projections images, and around
one hundred reference images for flat-field correction. Data acquisition for one
sample typically represents 2 Gigabytes, and enables the reconstruction of a (1024)3
tomographic image. Due to the parallel geometry, the 3D reconstruction problem
may be solved using a sequence of Filtered Back Projection algorithms run on each
slice of the volume, after rearranging the data in a set of corrected sinograms. To
avoid the duplication of the 2 Gigabytes of data, and save some computations, a
reconstruction program directly handling the radiographic images acquired during
experiment was developed. The program includes both pre-processing, and a 3D
version of the FBP algorithm adapted to 2D parallel projections. This algorithm was
parallelized on the workstation cluster of the ESRF, to speed up the reconstruction.
Using 4 machines, the mean reconstruction time obtained for (512) 3 volumes, is
approximately 2 hours, and depends on the workload of the system, since the system
is multi-user. Reduced reconstruction times are presently reached by devoting an
optimized computer to the reconstruction task.

3.3. Improvement in the signal to noise ratio in the 3D images


The synchrotron radiation source allows to dramatically reduce the exposure
times and improve the signal-to-noise ratio compared to a standard x-ray tube.
Figure 3.4 illustrates the differences of signal-to-noise ratio on the images of a
vertebra sample acquired once using the ID 19 Synchrotron microtomography setup,
and once a standard x-ray tube microtomography setup at IBT [RUE 96]. Figures
3.4a) and b) represent a slice through both 3D images, whose pixel sizes are
respectively 6.65 um, and 14 um. The image obtained at the ESRF is clearly less
noisy. To give an order of magnitude, the signal to noise ratio estimated under the
assumptions that the noise is stationary and uncorrelated, was found to be 70.8 on
the ESRF image and 5.8 on the IBT image. The peak signal-to-noise ratio
expressing the ratio of the image dynamic to the noise, are respectively 32.3 dB and
21 dB for these two images. These results come from the fact that the signal-tonoise ratio is proportional to the detected number of photons. The improvement of
the signal-to-noise ratio on the IBT image would be possible if the acquisition time
was increased, which may not be compatible with a 3D acquisition. The differences
are smaller on surface rendering displays of the 3D images as illustrated on figures
3.4c) and d). However, this display is obtained after segmentation of bone from
background, which is more difficult on a noisiest image. A detailed comparison of
these two techniques for the quantitative analysis of three-dimensional bone microarchitecture is reported in [PEY98] and [SAL98].

50

X-ray tomography in material science

Figure 3.4. Images of a vertebra sample obtained using the ESRF Micro-CT and the IBT
Micro-CT: a)-b): 2D slices extracted from the 3D images, c) d) 3D displays

3.4. Improvement in the spatial resolution


The availability of intense, parallel and monochromatic beams made it possible
to obtain images from very diverse materials, and to reconstruct the volume with a
resolution of the order of one u,m, much better than provided by laboratory
generators (limited in spatial resolution to about 20 urn). As already pointed out,
this spatial resolution is mainly determined by that of the detector, a CCD camera,
with suitable optical setups, specially developed for these experiments.
Increasing spatial resolution while keeping the same signal to noise ratio requires
to dramatically increase the number of photons. Under some estimations of the
signal to noise ratio in the reconstructed image, it may be considered that the

Microtomography at a third generation S R F

51

required number of photons grows as the third power of the number of pixels in the
image [PEY96]. As an illustration of the capabilities of micrometer synchrotron
micro tomography, figure 3.5 represents a reconstructed slice of a three dimensional
image of a fetal mouse bone, recorded with a voxel size of 1.8 um. An inferior
spatial resolution would not allow to observe micro-structures within this bone.

Figure 3.5. Reconstructed slice of a fetal mouse bone, pixel size : 1.8 \jan

Examples were an improved spatial resolution is a crucial point can be found in


the literature: this is the case of building materials (brick, concrete), where these
techniques allow to visualize the various components, as well as the pores. Models
for fluid diffusion (air, vapors) using as parameters the values deduced from the
images are in good agreement with experimental data [QUE98]. A synchrotron
radiation microtomography investigation of porous reservoir rocks, where both oil
and brine are visible on the reconstructions, was also published [COL98], and this
type of investigation is of growing importance. Other examples, as the penetration
of liquid Ga in Al-based alloys, can be found in the present volume (paper by
Ludwig and Bellet).

3.5. Quantitative measurements (absorption case)


A clear-cut tendency of absorption microtomography using synchrotron
radiation is the quantitative evaluation of the images. Thus the interest shifts from
just the architecture and porosity of the object to the densitometry of the solid parts.
The monochromaticity of the beam is the key point since this condition is a basic
assumption for tomographic reconstruction. This condition is not fulfilled when
using conventional polychromatic x-ray sources, and this may result in beam
hardening artifacts in the reconstructed images, due to the more important
attenuation of soft x-rays in the sample. Monochromaticity of the beam thus enables

52

X-ray tomography in material science

quantitative measurements of the absorption coefficient u (x,y,z), and consequently


quantitative density measurements.
Figure 3.6 is the illustration that it is now possible to access not only the
architecture and porosity of the object but also the densitometry of the solid parts: it
represents a reconstructed slice through a bone biopsy, where different gray levels
may be observed within the cortical region. This indicates the feasibility of mapping
3D bone mineralization, using a suitable calibration. The agreement between the
theoretical and reconstructed linear attenuation coefficients of hydroxyapatite
phantoms with different concentrations is shown on figure 3.7 [SAL99] .

Figure 3.6. Reconstructed slice through a human bone biopsy, showing different gray levels
within the cortical region, indicating differents levels of mineralization (voxel size: 10 /jm)

Figure 3.7. Linear attenuation coefficient of hydroxyapatite phantoms


of various concentrations

Microtomography at a third generation S R F

53

3.6. Present state of "local" tomography


Another emerging trend is the implementation of "local" or "zoom"
microtomography, i.e. the high-resolution reconstruction of an interesting region
within a matrix which gets only low-resolution reconstruction (or even no
reconstruction at all). This approach is essential for applications where it is not
possible or desirable to extract from the matrix a sample small enough to be entirely
illuminated by the beam.

Figure 3.8. Two reconstructed slices of the same sample a) with a 2 jam voxel size (local
tomography, region of 2mm in diameter), b) with a 6.6 jum voxel size ( 6 mm diameter sample
completely immersed into the beam)

Since the 2D detector is based on a 1024x1024 CCD, the size of the field of
view is determined by the pixel size in the image. Tomographic acquisition
theoretically requires that the field of view encompasses the entire transaxial extent
of the object at every angle. When the sample is only partly illuminated by the
beam, the projections are truncated, and the reconstruction problem is known as
'Local Tomography'.
Many efforts are devoted to obtain reliable Local
Tomography images, in spite of the missing information. Among them, let us
mention a wavelet-based algorithm for multiresolution tomographic reconstructions
[PEY99].
However if the region of interest is centered, and if the sample is globally
homogeneous, a good approximation in the center of the structure of the sample can
be obtained. Figure 3.8 shows that in this case the reconstructed image from
truncated projections is close to the image reconstructed from the complete data.
The projections from a 'composite with fibers' sample were recorded both with a
6.65 urn, and 2 urn, pixel size on the detector. In the second case the projections are

54

X-ray tomography in material science

truncated, which generates the important circular artifact at the border of the image.
However we may notice that even if the values in the center of the image may not
be used quantitatively, they provide an accurate information on the structure of the
sample.

3.7. Sample environment in microtomography

Figure 3.9. Snow samples resulting from the evolution of fresh snow, collected on the field a)
obtained by immersion in water at 0C, well-rounded grains, b) displaying faceted
crystallites, obtained by transformation under the action of a temperature gradient (lC/cm).
10 keV'X-rays.

Figuer 3.9 corresponds to a quite common porous medium, snow, which requires
to remain at low temperature to be investigated. The sample was located in a
cryostat especially designed for microtomography, featuring X-ray absorption that is
weak and independent of the angular position of the sample during its rotation. The
snow was maintained at -60C, in a regulated temperature nitrogen flow. It sitted
within a cylindrical enclosure with polished double plexiglass walls, 0.5 mm thick .
This device allows to establish a catalog of snows: fig. 3.8 shows that tomographic
methods provide data on the three-dimensional microstructure of snow that is
statistically significant because it represents a large number of grains, and at a high
resolution compared to the grain's scale [BRZ99]. Indeed, snow is a mixture of ice
particles, air and occasionally liquid water which can take different aspects. In most
cases, recent snow is a very loose powder, which can transform into hard, crusted or
pasty material, according to weather conditions and exposure. The growth of ice
particles is caused by vapor diffusion in dry snow and melt-freeze exchanges in wet
snow. Normally, dry snow covers are warmer at the bottom than on the top. The
value of the temperature gradient determines whether rounded (small gradient) or
faceted (large gradient) crystals will grow. These transformations have huge
consequences: changes over several order of magnitude in the physical and

Microtomography at a third generation S R F

55

mechanical properties of the different snow layers are commonplace. In some cases
the snow crystals are able to stick on vertical rocks, whereas under some conditions
a single skier can release a slab avalanche. The shape (specific area, local grain
curvature) and arrangement (grain connections) of the grains, and the quality of the
ice bonds will govern the snow properties. These parameters cannot be directly
derived from classical two-dimensional observations.
Other examples where the sample environment is a crucial part of the scientific
case are 1) the investigation of fatigue failure in silicon carbide particle reinforced
aluminum based composites, ([BUF97] and present volume), which employs a
traction machine specially designed for microtomographic experiments, or 2) the
'local tomography' in-situ investigation of an open-cell polyurethane foam at
several levels of compressive strain. This work correlates the macroscopic
behaviour (stress/strain curve) with the local structure modifications. It shows,
during the initial phase of compression (linear elastic response) the struts bending,
and, on a further compression stage (plateau in the stress/strain curve) the collapse a
whole band of cells [WINOO].
3.8. Phase Imaging
It is shown, in another paper of the present volume [Cloetens et al.], that the Xray beams produced at third generation synchrotron radiation facilities exhibit a
high degree of coherence. This allows to use them to record "phase images" by just
varying the sample-to-detector distance ("propagation technique"). The great
advantage of this new type of imagery is the increased sensitivity it provides, in
particular for light materials such as polymers, or for composites made up of
materials with neighboring densities (for example Al and SiC). This implies, of
course, that the spurious contrast due to inhomogeneities of the beamline
components has been eliminated [ESP 98]
Phase microtomography based on the visualisation of the edges was used, for
instance, to understand the mechanisms of degradation in aluminum-SiC
composites. It is possible not only to easily visualize the SiC reinforcing particles,
but also to observe the nucleation and propagation of cracks when the material is
submitted, in situ, to tensile stress. The cracks appear first in the elongated particles,
and this imaging technique has shown that their number is 50% more than suggested
by surface investigations [PEI 97, BUF 97].
Another example of application is the work on quasicrystals. These materials are
non-periodic solids with long-range order, discovered in 1984. Their growth
mechanism and stability is still a controversial topic. While they are not usually
considered as porous materials, the phase images show all the investigated high
quality icosahedral Al-Pd-Mn quasicrystals to contain internal holes, with
dodecahedral shape and orientation reflecting the icosahedral point symmetry of the
host [MAN98]. Their sizes exhibit a discrete distribution. The jump from one size to

56

X-ray tomography in material science

the next is consistent with the factor t3, where T is the golden mean, a basic
ingredient in all theoretical approaches of quasicrystals. The 3D reconstruction
resulting from phase microtomography shows that the average distance between
neighbouring holes is, again, about T3 times the hole size. The observed features are
in fair agreement with a geometrical approach which describes the quasicrystalline
structure in terms of a hierarchical self-similar packing of overlapping atomic
clusters, such that an inflation scale factor x3 preserves long range order but
generates a hierarchy of holes [JAN 99]. This geometrical approach appears to be
controversial among the concerned scientific community, and further experiments
are being performed to better understand the physical implications of these
observations.
Phase imaging based on the visualisation of the edges is not a quantitative
technique, and its spatial resolution is limited by the occurrence of the fringes used
to visualize the borders. A more quantitative approach of phase imaging and
tomography was recently developed. It is based on the combination of several
images recorded at different distances. An algorithm, initially developed for electron
microscopy by the Antwerp group, was successfully adapted to the X-ray case, and
allows the "holographic" reconstruction of the local phase, well beyond the images
of edges [CLO99a].
Once the phase maps are obtained through holographic reconstruction, there is
no conceptual difficulty in bringing together many maps corresponding to different
orientations of the sample, and in producing the tomographic, three-dimensional,
reconstruction. This combined procedure was applied to a polystyrene foam: for
each of 700 angular positions of the sample, the phase map was retrieved using
images recorded at four distances. The highest accessible spatial frequency is
determined by the resolution of the detector (~2 um our case). Quantitative phase
mapping and tomography ("holotomography") are now operational, and provide a
new approach to the characterization of materials on the micrometer scale
[CL099b].
3.9. Other new approaches in microtomography
The high intensity beams available at third generation synchrotron radiation
facilities are very favorable for X-ray scanning microscopies. In this approach, one
or more selected features of the sample's scattering diagram (diffraction,
fluorescence...) is plotted as a function of the position of the specimen as the latter
is scanned across the beam, to produce a mapping sensitive to crystalline phases,
impurities... Resolution in the micron range is obtained by focusing the beam.
Various focusing elements are currently used (curved mirrors or crystals, Fresnel
zone plates, refractive lenses, tapered capillaries...) to produce very small beams.
This kind of experiments is being extended to three-dimensional diffraction
tomography [KLE98] as well as to fluorescence microtomography, in which trace

Microtomography at a third generation S R F

57

elements can be mapped inside a sample [SIM99]. These techniques, and their
applications, will surely exhibit a rapid expansion in the next years, in connection
with the enhanced availability of the modern synchrotron sources.

3.10. Conclusion
X-ray microtomography is an invaluable tool to obtain 3D data on a large variety
of materials. The use of a third generation synchrotron radiation source, such as
ESRF, opens up new possibilities. The most important features, as far as absorption
microtomography is concerned, are the very broad choice available of photon
energy (typically between 6 and 120 keV), the quantitative evaluation of the
experimental data made possible by the beam being monochromatic and parallel,
and the improved spatial resolution. Obviously, some of the applications require an
even better spatial resolution. The detection of X-rays is performed through visible
light scintillators. The system is then diffraction limited. A possible way to
overcome this limitation is to use a lens to magnify the image before the scintillator.
Promising attempts have been performed using asymetrically cut crystals, or
parabolic refractive lenses [LEN99].
These techniques are well adapted to in-situ experiments, where the material, in
an adequate sample environment, is imaged as a function of an external parameter
(temperature, stress...). The very small angular size of the source provides, in an
instrumentally simple way, phase images which reveal phenomena hardly visible by
other means. Other approaches, using focus beams, and where diffraction or
fluorescence are measured, are also being developed.
3.11. References
[BRZ99] BRZOSKA J.B., et al. 3D Visualization of snow samples by
microtomography at low temperature. ESRF Newsletter 32, 22-23 (April 99)
[BUF97] BUFFIERE J.Y., et al.. Damage assessment in an Al/SiC composite during
monotonic tensile tests using synchrotron X-ray microtomography Mat. Science
and Engineering A234-236, 633-635 (1997)
[CLO97] CLOETENS P., et al. Observation of microstructure and damage in
materials by phase radiography and tomography J. Appl. Phys. 81, 5878-5886
(1997)
[CLO99a] CLOETENS P., et al. Hard X-ray phase imaging using simple
propagation of a coherent synchrotron radiation beam J. Phys. D: Appl.
Phys.32, A145-A151 (1999)
[CLO99b] CLOETENS P., et al. M Holotomography: quantitative phase
tomography with micrometer resolution using hard synchrotron radiation X-rays
Appl. Phys. Lett., 75, 2912-2914 (1999)
[COL98] COLES M.E., et al. Pore level imaging of fluid transport using synchrotron
X-ray microtomography J. Petroleum Science and Engineering 19, 55-63 (1998)

58

X-ray tomography in material science

[ESP98] ESPESO J.I., et al Conserving the coherence and uniformity of third


generation synchrotron radiation beams: the case of ID 19, a 'long'beamline at
the ESRF Journal of Synchrotron Radiation, 5, 1243-1249 (1998)
[FLA87] FLANNERY B.P., et al. Three dimensional X-ray Microtomography
Science 237, 1439-1444(1987)
[JAN99] JANOT C., et al.. Self-similar porosity in quasicrystals Mat. Res. Soc.
Symp. Proc. 553, 55-66 (1999).
[KAK88] Kak A.C., SLANEY M. Principles of computerized tomographic imaging.
IEEE Press, New York (1988)
[KLE98] KLEUKER U. et al. Feasibility study of X-ray diffraction computed
tomography for medical imaging Phys. Medicine and Biology 43, 2911-2923
(1998)
[LAB96] LABICHE J.C., et al. FRELON Camera: Fast REadout LOw Noise. ESRF
Newsletter, 25, 41-42 (1996)
[LEN99] LENGELER B., et al. Imaging by parabolic refractive lenses in the hard Xray range Synchrotron. Rad., 6, 1153-1167 (1999)
[MAN98] MANCINI L., et al. Investigation of defects in icosahedral quasicrystals
by combined synchrotron X-ray topography and phase radiography
Philosophical Magazine A, 78, 1175-1194 (1998)
[PEI97] PEIX G., et al. Hard X-ray phase tomographic investigation of materials
using Fresnel diffraction of synchrotron radiation SPIE 3149, p.149-157 (1997).
[PEY96] PEYRIN F., et al. Introduction to 2D and 3D tomographic methods based
on straight line propagation: X-ray, emission and ultrasonic tomography (text in
French) Traitementdu Signal 13, 381-411 (1996).
[PEY97] PEYRIN F., et al. Quantification of the trabecular structure from 3D
synchrotron radiation microtomography: comparison to histology, Osteoporosis
Int., 7, 268 (1997)
[PEY98] PEYRIN F., et al. Micro-CT examinations of trabecular bone samples at
different resolutions: 14, 7 and 2 micron level, Technology and Health Care, IOS
Press, 1998, vol 6(5-6), p. 391-401.
[PEY99] PEYRIN F., et al. Local tomography in 3D SR CMT based on a
nonseparable wavelet approach SPIE 44th Ann. Meeting, Developments In XRay Tomography II, Denver USA, (1999)
[QUE98] QUENARD D., et al. Micro structure and transport properties of porous
building materials: 3D modeling from 2D-SEM images and X-ray
microtomography Workshop on modeling of deterioration in composite building
components due to heat and mass transfer, 22-23/1/98, Tsukuba, Japan (1998)
[RUE96] P. RUEGSEGGER, et al. A microtomographic system for the non
destructive evaluation of bone architecture, Calcif. Tiss. Int., vol 58, p 24-29,
1996.
[SAL98] SALOME-PATEYRON M. Acquisition et quantification d'images du reseau
trabeculaire osseux en microtomographie tridimensionnelle utilisant le
rayonnement synchrotron, PhD thesis (Genie Biologique et Medical) INSA
Lyon, 1998.

Microtomography at a third generation S R F

59

[SAL99] SALOME-PATEYRON M. et al., Description of a synchrotron radiation


microtomography device for 3D trabecular bone imaging, Med. Phys., 26, n 10,
p. 2194-2204(1999)
[RAO93] RAOUX D Introduction to synchrotron radiation and to the physics of
storage rings Neutron and Synchrotron Radiation for Condensed Matter studies,
HERCULES, edited by Baruchel J. et al., Ed. de Physique and Springer-Verlag
(1993)
[SAS98J SASOV A. et al. Desk-top microtomography: gateway to the 3D world
European Microscopy and Analysis, 17-19 ( March 1998)
[SIM99] SIMIONOVICI A. et al. X-ray fluorescence microtomography: experiment
and reconstruction SPIE 3772, 304-310 (1999)
[WINOO] WINDLE A. et al. In-situ microtomographic investigation of the
compression of a polyurethane foam in press

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Chapitre 4

Introduction to reconstruction methods

This paper introduces reconstruction methods for X-ray transmission computed


tomography (CT) applied to materials science. Basic principles of analytic
reconstruction methods such as filtered back-projection (FBP) are recalled and
illustrated in 2D. Then we introduce algebraic reconstruction techniques (ART) that
can be implemented when conventional, complete data sampling cannot be
achieved.

4.1. Introduction
The purpose of a computed tomography (CT) system is to build a 2D or 3D
representation of the inner structures of an object, from a set of projection
measurements, acquired from a number of points of view. In the case of
transmission CT with X-rays or gamma-rays, the parameter that is reconstructed in
order to represent these structures is the linear attenuation coefficient u of the
object. It is assumed to be proportional, in most non-destructive testing (NDT)
applications, to the mass density (p in g/cm3) regardless of the chemical nature of
the object. Calibration procedures are usually necessary to transform the raw
measurements into quantitative projection data and to correct for X-ray
polychromaticity effects, but they are beyond the scope of this paper. In this paper
we intend to illustrate the basic concepts of reconstruction methods in parallel-beam
geometry, through a simulated example, rather than going into the details of
mathematical developments. References for this paper have been found in
[AMA85], [LEW 83], [CEN 83] and [HER80]. The reader can find a description of
recent developments including cone-beam or spiral CT in, for instance, [HIR97],
[GRA99] or [NAT99].

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X-ray tomography in material science

4.2. Description of projection measurements


Let us assume that the acquisition system is able to provide a set of projections
of /j. along straight lines, or source-to-detector "rays", in a so-called "parallelbeam" geometry. The object is supposed to be fixed, while a measurement system,
composed of one source and one collimated detector, translates and rotates around
the object, as shown in figure 4.1.

Figure 4.1. Acquisition geometry for parallel-beam tomography

In most NOT systems the source-detector system is fixed and the object moves,
but in order to explain reconstruction methods it is easier to place oneself in a
reference system attached to the object. Let (x,y) be the coordinates of a point M in
the reference system attached to the object. The origin O of this reference system is
at the axis-of-rotation. A source-to-detector ray is defined by parameters (r, 0) where
9 is the angle of the x axis with the perpendicular to the ray, and r is the algebraic
distance from the axis-of-rotation to the ray.
If $) is the number of photons delivered by the source, and <f> is the number of
photons after attenuation by the object, the Beer-Lambert law states that:
[1]

If one assumes that both

and

are measured by the acquisition system, then

the projection of u along a ray (r, 0) is expressed as follows :


[2]

Note that (r, o) do not correspond exactly to polar coordinates since generally :

Introduction to reconstruction methods


p(0,

p(o,

for

63

[3]

and r may be negative. We refer to as "a projection" the set of measurements


acquired for the same rotational angle. The set of projections over 180 (or 360) is
the Radon transform of function u. In parallel-beam geometry, 180 are sufficient
to represent the Radon transform since :

p(r,o,) = p(-r,0 + x)

[4]

The linear and angular sampling must be fine enough so that the projection data
can be mathematically considered as a satisfactory sampled version of the
continuous Radon transform, and function u, must be null outside the circle
defined by the acquisition system when it rotates. Obviously, real measurements are
not acquired with infinitely thin rays, but each ray has a width that is determined by
the focal spot size of the X-ray source, the detector width, the source-to-object
distance and the source-to-detector distance. Accordingly, the translation step must
be small enough to be consistent with this ray width and with the size of the
structures in the object. The number of angular projections must be between
and 1 4 times the number of pixels per projection.
The simulated phantom is made of a disk with /j = 1 including two elliptic
inserts with // = 2 . The simulation code is based on an analytic computation of the
lengths crossed by the rays in each component of the object. It does not include any
beam-hardening effect or other physical considerations such as scattering or energydependent detector efficiency. Such a realistic simulation code is available in our
laboratory [GLI98], but for the purpose of reconstruction, possible distortions due to
physical effects are supposed to be corrected for by adequate pre-processing of the
projections. We simulated 180 projections of 128 rays per projection, equally
spaced over 180. The reconstructed image is made of 128 x 128 pixels. Figure 4.2
shows the reconstructed image, which can be considered as the reference
representation of the object.

Figure 4.2. Reconstructed image of the object

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X-ray tomography in material science

If the projections are displayed in grey levels, one below the other, then the 2D
representation which is obtained (figure 4.3) is called a "sinogram" because a point
of the object describes a sinusoid in this representation, in effect, from figure 4.1 it
can be deduced that:

Figure 4.3. Right: sinogram or set of projections over 180 - Left: three projections

It can be seen on the sinogram that the long objects inside the main cylinder are
better detected when they are seen through their longest direction.
Let us assume now that projection data are available, and that the image whose
Radon transform corresponds to these measurement data is unkown.

Introduction to reconstruction methods

65

4.3. Backprojection
The first intuitive operation which can be implemented is backprojection. It
consists in assigning to each point of the object the average value of all the
projections at the corresponding location, as illustrated in figure 4.4. The result of
backprojection of the sinogram of figure 4.3 into a 128 x 128 pixels matrix is shown
in figure 4.5.

Figure 4.4. Backprojection in a point of the object

Figure 4.5. Backprojection of the sinogram


The backprojected image, when compared with the "perfect" object, is highly
blurred. As a result of the "projection-then-backprojection" process, each pixel
contains information about what the object really contains at the pixel location, but
this information is added to a blurred version of the rest of the object. An exact
mathematical correction of the "projection-then-backprojection" smoothing effect
can be done by an appropriate pre-filtering of the projections, as in the Filtered
Backprojection (FBP) algorithm. This can be demonstrated based on Fourier
considerations.

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X-ray tomography in material science

4.4. Projection-slice theorem


The "projection-slice theorem" is the basis of many reconstruction methods. It
states that the 1D Fourier transform p(R,0) of projection p(r,0) in the 0 direction
is equal to the cross-section, in the same direction 9, of the 2D Fourier transform
fr( vi, v2) of the original function //(*, y):

Figure 4.6. Magnitude of the Fourier transform of projection for 0 = 0.


Left: linear representation. Right: log representation

Figure 4.7. Magnitude of the Fourier transform of the object.


Left: linear representation. Right: log representation

This is illustrated by figure 4.6 and 4.7: figure 4.6 is a horizontal profile of
figure 4.7. Note that for this object the 2D Fourier transform contains 2 principal
components (one vertical and one horizontal) which correspond to the direction the
two ellipses inside the object. The representations of figure 4.6 and 4.7 are discrete
Fourier transforms; they are a valid representation of the continuous Fourier

Introduction to reconstruction methods

67

transform only if the Nyquist sampling conditions are satisfied. Let us recall that, if
Ar is the sampling step on the projections, and Nr the number of pixels per
projection, then the discrete Fourier transform of the projection is made of Nr points
and the maximum frequency which can be represented is :

4.5. Fourier reconstruction methods


From the projection-slice theorem can be built a reconstruction method: if
equally sampled projections are acquired over 180, then the set of their ID Fourier
transforms constitute a representation, on a polar grid, of the 2D Fourier transform
of u(x, y). If a polar-to-cartesian resampling is done, followed by a reverse 2D
Fourier transform, then the reconstruction is done, we will name this method the
"Fourier method".
Another method, referred to as the FBP method, can be deduced from the
Fourier method. The reverse 2D transform of /}( Vj , v2 ) is written :
dvldv2

[8]

If ( R ,6} are the polar coordinates in the ( v1 , v2 ) Fourier space it comes :

RdR dO

[9]

The change of variables may seem a little tricky since R varies over ]-oo,oo[ in
the ID Fourier transform of the projection p(R,0} , while R > 0 in the expression
of u(v 1 ,V2)in polar coordinates. Taking into account symmetry properties,
eventually, it comes :

which is the formula of the FBP reconstruction method. The first step of this
methods is :

68

X-ray tomography in material science

\R\dR

[12]

This is a filtering operation applied to the projection p(r, 6}, the filter being
represented in the frequency domain by /(/?) = R\ . This filter is noted HD because
it is the Hilbert transform of the first derivative. It is also known as the "ramp filter".

Figure 4.8. Filtered projection for 0 = 0.

Figure 4.9. Backprojection of filtered projections for 1, 2, 4 and 8 directions

Introduction to reconstruction methods

69

This filtering operation has the effect of creating negative components on the
filtered projection (see figure 4.8), which will compensate for the contribution of
other projections in the backprojection step (see figure 4.9).
The second step of the FBP reconstruction is :

which is the backprojection of the filtered projections. This operation is illustrated in


figure 4.9. It is important to understand that the averaging of all the projections in
the image pixels as explained in figure 4.3 is equivalent with the successive
spreading of the projections over the image as in figure 4.9.

4.6. Filtering in Fourier methods


In the presence of noise,
the "ramp" filter tends to
multiplied by an apodisation
high frequencies to decrease
the filter becomes :

is it even more important to filter the projections that


increase the high frequencies. Usually the filter is
function, such as a Manning window, which forces the
smoothly down to 0. If Rc is the cut-off frequency,

Figure 4.10. Reconstruction filters: ramp, ramp*Hanning (e=2), ramp*Hanning (e=6)

70

X-ray tomography in material science

Apodisation tends to reduce noise but also to blur the edges of the structures.
There is a trade-off to find between noise and spatial resolution as shown in
figure 4.11 (a gaussian random noise has been added to the projection data before
reconstruction)

Figure 4.11. FBP reconstruction of noisy data (all three images are displayed
with the same gray scale)

4.7. ART-type methods


The methods presented above are based on an analytical expression of the
inversion of the Radon transform. Discretization is introduced only at the time of
implementation. These methods assume that the measurement data constitute a
discrete representation of the Radon transform, which means that they must be
complete and equally spaced. When it is not the case, the problem may be written
directly in the form of a discrete linear system :

[15]
where p is the vector made of the measurement data,
x is a vector made of all the pixels of the image,
M is the projection matrix.
This can be written :

where i is an index of source-to-detector ray, j is an index of image pixel and mij is


a coefficient representing the contribution of pixel j to measurement i. There are
several ways of modelizing the projection matrix; usually mij coefficients are

Introduction to reconstruction methods

71

computed as the length crossed by ray j to measurement through pixel j. Several


other models exist in the literature, for instance the Xj may be considered as basis
functions with bell-shaped profiles on a circular, overlapping support [LEW 92] in
order to regularize and accelerate the reconstruction. In this paper we restrict
ourselves to conventional square pixels.
Since data are perturbed by noise, the inversion of the system is done in the least
square sense. The quadratic error to be minimized is :

The gradient of the quadratic error is :

The minimum of the quadratic error is found for x such that :

Even though many m^ coefficients are null, the size of the system is generally
huge, and the system is not inverted directly, but using a method iterative by blocks.
A block is a set of rays (or a set of rows in the matrix). Very often, a block will be
equivalent with a "projection", that is to say all the rays for the same rotational angle
(then the method is called the SART technique for "simultaneous algebraic
reconstruction technique"). At iteration q, one block of rays is taken into account,
and the current estimate x^' of x is refined in order to minimize the quadratic
error for the rays of this block :

The difference between the projection

M block . x (q) of the current image

estimate and the actual measurement Phiock for this block is backprojected in order
to update the image estimate. This can be written :

where

Pi

is the actual measurement across ray i,

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X-ray tomography in material science

is a relaxation factor, which prevents from going too fast towards the
solution corresponding to the current block, regardless of the other blocks,
mi
is the ilh row of matrix M, it corresponds to the projection along ray i.
This algorithm is made of two basis modules which are projection and
backprojection.
Projection : pi (q) = <mi,x ( q ) > = mij xj(q}
[22]
j
is the computed projection of the estimate X
along ray / (at the iteration q)

Backprojection :

[23]

is the backprojection into the image of Spi = pi - pi which is the error on


measurement i (at iteration q). The value which is backprojected into pixel j for
ray sum / is :

[24]
k on ray i

The weighting factor

gives the redistribution of the projection


kon rayi

error to the pixels crossed by ray i. If mij is homogeneous to a length and is


expressed in cm, then this weighting operation is equivalent with dividing the error
by the length crossed by the ray in the object. If the projection data are equivalent to
an attenuation ( u / ) then the reconstructed value will be u ( x , y } in attenuation per
cm.
This is the "basic" ART method. In order to regularize the problem in the
presence of incomplete or noisy data, a priori constraints are often taken into
account. Among them are found: positivity constraint (ju cannot physically be
negative), or support constraints (function u is known to be null outside a given
area). Filtering of the image or of the projection data may also be introduced. If
precautions are taken in order to ensure data consistency, ART methods can even be
used for "local" tomography :

Introduction to reconstruction methods

Figure 4.12. Local tomography is possible with SART.

We performed a simple backprojection and a SART reconstruction of the


phantom using only 3 projections at -30 (150), 0 and 30.

Figure 4.13. Reconstruction of 3 projections


Left: Backprojection, Right: SART reconstruction (30 iterations and A. = 0.1)

Figure 4.14. Horizontal profiles across the images reconstructed from 3 projections

73

74

X-ray tomography in material science

The vertical ellipse, which is in the direction of the projections used for the
reconstruction, can be seen on projection 9 = 0 (see figure 4.3), on the SART
reconstructed image (profile 1), and hardly on the backprojected image (profile 1).
The backprojected image is not quantitative, it has been divided arbitrarily by 50 in
order to be comparable to the other profiles. The SART reconstruction provides a
value of // which is at least of the good order of magnitude. The backprojected
image, and in a better way the SART reconstruction, also provide an information
about of the depth of this ellipse within the object. The quality of this information is
very dependent of the maximum angle between the projections (here, 60).
The horizontal ellipse cannot be located nor quantified since measurement data
along its main axis have not been used for this reconstruction.
This example is of course very simple, but it shows the potentialities of
reconstruction from few view angles, for instance for the detection of defects in
homogeneous media.
4.8. Conclusion
This paper has introduced basic FBP and ART methods in parallel beam in 2D
for the reconstruction of an image from its projections. Adaptations of these
algorithms are necessary in most applications in order to use ID or 2D detectors.
Simulated results for conventional CT and for very few (3) projections have been
shown.
4.9. References
[AMA 85] AMANS J.L., CAMPAGNOLO R.E., GARDERET P., Imagerie medicale :
methodes de reconstruction et techniques instrumentales, Note technique
CEA/LETI/MCTE N1511 du 10 dec 85.
[CEN 83] CENSOR Y., "Finite Series-Expansion Reconstruction Methods",
Proceedings of the IEEE Vol 71 N3 March 1983 p 409-419
[GLI 98] GLIERE A., "Sindbad: From CAD model to synthetic radiographs", Rev.
Of Progress in Quantitative Nondestructive Evaluation, Vol. 17A, 1998, pp 387394.
[GRA 99] GRANGEAT P., "Fully three-Dimensional Image Reconstruction in
Radiology and Nuclear Medicine", to be published in Encyclopaedia of
Computer Science and Technology.
[HER 80] HERMAN G.T., Image reconstruction from
projections: the
fundamentals of computerized tomography, Academic Press, New York, NY
1980.
[HIR 97] HIRIYANNAIAH H.P., "X-ray Computed Tomography for Medical
Imaging", IEEE signal Processing magazine, p 42-59, march 1997.

Introduction to reconstruction methods

75

[LEW 83] LEWITT R.M., "Reconstruction algorithms : transform methods",


Proceedings of the lEEEVol 71 N3 March 1983 p 390-408
[LEW 92] LEWITT R.M., "Alternatives to voxels for image representation in
iterative reconstruction algorithms", Phys. Med. Biol., 1992, N3, 705-716
[NAT 99] NATTERER F., Numerical methods in tomography, Acta-Numerica.
vol.8; 1999;p.l07-41 , 1999

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Chapitre 5

Study of materials
in the semi-solid state

A synchrotron X-ray source (ESRF, FRANCE), has been used to investigate the
microstructure of semi-solid materials. Two kinds of materials have been
investigated, Al-Cu alloys with a high volume fraction of solid to study hot tearing
and an industrial 356 alloy (Al-Si) which is the common material used for semisolid forming. Two imaging modes have been used, the absorption mode for the AlCu material and the phase contrast mode for the Al-Si. Discussion is presented on
the interest of such a technique to characterise semi-solid microstructures.

5.1. Introduction
The semi-solid state is a specific state in which the solid and the liquid phases
coexist. This state is obtained for every alloy with a solidification interval when it is
solidified from the liquid state (such as in the continuous cooling of metals), or
when it is reheated from the solid state (such as in semi-solid forming). In the first
case, during the solidification of the material, cracks can be generated in some alloys
(Al-Cu alloys in particular) owing to the deformation of the solid phase [FRE 79]
which leads to hot tearing. This phenomenon is not fully understood from a
theroretical point of view. The second case (reheating from the solid phase) is
related to the forming in the semi-solid state which is a competitive forming process
compared with liquid injection [Gffl 96]. This process involves the forming when
the material is reheated between the solidus and the liquidus with a solid fraction
close to 0.5. For the moment the alloys used in this technique are aluminum-silicon
alloys like 356 and 357 which are hypoeutectic alloys. The main advantage of this
process is to provide laminar filling of the mould during injection which avoids any

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X-ray tomography in material science

porosity formation and therefore allows to produce thin parts which can be heat
treated in addition to increase their mechanical properties.
Figure 5.la presents the microstructure of an Al-Cu alloy quenched from the
semi-solid state (T=570C). At this temperature the volume fraction of the solid
phase was 0.8. The solid phase is in grey and the black phase is the eutectic mixture
which was liquid when the material was in the semi-solid state. In the following the
eutectic will often be designated by the liquid. In this material, the solid phase can
be described as globules surrounded by the liquid. Figure 5.1b presents the
microstructure of an Al-Si alloy also quenched from the semi-solid state. The solid
phase is also surrounded by the fine eutectic mixture (which was liquid in the semisolid state). As previously, the solid phase can be described as globules embedded in
the eutectic liquid. Some liquid droplets are also observed in the solid phase.

Figure 5.1. Typical microstructure of (a) an Al-Cu alloy (b) an Al-Si alloy

However, 2D observations of such materials are not sufficient to describe the


microstructure. Some attempts have been made to get 3D images of the solid in
semi-solid materials. [ITO 92] studied an Al-Si alloy with a very low solid fraction
(0.2). The employed technique was to take micrographs of the sample, to polish it, to
take again micrographs and this procedure was repeated every 40 microns. Then the
volume was reconstructed. These images of the solid in a semi-solid alloy obtained
for the first time in 3D, even though at a very low solid fraction, indicate that
clusters of solid can not be properly characterised using 2D sections only. More
recently [VOL 97] have used the same technique on a small volume of a model SnPb alloy with a very high solid fraction (0.8). They took micrographs every 21
microns and reconstructed the volume. Their observations again clearly demonstrate
the limitation of 2D analysis for such a material. They found a complete
connectivity of the solid particles within the volume. The size of the solid particles
(around 0.35 mm) is large in the volume investigated (1.3 x 1.7 x 1.7 mm) and the
authors agree on the fact that the precision (21 microns) may create artificial

Study of materials in the semi-solid state

79

connections between particles. However, it must be noticed that this paper presents
the very first 3D images of a reasonable volume. Finally the last study published on
3D images of semi-solid materials is by [NlR 98]. This paper shows 3D images of
some solid particles obtained from an 2xxx alloy. The technique employed is the
same as that of the other papers except that the precision is higher, around 10
microns for the section spacing. However, there is no attempt in this paper to study
the connectivity of the solid phase and only few solid particles have been
investigated. Therefore, 3D characterisation of solid phase in semi-solid materials is
now becoming necessary to better understand microstructural evolutions, like
Ostwald ripening and coalescence processes, and deformation mechanisms. The aim
of this paper is to present a new technique which allows to get 3D images of any
semi-solid materials with a high resolution. This technique is high resolution X-ray
tomography carried out at ESRF. This paper will first present the experimental
device and then the materials under study. Finally 3D characterisations of these semi
solid materials will be presented.

5.2. Experimental device and procedure


The experimental device is available on line ID 19 at the ESRF and since three
years several studies were carried out with the X-ray tomography device. This is at
the moment the only way to get 3D images with a high level of resolution (of about
one micron). A X-ray beam with a high coherency and a high energy (up to 60 keV)
hits the sample and a CCD camera records the transmission image. The sample is
placed on a high precision rotating table and 600-900 transmission images are taken
while the table is rotating by 180. The CCD camera has 1024 x 1024 pixels and the
pixel size can range from 15 to 0.9 microns. Therefore the higher the resolution is,
the smaller the volume analysed is. In the investigated materials, two scales are
present in the microstructure, the globule size of the solid phase (around 100
microns) and the size of the liquid film between the globules (a few microns). In
order to image enough globules in the investigated volume and obtain a good
resolution to observe the liquid film, we have decided to work with the 2 microns
resolution. The samples were machined as cylinders of 1.6 mm in diameter and 3
mm in height.
X-ray tomography can be performed in several ways. The most classical is the
absorption mode, when the CCD camera is placed just behind the sample (3 mm for
example). This mode will provide images for which the contrast is obtained owing
to the difference in X-ray absorption of elements in the sample. This mode has been
used by [BUF 98] to study the spatial distribution of Al2Cu nodules in an Al-Cu
alloy. This mode was used also in this study for the Al-Cu alloys. However, this
mode does not allow to study multiphase materials when the absorption coefficients
of the various phases are not different enough. The contrast is then too low, which is
the case of the Al-Si alloy. It is then possible to use the phase contrast : this
particular mode requires the CCD camera to be placed far from the sample (up to

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X-ray tomography in material science

900 mm). Therefore the contrast is due to constructive interferences of X-rays


diffracted at the interface between phases. This special mode has been for example
used to study damage in metal matrix composites based on the Al/SiC system [BUF
99]. The phase contrast is enhanced when the distance between the sample and the
camera is increased, but the resolution of the interface between the phases becomes
lower.
In both Al-Cu and Al-Si alloys experiments, the energy of the X-ray beam was
fixed to 17.5 keV. A complete scan (800 projections) including references images
every 100 projections lasts about 10-15 minutes. It is important to notice that it is
not possible to do "in situ" scan on semi-solid alloys since the microstructure
changes when the material is held in the semi-solid state. Consequently, all the scans
were performed at ambient temperature on quenched samples from the semi-solid
state. The quenching must be very fast in order to get a very fine eutectic mixture in
between the solid phase, which will then appear homogeneous in contrast. This is
very important since, if the eutectic mixture is not fine enough, the high resolution
will allow to distinguish the two phases of the eutectic and therefore will cause
trouble to identify the solid globules.

5.3. Results on Al-Si alloys


In this section we will first present the best experimental conditions for this
material, then we will present several 2D sections of a 3D reconstructed volume and
finally we will study the influence of the remelting time on the microstructure of an
Al-Si alloy. The 356 material has been provided by Pechiney and it is mainly Al7wt% Si-0.5wt%Mg. It has been electromagnetically stirred during solidification in
order to get a non dendritic structure. This material was partially remelted in the
semi-solid state in an induction furnace at 583C (7C above the eutectic
temperature) and maintained at this temperature during 5 minutes. This time is
usually required before the forming of this material. Several X-ray tomography
experiments have been carried out for various distances between the sample and the
CCD camera and figure 5.2 presents 2D sections of the reconstructed volume of the
Al-Si alloy for 4 distances. As expected in absorption mode (distance=3mm), there
is no contrast between phases, whereas a good contrast is observed when the
distance is 200 mm or larger : indeed it is possible to distinguish all the phases
(liquid, solid and droplets of liquid). In order to keep good resolution of interfaces
between solid and liquid and to have enough contrast, the best distance seems to be
in between 200 and 600 mm. We have used 500 mm for the subsequent experiments.

Study of materials in the semi-solid state

81

Figure 5.2. Influence of the sample / camera distance on the contrast in Al-Si alloys

Figure 5.3 presents 2D sections every 4 microns. The microstructure is very


different between figure 5.3a and 5.3d although there is only a 12 microns distance
between the two sections. These changes concern the solid and the liquid phases.
Most of the droplets are effectively entrapped in the liquid when considering several
2D sections. However, some droplets of liquid which seem to be entrapped in the
solid phase are in fact connected to the interdendritic liquid (square box in figure
5.3). Until now, these droplets were assumed to be isolated in the solid phase owing
to morphological and metallurgical assumptions but it was really difficult to
distinguish between entrapped and connected liquid [SAL 96]. Concerning the solid
phase, within 12 microns, new solid globules can appear as illustrated in the dotted

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X-ray tomography in material science

box in figure 5.3 and connection between globules can appear also as illustrated by
the arrow. Therefore a resolution of 2 microns is at least necessary to get complete
information on the connectivity of the solid phase of industrial semi-solid materials.

Figure 5.3. Serial section on an Al-Si


These results therefore demonstrate that it is very important to make a real 3D
characterisation of such materials. The problem with the phase contrast technique is
that segmentation of the volume is not easy to perform. Apparently the edges of
each phase seem to be well defined (see figure 5.2) but this is not always the case.
The origin of this problem can arise from the experimental device but in our case it
is mainly due to the sample : as explained before quenching is sometimes not fast
enough so that the eutectic does not appear as homogeneous but as a mixture of two
phases : silicon and aluminium, which can not be distinguished from solid globules.
Therefore, it becomes delicate to get information on the connectivity of the solid
phase. As an automatic segmentation does not permit for the moment to know

Study of materials in the semi-solid state

83

precisely its influence on the connectivity, we decided to perform manual


segmentation on 2D sections every 2 microns and reconstruct part of the volume,
this procedure is long since it requires to draw by hand the globules and the liquid
phase using painting software. This technique allows also 3D information about
entrapped liquid and connectivity and shape of the solid, since segmentation is easy.
If information on the connectivity of the solid is only required, there is a quicker
way : the principle is to draw a line between connected globules in 2D in order to
get the skeleton. Then this 2D skeleton is placed on the next section and
modification of the connection can be added or suppressed. This faster technique,
however, must only be used to count solid phase globules in the volume and not to
get information about the morphology. Figure 5.4 presents a 3D reconstruction of
the material presented in figure 5.3 . Figure 5.4a illustrates a fully connected solid
phase, since all the globules have been found to be connected by 3D analysis of the
volume. This observation is very interesting since the 2D photographs of figure 5.3
do not suggest at all this high level of connectivity of the solid phase. This feature
indicates that partial remelting of a semi-solid Al-Si alloy during 5 minutes leads to
a highly connected solid phase. This explains why the material can be handle in this
state and does not collapse even if it contains 50% of liquid. Figure 5.4b presents the
entrapped liquid, which is not connected to the interdendritic liquid. As suggested by
the 2D sections presented in figure 5.3, these droplets are mainly spherical.

Figure 5.4. a) solid phase, b) entrapped liquid

The last experiment which was conducted was designed to study the evolution of
the microstructure during partial remelting with the same sample. As explained
earlier, it is not possible to perform in situ scan of these materials since the evolution
of the microstructure is very fast. Therefore, we decided to do what we call

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X-ray tomography in material science

interrupted in situ scans. A sample is scanned, then partially remelted during five
minutes, quenched and scanned again, remelted again for some time and so on. The
important point here is to put marks on the sample to be able to image the same part
of the sample after the remelting experiments. The sample was studied in the as
received conditions, after 5 minutes remelting at 587C and after 10 minutes. Figure
5.5 presents 2D sections of reconstructed volumes of the same region in the
specimen. It is therefore possible to see the evolution of the microstructure within 10
minutes remelting at 587C. It indicates that the evolution of the microstructure
during the time required for a complete scan is too important to perform real in situ
measurements. The microstructure evolves very rapidly during the 5 first minutes so
that it is difficult to follow the same region. Indeed coalescence of dendrite arms
occurs as generally observed which leads to the entrapped liquid [SEC 84]. Between
5 and 10 minutes, the evolution becomes slower and it is then easy to follow some
groups of globules as those underlined in black in figure 5.5.

Figure 5.5. Influence of remelting time on the microstructure of an Al-Si alloy

A 3D representation of a group of solid globules are shown in figure 5.6 for 5


and 10 minutes remelting. The morphology of the solid phase changes considerably,
since a small globule seems to disappear and the curvature of the solid phase
decreases.

Figure 5.6. Solid phase evolution during partial remelting

Study of materials in the semi-solid state

85

The main mechanism of this evolution is the well known reduction of the
liquid/solid interface area [VOO 84] and this figure is a real 3D representation of this
mechanism.

5.4. Results on Al-Cu alloys


A grain refined Al-8wt%Cu alloy was studied by X-ray microtomography in the
absorption mode. Figure 5.7 shows successive sections along the z-axis. Considering
the first and the last images (z = 0 and z = +10|jm) indicates that the two liquid films
present in the circle are not connected. The other sections of figure 5.7 conversely
show that these two liquid films are connected.
This kind of information about the connectivity of the liquid phase is very important
in the study of hot tearing phenomena. Indeed, if the liquid phase is totally
connected, the cracks will easily propagate into the liquid [FRE 79]. Sections closer
than 10 microns are thus required and it seems in this case that sectioning for every
4 microns gives a good information about the microstructure. 3D analysis of such a
volume indicates that there is no entrapped liquid in this volume.

Figure 5.7. Successive sections on the Al-Cu alloy

We also performed an interrupted in situ test for the Al-Cu alloy. For this alloy,
the air furnace temperature was 555C (the eutectic temperature is 548C) and four

86

X-ray tomography in material science

cumulated times were analyzed: 5, 15, 30 and 60 min. Figure 5.8 presents a 2D
section of the same sample after 30 and 60 min of partial remelting. As already
mentioned for the Al-Si material, there is an evolution of the microstructure which
obeys the Ostwald ripening process [Voo 84] but the evolution is lower since the
solid fraction is higher. During the partial remelting treatment, the liquid fraction
decreases from the Scheil equation value (0.19) to the equilibrium value given by
the phase diagram (0.1).

Figure 5.8. 2D sections at constant z during partial remelting experiments

5.5. Conclusion and perspectives


The microtomography is a very powerful techniques which allows to study the
microstructure of semi-solid materials. The resolution of 2 microns that is possible
to use at ESRF allows to study the connectivity of the solid phase in such materials
in 3D. We have shown that for the Al-Si materials the scan has to be made in the
phase contrast mode with a distance of 500mm and that the resolution of 2 microns
is a good trade off. In the case of Al-Cu materials the absorption contrast gives good
images and it seems that owing to the large solid fraction a resolution of 4 microns
might be sufficient. The first 3D analysis of the Al-Si shows that the solid phase is
entirely connected and lots of entrapped liquid are present. In the case of Al-Cu no
entrapped liquid has been found. We performed in both alloy interrupted in situ tests
in order to follow the evolution of the microstructure of the same sample. This gives
very interesting results concerning the solid phase morphology and entrapped liquid
in the case of Al-Si alloy. Future efforts will be concentrated on the evolution of the
microstrutructure during deformation and during partial remelting. This needs 3D
analysis of the volumes and therefore a good segmentation technique, which is
possible for Al-Cu but at the moment difficult for Al-Si.

Study of materials in the semi-solid state

87

5.6. References
[FRE 79] H.FREDRIKSSON and B.LEHTINEN, Solidification and Casting of Metals,
1979, p. 260-267
[GHI 96] G. GHIARMETTA , Conference Proceedings of the 4th International
Conference on Semi-Solid Processing of Alloys and Composites, 19-21 June
1996 Eds D.H. Kirkwoodand P. Kapranos, p204-208
[ITO 92] Y. ITO, M.C. FLEMINGS, J. A., Cornie Nature and Properties of Semi-Solid
Materials, eds J.A. Sekhar and J.A. Dantzig, 1992, p3-17.
[VOL 97] T.L. VOFLSDORF, W.H. BENDER, P.W. VOOHREES, Acta Mater. vo145,
n6, 1997, p 2279-2295
[Nm. 98] B. NlROUMAND , K. XlA, Conference Proceedings of the 4th International
Conference on Semi-Solid Processing of Alloys and Composites, June 1998
p637-644
[BUF 98] J.-Y. BUFFIERE, E. MAIRE, P. CLOETENS, J. BARUCHEL, R. FOUGERES,

Poceedings of ICAA 6 , Aluminium Alloys vol 1, 1998, p529-534.


[BUF 99] J.-Y. BUFFIERE, E. MAIRE, P. CLOETENS, G. LORMAND, R. FOUGERES,
Acta Mater vol 47 n5, 1999, p!613-1625.
[SAL 96] L. SALVO, M. SUERY, Y. DE CHARENTENAY, W. LOUE, Conference
Proceedings of the 4th International Conference on Semi-Solid Processing of
Alloys and Composites, 19-21june 1996 Eds D.H. Kirkwoodand P. Kapranos,
plO-16
[Voo 84] P.W. VOORHEES, M.E. GLICKSMAN, Met Trans A, vol 15A, 1984, pi0811089
[SEC 96] J.-F. SECONDE, M. SUERY , Journal of Materials Science, vol 19, 1984,
p3995-4006

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Chapitre 6

Characterisation of void and reinforcement


distributions by edge contrast

We have studied the inter-relation between reinforcing particle distribution and


void distribution prior to ductile failure in a model, ZrC>2 reinforced Al matrix, metal
matrix composite. Dual energy X-ray microtomography measurements above and
below a strong Zr absorption edge have been use to make reconstructions of ZrC2
and void distributions in failed metal matrix composite tensile test specimens. The
distribution of ZrO2 particles in the composite prior to testing is shown to be
spatially uncorrelated. There is a correlation between the local density of voids
nucleated during tensile straining and the density of ZrO2 reinforcement. However,
there is no evidence for preferential nucleation or growth of voids formed prior to
fracture in regions of higher particle density.

6.1. Introduction
In this study we have investigated the evolution of void volume fraction during
the plastic tensile straining of a particle reinforced metal matrix composite (MMC)
using X-ray microtomography (XMT). Previous studies of void evolution in MMCs
using conventional absorption contrast XMT have been unable to distinguish
between the contribution of void and reinforcement populations [MUM 93a, 95].
Recent work using coherent synchrotron X-radiation has been able to use phase
contrast to image individual reinforcement particles in model MMCs [BUF99].
However, this was only achieved with a model MMC containing very large SiC
reinforcement of diameter > 200 am.

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X-ray tomography in material science

Here we will describe a different approach used to characterise reinforcement


distributions tomographically. This is dual energy XMT, where the X-ray absorption
is measured at two X-ray energies either side of a critical X-ray absorption edge of
an element in the reinforcement material. This limits our selection of reinforcements
to those which possess a suitable absorption edge. Zr has an absorption edge at 18.2
keV and so model MMCs of ZrC>2 particles in an Al alloy matrix were used in these
studies. Combining the information from the two signals measured above and below
the absorption edge allows us to distinguish between the contribution of
reinforcement and voids to the X-ray absorption density. This enables the
tomographic reconstruction of separate images of the void distribution and
reinforcement distribution, allowing the relation between void evolution and local
reinforcement density to be studied.

6.2. Dual energy X-ray microtomography


XMT measurements were carried out on a "first generation" microtomography
apparatus. The details of this apparatus have been described elsewhere [ELL 90, 94]
and similar apparatus was used in our earlier studies of MMC fracture [MUM 93a,
93b, 95]. This apparatus uses a collimated, pencil beam of X-rays defined by a
lOum aperture. X-rays are detected by a single, energy dispersive, high purity Ge
detector. This is connected to a spectroscopy amplifier and then a calibrated 2048
channel multi-channel analyser (MCA). A laboratory microfocus X-ray source is
used with a Mo target run at typically 40 kV with a current of 2 mA. The resulting
beam is polychromatic and of 15um diameter at the specimen; this defines the
reconstruction resolution (voxel size). The specimen is translated through the beam
by a stage which positions to an accuracy of better than 0.5 (am. To provide the data
to reconstruct a single 2-dimensional slice, the specimen is stepped to provide a line
projection of 128 measurements. It is then rotated through equal angular intervals of
1.434 to obtain 251 line projections of X-ray absorption over 360. A standard
filtered back projection algorithm is used to reconstruct the data from each slice onto
a 256 x 256 pixel array. Three-dimensional reconstructions are obtained by
collecting data from a series of slices.
In dual energy XMT, two independent sets of transmitted X-ray intensity are
made at two different energies along identical beam paths through the specimen. In
order to achieve this, the MCA is used to distribute the X-rays detected by the Ge
detector into different energy bins of 0.025 keV width. In order to get independent
data sets for this technqiue, the ratio of matrix to reinforcement X-ray absorption
coefficient should be as different as possible at the two X-ray energies chosen. This
can be most easily achieved if the reinforcement has an X-ray absorption edge in the
energy range available from the X-ray source. In this case a suitable model
reinforcement is ZrO2 with the Zr absorption edge at 18.2 keV.

Characterisation of void and reinforcement distributions

91

In conventional XMT, the reconstruction provides a spatial distribution of linear


X-ray absorption coefficient //. In each reconstructed voxel the absorption
coefficient is made up of three components:
u voxel =
where V is the volume fraction of each component matrix, particles and void,
defined by subscripts m, p and v respectively. The general method of reconstructing
elemental quantified XMT data using multi-energy X-ray absorptiometry has been
described elsewhere [KOZ 99]. In dual energy XMT, the absorption coefficients of
each phase are not separately reconstructed; instead, the individual contributions of
the matrix and reinforcement to the total absorption are decoupled. This requires the
use of the mass absorption coefficient, which is the linear X-ray absorption
coefficient of fully dense material divided by its theoretical density. We use the
notation mc,? to represent the mass absorption coefficient of component c at
energy E2. At energy E\ the absorption measured is thus:

where p is the density of the component in the voxel, r is the specimen thickness and
I and I, are the intensities of the incident and transmitted beam respectively. Note
that because a void has a mass absorption coefficient taken to be zero, it is not
included in the above calculation. Equation 2 can be rewritten for the second X-ray
energy E2 and combined to give a solution for the local particle component density:

This calculation is carried out on the X-ray intensity values collected at each
specimen position. This results in "intensity of density" values on which
reconstruction is carried out directly yielding voxel particle density:
Ip=exp-[Joppdx|

[4]

The above equations 2-4 can also be solved for pm. Once the values of pm and
pp are known for an individual voxel, the void content of that voxel can also be
calculated by

[5]
Pp
Pm
where pp' and pm' are the theoretical densities of the particles and reinforcement.

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X-ray tomography in material science

Dual energy XMT reconstruction was carried out on data collected at X-ray
energies of 17.4 keV and 19.6 keV. These energies correspond to the MoKa and
MoKp characteristic X-ray energies and were chosen because the characteristic count
rates are high. The strong X-ray absorption of ZrO2 restricts the maximum diameter
and reinforcement volume fraction of the specimens that can be examined. Thus, a
maximum reinforcement volume fraction of 7.5% was used which allows a
maximum specimen thickness of about 1mm. The typical data collection time on
these specimens was 14 hours per slice; a minimum of 20 slices with 50 urn
separation between each slice were reconstructed for each specimen examined.

6.3. Experimental materials


All materials were formed using a standard powder metallurgical fabrication
route of vacuum hot pressing followed by extrusion. The matrix Al alloys chosen for
this study were commercially pure Al (1100) and a Mg and Si containing
precipitation hardening alloy (6061). Argon gas atomised powders were supplied by
Alpoco. The Al 1100 and Al 6061 powders had quoted mean particle diameters of 7
fim and 45 u,m respectively. The morphology of both powders was spherical. The
reinforcing particles used were cubic Mg stabilised ZrO2 (Johnson Matthey) of
sieved particle range 28 - 45 urn.

Figure 6.1. Variance of local area fraction of ZrO2 particles in a 7.5% ZrO2 reinforced Al
6061 matrix, plotted against the size of the area used for measurement (logarithmic scale for
both axes)

Quantitative measurements of the microstructure were made using a Kontron


IBAS V2.0 image analysis system connected to an optical microscope. The spatial

Characterisation of void and reinforcement distributions

93

distribution of the reinforcements was determined by measuring the local volume


fraction of reinforcements in sub-areas within 4 fields. An important question is
whether this distribution in local area volume fraction reflects a truly random
distribution of particles or whether some clustering or ordering occurs.
If a distribution of points is truly random in space, there should be no influence
of the scale of the measurement unit on results. For particle clustering, this can be
determined by plotting the logarithm of the variance of the measured local area
fraction of particles against the log of the measured area [MIL 61, LI 92, WOR 96].
This is similar to a Richardson plot in fractal analysis. If the distribution is random
over all the length scales of the measurement, this plot should be linear with a
gradient of -1. Gradients between -1 and 0 indicate a fractal dimension < 3,
characteristic of the spatial distribution of points. For example, if the points are
distributed on randomly distributed planes (perhaps on grain boundaries), at certain
length scales, a fractal dimension would be measured between 2 and 3, and in our
plot a gradient > -1 would be measured.
When a deviation from linearity occurs on the plot, this indicates a change in the
characteristics of the particle distribution, e.g. clustering, at a scale characteristic of
that measured area. Figure 6.1 shows such a variance plot for an Al 6061 matrix
MMC on measurements parallel and perpendicular to the extrusion direction. The
gradient is closer to -1 on measurements made perpendicular to the extrusion
direction, but both directions show no change in slope characteristic of clustering at
a particular areal length scale.

Figure 6.2. Schematic illustrating the location of XMT specimens machined


from failed tensile specimens

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X-ray tomography in material science

For XMT characterisation of undeformed MMCs, a 1 mm diameter cylinder of a


fully dense Al 1100 containing 7.5 vol% ZrO2 was machined from an extruded rod.
Specimens were also extracted from failed tensile specimens just below the fracture
surface by electro-discharge machining (figure 6.2). They were of square section,
approximately 1 mm x 1 mm. These specimens were used in a parallel study on
acoustic emission prior to fracture]. Three specimens were used for fully
quantitative XMT studies containing nominally 7.5% by volume of ZrO2 in annealed
Al 1100, peak aged Al 6061 and over aged Al 6061.

6.4. Results and discussion


Figure 6.3a shows conventional XMT reconstructions of a single slice from the
fully dense 7.5% ZrO2 Al 1100 MMC measured below and above the Zr absorption
edge at 17.4 and 19.6 keV respectively. The same features can be identified below
and above the absorption edge at 18.2 keV. The apparent low density halo seen at
the specimen edge in the 19.6 keV reconstruction is an artefact generated by the
edge pixels being incompletely occupied by material. Figure 6.3b shows a separate

Figure 6.3. Reconstruction of a single slice obtained from dual energy XMT measurements on
a fully dense, extruded bar of 7.5vol% ZrO2 reinforced Al 6061 MMC. a) Single energy
reconstruction of absorption density from 17.4 keV and 19.6 keVX-rays either side of the Zr
K-edge. b) Reconstruction of Al and ZrO2 density computed from the data in (a)

Characterisation of void and reinforcement distributions

95

reconstruction for each of the Al and ZrO2 distribution data sets obtained from the
data of figure 6.3a. It is clear that regions of high ZrO2 density correspond with
regions of low Al density. The reinforcement volume fraction averaged across this
slice was measured at 4.5%. The maximum reinforcement volume fraction of a
single voxel was 56%, which is attributed to a combination of the interpolation
carried out during back-projection reconstruction and the similarity between
reinforcement particle size and voxel linear dimension. The void content averaged
over this slice was measured as 0.4%.
Figure 6.4 shows images of ZrO2 density distribution and total material density
distribution. The void density distribution is the inverse of the total relative density.
These have been calculated from two slices of a dual energy XMT reconstruction
from beneath the fracture surface in the peak aged 7.5% ZrO2 Al 6061 MMC. Slice
numbering is arbitrary with increasing number towards the fracture surface. Both
images in slice 16 show a common feature corresponding to a section of the fracture
surface intersecting the slice. Regions of high void density correlate with regions of
low ZrO2 density as expected.

Figure 6.4. Dual energy XMT reconstructions from a peak aged 7.5vol% ZrO2 reinforced Al
6061 MMC showing ZrO2 particle distribution and totsl density distribution. Two slices are
shown, slice 12 is from the bulk of the specimen while slice 16 intersects the fracture surface:
a) total density distribution (light regions are voids), b) ZrOz density distribution

96

X-ray tomography in material science

It is possible to analyse the quantitative XMT data in a number of ways [MUM


93a, 93b, 95]. Changes in sample external dimension can be used to measure local
strain. The void content can be averaged over complete slices of material which
have undergone a known plastic strain to determine the local void content as a
function of strain [MUM 93a]. The reinforcement volume fraction can also be
averaged over a complete slice of material. It is also possible to determine the
reinforcement and void content in each individual voxel and compute the probability
distributions of these measures. It is thus possible to investigate whether there is any
correlation between the particle and void distributions over a range of length scales.
Finally, variance analysis can be carried out on both the reinforcement and void
density distributions in any single slice of material to determine the extent of any
void clustering as a function of plastic strain.
Measurements of ZrO2 volume fraction from each complete slice in the three
fractured specimens were in the range 5.7 - 7.4%. This is lower than the nominal
volume fraction of ZrO2 present (7.5%) and is also lower than that measured by
optical metallography in this study (8.3% for the Al 1100 MMC and 8.2% for the Al
6061 MMC). The precise reasons for this divergence are unclear but are probably
artefacts of both the tomographic reconstruction algorithms and the determination of
3-dimensional information from the 2-dimensional data of quantitative optical
metallography. The maximum reinforcement content measured in any reconstructed
voxel from the fractured specimens was 18.5% (figure 6.5). This is significantly
lower than that found with the as extruded specimen (56%). This may indicate an
accumulation of damage in the regions with the greatest local reinforcement volume
fraction. Figure 6.5 also shows no systematic variation in maximum reinforcement
content with distance up to 1mm from the fracture surface, this suggests that all high
reinforcement content regions have associated voids throughout this region near the
fracture surface.

Figure 6.5. Maximum ZrO2 volume fraction measured in an individual voxel on each
reconstructed slice as a function of distance from the fracture surface

Characterisation of void and reinforcement distributions

97

Figure 6.6 shows the results of variance analysis on both reinforcement and void
distribution within each slice of an XMT reconstruction. The resulting straight lines
have gradients between ~ -0.8 and - 0.5. These are similar, if a little further from the
ideal case of -1, to those found for the distribution of particles on optical crosssections. Thus, we might infer there to be no significant clustering of voids.
However, the algorithm used during filtered back projection reconstruction of an
XMT slice introduces a correlation between adjacent voxels, hence leading to a
reduction in variance at small sampled areas, as can be clearly seen from the gradual
change in slope as the sampled area decreases. This reduces the utility of variance
analysis with this form of tomographic reconstruction algorithm, however, the
absence of any abrupt change in slope suggests that there is no clustering within the
length scales sampled.

Figure 6.6. Variance analysis with gradient of plot, b, shown of a) Zr02 distribution and b)
void distribution, determined from dual energy XMT slice reconstruction data

98

X-ray tomography in material science

Figure 6.7. Local void content as a function of local reinforcement volume fraction measured
from a dual energy XMT reconstructed slice 300 fjmfrom the fracture surface of a peak aged
7.5vol% ZrO2 reinforced Al 6061 MMC. Linear regression plots are shown for two different
sampled areas

Finally we can consider representing a direct relationship between local


reinforcement content and local void content in any reconstructed slice, i.e. at
constant distance from fracture surface and hence, constant nominal strain. The
measure of a local value of any parameter with a degree of inherent randomness
depends on the measured area. Figure 6.7 shows the relation between local void
content and reinforcement volume fraction for the peak aged Al 6061 MMC
measured over 12 x 12 pixel (180 x 180 um) and 16 x!6 pixel (240 x 240 um) areas.
There is considerable scatter but in both cases a straight line can be fitted by
regression analysis with a reasonable correlation coefficient. Table 6.1 shows the
correlation coefficient between local particle density and void fraction as a function
of distance from the fracture surface and sampling area for the annealed Al 1100 and
peak aged Al 6061 MMCs. With the Al 1100 MMC there are only significant void
volume fractions within about 250 urn of the fracture surface (figure 5a). In this
region the correlation coefficient is in the range of 0.3 - 0.4. The peak aged Al 6061
MMC has a significant void fraction throughout the volume sampled and a higher
fraction than the Al 1100 MMC at most sections (figure 5a). This shows a stronger
correlation with a coefficient typically in the range of 0.3 - 0.8. In this material there
are a few "rogue" slices (e.g. at 300um and 600 um) with a systematic anomaly in
the correlation. The 24 x 24 sampling is more susceptible to rogue results,
presumably because its size limits the number of data points. In both MMCs there is
no systematic change in correlation coefficient with sampling size which is
consistent with there being no clustering of voids.

Characterisation of void and reinforcement distributions

Distance
4x4
6x6
Annealed 7.5% ZrO2 Al 1100
0.25
0.18
50
0.38
0.33
100
0.34
150
0.35
0.29
0.39
200
250
0.35
0.33
0.12
300
0.18
350
0.16
0.27
0.24
0.32
400
0.04
450
0.05
0.21
500
0.05
0.14
550
0.00
0.05
600
0.01
650
0.20
0.09
0.34
0.20
700
0.04
750
0.01
Peak Aged 7.5% ZrO2 Al 6061
50
0.45
0.50
100
0.34
0.35
150
0.42
0.41
200
0.44
0.38
250
0.31
0.30
300
0.60
0.65
350
0.44
0.42
400
0.46
0.43
450
0.37
0.27
500
0.51
0.53
550
0.41
0.46
600
0.01
0.05
650
0.33
0.32
700
0.33
0.29
750
0.33
0.20

99

Sampling Area (Voxels)


8x8

12x12

16x16

24x24

0.22
0.29
0.41
0.40
0.34
0.09
0.22
0.46
0.08
0.19
0.18
0.02
0.29
0.44
0.07

0.29
0.28
0.21
0.44
0.34
0.19
0.12
0.40
0.18
0.07
0.16
0.18
0.48
0.54
0.06

0.46
0.29
0.25
0.39
0.03
0.22
0.11
0.50
0.08
0.07
0.22
0.10
0.45
0.40
0.23

0.52
0.09
0.04
0.38
0.58
0.43
0.39
0.52
0.38
0.74
0.02
0.71
0.97
0.47
0.79

0.59
0.44
0.43
0.35
0.37
0.70
0.50
0.43
0.33
0.58
0.51
0.13
0.32
0.47
0.20

0.57
0.33
0.18
0.41
0.36
0.85
0.24
0.61
0.15
0.65
0.76
0.30
0.06
0.33
0.88

0.88
0.45
0.60
0.40
0.27
0.89
0.43
0.43
0.08
0.73
0.74
0.32
0.30
0.57
0.24

0.81
0.38
0.83
0.66
0.89
0.95
0.34
0.99
0.24
0.74
0.90
0.37
0.89
0.32
0.62

Table 6.1. Linear correlation coefficient between local reinforcement volume fraction and
local void fraction as a function of distance from the fracture surface and different sampling
areas

100

X-ray tomography in material science

Let us now consider the evidence for any relationship between local particle
volume fraction and local void volume fraction in these materials after straining.
These materials were produced by powder metallurgy and our analysis of the
particle distribution using a Richardson (variance) plot indicates a self similar
distribution with fractal dimension between 2 and 3. There is no apparent change in
slope seen on the plot over the range of sampled areas selected and thus no
significant change in distribution character. Similar random distributions are seen
when the XMT data of void and particle distribution are analysed, with the caveat
concerning possible autocorrelation introduced during reconstruction. Linear
regression analysis indicates a significant correlation between void fraction and
reinforcement content. However, this correlation is independent of plastic strain and
sampled area. Thus there is no evidence for either an increased void nucleation rate
or growth rate in regions of higher local reinforcement content. Our results are
consistent with a model of random void nucleation at particles and subsequent
growth independent of local environment; i.e. there is greater void volume in regions
of high reinforcement content purely because there are more nucleation sites.
These results only apply to our materials with random particulate distributions
and may not apply to highly clustered MMCs obtained by casting routes [LLO 91].
There is some evidence from acoustic emission experiments that artificially
constructed MMC microstructures with reinforcement clusters nucleate damage at
lower strains than random microstructures [BUR 97]. Indeed, there is some very
limited evidence from our results that might support this hypothesis. Highly
clustered regions of reinforcement are rare in our material, but their presence was
identified in the undeformed material where some voxels in the tomographic
reconstruction had reinforcement contents in excess of 50%. Beneath the fracture
surface, we never found any voxels with reinforcement contents greater than 20%.
Thus, the albeit rare regions of high reinforcement disappear after straining. Clearly
more work is required to address the fracture behaviour of more clustered
microstructures during tensile straining.

6.5. Conclusions
Dual energy XMT has been used successfully to determine the spatial
distribution of voids and reinforcement in model ZrO2 reinforced Al alloy MMCs. It
has not been possible to demonstrate the equivalence of reconstructed XMT sections
with coincident metallographic sections, because the system resolution was below
that required to image individual ZrO2 reinforcement particles. However, the ability
to measure local reinforcement density in each reconstructed voxel allowed the
analysis of local particle clustering.
The initial ZrO2 reinforcement distribution appears to be random and with no
significant clustering as determined by variance analysis. Void distributions after
straining had similar properties. Unfortunately because of correlations introduced by

Characterisation of void and reinforcement distributions

101

the tomographic reconstruction algorithms we cannot be certain that this analysis is


valid for the XMT data. There appears to be a weak but consistent correlation
between void density and particle density. This supports the hypothesis that in
powder route fabricated MMCs, void density during plastic straining is directly
related to particle density and that no enhanced void nucleation or growth occurs in
regions of high reinforcement concentration.
Acknowledgements
We would like to acknowledge the EPSRC for the provision of funding to
support this project through its composite materials programme, reference
GR/H33817 and GR/J25628. IJJ would also like to acknowledge the EPSRC for the
provision of a postgraduate research studentship.
6.6. References

[BUF 99] BUFFERS J.-Y., MAIRE, E., CLOETENS P., LORMAND G. and FOUGERC R.,
Acta Mater, vol. 47, p. 1613 (1999).
[BUR 97] BURDEKIN N.A., STONE I.C. AND MUMMERY P.M., presented at 4th Inter.
Conf. Compos. Eng. (1997), unpublished.
[ELL 90] ELLIOT J.C., ANDERSON P., DAVIS G.R., DOVER S.D., STOCK S.R.,
BREUNIG T.M., GUVENILIR A. AND ANTOLOVICH S.D., /. X-Ray Sci. Tech. vol.
2, p. 249(1990).
[ELL 94] ELLIOTT J.C., ANDERSON P., DAVIS G.R., WONG F.S.L., and DOVER S.D.,
JOM-J. Min. Met. Mater. Soc. vol.46, p. 11 (1994).
[HIL 61] BILLIARD J.E., CAHN J.W., Trans. Metall Soc. AIME vol. 221 p. 344, 1961.
[KOZ 99] KOZUL N., DAVIS G.R., ANDERSON P. AND ELLIOT J.C., Meas. Sci.
Technol. vol. 10, p. 252 (1999).
[LI 92] LlQ.F., SMITH R., McCARTNEY D.G., Mater. Char. vol. 28 p.189 1992.
[LLO 91] LLOYD D.J., in Metal Matrix Composites - Processing, Microstructure and
Properties, Proceedings of the. 12th Ris0 Inter. Symp. Mater. Sci., p. 81 1991
Ris0 National Lab., Roskilde, Denmark.
[MUM 93a] MUMMERY P.M., ANDERSON P., DAVIS G.R., DERBY B. and
ELLIOTT J.C., Scripta Metall. Mater, vol. 29, p. 1457 (1993).
[MUM 93b] MUMMERY P.M. and DERBY B., in Prcoeedings of the 9th International
Conference on Composite Materials. , Vol. 1, Metal Matrix Composites, p. 424,
1993, Woodhead Publishing, Cambridge, UK.
[MUM 95] MUMMERY P.M., ANDERSON P., DAVIS G.R., DERBY B. and
ELLIOTT J.C., J. Micros, vol. 177, p. 399 (1995).
[WOR 96] WORRALL C.M., WELLS G.M. Proceedings of the European Conference
on Composite Materials, London, p. 247 1996.

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Chapitre 7

Characterisation of MMCp
and cast Aluminium alloys

This paper describes recent results on the application of high resolution X-ray
tomography to the study of metal matrix composites and cast aluminium alloys. The
advantage of phase contrast X-ray tomography over classical attenuation X-ray
tomography is shown in the case of an Al/SiC metal matrix composite. The
possibility of studying in situ damage initiation and development within a material
under stress is also illustrated. Finally, examples of quantitative results extracted
from reconstructed three dimensional images are given with respect to
microstructure and damage characterisation of different structural materials.

7.1. Introduction
Almost all structural materials contain micro-heterogeneities such as precipitates,
reinforcing particles, holes, etc. Generally the mechanical properties of those
heterogeneities are different from those of the base material (the matrix). Therefore,
those heterogeneities form a preferential site for the nucleation and development of
damage inside structural materials under stress.
Ceramic reinforcements can be added, for instance, to a metal matrix in order to
obtain a Metal Matrix Composite (MMC) with a high specific elastic modulus.
However, the co-existence of a brittle material with a very ductile matrix induces
some elastic and plastic incompatibilities which result in poor fracture properties. A
lot of attention has been paid to the investigation of the damage mechanisms of
Metal Matrix Composites (MMC) under stress. However, most of the work carried
out so far relies on surface observations of samples mainly because experimental

104

X-ray tomography in material science

evidences of the damage mechanisms occurring in the bulk of the samples are rather
difficult to obtain.
Another example of micro-heterogeneous structural materials are cast aluminum
alloys. These materials offer various advantages over wrought aluminium alloys
when one is concerned with the manufacturing of an object with a very intricate
shape, like, for example, hollow shapes. However, aluminium, like other metals,
contracts when it solidifies and besides, hydrogen dissolves very easily in the molten
metal. Therefore, unless special (expensive) processing methods are used, aluminium
cast objects always contain a certain amount of porosity. These pores are a major
problem because of their detrimental effect on the mechanical properties of the
finished object. For this reason, a lot of research is being carried out on the study of
porosity in cast aluminium alloys and on its influence on mechanical properties.
However, like in the case of MMCs, the characterisation of porosity in cast alloys is
quite difficult to achieve experimentally through classical metallographic
examination.
For the moment, X-ray Computed Tomography (XRCT) is the only non
destructive characterisation technique which provides direct images of the bulk of
heterogeneous materials. As a matter of fact, this method has been used extensively
in medicine for years, but the low resolution of the images obtained (around 100 um)
impeded its use in materials science. In the last ten years, however, the use of
synchrotron X-ray radiation coupled with new detectors has opened new possibilities
in this field. 3D images of the interior of micro-heterogeneous materials have been
obtained with a resolution of a few microns (see for example [CLO 97] for a
review).
In this paper we present some recent results in the study by XRCT of damage
initiation and development inside a notched sample of MMC. The aim of the
experiment is to evaluate the influence of the non uniform stress state on damage
development within the material. Moreover, the same technique has also been used
for the characterisation of model cast alloys. Some quantitative results on the
description of the pore population in these alloys are shown.
7.2. Experimental methods
7.2.1. Materials.
7.2.1.1. Al/SiC composite
The composite studied in this work was a 6061 Al alloy reinforced by a 10 %
volume fraction of SiC particles. The average size of the reinforcement, 120 fam, was
large compared to industrial material. This size had been chosen in relation with the
resolution of the 3D imaging technique (see below). The average aspect ratio of the
particles was 1.6. The material was processed through a rheocasting route under

Characterisation of MMCp and cast Aluminium alloys

105

nitrogen and was subsequently extruded at 813 K with an extrusion ratio of 16 and a
ram displacement rate of 100 um.s"1. The extruded bars were solutionised at 803 K
for 2 hours, quenched in water and matured at room temperature for 2 weeks (T4
heat treatment) before testing.
7.2.1.2. Al cast alloys
Three different model Al cast alloys have also been studied and characterised by
X-ray tomography. The nominal composition of the three alloys is given in table 7.1.
Those alloys were chill mould cast by Pechiney. Different amounts of hydrogen (H2)
and Argon (Ar) gases were introduced in the melt thanks to a propeller. At the
beginning of solidification, part of the gas content was rejected and formed artificial
pores. By varying the H2/Ar ratio (2%, 7% and 10%) three different average sizes of
pores were obtained for each alloy (alloy A, B and C, respectively). Thin cylinders
(diameter 3mm) were machined from the ingots for XRCT characterisation. The
volume of material investigated during each scan was around 170 mm3.

Si

Fe

Mg

Ti

Sb

6.6-7.0

0.09-0.14

0.29-0.34

0.11-0.14

0.12-0.14

Cr
<0.01

Others
<0.01

Table 7.1. Chemical composition (wt%) of the studied castAl alloys

7.2.2. Attenuation vs. phase contrast tomography


High resolution XRCT experiments have been carried out at the European
Synchrotron Radiation Facility (ESRF) in Grenoble on line ID 19. A schematic view
of the experimental set up used can be seen on figure 7.1. The X-ray beam coming
out of the ring first encounters a double silicon monochromator before hitting the

Figure 7.1. Schematic view of the experimental set up used for the tomography experiments
on line ID 19 at ESRF. Note the unusual large distance between source and detector which
results in a large coherence of the X ray beam.

106

X-ray tomography in material science

studied specimen which stands on a rotating stage. The transmitted X-ray beam, is
converted into visible light before being recorded by a 1024*1024 CCD detector
specially designed at ESRF. A tomographic scan comprises 600 2D projections of
such type. They are obtained by a 180 rotation of the sample around its vertical
axis with a 0.3 step. Those projections are used to reconstruct a 3D numerical
image of the sample through a classical filtered back projection algorithm [ROB 99].
The voxel size in the reconstructed volume, fixed by the experimental setting of the
detector, was about 6.5*6.5*6.5 um3 for the materials studied in this work.
In classical tomography, the contrast obtained on the reconstructed images
comes from differential X-ray attenuation between the constituents of the studied
material. The pores in the studied cast al alloys show an X-ray attenuation very
different from the matrix. Therefore, they give a good contrast on the 2D projections
and in the reconstructed images.
The case of the Al/SiC composite is slightly more problematic as the X ray
attenuation of the SiC particles is very close to that of the matrix. Thus, the contrast
of the SiC particles in the reconstructed images is very faint. This is illustrated on
figure 7.2a. To circumvent this problem, the so called phase contrast tomography
has been used. This technique, which is based on the high coherence of the X-ray
beam on line ID 19, greatly improves the detection of SiC particles (see figure 7.2b).
It has been shown, besides, that the phase contrast also enhances the detection of
damage (cracks) within reinforcements in MMCs [BUF99].

Figure 7.2. Reconstructed images of two different cross sections of the studied Al/SiC
composite obtained by a) attenuation tomography and b) phase contrast tomography. On the
left, the contrast given by the SiC particles is very faint because of the small difference in Xray attenuation between SiC and Al. Reconstruction rings are also visible because the
contrast of the image has been enhanced to visualise the SiC particles. On the right, thanks to
the phase contrast technique available on ID 19 beamline at ESRF, the contrast between
matrix and reinforcement is enhanced by the presence of bright/dark fringes at each
particle/matrix interface. Those fringes are obtained by simply setting the CCD detector at 83
cm behind the sample

Characterisation of MMCp and cast Aluminium alloys

107

7.2.3. Mechanical tests


The mechanical tests have only been performed on the Al/SiC composite. A
double shouldered tensile sample cut along the extrusion direction was used. The
cross-section of this sample was 2*2 mm2 and its gage length was 4 mm. A notch
was cut in the central part of the sample using a diamond saw. Its height and depth
were 365 urn and 500 urn respectively. The radius of curvature at the root of the
notch was around 130 urn. Before testing, the flat faces of the sample were
mechanically grinded using SiC paper down to 1200 grit.
The tensile tests were conducted at room temperature using a specially designed
tensile testing device which was set directly on the goniometer and which
experienced the same rotation as the sample during the scans. In order to avoid the
frame of the machine to hide the beam during the 180 degree rotation, a PMMA tube
was used to transmit the load between the upper mobile grip and the lower grip fixed
on the goniometer. This tube was carefully polished and gave a weak attenuation
(which was corrected in the reconstructed images) on the 2D radiographs. The
machine could be used in tension or in compression with a maximum load of 2500
N. The force and the crosshead displacement were recorded on a computer and
monitored during the test.
A constant crosshead displacement rate of 150 um.min'1 was used. This
corresponded to an average strain rate of 6 10"4 s"1 in the sample. Five tomographic
scans were performed corresponding to the initial undeformed state and to four
consecutive steps at increasing values of the applied stress (40, 95, 130, 140 MPa).
These steps will subsequently be referred to as steps 0, 1, 2, 3 and 4. For each scan,
the sample was maintained with a constant crosshead displacement on the tensile
testing device. All observations were consequently made in the loaded state.
For the initial state and also for each stress step, one 3D volume of the sample
was reconstructed. Only a restricted zone (2*2*1.7 mm3) around the notch has been
considered in the reconstruction in order to reduce the volume of data to handle.
7.3. Results and discussion
7.3.1. Al/SiC material
Figure 7.3 shows three reconstructed images of the same internal section of the
AlSiC sample at step 0, 1 and 2. The analysis of this figure shows, first, that some
voids induced by the extrusion process were present at some particle/matrix interface
at the initial state. A few cracked particles were also observed. For the experimental
conditions investigated, the voids induced by the extrusion process did not tend to
propagate under stress and no clear evidence of particle matrix de-cohesion could be
seen. The main damage mechanism was the mode I cracking of the SiC particles as

108

X-ray tomography in material science

already observed for the same material during tensile test on a smooth sample [BUF
99]. The evolution of the cracked particles spatial distribution within the sample, all
along the test, is shown on figure 7.4.

Figure 7.3. Reconstructed images of the same internal section of the AlSiC sample at step 0,
1 and 2. The arrows indicates the presence of a crack in a SiC particle at the root of the
notch where the stress level is high

It can be seen, on that figure, that the particles tend to break first near the root of
notch where a higher stress level is obtained. When the stress is increased, however,
the size of the volume containing the cracked particles steadily increases.
The presence of a tri axial state of stress in the studied sample is generally
believed to alter the mode of damage, by promoting particle matrix decohesions
[CLY93]. In our case, however, the mode of damage ( mode I particle cracking)
seems to be the same as that observed in a smooth sample in the same deformation
conditions. At least two effects can account for this observation. One is related to the
phase contrast technique. A thin interfacial crack between matrix and reinforcement
would give an extra fringe in the reconstructed image which would probably be quite
difficult to detect with a 6.65 urn resolution. The second reason is related to the
material itself. In MMCs indeed, a large size of the reinforcements is known to
promote particle cracking at the expense of other damage modes. Thus, the large size
of the SiC particles studied here are likely to favour only the particle cracking as
damage mechanisms in the early stages of straining. Further work with a material

Characterisation of MMCp and cast Aluminium alloys

109

containing smaller particles (around 20 urn) and with a higher (2 urn) resolution
should help to clarify this point.

Figure 7.4. 2D projection (as indicated by the arrows on the 3D sketch on the right) of the
SIC particle centroids in the reconstructed volume of the material. The different symbols used
on the figure indicate at which step a particle broke. The tensile stress was applied vertically.
The superimposed square indicates approximately the zone where a higher number of broken
particles was found at the first stages of deformation

In order to study quantitatively by 3D image analysis the evolution of damage in


the material all along the test, the reconstructed images were binarised. The average
grey level in the SiC particles was quite close to that of the matrix [CLO97],
impeding the use of simple well known threshold-based methods. Instead, the
binarisation process was carried out on the 2D projections with an edge detection
algorithm. The resulting binary images were analysed with a 3D software OTIP 3D
specially designed for the classification of 3D images [MIC 98]. For each particle, of
the 3D volume, a set of parameters was determined by the software (volume of the
particle, centroid coordinates, size of the surrounding box ...). In this work, 260
particles were analysed individually around the notch. For each of them, the state of
deformation (broken or not broken ) was studied manually on the 1250 sections of
the different 3D volumes.
From those results, a Weibull analysis of damage was undertaken. The Weibull
probabilty Pr(i) for the rupturebof a particle i is given by the following formula:

110

X-ray tomography in material science

V0 is a reference volume which is a constant, V, stands for the volume of particle i,


oi is the stress in the particle, m and a0 are the Weibull distribution coefficients
which are to be determined.
The volume Vi can be obtained directly from the results of image analysis on the
3D images. The stress cri arises from elastic and plastic incompatibilities between
matrix and reinforcements. Its value, is obtained through quite complex analytical
calculations which take into account the local stress value. This local stress being
obtained via a 3D FEM model of the sample.
By coupling this calculation and the result of the analysis of the 3D reconstructed
volumes, the rupture stress of each particle was determined. From this data a plot of
the particle rupture probability as a function of the stress in the particles was
obtained. The shape of this curve suggests that the particle failure probability does
follow a Weibull law as already observed in MMCs [LEW 95]. The corresponding
Weibull parameters m and a0 were found equal to 3.2 and 1000 MPa, respectively.
The value of the Weibull modulus m calculated in the present study is relatively
low, suggesting that the rupture of the SiC particles is spread over a large stress
range. As a matter of fact, the analytical calculation of oi does not take into account
several parameters such as the introduction of damage in the particles during
specimen preparation or the degree of clustering of the particles (a high local
volume fraction should enhance the stress level in the particles). Such factors could
probably account for a large distribution of the rupture stresses. Thus, the Weibull
parameters obtained in this study should be regarded as those of the studied SiC
particles embedded in a deforming matrix, rather than the inherent fracture
behaviour of the particles themselves.
7.3.1. Cast aluminium alloys
Figure 7.5 shows a volume rendering of the internal pores inside alloy A and B
as observed by X-ray micro-tomography. It can be seen, from this figure that the
size and the volume fraction of the pores increases when the amount of hydrogen
introduced in the melt increases. Besides the shape of the pores appear to vary a lot,
from rather round shapes to more tortuous ones.
By comparing reconstructed sections of the material with the corresponding 2D
optical micrographs, it was shown that the reconstructed images of the pores with a
6.65 urn resolution do correspond (both in shape and size) to the actual pores in the
material [SAV 98]. On that basis, a quantitative study of the pores was carried out
from the 3D reconstructed images. As already mentioned, the differential X-ray
attenuation between a gas pore and the aluminium matrix being large, the pore grey
level in the reconstructed images is very different from the matrix grey level and
thus, binary images of the pores could be obtained by simple thresholding of the

Characterisation of MMCp and cast Aluminium alloys

111

images. The binary images have been studied by automatic 3D image analysis. Two
stereological parameters have been defined to try and characterise the shape and size
distributions of the pores. The first one, called the equivalent size, is defined as the
diameter of a sphere which would have the same volume as the considered pore.
The second one, called the sphericity s, is defined from the ratio of the volume of
the pore to its surface. A perfect sphere would have a sphericity parameter of 1
while a pore with a very tortuous shape would have a sphericity much smaller than 1
[SAV 98].

Figure 7.5. Reconstructed images of internal pores in two model cast aluminum alloys.
Artificial pores have been obtained by introducing H2 and Ar gases in the melt metal. As the
solubility of hydrogen decreases with temperature, when the metal solidifies, H2 is rejected
and forms gas pores which are easily visualised using X-ray tomography. Two different
H/Ar ratio have been used: 2% (left) and 7% (right). The edge size of both cubic boxes is
1.33 mm
Figure 7.6 shows a plot of those two parameters for the three investigated alloys.
It can be seen from this figure that at least two population of pores (cooresponding
to two clouds of points on the plot) can be found in the material. The first one, in the
lower part of the plot (equivalent size lower than 50 um), shows a weak correlation
between shape and sphericity and is represented for the three alloys. The second one
on the contrary can be found for sizes larger than 50 um and shows a strong
correlation between size and shape. The volume fraction of the pores belonging to
this last population can be seen to increase when the amount of hydrogen introduced
in the liquid metal is increased.
The two populations have different origins. One corresponds to microshrinkages when the metal solidifies while the other corresponds to artificial gas
pores. The latter appears during the whole solidification process while the former
appear at the end of it. Both types of pores have to form between the growing
dendrite arms network. Thus the growth of large pores is geometrically hindered by

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X-ray tomography in material science

the dendrites and the resulting shape is tortuous (low sphericity). By analysing
carefully the data it is possible to show [SAV 00] that the volume fraction of microshrinkage pores remains roughly constant for the three investigated alloys while the
volume fraction of gas pores increases exponentially with the H2 content as already
observed in the literature.

Figure 7.6. Plot of the equivalent size of the pores inside alloys J, K and L, as a function of
their sphericity. Two populations of pores can be seen respectively below and above an
equivalent size of about 50 jam. Those two populations correspond to artificial gas pores
(equivalent size larger than 50 pm) and to micro-shrinkages (below 50 /jm)

7.4. Conclusion
We have shown in this paper how X-ray tomography can be used to study
quantitatively structural micro heterogeneous materials. Two examples have been
given corresponding to the case on an Al/SiC particulate metal matrix composite
and to model cast aluminium alloys. Although 3D X-ray images of internal pores in
cast alloys are quite easy to obtain thanks to the large X-ray attenuation difference
between gas pore and aluminium matrix, the visualisation of the SiC reinforcements
in an aluminium matrix is not possible with classical tomography. In that case, it is
necessary to use phase contrast tomography which can be obtained with a coherent
X ray beam like the one delivered on the ID 19 beamline at ESRF. This technique
also improves the detection of damage in reinforcements.
With regard to the composite material, it was possible to follow the initiation and
development of damage inside a notched sample during in situ tensile deformation.

Characterisation of MMCp and cast Aluminium alloys

113

No influence of the tri axial stress state could be found on the mode of damage
(mode I cracking of the particles) which appears to be localised near the notch root
at the begining of the deformation process. By coupling the 3D data on the SiC
particles and analytical calculation a Weibull analysis of the particle fracture was
carried out, leading to Weibull modulus of 3.2 and a a0 constant of 1000 MPa.
For the model cast aluminium alloy, the 3D data obtained by tomography has
been used to characterise the pore population for three different processing
conditions. From this characterisation it is possible to distinguish between degassing
pores and micro-shrinkage pores.
7.5. References
[CLO 97] CLOETENS P., et al. Observation of microstructure and damage in
materials by phase sensitive radiography. Journal. Appl. Phys. 81,9 p.5878,
1997.
[ROB 99] ROBERT-COUTANT C, et al. Introduction to reconstruction methods
This Workshop.
[BUF 99] BUFFIERE J.-Y., et al. Characterisation of internal damage in a MMCp
using X-Ray synchrotron phase contrast microtomography Acta Mater. 47, 5,
pp.1613-1625, 1999.
[CLY 93] CLYNE T.W., WITHERS P.J., An Introduction to Metal Matrix
Composites Cambridge University Press, 1993.
[MIC 98] MICHOUD P., DARSONVILLE F., Segmentation et visualisation d'images
3D application par croissance de region a I'imagerie medicate dentaire PhD
thesis Saint EtienneUniversity June 1998.
[LEW 95] LEWIS C.A., WITHERS P.J., Weibull modelling of particle cracking in
metal matrix composites Acta metall. mater., 43, 10 1995.
[SAV 98] SAVELLI S., et al. Characterisation by synchrotron X-ray
microtomography of internal features and their detrimental effects with respect
to the fatigue properties in aluminium cast alloys Proc. of ICAA 6 Toyobashi
Japan p.529 1998 .
[SAV 00] SAVELLI S., PhD thesis INS A Lyon 2000 to be published.

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Chapitre 8

X-ray tomography of Aluminum foams


and Ti/SiC composites

The High resolution X ray tomography technique has been used to investigate
the internal structure during the deformation of two very different materials : an Al
foam and a SiC fibre reinforced titanium matrix composite. The observations show
that the metallic foam deforms via local buckling events. This collapse mechanism
is also studied by means of a modelling technique based on the finite element
method. The microstructure of the metal matrix composite is also easily revealed
with a sifficient resolution despite the high attenuation of the matrix. Cracks can be
observed during the straining on a fibre touching the surface of the sample. It was
not possible to show if this preferencial rupture was due to the weakness of this fibre
or to the stress field which is different close to the surface.

8.1. General introduction


This paper presents the investigation, with a single technique, of two completely
different materials. As a consequence, it is divided into two parts. The first part is
devoted to the characterisation of the microstructure of an aluminium foam and its
evolution during a compression loading. The second part is devoted to an
investigation of the microstructure and damage of a Ti/SiC composite during in situ
tensile straining.

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8.2. Aluminium foams


The newer low density cellular materials such as aluminium foams are being
produced at low cost by several companies thanks to recent developments in
manufacturing methods [MCC 99]. These materials show potential for use in lightweight structures. One of their interesting properties is the amount of energy
absorbed during the deformation which is directly related to the way the material
collapses in compression. We will focus our study on the compression behaviour of
these aluminium foams. We performed 3D inspections by means of X ray computed
microtomography (XRCMT) [KAK 88] on a commercial foam at different
deformation stages in compression. XRCMT has recently emerged as a powerful
technique capable to give a non destructive picture of the interior of the structural
materials including foams. We also present a method to transform the images of the
actual microstructure into a mesh which can be used to model the behaviour by
finite element calculations. We finally use these calculations to assess the stress
distribution inside the compressed walls.

8.2.1. Experimental set-up and results


&.2.I.I. Set-up
The tomograph used is based on the principle of fan-beam X-ray computed
tomography scanners. A schematic view is shown in Fig. 1 and a more complete
description can be found in [KAF 96]. An X-ray tube (Pantak HF 100) is used to
irradiate a thin slice of the scanned object. The transmitted intensities are measured
by means of an X-ray linear detector constituted by a unique row of 1024 sensitive
elements with a pitch of 0.225 mm. The height of the sensitive row is 0.5 mm.
Within each sensitive diode, a scintillator converts X-ray photons into visible light
which is detected by a photodiode. A charge-coupled device allows multiplexing of
the individual charges accumulated in each photodiode and delivers, after offset and
gain calibration, a one-dimensional signal of 1024 points encoded on 8 bits. The line
integration time is 8 ms.
The scanned sample is set between the focus and the detector, at a distance
allowing a geometrical magnification of 1.5. As the pixel size, measured along the
linear detector, is 0.225 mm, the corresponding elementary feature imaged at the
level of the sample is therefore 150 urn wide and 300 urn high. A first stepping
motor allows to rotate the sample by steps of 360/N degrees. The rotation axis must
be set perpendicular to the array and to the beam axis.
The acquisition of N successive lines delivers a complete sinogram which is
then processed by computer (computed tomography) to reconstruct the map of the

X-ray tomography of Aluminium foams and Ti/SiC composites

117

slice. For the present application, N was set to 900. A second stepping motor then
generates a translation of the sample along a direction parallel to the rotation axis
and a new adjacent slice can thus be imaged. The acquisition of the data
corresponding to a single slice lasts about 3 min.

Figure 8.1. Schematic description of the experimental setup for the tomograph used

Reconstruction is achieved using a C-language program written by the CEALETI (Commissariat a 1'Energie Atomique - France) and based on the Feldkamp
algorithm [FEL 84]. A ramp filter is selected, thus preserving the spatial resolution.
A DEC 500 MHz workstation is used to reconstruct the entire volume, slice by slice.
Reconstruction of the complete volume (350 x 340 x 128 voxels) lasts
approximately 1 hour.
We have translated the sample of 300 (jm between each slice in z, a value which
corresponds to the height of the diodes. In order to get an isotropic 3D
representation of the sample (i.e. reduce the resolution in the z direction to 150 |jm ),
we have numerically added extra slices in between the slices in z. We calculated the
grey level in these extra slices by linearly interpolating the grey levels in the
corresponding x, y voxels of the two adjacent slices.
8.2.1.2. Results
The sample was scanned for tomographic analysis in its initial state. It was then
compressed at three increasing values of remnant strain (true strain measured after
unloading). The internal microstructure was imaged using tomography at these three
steps after removal of the compression load. We then have a picture of the interior

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of the sample at four values of the remnant true strain in compression: 0, 0.065, 0.2
and 0.6.
A 3D view of the analysed sample is shown in figure 8.2. The cell walls are
clearly imaged and the 3D structure can be analysed. However, it is quite difficult to
visualise the deformations with this kind of representation especially in the of closed
cells for which the outer walls hide the inner ones. In what follows the qualitative
results will be shown under the form of 2D reconstructed slices which are easier to
analyse. Figure 8.3 (a and b) show a set of 2 D images of the same zone of the
sample numerically extracted from the volume at 0 to 6.5 % of remnant strain
respectively. These slices are parallel to the compression axis which is vertical on
the figure. One can clearly observe the deformation mechanism of the studied foam
in compression by comparing these two figures. The large value of the plastic strain
at this stage is obviously not due to a homogeneous plastic straining of the whole
sample, but to the local buckling of several walls like these surrounded by circles on
the picture. From the observation of the entire population of buckled walls, we have
observed that they are located in a band perpendicular to the loading axis (see figure
8.3b) i.e. the centre of gravity of these buckled walls is located in a narrow range in
the z dimension (roughly between z=60 and 100 pixel compared to a total height of
255 pixel for the sample).
Between the second and the third step, the number of new buckled walls is
small. The deformation process leads to the complete closing of the already
collapsed cells instead of the appearance of new ones. Some new collapsed cells can
be seen in step 3, but even at this very large plastic strain, some regions of the
sample are not deformed at all.

Figure 8.2. 3D view of the sample before compression

X-ray tomography of Aluminium foams and Ti/SiC composites

119

Figure 8.3. Part of a 2D reconstructed slice of the same zone at two deformation steps
initial state (left) and 6 % (right)

8.2.2. Finite element modelling


The internal structure of the studied foam is extremely complex: the cell size and
the length of the walls are parameters which are widely spread. The non periodic
character of the structure leads also to a very difficult calculation of the actual force
applied to each wall compared to the case of honeycombs which is another class of
cellular materials. The complexity of this entanglement lead us to analyse the
distribution of the stress and deformation in each wall using an appropriate tool: the
finite element analysis. In what follows, we present an easy way to use this 3D
picture to generate meshed models of the actual microstructure. These models are
readable by the ABAQUS commercial code which we have used to perform the
calculations in 3D.
8.2.2.1. Direct meshing of the actual microstructure
The result of a tomographic inspection (after reconstruction) is a 3D table of
gray levels. Each point of this table (voxel) defined by its coordinates x, y and z,
represents the linear attenuation coefficient of the X-rays within the elementary
volume of the material at this location. Given the experimental resolution of the setup used, the volume of the element exhibiting this transmission coefficient is 150um
x ISO^m x 150um in our study. The grey level is high if the voxel is situated inside
a cell and it is low if the voxel is situated inside an aluminium wall. The method
described below is based on a simple idea: each voxel in the 3D image can be
represented by a cubic element in a finite element mesh. We developed a software to
produce models meshed according to the following procedure :
- a 3D parallelepipedic set of nodes is generated with a regular and identical
spacing in the three directions. This spacing is equal to 150 jam. The number of
nodes is governed by the number of voxels in the actual sample in the three
directions (number of nodes = number of voxels +1);

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- this set of nodes is used to define cubic-eight-nodes-brick-elements according


to the standards used in the ABAQUS commercial code (element type C3D8).
- the table of the values of the local transmission coefficient in the sample is
read in parallel with the 3D mesh. The elements located in the cells (high grey level)
are removed from the mesh and the elements located in the walls (low grey level)
are kept in the model.
We considered that the boundary between the steel plates of the rig and the
aluminium foam was perfect. The displacement of the lower nodes were fixed in the
three directions. We generated a steel plate perfectly bounded to the upper nodes
and applied a displacement along the compression direction to the upper nodes of
this steel plate.
8.2.2.2. Results
Given the number of degrees of freedom of the problem to be solved, it was not
possible to treat the complete foam in 3D. We firstly grouped 8 voxels into one
voxel which lead to a resolution of the mesh twice lower than this in the initial
picture. We calculated the deformation of a 503 voxels block which represents a 1003
voxel block in the initial foam i.e. approximately one eight"1 of the entire volume of
the studied foam. The calculation was performed in the elastic regime. The
deformed and undeformed models are compared in figure 8.4 a and b respectively.
One can see the deformed shape of the walls.

Figure 8.4a. FEM undeformed model

Figure 8.4b. FEM deformed mode

X-ray tomography of Aluminium foams and Ti/SiC composites

121

8.3. Titanium composites


8.3.1. Experimental procedure
8.3.1.1. Imaging setup
This part of the experiment has been carried out at ESRF on beam line ID 19.
The electron beam energy was 6 GeV. The white beam was restricted by slits and
monochromated by a set of two parallel silicon single crystals selecting the photons
exhibiting the chosen energy (33 keV for the present application). The unusually
large distance of 140 m between the source and the experimental hutch on ID 19
leads to a high lateral coherence of the photons. The distance between the sample
and the detector (a cooled CCD camera developed at ESRF) was set to about 70
mm. This particularity in the setup combined with the high lateral coherence of the
photons has been shown [CLO 97] to lead to an improvement in the detection of
phase features (like cracks) thanks to a so called 'phase contrast' which is added to
the regular attenuation contrast. More details about this technique can be found in
the article by Cloetens et al. which will be published in the present proceedings.
In addition to simple x-ray radiography, the ID 19 beam line allows tomographic
observations to be performed on structural materials. Tomography is a new non
destructive technique which allows the 3D internal structure and damage of a
sample to be imaged [BUF 99] with a resolution down to 1 (jm. The sample can be
fixed on a turntable and rotate in the beam to provide a set of 900 radiographs which
are used by a reconstruction software to give a 3D numerical image of the studied
material.
8.3.1.2. Sample

Figure 8.5. Schematic description of the sample used

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X-ray tomography in material science

Figure 8.6. Tomographic reconstruction of the sample in its initial state.


View along the z axis. The three plys can be observed

Figure 8.7. Tomographic reconstruction of the sample in its initial state.


View along the y (right) and the x (left) axis

X-ray tomography of Aluminium foams and Ti/SiC composites

123

The sample used for this study was made of three layers of monofilamenatry SiC
fibers embedded into a titanium matrix. The schematic geometry of the sample is
shown in figure 8.5. The initial state was characterised using the tomographic setup
described above. The results are shown in figures 8.6 and 8.7 under the form of 2D
reconstructed tomographic slices along the 3 principal directions of the sample
according to the geometry defined in figure 8.5. The internal structure of these
composites can be clearly imaged at the resolution of 6.65 um used for the present
study.
8.3.1.3. Tensile rig and testing procedure
A tensile rig has been especially designed to allow the observation of damage by
tomography during the deformation of materials [BUF 99]. This rig can be set on
the turntable. In order to avoid the frame of the machine to hide the beam when
rotation is necessary (for the tomographic inspection) a PMMA tube is used to
transmit the load between the upper mobile grip and the lower fixed grip. This tube
was carefully polished and gave negligible attenuation nor phase contrast on the 2D
radiographs. The force and the crosshead displacement were recorded on a
computer and monitored during the test.
A crosshead displacement rate of 150 um.mn 1 was used for the tests
corresponding to an average strain rate of 5.10 s'1. Once sample 1 was set in the
machine, a first radiograph was recorded in order to characterise the initial state.
The sample was then loaded step by step in tension : during the test, the crosshead
displacement was stopped at increasing values of the deformation and a radiograph
was recorded during each of these steps.

8.3.2. Results
Figure 8.8 shows the observation of the evolution of damage during the straining
of the sample. After the first step, one fiber was broken in two locations. After the
second step, the same fiber was broken in a third location. These were the only
visible events detected during the straining which then had to be stopped because
the sample was too strong compared to the limited capacity of the tensile rig. The
fiber which broke was this at the bottom left corner of the sample in figure 8.6. This
fiber was the only one cut by the free surface. It is not clear if the early damage of
this fiber is due to the fact that its intrinsic resistance was reduced because of pre
damage during the sample preparation or if the stress field inside this fiber was
modified by the effect of the presence of the surface.

8.4. General conclusion


The collapse mechanism of a closed cell foam has been studied during
compression thanks to X ray tomography experiments. The resolution in this first
case was 150 |im, a value which was chosen because of the big size of the sample.
The deformation mechanism by buckling of the walls of the foam has been
evidenced. These microbuckling events are located in a band perpendicular to the
compression axis. A software has been developed to transform the actual voxel
information into a meshed model. The deformation of a part of the foam has been
calculated by the finite element method in the elastic regime. In future work, we will
try to define a criterion for local buckling of the walls from the comparison of the
actual buckling configuration observed and the calculation of the stresses inside the
walls. The microstructure and damage of a titanium composite reinforced with SiC
long fibres has also been clearly imaged with the same kind of technique but

Figure 8.8. 2D reconstructed tomographic slices showing the evolution of the microstructure
of a same zone for the three steps of the tensile test: inital step, fisrt step (center) and second
step (right)

X-ray tomography of Aluminium foams and Ti/SiC composites

125

with a much higher resolution (6.65 urn in the resent case). This resolution was
achieved using synchrotron radiation. The observation of damage was carried out in
tension. Unfortunately, the sample was too strong for the tensile rig, but the
observations made during this primarily experiment are promising. We were able to
visualise several ruptures in a same fibre at different steps during the test.

Acknowledgements
The tomographic scans on the Al foam were performed with the help of G. Peix
using the equipment of the CNDRI laboratory in Villeurbanne. The Ti/SiC samples
were provided by Alex Madgewick and Phil Withers from the UMIST in
Manchester and the tomographic scans were made at ESRF in collaboration with
J. Baruchel and P. Cloetens.

8.5. References
[BAR 98] H. BART-SMITH, A.F. BASTAWROS, D.R. MUMM, A.G. EVANS,
DJ. SYPECK, and H.N.G. WADLEY. Acta mater. (1998). 46, N 10, PP 35823592.
[BUF 99] J.-Y. BUFFIERE, E. MAIRE, P. CLOETENS, G. LORMAND, R. FOUGERES.
Characterisation of internal damage in a MMCp using X-ray synchrotron phase
contrast microtomography. Acta Met. (1999) vol. 47, N5 pp 1613-1625.
[CEN 99] CENDRE E., DUVAUCHELLE P., PEIX G., BUFFIERE J.-Y. and BABOT D.
Conception of a high resolution X-ray computed tomography device ;
application to damage initiation imaging inside materials. Proceedings of the 1st
World Congress on Industrial Process Tomography (1999) BUXTON (U.K.),
14-17avril.
[CLO 97] P. CLOETENS, M. PATEYRON-SALOME, J.-Y. BUFFIERE, G. PEIX,
J. BARUCHEL, F. PEYRIN, J. SCHLENKER. J. Appl. Phys. (1997), 81,9.
[DAY 83] G.J. DAVIES and S.J. ZHEN. Mater sci. (1983), 18, 1899.
[PEL 84] L.A. FELDKAMP, L.C. DAVIS, J.W. KRESS. Practical cone-beam
algorithm. J. Opt. Soc. Am. (1984), 1 N 6, pp. 612-619.
[KAK 88] C. KAK, M. SLANEY. Principles of Computerized Tomographic Imaging.
(1988). Cotellessa RF (Editor). New York : IEEE Press (Phs).
[KAF 96] V. KAFTANDJIAN, G. PEIX, D. BABOT and F. PEYRIN. J. of X ray Science
and Technology (1996). 6, 94.
[MCC 99] K.Y.G. McCuLLOUGH, , N.A. FLECK and M.F ASHBY. Toughness of
aluminium alloy foams. Acta Mater. (1999), 47 pp. 2331-2343.

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Chapitre 9

Simulation tool
for X-ray imaging techniques

A computer code was developed to simulate the operation of radioscopic or


tomographic devices. This code can be helpful to predict and optimise the
performance of any imaging system. The use of computer aided drawing (CAD)
models allows to carry out simulations with complex three-dimensional (3D)
objects. The whole geometry of the system, from the source to the detector, can be
defined and monochromatic or polychromatic beams can be chosen. Computed
images present the advantage to contain no photon noise. Nevertheless, if necessary,
noise can be added to the images afterwards, with an adjustable level. Movements of
the object can be performed automatically, in order to simulate, for example, the
acquisition of a sinogram. 2D tomographic images of a spatial resolution phantom,
simulated with different sets of parameter values, have been reconstructed. A 3D
tomography has also been carried out on a geometrically complex sample. The
results prove overall coherence of our simulation tool and show rich possibilities.

9.1. Introduction
X-ray imaging techniques, such as radiography, radioscopy and tomography, are
used in a wider and wider range of specific applications, notably in the medical field
and in materials science [PEL 89][PEI 97]. To develop new imaging systems, or
optimise existing ones, it is generally necessary to carry out long and expensive
series of tests and measurements. Proceeding in such a way, by trials and errors,
often reveals itself unrewarding because it is practically difficult to study the
influence of the many parameters (beam energy, focal spot size of the X-ray tube,
detector type, geometric parameters, etc) that condition the final image quality.

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To go beyond those material limitations, simulation tools can be appealed to,


with the aim to create a virtual imaging environment. Thus complex situations can
be investigated, with important saving of time and low cost [INA 98]. When
developing a new system, simulation offers powerful means to predict and optimise
the future device performance, and to choose the most suitable components.
Simulation can also be very helpful to interpret complex experimental data, by
comparing them to the corresponding simulation results [KOE 98]. Finally,
simulation can also be a tool to train operators.
In that context, a four years research program was initiated 12 months ago in the
laboratory "Controle Non Destmctif par Rayonnements lonisants", to model and
simulate the functioning of any X- or y-ray imaging chain, from the photon emission
phenomena, up to the detector behaviour, including the photon-matter interactions
within any 3D object. During this first period, we started with photon attenuation in
the object, and we have laid emphasis on 3D geometric aspects.
This paper presents the basic principles we have used, the possibilities offered
by the computer code we have developed and a few examples of simulated images,
especially in tomography.

9.2. Background
Our simulation software requires various input data, intended to describe an
experimental situation with maximum accuracy. From the geometric point of view,
we have to define the source (shape, size, position, orientation), the detector
(position, orientation, pixel number and size), and the sample. The use of a
computer aided drawing (CAD) model describing the object offers great advantages:
complex 3D samples can be drawn in a short time with automatic surface mesh
generation (triangular meshes), and with high accuracy. The object may consist of
several parts, possibly of different materials.
Ray-tracing techniques, together with the X-ray attenuation law, are the basis of
our computer code. From each source point, a set of rays is emitted towards every
pixel centre of the detector. Each ray may intersect a certain number of meshes on
the object surface (fig. 9.1). The attenuation path length in every object phase is
calculated by determining the coordinates of all those intersection points. The
photon number N(E) that emerges from the sample and reaches the detector
surface is given by the attenuation law:
N(E) = N0(E) A0Q[])xp[-//,()*,.]

[1]

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129

where N0(E) refers to the number of photons with energy E, emitted by the source
per solid angle unit, AQ is the solid angle corresponding to the pixel, observed from
the source point, ui(E) designates the attenuation coefficient associated to the
material i at energy E, and xi the total path length through the material i.
The image computed by using equation [1] does not take into account the
contribution of scattered photons. Moreover, the simulated image does not contain
any photon noise. So far, we have used a perfect detector, in which every pixel is
able to count all of the photons that hit its surface. The Compton and Rayleigh
scattering contributions to the image and the photon interactions with a real detector
will be investigated in a future work [DUV 98].

Figure 9.1. Principle of radiography simulation. A point source, a matrix detector, and a
CAD model of the object with triangular meshes are used

9.3. Simulation possibilities


9.3.1. Source geometry
As mentioned before, the simulation is based on ray-tracing from a source point.
Consequently, if a unique source point is used, the simulated image does not take
into account any image degradation due to geometric unsharpness. Accurate
evaluation of geometric unsharpness is of great importance, e.g. in diagnostic
radiology [SCH 98], but it is a very delicate task, because the unsharpness associated
to a point in the object depends on several parameters:

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the position of the point in the object


the shape, size, position and orientation of the gamma or X-ray source
the position and orientation of the detector.

To carry out realistic simulations, we chose a straightforward method, which


consists in cutting the source area into elementary source points, and repeating
image computation with each of the latter (fig. 9.2). The source shape (rectangular or
elliptic) can be chosen, and the number of source points as well as their spacing in
the two directions are adjustable. In this way, the influence of geometric
unsharpness can be evaluated, even in complex situations. This can be useful to
determine the best geometric adjustment of an imaging system.

9.3.2. Beam spectrum


The photon spectral distribution of the incident beam is another important aspect
we had to give care to. To simulate an image, the photon attenuation calculation has
to be repeated with a set of discrete energy values. So far, we have used the Birch
and Marshall catalogue [BIR 79], in which semi-empirical spectral data, in the tube
voltage range 30 to 140 kV, are tabulated. The corresponding attenuation

Figure 9.2. Simulation of geometric unsharpness. The sample is a thin square plate with a
circular hole 1 mm in diameter. The detector is composed of 80 x 80 square pixels, 0.1 mm
wide. Simulation A: point source (geometric unshrapness UA = 0 mm); B: 1 mm wide square
source (UB = 1 mm); C: 2 mm wide square source (Uc = 2 mm). The grey level profile
corresponding to the central column of the detector is presented in each case. The profile C
reveals a degradation of the image contrast, due to geometric unsharpness

Simulation tool for X-ray imaging techniques

131

coefficients, associated to any elementary or compound substance, can be obtained


by means of available databases, such as XGAM [BER 88] or EPDL97[CUL97].
When performing a simulation, energy intervals (or channels) with adjustable
width can be defined, and a set of images associated to each one is stored. A global
image, obtained by adding all those partial images is computed too. It is therefore
easy to monitor the spectrum evolution (beam hardening) when the beam goes
through the object (fig. 9.3). The influence of a filter, wherever it is located in the
imaging chain, can also be visualised. Simulation of dual energy imaging techniques
can be carried out as well.
By comparing simulation results obtained at different tube voltages, it is possible
to predict the more favourable energy, leading to optimal image quality, in any
specific application. For example, when the photon energy rises, the quantity of
transmitted photons is more important and the relative photon noise is smaller.
However, the image contrast is lower and therefore a compromise has to be found.
To determine the latter, simulation can be a helpful tool.
9.3.3. Sample movements
To simulate the functioning of radioscopic or tomographic systems, multiple
simulation with automatic movements of the sample is necessary. Those movements
play the same role as stepper motors in experimental setups and they can be a
combination of translations and rotations. For example, radioscopic image
acquisition can be performed by means of a linear detector, with a sample
translation, perpendicular to the plane constituted by the X-ray focal spot and the
detector [KAF 95]. Tomographic devices can be simulated as well, with automatic
computation of all the projections that compose the sinogram.
Depending on the simulation type (simple radiographic projection, 2D
tomographic slice, 3D tomography with a matrix detector) and parameters (detector
resolution, number of source points, mono or polychromatic beam, complexity of
the sample), the computation time order of magnitude can vary from 0.1 second up
to several hours on a PC, with a 400 MHz microprocessor.

9.3.4. Phone noise


An interesting characteristic of our simulation code is its deterministic principle.
The same experiment, if it is simulated several times, will always yield exactly the
same results. Moreover, the synthetic images have the advantage not to contain any
photon noise. If necessary, photon noise, i.e. Gaussian random fluctuations, can be
added to the image, when the simulation is complete. The effect of different noise
levels can thus be evaluated with a single simulation.

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X-ray tomography in material science

Figure 9.3. Radiograph simulation of a gate, with a step wedge. A polychromatic beam is
used and the detector is split into 100 energy channels with a 1 keV interval, (a): CAD model
of the gate, (b): Simulated radiograph, (c): Incident beam spectrum, (d): The transmitted
photon spectra associated to the points labelled a to c reveal a beam hardening phenomenon,
stronger where the part is thicker, i.e. close to the edge

9.4. Simulation examples in tomography


9.4.1.2D tomography on a spatial resolution phantom
As a first application, we decided to simulate 2D tomographic experiments, with
a linear detector (fig; 9.4). Several sinograms were simulated with different source
sizes to assess the geometric unsharpness influence on spatial resolution.
We used a CAD model of an aluminium spatial resolution phantom, cylindershaped, with square holes from 0.4 mm to 2.5 mm in width. This phantom was
defined in the frame of an industrial tomography workgroup, in order to quantify the
performance of a tomographic system.
We have also studied the effect of beam spectral distribution. When a
monochromatic beam is used, the reconstructed numerical value of the linear
attenuation coefficient is constant in the homogeneous aluminium phase, and

Simulation tool for X-ray imaging techniques

133

Figure 9.4. Simulation of a tomographic slice on an aluminium spatial resolution phantom,


(a): Simulated setup and CAD model of the phantom. The detector is linear, composed of 500
pixels (0.2 mm wide). 800 projections were computed, (b): Reconstructed slices. Left: point
source; right: 4 mm wide source, cut into 15 elementary source points (geometric
unsharpness associated to the centre of the phantom: U - 1.7 mm). In both simulations, the
beam is polychromatic (100 kV tube voltage), (c): The grey level profiles, corresponding to
the lines labelled A and B show the effect of geometric unsharpness. Computation time: 10
min (point source) and 2.5 h (large source)

corresponds, as expected, to the attenuation coefficient of aluminium at the beam


energy (fig. 9.5). This quantative result proves that the whole simulation process is
coherent. If the beam is polychromatic, it hardens itself when penetrating into the
part, causing a "cupping effect"[CEN 98][KAK 88].
If necessary, it is also very simple to add photon noise, i.e. Gaussian fluctuations
to the sinogram and to the reference image (obtained when the sample is removed
from the beam) before reconstructing the tomographic slice. In this way, different
noise levels can be visualised easily (fig. 9.6). Experimentally, photon noise is
conditioned by the choice of tube voltage, current intensity, filters, exposure time
and geometric parameters.

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Figure 9.5. Influence of the incident beam spectrum on a reconstructed slice (a):
monochromatic 100 keV beam, (b): polychromatic beam with 100 kV tube voltage. In both
cases, a point source was used, (c): (-n) reconstructed value profiles (n designates the linear
attenuation coefficient). When a monochromatic beam is used (graph A), the baseline of the
profile has a constant value, equal to the value of(-u) associated to aluminium at 100 keV. In
contrast, when the source is polychromatic, the beam hardens itself in the object, causing a
"cupping effect" (graph B)
9.4.2.3D tomography on a complex mechanical part
Finally, we simulated a 3D tomographic system, with a matrix detector,
consisting of 250 x 220 pixels. The whole volume of the object was reconstructed
successfully. As the beam was polychromatic, cupping effect, as well as streaks, are
visible in the reconstructed slices (fig. 9.7).

Simulation tool for X-ray imaging techniques

135

Figure 9.6. Influence of Gaussian photon noise. Gaussian fluctuations have been added to the
sinogram and to the reference image (obtained by performing an acquisition without sample)
before reconstruction, (a): The photon number reaching the central pixel of the detector,
during the first projection, is equal to 50. (b): The photon number is 10 times greater, (c):
Grey level profiles corresponding to the lines labelled A and B

9.5. Conclusion and future directions


This preliminary work phase allowed us to develop the framework of a computer
code, able to produce within a short time realistic synthetic images, simulating the
operation of radiographic, radioscopic or tomographic devices. The strong points of
this tool are the use of CAD models to describe complex 3D objects, the ability to
simulate geometric unsharpness and to deal with a polychromatic beam. The

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Figure 9.7. 3D computed tomography, (a): Schematic view of the simulated setup and CAD
model of the sample. A matrix detector (250 x 220 pixels) and a point source were used. The
dotted lines labelled A, B and C indicate schematically three slices presented on the right (b)

computed images present no photon noise, but Gaussian random fluctuations can be
added afterwards, if needed.
Several issues need further development and will be addressed in the next phase
of our research program. As a priority, we envisage to enrich our simulation tool, by
taking into account the scattering contribution. The 3D mapping of the absorbed
dose in the sample will be broached simultaneously. Modelling and simulating the
influence of the detector response on the image quality will also be an essential task.
Finally, quantitative experimental validations will be necessary.
Possible application areas are numerous. Simulation can be useful, when
developing any specific application, to choose the best components, optimise the
experimental parameters and save time by reducing the number of experimental
tests. Simulation also presents an important potential, to test the performance of
image processing procedures in a virtual environment, where all parameters are
fully controlled.

9.6. References
[BER 88] BERGER, M. J., "MIST Standard Reference Database 8, X-ray and Gamma-ray
Attenuation Coefficients and Cross Sections, XGAM", distributed by Office of Standard

Simulation tool for X-ray imaging techniques

137

Reference Data, National Institute of Standards and Technology, Gaithersburg,


Maryland 20899, 1988.
[BIR 79] BIRCH, R., MARSHALL, M., ARDRAN, G. M., Catalogue of Spectral Data For
Diagnostic X-rays, The Hospital Physicists' Association, 1979.
[CEN 98] CENDRE, E., Tomographie a haute resolution par rayons X, application a I'etude de
la perte osseuse chez le sujet age, these de doctorat, Institut National des Sciences
Appliquees de Lyon, 1998.
[CUL 97] CULLEN, D. E., HUBBEL, J. H., KISSEL, L., "EPDL97: The Evaluated Data Library,
'97 Version", UCRL-ID-50400, Vol. 6, Rev. 5, 1997.
[DUV 98] DUVAUCHELLE, P., Tomographie par diffusion Rayleigh et Compton avec un
rayonnement synchrotron: application a la pathologic cerebrale, these de
doctorat, Universite Joseph Fourier - Grenoble 1, 1998.
[PEL 89] FELDKAMP, L. A., GOLDSTEIN, S. A., PARFITT, A. M., JESION, G., KLEEREKOPER, M.,
"The direct examination of three dimensional bone architecture in vitro by computed
tomography", Journal of Bone and Mineral Research, vol. 1, n 4, p. 3-11, 1989.
[INA 98] INANC, F., GRAY, J. N., JENSEN, T., Xu, J., "Human body radiography simulations:
development of a virtual radiography environment", Part of the SPIE Conference on
Physics of Medical Imaging, Vol. 3336, p. 830-837, 1998.
[KAF 95] KAFTANDJIAN, V., Reconnaissance automatique de defauts dans les produits
metalliques par radioscopie numerique, these de doctorat, Institut National des Sciences
Appliquees de Lyon, 1995.
[KAK 88] KAK, A. C., SLANEY, M., Principles of Computerized Tomographie Imaging, IEEE
Press, 1988.
[KOE 98] KOENIG, A., GLIERE, A., SAUZE, R., RJZO, P., "Radiograph Simulation to Enhance
Defect Detection and Characterization", Proceedings of the 7tn European Conference on
Non-Destructive Testing, Vol. 1, p. 444-451, 1998.
[PEI 97] PEIX, G., BUFFIERE, J.Y., CARDINAL, S., CLOETENS, P., SALOME, M., PEYRIN, F.,
BABOT, D., "Caracterisation de rendommagement dans les materiaux de structure par
tomographie haute resolution a rayons X", Revue des composites et des materiaux
avances, Vol. 7, n hors serie, p. 59-67, 1997.
[SCH 98] SCHIABEL, H., SlLVA, M. A., C-LIVEIRA, H. J. Q., MARQUES, P. M. A., FRERE, A. F.,

"A computer simulation technique to preview the influence of the recording system on
the image sharpness in mammography", Part of the SPIE Conference on Physics of
Medical Imaging, Vol. 3336, p. 602-609, 1998.

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Chapitre 10

Micro focus computed tomography


of Aluminium foams

X-ray microfocus computed tomography (CT) is a non-destructive inspection


method that provides the true cross-sectional images of the internal details of a
component. Due to their X-ray absorption properties, CT technique has been found
to be very useful for the internal investigation and quality control of metal foams.
Therefore, some non-destructive tests have been performed on closed cell
aluminium foams produced by powder metallurgical and casting processes. This
method provides a detailed microstructure characterisation of any cross-section of
the sample as well as a three-dimensional (3D) visualisation of the specimen using
backprojection algorithms. Moreover, digital imaging with CT technique enables the
description of the deformation mechanisms within the foam at different strain
values.

10.1. Introduction
Metallic foams are porous metals with high porosity (from 50 to 99 %). In the
past few years there has been a considerable increase in interest for metal foams,
especially made of aluminium or aluminium alloys. The unique properties of
aluminium foams like high stiffness to weight ratio, high energy dissipation, low
density, reduced acoustic, thermal and electrical conductivity, chemical resistance,
easy recycling etc..., make them potentially useful in many high technology
industries such as automotive and aerospace. Therefore, they are currently used for
energy impact absorbers [GIB 88, EVA 99], in lightweight structures (in the cores of
sandwich panels) [DAY 83, GIB 88, KRE 99], heat exchangers [GIB 88, BAR 98, EVA
99], sound absorbers or silencers [DAV 83, GIB 88] and filters [GIB 88]. However,
successful thermostructural implementation relies not just on their thermome-

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chanical properties, but on additional attributes such as manufacturing cost,


environmental durability and fire retardancy [EVA 99]. Efficient use of foams
requires detailed understanding of their mechanical behaviour. Therefore, simples
equations related to their structural features and the properties of the material from
which they are made have been derived [GIB 88, THO 75]. Thereby, computed
tomography which is a non-destructive technique of characterisation, has been used
for a detailed 3D description of the microstructure (which can not be achieved by a
commonly used 2D characterisation technique) as well as for the investigation of
deformation mechanisms within the foam at different strain values. Furthermore,
input parameters for both the optimisation of production process and for the
modelling can be expected as feedback.

10.2. Production process of Aluminium foams


Aluminium foams can be produced by various methods [DAY 83, GIB 88]. For
our tests two types of Al-foam samples with closed cell structure have been used.
These specimens were made by a powder metallurgical process and by a continuous
foam-casting route.

10.2.1. Powder metallurgical process


Aluminium foam samples made by powder metallurgical route were produced by
LK Ranshofen [KRE 99], a department of the Austrian Research Centres. The
process, that is based on the Alulight-technique, is described schematically in
figure 10.1. Aluminium alloy is prepared by mixing metal powder in the appropriate
relations. The foaming agent, titanium hydride or zirconium hydride is then added

Figure 10.1. Schematic illustration of the powder metallurgical process

for making metal foams

Micro focus computed tomography of Aluminium foams

141

to the mixture. The content of the foaming agent depends on the metal to be foamed
and the desired density. The mixture, containing the agent, is then compacted by
extrusion. As a result a semi finished product is obtained in which the foaming agent
is homogeneously distributed within a dense, virtually non-porous metallic matrix.
This foamable material is processed into pieces of the desired shape by rolling and
cutting. Finally, foamed metal parts were obtained by heating the material to
temperatures above the melting point of the matrix metal. The metal melts and the
foaming agent releases gas in a controlled way, so that the metal transforms into
foamy mass which expands slowly.
The foaming takes place inside simple closed moulds which are completely filled
by the foam. After the mould is filled, the process is stopped by simply allowing the
mould to cool to a temperature below the melting point of the metal. The density of
the metal foams is controlled by adjusting the content of foaming agent and by
varying the heating conditions. The resulting foamed blocks have closed outer skins
(figure 10.2) which can be removed by cutting them into samples of the desired
dimensions.

Figure 10.2. Aluminium foams made by powder metallurgical process, the right picture
is a sample with closed outer skins, and the left one is a sample without skins.

10.2.2. Continuous foam-casting process


Another production method for aluminium foams is the continuous foam-casting
route developed simultaneously and independently by Alcan and Norsk Hydro in the
late 1980's [ASH 99, SAN 94]. A principle sketch of the process is given in figure
10.3.
Gas is dispersed into small bubbles in an aluminium composite melt by rotor
impellers. The walls of the created bubbles are stabilised by dispersed refractory
particles avoiding coalescence between them. The bubbles rise to the surface where
they accumulate. The accumulated foam on the melt surface is then transferred to a
conveyor belt, where it solidifies and cools. The melt may constitute of different
alloys and refractory particles. The most common alloys and particles are AlSiSMg
(or equiv.), AlSiSMgCuNi with SiC particles and AA6061 (or equiv.) with A12O3

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particles. The particle size ranges from 10 to 30 um and their amount in the melt is
comprised in the interval of 10 to 30 vol%.

Figure 10.3. principle sketch of the foam-casting route employed by Nosk Hydro

Figure 10.4. Aluminium foams made by casting process, the right picture is a sample
with density 0.3 g/cm, and the left one is a sample with density 0.18 g/cm

Foams may be produced in densities from 0.1 to 0.5 g/cm3 by this method. The
density is controlled by the process parameters, the most important being the rotor
speed, the gas flow through the rotor and the amount of particles in the melt. At the
present stage the production is directed towards slabs having typically 8-12 cm
thick, 70 cm wide and 200 cm long; however samples of the desired dimensions
(figure 10.4) can be cut out from these slabs.

10.3. Mechanics of foams


A first impression of the mechanical behaviour of foams can be obtained by a
uniaxial compression test, because in most applications, foams are loaded in
compression. A typical compressive stress-strain curve is shown in figure 10.5. One

Micro focus computed tomography of Aluminium foams

143

can see an initial quasi-static increase of stress for small deformations followed by a
long collapse plateau, truncated by a regime of densification where the stress steeply
rises.

Figure 10.5. Schematic compressive stress-strain curve for an elastic solid and a foam made
from the same solid, showing the three regimes of compressive behaviour and the dissipated
energy at a given peak stress for both foam and the solid from which the foam is made

Gibson and Ashby [GIB 88] have developed models to describe the typical
mechanisms responsible for the different mode of deformation of foams. The
mechanical properties of foams can be described by equation [1] derived using
dimensional analysis:

[1]

where X and p are the mechanical property and density of the foam, Xs and ps are
those of the solid cell wall material and (|) is the volume fraction of solid contained in
the edges, C and a are constants.
Foams are especially good for energy absorption. Energy absorption in a foam is
related to the area under its stress-strain curve in figure 10.5, energy absorption of a
foam for a given peak stress is compared to that of the solid from which it is made.
For the same energy absorption, the foam always generates a lower peak force, but
the stress is limited by the long flat plateau of the stress-strain curve [GIB 88].
Thereby, by choosing the right cell wall material and relative density, best
combination of the properties can be achieved for energy absorbers.

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X-ray tomography in material science

10.4. Non-destructive investigation of Aluminium foams


Previous models for mechanical performance of foams (equ.[l]) have focused on
their dependence on the variation of the apparent density, the properties of the solid
material from which the cell face are made, and the cell geometry. The geometrical
feature include cell shape and size, distribution in cell size, defect and flaws in the
cell structure as well as the microstructural parameter like cell wall and edges
thickness and material distribution between cell face and cell edge.
X-ray microfocus computed tomography (CT) is a non-destructive inspection
method that provides the true cross-sectional images of the internal details of a
component. Due to their X-ray absorption properties, CT technique has been found
to be very useful for the internal investigation and quality control of metal foams.
Unlike conventional microstructure characterisation methods [GRO 99], no previous
preparation of the sample is required when using CT technique. This method
delivers any cross-section of the sample as well as a three-dimensional (3D)
visualisation of the specimen using back projection algorithms. Moreover, digital
imaging with microtomography enables to the description of the deformation
mechanisms within the foam at different strain values.
10.4.1. Principle of microfocus computed tomogrphy
Microfocus computed tomography technique is based on X-ray attenuation
inside an object [BRU 92 - MAI 89]. The attenuation depends on the material's
atomic number, density and thickness of the sample and on the energy of X-ray
beam. A diagram showing the basis of CT technique is given in figure 6. The object
to be inspected is mounted on a turntable. Rotation and translations are controlled
par stepping motors. A conical X-ray beam is generated from an X-ray source and
focused on a detector located on the opposite side of the specimen. After traversing
the sample, the beam is recorded by an X-ray CCD camera. Several projections are
needed to fully construct the two-dimensional cross-section. There are obtained by
rotating the object through 180 degrees. Conversion of these projections to the final
image is conducted using a back projection algorithm [BRU 92].

Figure 10.6. Basis of method for X-ray microfocus computed tomography

Micro focus computed tomography of Aluminium foams

145

The CT images obtained by this method represent cross-sectional slices through


the specimen in a horizontal plane perpendicular to the rotation axis of the turntable.
Magnifications up to 100 are possible on small objects resulting in a high resolution
(10 um) and therefore, very small details can become visible.
10.4..2. Results
Samples of Al-foams made by both powder metallurgical (LKR) and casting
(Norsk Hydro) processes were chosen for non-destructive testing. The typical
dimensions of the specimens were approximately 50 x 50 x 50 mm3. The density of
the Hydro samples were measured to be 0.31, 0.18, and 0.10 g/cm3 while the density
of the LKR specimens were measured to be 0.35 and 0.22 g/cm3.
The desktop X-ray microtomograph used for scanning contains a microfocus
tube, an X-ray CCD camera and a Pentium computer with an integrated software
package called TOMOHAWK running under Windows NT V4.0. The
TOMOHAWK software developed and commercialised by AEK Technology
Company in OXON (UK) provides a package of programs for calibration, data
acquisition, processing, display and analysis of both computed tomography and
digital radiography data. The samples were placed at such distances from the X-ray
source and the imaging system to achieve a magnification of 2.3 and a resolution of
200 um. To acquire the information needed for tomography, the specimens are
rotated for 180 degrees in steps of 0.5 degree. To increase the signal-to-noise (SNR)
ratio, the image processing hardware is first used to digitise the real-time TV images
into arrays of 512 x 512 pixels, each having 8 bits of intensity information.
Integration of 256 TV frames is then used to increase the SNR by a factor of 16. The
data collected as described above are processed to obtain the cross-sectional CT
images using an appropriate filtered backprojection algorithm [BUR 92]. Several
different sets of data at various heights can however be readily extracted
simultaneously (up to 50 slices) from the integrated TV images. The total data
acquisition time is about 70 minutes and the CT reconstruction lasts about 20
minutes.
10.4.2.1. Qualitative micro structure characterisation of Al-foams
Figure 10.7 shows CT images of Al-foam samples made by Norsk Hydro casting
process. The specimens have an average density of 0.10, 0.18 and 0.31 g/cm3. The
pictures reveal a broad density distribution through the samples. Regions with a high
density (figure 10.8) consist of spherical cavities embedded in the metallic matrix
while for those with a lower density, individual cells can fell the presence of
neighbouring cells during solidification [PRA 95].

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X-ray tomography in material science

Figure 10.7. CT images of cross-sections of Norsk Hydro Al-foams; (a) sample with average
density of 0.10 g/cm3, (b) sample with average density of 0.18 g/cm, (c) sample with average
density of 0.31 g/cm

We can also distinguish from figure 10.7 that the cells are oriented in a preferred
direction (perpendicular to the outer skins) and on the other hand that there is a
broad cell size distribution. A qualitative description of the material distribution
between cell walls and cell edges is shown in figure 10.9. Different situations that
influence the mechanical properties of foams through the factor <j> in equation [1] are
specified.

Figure 10.8. CT images of cross-sections of Norsk Hydro Al-foams showing regions of high
density and others of lower density; (a) sample with average density of 0.18 g/cm , (b) sample
with average density of 0.31 g/cm

Micro focus computed tomography of Aluminium foams

147

CT images of Al-foam specimens made by LKR powder metallurgical route are


given in figure 10.10. The samples have an average density of resp; 0.22 and 0.35
g/cm3. Two slices at two different heights have been extracted for each sample.

Figure 10.9. CT images of cross-sections of Norsk Hydro Al-foams showing the material
distribution between cell walls and cell edges: (a) concentration of the material in the cell
walls, (b) concentration of the material in the cell edges, (c) equal distribution of the material
between cell walls and cell edges

Cell size distribution seems to be homogeneous but the presence of big holes
around the centre of the structure leads to a broad density distribution through the
specimens. These holes might be caused by the foaming process itself because the
latter is stopped by simply allowing the mould to cool. The temperature in the centre
of this mould is still sufficiently high to enabling the foaming process to continue
while it has stopped elsewhere.
In figure 10.11 the image obtained by a zooming of the circled region (figure
10.11(a)) in the CT slice of the specimen, reveals a significant decrease of the
resolution. To overcome this problem, a scanning of a smaller sample is done (figure
10.1 l(b)). Therefore, the size of the specimen has to be chosen carefully to achieve
the required resolution.

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X-ray tomography in material science

Figure 10.10. CT images of cross-sections of LKR Al-foams showing the presence of big
holes in the foam structure: (a) sample with average density of 0.35 g/cm, (b) sample with
average density of 0.22 g/cm3

Figure 10.11. C7 images of cross-sections of Norsk Hydro Al-foams: (a) picture obtained by
a zooming of the circled region, (b) picture obtained by scanning a smaller specimen of 10 x
10 x 30 mm leading to a resolution of 90 [im

Micro focus computed tomography of Aluminium foams

149

10.4.2.2. Description of the deformation mechanisms


CT technique has been found to be very useful for the investigation of
deformation mechanisms of Al-foams at different strain values. Hydro samples of 20
x 20 x 30 mm3 have been strained up to 10% and scanned again to show the
deformations that occur within the specimen, the CT slice of unloaded sample was
taken as a reference.

Figure 10.12. CT images of cross-sections of Norsk Hydro Al-foams having typical


dimensions of 20 x 20 x 30 mm3: (a) picture of the unloaded specimen, (b) picture after 10%
straining showing the deformation mechanisms within the foam.

From figure 10.12 we can see that deformation was concentrated in a local area
having the lowest density of the sample [KRI 99, BAR 98]. The main observed plastic
deformation mechanisms were bending and buckling of cell walls, nodes which are
centre of high concentration of metallic material were left unchanged in most cases,
some of them seemed to undergo a slight rotation. Some cells were even found to be
completely intact, they had only undergone a translation. 10% straining is perhaps
too much to describe the onset of the deformation bands in the specimen, so in
subsequent tests, samples will be strained at lower values (2 - 4 %) to identify the
cells that initiate the bands and to provide a morphological explanation to the
importance of band formation in plastic deformation.
10.4.2.3. Three-dimensional (3D) reconstruction of Al foam structure
CT technique provides 3D information of the scanned specimen concerning cell
arrangement like orientation, gradient, homogeneity, etc. Images of contiguous
planes can be stacked by mean of a reconstruction algorithm, called T3D, to form
3D images of a section or if the entire part has been scanned, a full volumetric image
of the specimen. T3D is a scientific visualisation application for graphically

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X-ray tomography in material science

analysing volumetric data. It has been developed and commercialised by Fortner


Software Company.

Figure 10.13. 3D reconstruction of Al-foam structure using T3D software: (a) 3D


reconstruction of a Norsk Hydro Al-foam structure based on 50 CT slices, (b) numerical
oblique slice through the 3D data volume

Figure 10.14. 3D reconstruction of Al-foam structure using T3D software: (a) 3D


reconstruction of a Norsk Hydro Al-foam structure based on 50 CT slices with a numerical
cut-out, (b) 3D reconstruction of an LKR Al-foam structure based on 50 CT slices with a
numerical cut-out

TT

Once data is imported, the reconstruction algorithm can quickly generate slices
in any orthogonal plane or at oblique angles through the 3D data volume (figure
10.13) as well as creating cut-outs in the reconstructed 3D foam structure (figures
10.14, 10.15). The presence of the big holes in the Al-foam specimens produced by
LKR powder metallurgical process is clearly shown in figure 10.15

Figure 10.15. 3D reconstruction of an LKR Al-foam structure based on 50 CT slices,


the presence of big holes in the structure is clearly shown

10.5. Conclusion
Aluminium foams of similar relative density can exhibit a wide dispersion of the
mechanical properties due to various effects, such as, gradient of density
distribution, preferred pore orientation, cell size distribution and cell shape features
[SIM 99, GRA 99, SIM 98, GIB 88]. Therefore a clever characterisation of these
material is required.
Besides the fact that microfocus computed tomography is a non-destructive
technique of investigation, it brings a fundamental change to the microstructure
characterisation by delivering 3D data as well as it provides a powerful tool to
describe the deformation mechanisms within the specimen at different strain values.

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Future work will focus on the use of microfocus computed tomography for
quantitative characterisation of Al-foams as well as the identification of the cells that
initiate the deformation bands by straining the specimens at lower values (2-4 %).
Furthermore, input parameters to support modelling work can be expected.
Acknowledgements
We wish to acknowledge the financial support of Renault S.A. Company. The
authors would like to thank Claude Peytour-chansac and Christophe Grolleron from
Renault S.A. for their support and useful discussion.

10.6. References
[BUR 92] BURCH S.F., LAWRENCE P.P., "Recent advances in computerised X-ray
tomography using real-time radiography equipment", British Journal of NOT,
Vol. 34, n 3, p. 129-133, 1992.
[CEN 96] CENDRE E. et al., "High resolution X-ray computed tomography applied
to bone structure characterization", Proceedings of the 14th Word Conference on
Non Destructive Testing, p. 1211-1214, 1996.
[SAS 98] SASSOV A., "Desktop X-ray microtomography", Proceedings of the 7h
European Conference on Non Destructive Testing, p. 2837-2836, 1998.
[MAI 89] MAISL M., REITER H., "Non destructive investigation of new materials
and electronics by microfocal radiography and high resolution X-ray computed
tomography", Proceedings of the 12th Word Conference on Non Destructive
Testing, p. 1667-1672, 1989.
[GRO 99] GROTE F., SCHIEVENBUSH A., "Characterization of cast and compressed
foam structures by combined 2D-3D analysis", Proceedings of the International
Conference on Metal Foam and Porous Metal structures, p.227-232, 1999.
[GIB 88] GIBSON L.J., ASHBY M.F., Cellular Solids: Structure and Properties,
Pergamon Press, 1988.
[SUG 97] SUGIMURA Y. et al., "On the mechanical performance of closed cell Alalloy foams", Acta Mater., Vol. 45, n12, p.5245-5259, 1997.
[THO 75] THORNTON P.H., MAGEE C.L., " The deformation of Aluminium foams",
Metallurgical Transactions A, Vol. 6A, p. 1253-1263, 1975.
[BAR 98] BART-SMITH H. et al., "Compressive deformation and yielding
mechanisms in cellular Al alloys determined using X-ray tomography and
surface strain mapping", Acta Mater., Vol. 46, n10, p. 3583-3592, 1998
[GRA 99] GRADINGER R., RAMMERSTORFER F.G., "On the influence of mesoinhomogeneities on the crush worthiness of metal foams", Acta Mater., Vol. 47,
n l , p . 143-148, 1999.
[SIM 98] SlMONE A.E., GIBSON L.J., "Effects of solid distribution on the stiffness
and strength of metallic foams", Acta Mater., Vol. 46, n 6, p. 2139-2150, 1998.
[PRA 95] PRAKASH O. et al., "Structure and properties of Al-SiC foam", Materials
Science and engineering A199, p. 195-203, 1995.

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[DAV 83] DAVIES G.J., ZHEN S., "Metallic foams: their production, properties and
applications", J. Mater. Sci., Vol. 18, p. 1899-1911, 1983
[SAN 94] SANG et al., "Process for producing shaped slabs of particle stabilized
foamed metal", US Patent 5334236, 1994.
[EVA 99] EVANS A.G., HUTCHINSON J.W., "Multifunctionality of cellular metal
systems", Proceedings of the International Conference on Metal Foam and
Porous Metal structures, p.45-56, 1999.
[KRE 99] KRETZ R. et al., "Manufacturing and testing of aluminium foam structural
parts for passenger cars demonstrated by example of rear intermediate panel",
Proceedings of the International Conference on Metal Foam and Porous Metal
structures, p.23-27, 1999.
[ASH 99] ASHOLT P., "Aluminium foam produced by the melt foaming route
process, properties and applications", Proceedings of the International
Conference on Metal Foam and Porous Metal structures, p. 133-140, 1999.
[SIM 99] SlMANClK F., Reproducibility of aluminium foam properties", Proceedings
of the International Conference on Metal Foam and Porous Metal structures,
p.235-240, 1999.
[KRI 99] KRISZT B. et al., "Deformation behaviour of aluminium foam under
uniaxial compression (a case study)", Proceedings of the International
Conference on Metal Foam and Porous Metal structures, p.241-246, 1999.

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Chapitre 11

3D observation of grain boundary penetration


in Al alloys

Synchrotron radiation X-ray microtomography is used to investigate the


penetration of liquid gallium into the grain boundaries of aluminium.Penetration and
wetting processes play a key role in the understanding of liquid metal
embrittlement.The large difference in absorption coefficients between Ga and Al
allows micrometer and sub-micrometer thick liquid Ga films to be observed as they
are wetting grain boundaries of Al. The tomographic reconstruction are compared to
electron backscattering diffraction mappings recorded on the sample surface.
Morphologic segmentation of the tomographic dataset opens the way to analyse and
visualize the three-dimensional microstructure of the material.

11.1. Introduction
The phenomenon of liquid metal embrittlement (LME) can be defined as the
brittle fracture (or loss of ductility) of normally ductile metals and alloys when
stressed while in contact with a liquid metal [PER 97]. LME leads to a significant
deterioration of the mechanical properties of the solid metal: liquid Ga for example
(melting point Tm= 29.8 C) is known to induce brittle fracture in polycrystalline Al
at stress levels far below the fracture strength of the material in air. Typically this
deterioration is observed only over a limited range of temperatures near the melting
point of the embrittling agent ('temperature trough' [NIC 79]). Strictly speaking,
LME concerns metals and alloys under stress. However, it is known, that for some
particular systems, intergranular penetration occurs even at zero applied stress. The
observed kinetics are far beyond the rates expected for grain boundary diffusion.
There is experimental evidence that the penetration may be considered as a wetting
process which is governed by the ratio of the grain boundary energy ygb and the

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X-ray tomography in material science

energy y sl of the liquid metal - solid metal interface. The equilibrium dihedral angle 6
at the solid metal is given by: 9 = 2cos"1(ygb/2ysl). Once the wetting condition
2ysl <ygb is fullfilled, 6 equals zero and the grain boundary will be replaced by the
liquid metal [Str 94].

Figure 11.1. a) grain boundary groove with equilibrium dihedral angle d >0 (T<TJ b)
wetted grain boundary with 9=0 (T>TJ c) Temperature dependance of surface and grain
boundary energies d) resulting temperature dependance of equilibrium dihedral angle for
different grain boundaries [Str 94]

However the formation of micrometer thick liquid layers cannot be explained


within this simple framework and different models have been proposed to account
for [Rab 97], [Gli 99]. As penetration and wetting are involved in the mechanism of
LME, a more detailed characterisation of these processes might be considered as
key steps towards a future understanding of LME.
Up to now the occurrence of grain boundary wetting has mainly been detected
by standard metallographic observation methods like Auger electron spectroscopy,
TEM and SEM. Recently some in-situ transmission electron microscopical
observations of the penetration process itself have been reported [Hug 98]. These
observation methods provide excellent spatial resolution but are intrinsically limited
to the sample surface or thin foils. Quite recently synchrotron radiation X-ray
microtomography was applied for bulk observation of penetrated grain boundaries
at the micrometer level [Lud 99]. The present paper gives an overview of results
obtained with this new technique.

3D observation of grain boundary penetration in Al alloys

157

11.2. Experimental set-up


The experiments were carried out at the ID 19 beamline of the European
Synchrotron Radiation Facility (ESRF). ID 19 is devoted to high resolution imaging
and features an energy tunable (7-100 keV) X-ray beam of low divergence (~ 1
urad). The dedicated micro-tomographic set-up consists of a precision mechanics
sample stage (rotation and translation) combined with a fast, high resolution
detector system (Fig. 11.2). The detector system itself consists of a fluorescent
screen (YAG: Ce) which transforms the X-rays into visible light and microscope
optics to project the image on the cooled 10242 CCD camera, with a dynamic range
of 14 bits, fast readout (0.22 s/frame) and low noise electronics (3 e-/s) [Lab 96]. The
spatial resolution, limited mainly by scattering in the fluorescent screen, was
determined with the knife-edge method to be 1.7 jam for the optical magnification
used in our experiments (effective pixel size: 0.98 urn). The need for ultimate spatial
resolution in order to resolve the Ga decorated grain boundaries of micron and
submicron size restricts the maximum sample diameter to approximately 1 mm.
In order to avoid beam-hardening artefacts, the incoming 'white' synchrotron
radiation was monochromatized to 15 keV using a Rb-B4C multilayer with large
energy bandwidth (AAA=10"2). Typical scan times (1000 projections over 180
degrees, 13 bit dynamic range) are of the order of 25 min.
The samples were prepared from a piece of polycrystalline Al 5083 alloy
(composition in at.%: Si (0.15), Fe (0.19), Cu (0.04), Mn (0.56), Mg (4.1), Cr
(0.12), Ti (0.02)). The extruded material was annealed at 700 K for 24 h, then at 800
K for another 24 h. Optical inspection after surface etching (10 % HF) clearly

Figure 11.2. Schematic view of the experimental set-up showing multilayer monoehromator,
sample rotation and translation stage and the detector system. The sample is rotated stepwise
from 9 0 to 180 and 2D projections are recorded for each angular position 9. The
spatial distribution of the linear attenuation coefficient in the sample can be reconstructed
using a standard tomographic reconstruction algorithm

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X-ray tomography in material science

revealed the columnar structure of the material. In the plane perpendicular to the
deformation direction, grain size ranges from tens to hundreds of microns.
Cylindrical samples with a diameter of 0.8 mm were machined from this material,
with the cylinder axis parallel to the major axis of the elongated grains. In order to
promote surface wetting by liquid Ga, the sample was dipped in a 10% NaOH
solution for about 30 seconds in order to remove the Alumina layer covering the
surface and a droplet of Ga was deposited on the surface immediately afterwards.

11.3. Results
Figure 11.3 shows a reconstructed slice of a sample which has been penetrated
by liquid gallium. Lighter gray-levels in the reconstructed images correspond to
stronger absorption. The bright lines, dividing the image into smaller, closed cells
can be clearly attributed to the presence of highly absorbing Ga (Z=31, attenuation
length =19 |jm at 15 keV) layers inside the Al matrix (Z=13, attenuation length =
506 |tim at 15 keV). The spatial resolution of the used optical set-up is restricted to
about 1.7 (am. However it is possible to detect features below this limit ('partial
volume effect'): the locally enhanced absorption in a subregion of a volume element
(voxel) will change the mean attenuation for the entire voxel. The fact that some of
the wetted grain boundaries show only weak contrast might be attributed either to
different composition or density of the absorbing material, or to a different (subpixel) size of the observed features. As Al shows a very limited solubility in Ga at
low temperature [Mon 76] the differences in attenuation can not be explained by
differences in composition of the liquid itself. As a consequence, the amount of
liquid Ga present per unit volume must be different, or in other words, the width of
some wetted grain boundaries is smaller than the pixel size.
11.3.1. Comparison with EBSD surface mapping
As mentioned above, the thickness of the liquid layer varies considerably from
grain boundary to grain boundary. A first attempt has therefore been undertaken to
correlate the information from electron backscattering diffraction (EBSD) mapping
(Fig 11.4c) before application of liquid Ga and microtomographic reconstruction of
the same zone on the sample surface after penetration by liquid Ga (Fig. 11.4a,b).
The sample was penetrated with liquid Ga and a first tomographic scan was
performed after an initial anneal for 30 min at 50C (Fig 11.4a). The second
tomographic scan (Fig 11.4b) followed after an additional anneal of 60 min at
150 C.

3D observation of grain boundary penetration in Al alloys

159

Figure 11.3. a) Reconstructed tomographic slice (pixel size: 1 \jan) through a cylindrical
Al sample which has been exposed to liquid Ga for 4h at 320K: the wetting of the grain
boundaries by liquid Ga can be clearly detected; the magnified image shows the varying
thickness of the Ga layer

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X-ray tomography in material science

A series of circumstances contributes to the fact, that the contours observed with
both techniques do not compare perfectly: a) corrosion and dissolution processes of
excess liquid Ga on the sample surface may lead to changes in the size and shape of
the surface grains, b) the tomographic cut defines a geometrically perfect plane
whereas the (mechanically and electrochemically polished) sample surface analysed
by EBSD does not, c) the spatial sampling rate of 5um in the EBSD mapping
different from the pixel size of Ijam in the tomographic reconstruction d) spherical
aberations of the electron microscope at low magnification leed to distorsions of the
EBSD mapping.
It is interesting to note, that grain boundaries which cannot be observed after the
first anneal at 50C, e.g. boundaries B'-B2 and C'-C2, are preferentially those of
small relative misorientation (close colour codes in the EBSD mapping). These
boundaries become visible after the second anneal at 150 C - in accordance with
the qualitaive model presented in Fig. 1 [Str94].
11.3.2.3D visualization of a polycrystal
The comparison of the tomographic reconstruction after the second anneal at
150C with the EBSD surface mapping (Fig. 7.4b&c) shows, that even with the
above mentioned limitations a good agreement is achieved. The tomographic
reconstruction of a penetrated polycrystal might therefore be used to analyse and
visualize the microstructure of the material in three dimensions. For this purpose the
experimental raw-data need to be refined using morphological image processing
methods. The applied three-dimensional segmentation algorithm, an implementation
of the "watershed" method [Bou 99], transforms the experimetnal raw data (Fig.
7.5a) into binarised volume-data containing closed cells (Fig 7.5b). In a final step, a
"label" (e.g. a number or a specific colour) is attributed to each voxel belonging to
the same cell. The size and the shape of the individual grains in the polycrystalline
material can now easily be analysed and visualized using a dedicated volume
rendering software (Fig 7.5c).
11.4. Conclusions
The present study is a new example showing the interest of synchrotron
radiation X-ray microtomography as a non destructive bulk characterization method
of materials at the micrometer scale. The presence of liquid Ga at the grain
boundaries of polycrystalline Al leads to locally enhanced absorption and standard
tomographic reconstruction methods allow to observe the wetting state of grain
boundaries inside the material. The complementary information provided by
micotomography and EBSD allows to correlate the wetting state of grain boundaries
with the relative misorientation of the adjacent grains. We do not yet have enough
data to draw quantitative conclusions, however we may confirm from our

3D observation of grain boundary penetration in Al alloys

161

experimental results that, as expected, low angle grain boundaries are less
penetrated than general grain boundaries.

Figure 11.4. Comparison of tomographic reconstructions (a,b) of the sample surface with
electron backscattering diffraction mapping (c). The EBSD mapping was obtained before
application of liquid gallium. Two tomographic scans were taken after the penetration: a)
after an anneal of SOmin at 50 C and b) after additional anneal of 60 min at 150 C. Note
that the low angle grain boundaries B'-B2 and C'-C2 are only detected after the second
anneal

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X-ray tomography in material science

Figure 11.5. a) tomographic reconstruction of same sample as in Figl after


additional anneal of 2h at 300 C. b) result of 3D morphological filtering and
segmentation c) volume rendering of a small part of the sample
Apart from the scientific interest in studying the penetration of liquid metals, one
might also think of some practical use of the microtomographic observation of Ga
decorated grain boundaries. Under the assumption that all boundaries are detected in
the tomographic reconstruction, one can use the segmented volume-data in order to
analyse and visualize the microstructure of a polycristal in three dimensions. This
technique might for example be applied to study the influence of grain boundaries
on the propagation of cracks in prefatigued aluminium alloys.

3D observation of grain boundary penetration in Al alloys

163

Acknowledgements
We would like to thank E. Boiler and P. Cloetens for their help during the microtomography experiments. We gratefully acknowledge useful discussions with
J. Baruchel and Y. Brechet.

11.5. References
[PER 97] FERNANDES P.J.L., JONES D.R.H., "Mechanisms of liquid metal induced
embrittlement",International Material Reviews 42, p. 251, 1997.
[NIC 79] NICHOLAS M.G., OLD C.F., " Review Liquid Metal embrittlement",
Journal of Materials Science 14, p. 1-18, 1979.
[Str 94] STRAUMAL B., GUST W., MOLODOV D., "Tie lines of the grain boundary
wetting phase transition in the Al-Sn system", Journal of Phase Equilibria
Vol.15, 4, p. 386-391, 1994.
[Rab 97] RABKIN E., "Coherency strain energy as a driving force for liquid
grooving at grain boundaries", Scripta materialia, vol.39, No.6, pp 685-690,
1998.
[Gli 99] GLICKMAN E., NATHAN M., "On the kinetic mechanism of grain
boundary wetting in metals", J.Appl.Phys.,85, p. 3185-3191, 1999.
[Hug 98] HUGO R.C., HOAGLAND R.G., "In-situ observation of Aluminium
embrittlement by liquid gallium", Scripta Materialia, 38, p., 523-529, 1998.
[Lud 99]LUDWIG W., BELLET D., "Penetration of liquid gallium into the grain
boundaries of aluminium: A synchrotron radiation microtomographic
investigation", J. Mater. Science Eng. A, in press.
[Lab 96] LABICHE J.C., SEGURA-PUCHADES J., VAN BRUSSEL D., MOY J.P.,
ESRF Newsletter 25 p. 41-43, 1996.
[Mon 76] MONDOLFO L.F., Aluminium Alloys: Structure and Properties,
Butterworths, London, 1976.
[Bou 99] BOUCHET S., Segmentation et quantification d'images tridimensionnelles,
rapport de stage 36me annee, Ecole des Mines de Paris, 1999.

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Chapitre 12

Determination of local mass density


distribution

Closed cell aluminium based foams are chosen for performing digital transmission
radiography and X-ray computed tomography (CT). Transmission radiography yields
information on the heterogeneity of mass distribution, if two dimensional local mean mass
density maps are computed. CT provides data of the three-dimensional mass distribution.
Three-dimensional local mean density maps are proposed to identify hard and soft regions in
a cellular structure and they are used for modeling the mechanical behavior of aluminium
foams. High resolution CT enables a detailed structural analysis of the foam.

12.1. Introduction
Industrial production of foamed metals [ASH 99, BAU 99, HOP 99, KRE 99, MIY 99,
SEE 99] and metal matrix composites [DEC] is in progress for some specific
applications. Being in a developmental stage there are no generally acknowledged
specifications. Quality definitions for heterogenous materials have to be defined.
One of the main structural features correlated to properties is the local distribution of
the second constituent (either reinforcement or pores) within the matrix metal. The
aim of this work is to develop a quantitative description of "heterogeneity" of such
composites which can be applied for quality control. Foamed aluminium is chosen to
demonstrate the determination of local mass distribution by transmission
radiography or computed tomography. The recorded intensity distributions form the
basis for the calculation of local mass density distributions. Since the density is the
most important parameter which correlates the mechanical properties of a foam to
those of the dense bulk material [GIB 97], density distributions can be used for the
simulation of the mechanical behaviour and can be correlated to experimentally
determined properties.

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X-ray tomography in material science

12.2. Material
Samples of foamed aluminium with closed cell structure were chosen for testing.
The ALULIGHT material [MEP 96] of AlSiMg (AA 6xxx) wrought and of AlSil2Mg
cast alloys were produced by LK-Ranshofen [KRE 99] and by SAS-Bratislava [SIM 99]
and are originally covered by a skin of the matrix alloy, respectively its oxide.

12.3. X-ray radiography


In transmission radiography the recorded intensities provide an integral
information about the attenuation of the X-ray beam along its path, whereas in CT
the recording of intensities from a large number of different views allows the
mathematical reconstruction of the local attenuation at any point of the object [COP
94]. For both methods the attenuation values can be correlated to the mass density, if
the material composition is known.
The following X-ray sytems have been used: a Philips Tomoscan SR7000
medical tomograph to provide digital transmission radiography and computed
tomography as well and a GAMMASCAN micro-CT system [BAM 97]. Medical CT
can be applied to cellular aluminium yielding a resolution of about 0.7 mm
(comparison with a metallographic light microscopic picture was given in [DEG 99]).
The main features of the cellular structure can be revealed even in X-rayed cross
sections of more than 250 mm in diameter. The GAMMASCAN 3d-tomograph with
a 200 kV microfocus tube and a 12 inch area detector provide a resolution of about
1/1000 of the tested object's size (but not better than 10 um). High resolution
technical CT is a powerful research tool to characterise structural features in 3D to
correlate them to materials properties and their scatter [EVA 99, FOR 98] and to
stimulate modelling [DAX 99].
Two dimensional (2D) local mean mass density maps of flat parts were derived
from transmission images, where the pixel value p(/v) correlates to the mass density
of the corresponding column traversed by the beam (Fig. 12.la). Averageing over a
surrounding area of n x m pixels gives the local density value at the location of the
central pixel. Calculating this average pa (rtj) for every point /v yields a local mean
mass density distribution of the component:

where g(r ij-r ij) is the weight of each surrounding pixel. In Fig. 12.1bp(;c.) is a
schematic onedimensional representation of the pixel values of the transmission
image. A mean local density function pa(xi)is calculated by averaging over an
intervall of [;t - 34, xi + 35] with a constant weigth function g = 1 /70.

nD efot eloca
r sml idnemas
ant ysi oi t d i s t r i bn u t i o7

16

Figure 12.1. (a) principle of calculating a local density value from a transmission image; (b)
the density
values p(x
scheme) derived from the transmitted intensities
t} (onedimensional
are the result of a physical averaging over the column taversed by the beam.
pa (xt ) illustrates the effect of mathematical averaging over an interval of Ax=70 pixel

CT experiments reveal a three dimensional (3D) data set of volume elements


(voxels) containing the 3D mass distribution of the tested object. This data set is
appropriate to investigate the cellular structure [GRO 99, COR 99] and to calculate a
mean local density distribution [KRI 99a] by averaging over a certain surrounding
volume of each voxel (Fig. 12. 2a). Considering a foam (or an MMC) the material is
described by voxel
values
0 in pores
p(r ( p(rijk ) = pR for reinforcement) and
ijk ) =
p(r.
jk ) = ps in cell walls, edges and nodes ( p(rijk ) = pM for the matrix). The mean
local
of the voxel
functionlocated
p
at point rijk
a (rjjk )density

is then defined

analogous to Eq. 1 as: p

Figure 12.2. (a) principle of calculating a local density value from a volumetric CT data set;
(b) onedimensional representation p(xt) of a cellular structure and local density p(l(xj).
Limits of the mean local mass density around the overall average density pm are indicated to
discriminate "hard" (pa > pm + Ap) or "soft" (pa < pm - Ap) regions

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X-ray tomography in material science

The averageing process neglects fine structural details and allows to determine
local differences in the material distribution. Figure 12.2b shows a onedimensional
model p(xi)of a cellular structure with massive walls of the solid density psand
empty pores in between. Averaging the mass densities over intervals [*, - 34, ;c, + 35]
with g = I/70yields the mean local density function pa(xi).

12.4. Results
12.4.1. Mass Distributions calculated from Transmission Radiographs

Figure 12.3. X-ray transmission of ALL/LIGHT plate: a) transmitted intensity of each pixel
(0.6 x 0.6 mm2); b) contour plot of the 2D mean local mass density

Determination of local mass density distribution

169

Figure 12.3a demonstrates a digital recording of the X-ray intensity transmitted


through a part of a cellular wrought alloy slab (200 x 130 x 20 mm3), average density
pm - 0.57 g/cm3) with skin. The intensity in each pixel oscillates strongly, which
complicates the interpretation of local density variations. The contour plot of 2D
local mean density is shown in Figure 12.3b varying from less than 0.2 g/cm3 to
more than 2 g/cm3. It was computed by averaging the mass densities over areas of
11x11 pixels (6.4x6.4 mm2) as schematically shown in Fig. la. Although the
original information is smeared over a given area, the averaging process reveals
much clearer mesoscopic inhomogeneities in local mass distribution. The example
reveals the drainage effect the sample suffered by foaming in an upright position.
Some big pores (> 4mm) are visible too, where the mean mass density of a
transmitted column of the averaging cross section amounts below one tenth of the
average density of the whole sample.

12.4.2. Mass Distributions calculated from 3D-Tomograms


3D-CT recordings of cellular metals serve as basis for 3D density mappings.
Fig. 12.4 depicts the mass distribution recorded by CT along 3 perpendicular cross
sections of the same sample as shown in Fig. 12.3. Fig. 12.4a represents the mass
distribution in each voxel. Fig. 4b shows the corresponding 3D mean local mass
density maps for the voxels along these cross sections. The cells bigger than 4 mm
can be clearly identified even in the 3D mean local density map.
Mass density limits can be defined in 3D mean local density maps to distinguish
regions with high or low mass density. Mean local density values of volumes of
2 x 2 x 2 m m 3 of an AlSil2-ALULIGHT compression test sample measuring
22x22x30 mm3 had been computed. A lower limit of 1.67-times the average
density of the sample pm was chosen to discriminate "hard" regions of higher mass
density. The iso-surface in Fig. 12.5a encloses the voxels with values above that
limit. The density limit is reduced to 1.33-/?m and the averaging volume is increased
27-times yielding the iso-surface given in Fig. 12.5b. Figure 12.5a and b demonstrate
the influence of the chosen density limit in combination with the averaging volume
of the mean local density mapping. The influence of the selection of the averaging
volume alone on the localisation of "soft" regions is compared in Fig. 12.5c and d,
where the iso-surface at 0.67-pm encloses the regions of lower mean local mass
density. The averaging volume is changed from a cube of 6 x 6 x 6 mm3 in Fig. 12.5c
to a more than twice as big parallelepiped with one third of the edge lengths of the
sample, i.e. 7x7x10mm 3 in Fig. 12.5d. The smaller the averaging volume the
bigger the scatter in mean local density will be.

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X-ray tomography in material science

Fig Ure l 2 4

,
, ' - MaSS dmsity distribution on the surfaces of a parallelepiped recorded by
technical CT: a) CT cross section images from the 3D data set (voxelsize 0.3x0.3x0 3 mm3)
b) contour plots of 3D mean local density maps for an averaging volume of 4.3x4.3x4 3 mm>
(15x15x15 voxels) for the voxels along the planes shown in (a)

The iso-surface presentations of the limits of mean local mass density reveal as
well the 3D arrangement of the corresponding hard or soft regions across the sample
Fig I2.5b shows a V-like interconnection of hard regions across the sample which
will increase the compression resistance in the long direction. The soft regions of
that sample - see Fig. 12.5c, d - are oriented rather parallel to the direction of
compression suggesting, that they will not be identical with deformation bands [KRI
yybj. Consequently the spatial distribution of hard and soft regions has to be
considered too as an additional quality criterion.
High resolution CT reveals details in the cellular structure as shown in Fig 126
The 3D iso-surface representation of the structure shows cell walls down to about
100 Mm thickness as well as tiny shrinkage pores in cell wall nodes. Such CT data
can be used to study deformation mechanisms by computing 3D-displacements of
structural features [FOR 98].

Determination of local mass density distribution

171

Figure 12.5. Iso-surfaces of mean local mass densities in one AISU2-ALULIGHT test sample
(a = b = 22 mm, c = 30 mm) of average density pm= 0.5 g/cm3: a) hard regions of mean
local densities p > 1.67-pm in averaging volumes of 2x2x2 mm3, b) hard region of p >
1.33-pn, within 6x6x6 mm3, c) soft regions of p < 0.67- pm within 6x6x6 mm3, d) same
density limit as c) but within 7 x 7 x 10mm3, i.e. 1/3 of the edge lengths of the sample

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X-ray tomography in material science

Figure 12.6. Iso-surface at a level of 50% of pAI computed from high resolution 3D technical
CT data (voxelsize: 40x40x 40 fjm3). The volume of 8x8x8 mm3 within a casting alloy
ALL/LIGHT sample (same as in Fig. 5) shows a few cells, where the roughness of the cell
walls, defects in cell walls, shrinkage pores in nodes and an ensemble of neighbouring cells
can be seen

12.5. Application of the mean local density distribution


X-ray transmission images of cellular samples are ambiguous in detecting big
pores. Any conventional X-ray transmission system including medical CT is
suitable for identification of density variations of cellular metallic parts of regular
shape, based on 2D mean local density maps.
3D X-ray computed tomograms of even moderate resolution provide the basis
for the calculation of 3D mean local mass densities to identify soft and hard regions
and their spatial arrangement within the component. However the experimental
results show, that the arrangement of these regions has to be considered when
describing the mechanical behavior of foams (macroscopic anisotropic behavior).
Fig. 12.7 shows the measured compressive stress-strain curves and the density
distribution of two samples viewed from perpendicular directions. The density
distribution is derived from medical CT measurements. The 2D local mean densities
were calculated by averaging the CT data over columns having the thickness of the
sample (20 mm) and a cross-section of 5 x 5 mm. The largest extension of the
columns is oriented in y-direction (z-direction) for the xz-mapping Cry-mapping).
The yield strength shows a variation of about 20%, although the average density of
samples was fixed at 480 kg/m3. This high variation of yield stress can be explained
by the density distribution. The sample A is characterized by the lower yield stress
and shows a soft zone of low density, oriented nearly perpendicular to the loading
direction; sample B has a higher strength and has a hard zone of high density

Determination of local mass density distribution

173

parallel to the loading direction. Density variation limits can be chosen as quality
criteria, but have to be combined with a reasonable choice of averaging volume.

Figure 12.7. Compressive stress-strain curves of Alulight (cast alloy) samples, both having
an average density of 0.48 g/cm3 but different local density distribution as shown by
mappings of these samples in xz and xy planes

Figure 12.8. The sample A: a) The cellular structure along the observed surface recorded by
a digital camera at 2% overall strain. Deformation zones are marked by the white lines; b)
distribution of the corresponding calculated equivalent plastic strain (PEEQ) on this surface

The assessment of the spatial arrangement of such hard and soft regions in
mechanically loaded components can also be used for the meso-mechanical
simulation of heterogeneous materials. The results of this simulation for foamed
aluminium are presented, by demonstrating the calculated elastic-plastic behavior of
a sample. A 3D density mapping which was calculated with an averaging volume of
5 x 5 x 5 mm3 was used in this finite element simulation. The detailed modeling has

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X-ray tomography in material science

been described in [KRI]. Fig. 12.8b shows the distribution of the equivalent plastic
strain [HIB 98] occurring on the sample's surface, which was observed in the
experiment.
The calculated maximum strain is in the same position as observed in the
experiment by optical recording (Fig. 12.8a). The capability of the 3D model
enables to follow the forming of deformation bands in the interior of the sample too.
The calculated 3D plastic strain field for this sample is given in Fig. 12.9. Four
stages, showing the growth of deformation bands, are depicted in this figure by
indicating the regions having more than 1% equivalent plastic strain.

Figure 12.9. Simulated 3D propagation of plastic regions in the interior of the sample A at
a) 0.7%; b) 1.0%; c) 1.23% and d) 1.5% overall strain. Direction x is the compression
direction

Acknowledgements
The authors gratefully acknowledge: the provision of ALULIGHT samples by
Leichtmetall-Kompetenzzentrum Ranshofen (A) and Slovak Academy of Science,
Bratislava (SK); the admission to use CT at the Department of Radiology, Division
of Osteoradiology, University of Vienna (A) and the Ferderal Institute for Materials
Research and Testing, Berlin (D). The work was funded by the Austrian Ministry of
Science and Transport.

Determination of local mass density distribution

175

12.6. References
[ASH 99] ASHOLT P., "Aluminium Foam Produced by the Melt Foaming Route Process Properties and Applications", MetFoam99 a>, p. 133-140, 1999.
[BAM 97] "Computertomographie", Leaflet, Federal Institute for Materials
Research and Testing, Berlin (Germany), 1997.
[BAU 99] BAUMGARTNER F., GERS H., "Industrialisation of P/M foaming
process", MetFoam99 a>, p. 73-78, 1999.
[COR 99] CORNELIS E., KOTTAR A., SASOV A., VAN DYCK D., "Desktop X-ray
micro-tomography for studies of metal foams", MetFoam99 a), p. 233-240, 1999.
[COP 94] COPLEY D., EBERHARD A., MOHR A., "Computed Tomography Part I :
Introduction and Industrial Applications", Journal of Materials, vol. 46, no 1, p.
14-26, 1994.
[DAX 99] DAXNER T., BOHM H.J., RAMMERSTORFER F.G., "Influence of microand meso-topological properties on the crash-worthiness of aluminium foams",
MetFoam99 a>, p. 283-288, 1999.
[DEG] DEGISCHER H.P., DOKTOR M., PRADER P., "Assessment of metal matrix
composites for innovations - a Thematic Network within the 4th EUframework", Euromat 99 (to be published).
[DEG 99] DEGISCHER H.P., KOTTAR A., "On the Non-Destructive Testing of
Metal Foams", MetFoam99 a), p. 213-220, 1999.
[EVA 99] EVANS A.G., HUTCHINSON J.W., "Mutifunctionality of Cellular Metal
Systems", MetFoam99 a>, p. 45-56, 1999.
[FOR 98] FOROUGHI B., "Study of cellular deformation of Al-Foam under
Compressive Loading", Junior Euromat, 1998.
[GIB 97] GIBSON L.J., ASHBY M.F., Cellular Solids : Structure and Properties,
2nd Ed., Cambridge University Press, 1997.
[GRO 99] GROTE F., SCHIEVENBUSCH A., "Characterization of cast and
compressed foam structures by combined 2D-3D analysis", MetFoam99 a), p.
227-232, 1999.
[HIB 98] HIBBIT, KARLSSON and SORENSON INC., HKS ABAQUS/Standard
user manual, Version 5.8, 1998.
[HOP 99] HOPLER E., SCHORGHUBER F., SIMANCIK F., "Foamed aluminium
cores for aluminium castings", MetFoam99 a>, p. 79-82, 1999.
[KRE 99] KRETZ R., HOMBERGSMEIER E., EIPPER K., "Manufacturing and
testing of aluminium foam structural parts for passenger cars demonstrated by
example of a rear intermediate panel", MetFoam99 a>, p. 23-28, 1999.
[KRI] KRISZT B., FOROUGHI B., KOTTAR A., DEGISCHER H.P., "Mechanical
Behavior of Aluminium Foam Under Uniaxial Compression ", Euromat 99 (to be
published).
[KRI 99a] KRISZT B., KOTTAR A., DEGISCHER H.P., "Strukturanalyse von
geschaumten
Aluminium
mittels
Computertomographie",
Metalle/Werkstoffwoche 98, Symposium 8, Ed.: R. Kopp, Bd. 6, p. 687-692,
Wiley-VCH, 1999.

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[KRI 99b] KRISZT B., FOROUGHI B., FAURE K., DEGISCHER H.P., "Deformation
behavior of aluminium foam under uniaxial compression (a case study)",
MetFoam99 a), p. 241-246, 1999.
[MEP 96] "Alulight", Leaflet, Mepura Ges.m.b.H., Ranshofen/Austria, 1996.
[MIY 99] MIYOSHI T., ITOH M., AKIYAMA S., KITAHARA A., "Aluminuim Foam,
'ALPORAS': The Production Process, Properties and Applications",
MetFoam99 a>, p. 125-132, 1999.
[SEE 99] SEELIGER H.-W., "Application Strategies for Aluminum-Foam-Sandwich
Parts (AFS)", MetFoam99 a>, p. 29-36, 1999.
[SIM 99] SIMANCIK F., MINARIKOVA N., CULAK S., KOVACIK J., "Effect of
foaming paramters on the pore size", MetFoam99 a\ p. 105-108, 1999.
a)

Metal foams and porous metal structures, International conference, 14th-16th


June 1999, Bremen (Germany), Ed.: J. Banhart, M.F. Ashby, N.A. Fleck

Chapitre 13

Modelling of porous materials evolution

By providing 3D images of the micro-geometry, synchrotron micro-tomography


is offering huge possibilities to porous materials evolution modelling. Through three
examples, reservoir rock diagenesis, carbon-carbon composite densification and
ceramics sintering, this text illustrates those possibilities and puts into evidence the
need of a strong theoretical framework. The volume averaging method is succinctly
presented in the case of pressure solution in sandstone reservoirs. The fundamental
concept of Representative Elementary Volume is introduced. Various problems
specific of the considered materials are described and solutions to be used during
the acquisition or in post-processing are outlined.

13.1. Introduction
Understanding the evolution with time of natural or artificial porous materials is
essential for many applications. In this paper, three examples that are presently
studied within the research group CM3D* from Bordeaux, will be considered:
- mineral diagenesis of reservoir rocks for oil exploration and production,
- carbon/carbon (C/C) composites elaboration by vapour-phase densification of
carbon-fibre preforms for thermostructural materials production,
- sintering of advanced ceramics with controlled porosity distribution for
mechanical properties enhancement (strength and toughness).
In porous media physics the concept of "change of scale" is fundamental. The
common objective of all the methods used to perform the change of scale (volume
averaging, homogenisation, etc...) is to move from the local scale (the pore scale for
the cases considered here) to a larger one where the porous material behaves as an

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equivalent continuous material characterised by effective properties. In this paper


we will only make use of the volume averaging method.
At the local scale everything is known; the equations and the associated
boundary conditions governing the physical phenomena, the values of the physical
parameters appearing in those equations and the geometry. Applying the change of
scale operator to the problem defined at the local scale will make the equations of
the large scale physics emerge. The effective properties appearing in those equations
can be calculated from solutions of differential problems (eventually integrodifferential) stated at the local scale: the closure problems. Furthermore some
methods, like volume averaging, provide conditions that must be verified to insure
that the change of scale is possible. Depending on the treated problem, those
conditions might be more or less difficult to verify, as illustrated by the three
examples examined here.
Mineral diagenesis of reservoir rocks is an evolution process for which the
above-cited conditions are easily verified. Indeed, it is a very slow process that takes
place within very large domains that are rather homogeneous. In this case the
change of scale puts into evidence an evolution governed by physical phenomena at
the pore scale but having a kinetics directed by fluxes at the large scale (fluid and
mater fluxes).
For C/C composite elaboration, the change of scale might be difficult if the size
of the sample is too small with respect to the characteristic dimensions of the textile
architecture or if the characteristic time of the chemical reactions responsible for the
densification is too short. Practically, this last case is avoided because it produces
reaction fronts and heterogeneities that drastically reduce the mechanical properties.
For large enough samples, the change of scale is possible and all the remarks made
for mineral diagenesis are valid. For small samples, direct simulation is still possible
but one cannot define effective properties intrinsically related to the porous material.
In particular, the equivalent properties would be affected by the boundary
conditions applied at the "large" scale.
In the case of sintering, particles are very small and the conditions for the change
of scale are generally easily verified. Evolution, i.e. sintering, is caused by diffusion
within the solid phase. This diffusion is governed by the local curvature of the
interface and the kinetics is controlled by large-scale parameters, like temperature
for instance. The corresponding coupling is weaker than for mineral diagenesis
because those parameters are constant at the local scale (it is not the case for the
local fluid flow for instance).
Because of the differences pointed out above, the modelling strategy will slightly
differ for each of these three examples. Nevertheless, a good characterisation of the
3D micro-geometry is always essential. For this purpose, computed microtomography (CMT) is a very well adapted tool, as it will be shown in the following
paragraphs. In the first one, the volume averaging method is succinctly introduced

Modelling of porous materials evolution

179

through its application to an important mechanism of mineral diagenesis: pressure


solution. The usefulness of CMT will appear clearly in this example and will be
reinforced by the two ensuing paragraphs where preliminary but encouraging results
will be given for C/C composites and ceramics sintering.
13.2. Evolution of sandstone reservoir rocks by pressure solution
Rock deformation by pressure-solution is due to the variation of the chemical
potential with stress; in some conditions, the stress concentration at the grain-tograin contacts (Figure 13.1) induces an accelerated dissolution of minerals in these
zones and a precipitation of those minerals at interfaces under low stress. This
microscopic mechanism is the origin of one of the three most important deformation
modes of earth crust. More practically, research of a better understanding of this
mechanism is justified by the fact that in deep hydrocarbon exploration (more than 3
km), compaction and cementation of the quartz matrix is the main cause of error in
sandstone hydrocarbons reservoir quality evaluation.
In the literature there are two main theoretical models for pressure solution:
- the free-face pressure solution model adopted in this work, where dissolution
occurs at the periphery of the contacts. This process leads to a reduction of the
contact area, plastic deformation and finally collapse of this zone.
- the water-film diffusion model where dissolution is supposed to occur within
the grain-to-grain contacts. In this model, the existence of a thin water film able to
support a high normal effective stress is necessary. Dissolved species are transported
from the film to pore space by diffusion.
13.2.1. Local equations and volume averaging
The pore scale configuration is pictured on Figure 13.2. The two phases, the
fluid P and the solid a, are in contact at Apa their interface. A dissolved compound a
is moving within the fluid phase by diffusion (to simplify the demonstration,
convection is not considered here). The compound a can react with the solid phase
at the interface. Equations [1] and [2] govern the transport at the local scale.
- = V.(DVCfl)

in the p phase

- npo . (DVCa) = k (Cfl - C*)

on the interface A po

[1]
[2]

where Ca is the concentration of the compound a in the p phase, D its molecular


diffusivity, t the time, k the reaction rate coefficient and C* the equilibrium
concentration. C* is a function of pressure, temperature and stress.

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X-ray tomography in material science

Figure 13.1. Tangential stress concentration in


a simple spheres packing: all the zones having a
stress value greater than 20% of the maximum
are near the contacts

Figure 13.2. Local scale geometry and


notations used in the text

The intrinsic phase average of the concentration is defined by:


[3]

where V is the Representative Elementary Volume. Applying this operator to


equations [1] and [2] and using the spatial averaging theorems [WHI 99], the
following equation is obtained:

where GRAY's decomposition (equation [5]) of the local concentration has been
used to distinguish the smooth part, the averaged concentration linked to transport at
the large scale, from the spatial deviation produced by the reaction at the interface
and by the interface itself.

In a similar way the equilibrium concentration is decomposed into two terms:

Modelling of porous materials evolution

181

Assuming that k is constant and introducing the specific surface av defined by:

equation [4] can now be written:

[8]

Equation [8] is still containing microscopic terms that have to be eliminated.


Following the same way as [WHI 99], it can be inferred that the spatial deviation of
the concentration can be represented by the following expression:

where f is a vector and s a scalar. Both are solutions of partial-differential problems,


called closure problems, which have to be solved at the local scale:

f mainly takes into account the effects of the micro-geometry on diffusion and s
takes into account the previous effects plus the effects of the chemical reactions on
the interface. The problems [10] are similar to the closure problems classically
obtained for diffusion-reaction in porous media, the specific effects of local stress
concentration being carried by * Indeed, this term is not an unknown for transport
equations. It is a local property of the interface that has to be calculated by solving
an almost decoupled local mechanical problem.
The transport equation at the large scale can now be written:

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where the effective diffusivity is given by [WHI 99]:

[12]

The local flux of matter can be expressed by equation [13]. A new version of the
model, taking into account the existence of water films at the grain-to-grain
contacts, is under development. When the new expression of the local flux will be
available, it will be possible to compare the evolutions predicted by both models for
the same starting geometry. In parallel, both models will be confronted to real data
( 13.2.3) looking for arguments supporting a choice between them.
13.2.2. REV size of a Fontainebleau sandstone sample
The concept of Representative Elementary Volume (REV) is central in the
change of scale theory for porous media. However there is no explicit formula for
the REV size ro, the main indication being that it has to be large enough compared to
the local scale characteristic lengths (lp, la) and small enough compared to the largescale characteristic length (L):
[14]

Using tomography data acquired at the ESRF (ID 19) for ELF-EP, the 3D microgeometry shown on Figures 13.3 and 13.4 has been reconstructed. It is the central
zone of cylindrical sample (diameter of 6 mm). The voxels are cubic (edges of 10
jam) and the complete data set comprises 256 x 256 x 256 voxels.
To estimate the REV size of this Fontainebleau sandstone sample for different
physical properties, the following numerical experiments have been performed:
- cubic volumes of different sizes have been extracted from the central region of
the complete data set;
- those volumes being considered as REV, three physical properties have been
computed:
- porosity values from the number of voxels belonging to the fluid phase,
- effective diffusivity values using equation [12] after resolution of problem
[10],

Modelling of porous materials evolution

183

-permeability values after resolution of a closure problem obtained by


volume averaging of Stokes equations [BER 95];
- the results have been plotted as functions of the volume size (Figure 13.5).

Figure 13.3. Visualisation of the solid phase


of a Fontainebleau sandstone sample

Figure 13.4. Visualisation of the fluid phase


of the same sample

Figure 13.5. Evolutions of porosity, effective diffusivity and permeability


with the size of the computational cell

Figure 13.5 is clearly demonstrating that it is possible to obtain, using CMT, 3D


images of porous samples large enough to attain the REV size for various physical
properties. 10 times the average grain diameter can be considered as a good

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X-ray tomography in material science

approximation of the size of a cubic REV for simple granular porous media. The
subsequent and complementary question is now: what is the required size for the
voxel in order to characterise correctly the fluid-solid interface? The importance of
this aspect is obvious when dealing with more complex porous media and with
coupled phenomena like in the following example.

13.2.3. An example of pressure solution evolution from the ELLON field


Among the numerous difficulties encountered when studying mineral diagenesis
of reservoir rocks, two are rather specific:
- phenomena occur at very different scales (from the pore scale -100 urn- to the
basin scale -500 km) and are strongly coupled,
- the initial state (-100 My) is not directly accessible.
Having that in mind, the Ellon field (Alwyn area, North Sea) can be considered
as exceptional. Indeed, in an early stage of its evolution this sandstone reservoir has
been drastically and quickly modified by two diagenetic events [POT 97]: first a
general and almost complete calcite cementation (porosity initially around 40% and
about 3% after cementing) and secondly a localised dissolution of the calcite cement
leading to an heterogeneous formation composed of two domains separated by sharp
fronts (Figure 13.6). During the subsequent evolution, the cemented zone remained
unchanged (Figure 13.7) and the uncemented zone has been modified by pressuresolution and quartz over-growths (Figures 13.8-9) giving an actual porosity of about
20%. Those processes mainly occurred at the pore level with small coupling with

Figure 13.6. Sandstone sample from the


ELLON field showing the interface between
the cemented (C) and the non-cemented
(NC) zones

Figure 13.7. Reconstructed section (512x512


pixels of 6.5 um) of a sample at the C-NC
interface. Black zones are pores, dark grey
zones are quartz grains and light grey zones
correspond to calcite

Modelling of porous materials evolution

Figure 13.8. Reconstructed section


(512x512 pixels of 6.5 urn) of a NC
sample. Black zones are pores and dark
grey zones are quartz grains

Figure 13.9. Reconstructed


(700x700 pixels of 1.8 urn) of
sample. Quartz overgrows are
visible. Pores are partly filled with

185

section
a NC
clearly
clay

larger scales (no water flow) and the initial state has been frozen by calcite
cementation; it is why the Ellon field is an exceptional case to study.
Examining Figures 13.7 and 13.8, it is evident that this sandstone is more
complex than Fontainebleau sandstone. Porosity is larger but spatial distribution of
this porosity is completely different. Both were rather similar quartz grains packing
at the deposit (Figure 13.7) but the diagenetic mechanisms that took place have been
different. The combination of classical CMT (Figures 13.7, 13.8) and local CMT
(Figure 13.9) seems to be a promising solution to problems where more than one
scale are relevant.

13.3. C-C
Carbon/carbon composites are well known high-performance materials for
thermostructural applications, such as rocket nozzles or aeroplane brakes, and their
market is in appreciable extension. They are usually produced either by
impregnation of a preform made of carbon fibres by pitches or mesophases or by
vapour-phase densification of the same preform [NAS 99]. Chemical Vapour
Infiltration (CVI) is a variant of the Chemical Vapour Deposition (CVD) process
involving the cracking of gaseous species (precursors) which lead to the deposition
of a solid phase on a hot substrate by heterogeneous reaction. For instance, a
mixture of hydrocarbons and hydrogen is used to obtain a pyrocarbon deposit. The
gaseous species are transported inside the preform by viscous flow or by diffusion.

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X-ray tomography in material science

In isobaric-CVI (I-CVI) low pressures are required in order to avoid diffusional


limitations and premature pore plugging. As high temperatures are required for the
heterogeneous reaction, one has to deal with transport by Knudsen diffusion (also
called Klinkenberg effect or slip flow), in addition to ordinary diffusion. The role of
porous medium transport is fundamental for the monitoring and optimisation of the
CVI process, and it may be easily understood that it depends in a rather complex
way on the preform geometry.
One of the possible ways to investigate precisely the properties of interest either
for direct use (mechanical, thermal) or for processing (permeability, diffusivity, and
specific surface...) is to obtain accurate data concerning the 3D architecture of real
fibrous preforms at various stages of densification. For this, CMT is a powerful tool
having a resolution compatible with the size of an isolated single carbon fibre (7-8
jam diameter). Furthermore, the 3D character of the method yields essential
information about the connectivity of the porous and solid phases.
It is possible, on the basis of the reconstructed 3D images where the interface
between porous and solid phases is visible, to compute the essential geometrical
properties [LEE 98] and effective transport properties (permeability [BER 95],
diffusivity and Knudsen diffusivity [VIG 95] as well as mercury penetration curves
for the porous phase [HAZ 95], thermal and electrical conductivity [QUI 93],
stiffness tensor... [POU 96]). It is also possible to perform on such images
simulations of the evolution of the microstructure under some constraints, such as
matrix deposition or infiltration, and chemical or mechanical degradation.
Images were collected at the ID 19 beam line of ESRF (European Synchrotron
Radiation Facility). The outstanding quality of the secondary beam allows to image
samples at resolutions as good as 0.8 jam. Here, a resolution of 1.8 urn has been
chosen because of the wide size of the representative elementary volume (REV).
Accordingly, the studied samples measured less than 2 mm in diameter. Even
though, it is not claimed that 2-mm width images do contain a C/C composite REV.
The problem that arises specifically when imaging C/C composites is linked to the
low absorption coefficient of C at the frequencies of use, together with the important
coherence of the beam, and the order of magnitude of the resolution. In such
conditions, the X-ray beam reveals itself much more sensitive to phase shifts than to
intensity absorption [CLO 96]. When the detector plane is placed roughly at one
centimetre behind the sample, the image obtained after reconstruction displays an
enhancement of the void-solid interface under the form of a bright-dark double
band, while the interior of both phases are of approximately the same mean grey
level (Figure 13.10). The double band is the result of an interference between the
coherent rays passing close to the interface, through both phases, one of which
(carbon) induces a phase shift.

Modelling of porous materials evolution

Figure 13.10. Image extracted from


one slice of a reconstructed 3D image

of a C/C partially densified preform


obtained by synchrotron X-ray CMT

187

Figure 13.11. 3-D rendering of the treated


sample. The circles focus on rounded fibre

tips

If phase contrast allows the immediate production of human-understandable


images, it is not suited for subsequent computations. Nevertheless, the important
information is contained inside the phase-contrast image, since for most of the
interface, the bright layer is always on the same side of the interface (e.g. the fluid
side) and the dark layer lies always on the other. A variety of methods may be
designed to answer to the following question: for any point (voxel) of the
discretized image, what is the phase it lies in?
An image treatment sequence has been designed to extract pertinent information
from C/C tomographs displaying a phase contrast structure enhancing the void/solid
interface. After having applied the algorithm, the image is fully binary. However,
some closed porosity remains, which is removed using a classical percolation
algorithm. It is also possible to use a mask and recover the exact grey-level values
of the pixels that touch the interface, in order to use subsequently accurate surface
tessellation procedures.
Phase contrast images, after this treatment, are now suited for subsequent
physico-chemical computations at pore-scale. As an example, the image treatment
suite has been applied to a 200x200x50 voxels sub-sample of a tomography taken at
2 urn spatial resolution (Figure 13.10). The result is shown on Figure 13.11.

13.4. Ceramics sintering


Sintering is known as the process allowing the transformation of a powder into a
compact material presenting at least some mechanical properties. The widest used
model of solid state sintering considers the ceramic as ideal packing of facetted

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X-ray tomography in material science

grains with its associated porosity situated on the grain edges [COB 61]. In this
representation the process is completely defined by two parameters: the grain size
and the density. In real systems, grain size distribution and initial packing
inhomogeneities lead to internal stress gradients originating differential
densification phenomena (constrained densification). Pore evolution should be
considered and analysed independently of density and grain size changes.
Sintering of a powder deposited on a dense and rigid substrate (Figure 13.12) of
the same chemical nature, is an interesting model to investigate constrained
sintering at the macroscopic scale.

Figure 13.12. Schematic of (a) a powder sintered without constraints (free sintering)
(b) a powder layer sintered on a rigid substrate (constrained sintering)

A new phenomenological model of solid state sintering has been developed. In


this model, pore size is explicitly considered [LET 94]. This parameter can be
determined by image analysis of polished sections permitting a correct description
of free and constrained sintering. If macroscopic shrinkage behaviour is correctly
obtained, development of localised microstructural phenomena cannot be taken into
account in this framework. For instance, large pore defects present in the compact
can evolve and lead to de-sintering phenomena [LAN 89, HEI 94]. So, improvement
of sintering modelling needs more detailed analyses of densifying phenomena,
especially at a lower scale. It requires a more accurate description of porosity and
CMT associated to 3D reconstruction techniques looked as the up to date technique
to investigate pore structures in real ceramic samples at the appropriate scale (grain
scale).
Experiments were carried out on a well-known ceramic material, i.e. A12O3. The
powder was a pure alumina powder (Baikowski DF 1200) and the average grain size
was estimated to be 4 urn. A reference sample (initial state) was obtained by cold
pressing this powder and then by sintering it at low temperature (1300C, 1 min.) in
order to get a minimum of cohesion without any significant change of the
microstructure. The role of a constraint on the sintering and on the development of
the porosity was investigated by comparing free sintered samples (powder naturally
sintered) to constrained samples (powder layer deposited on a sapphire, i.e. dense
alumina, substrate and sintered). The sintering temperature was fixed to 1600C and

Modelling of porous materials evolution

189

the sintering times were 15 min, 30 min and 60 min. Due to the large initial grain
size, relative density of the free samples remained low and was 62.5 %, 67 % and
68 % respectively. The constrained samples were assumed to exhibit even lower
relative densities [LET 94].

Figure 13.13. 2D sections of alumina ceramics samples sintered during 30 min. at 1600C
(image size: 512x512 pixels, pixel size: 0.9 /jm2). Free sintering on left and constrained
sintering on right (on left is the sapphire substrate)

Figure 13.14. 60 min. free sintered ceramic. Formation of a denser shell around a large pore
is observed while no change in density can be noticed along the crack. The first effect may be
attributed to differential sintering (localised constrained sintering phenomenon) as it has
been predicted and observed in 2D within ceramic and composites [LAN 96]. Image
processing analysis tools will be used to obtain 3D information on the micro structure around
the pore to relate them to previous studies

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X-ray tomography in material science

X-ray computerised micro-tomography of these alumina ceramics were


performed on ID 19 beamline. All specimens were scanned at the two lowest
resolutions (0.8 jam and 1.8 jam), using a monochromatic beam (17.5 keV) obtained
using a bent multilayer device (strong decrease of the acquisition time). A control
section was numerically reconstructed for each sample. Unfortunately, as it can be
seen on Figure 13.13, phase contrast artefacts related to the low grain size (large
number of solid-gas interfaces) superimposed themselves on the grey level image,
preventing an easy separation of the two phases (pore/matter) at the micrometer
scale.
Nevertheless, numerical analysis of the 3D signal is planned to extract average
density fields close or far from the substrate. Furthermore, some samples reveal
interesting features justifying an deeper exploration: for example, a free sintered
specimen (60 min.) shows two types of internal defects producing different
microstructural modifications (Figure 13.14).
13.5. Conclusions and forthcoming works
The three examples presented in this paper illustrate the huge possibilities
offered by CMT to porous materials evolution modelling. Recent developments
(phase contrast imaging, local tomography) increased notably the quality of the data
that can be obtained and extended the domain of application to new fields.
CMT is opening very promising perspectives but one must keep in mind that,
because of the amount of data that is generated, an efficient use of this tool requires
consequent intellectual and material investments. CM3D* is orienting its activities
towards those goals: volume averaging is providing the theoretical framework for
data exploitation, new codes are developed for data treatment and physical
properties computation, new computing facilities will be available in near future
(next camera will generate images of 2048 x 2048 pixels!!!).
If data acquisition has been rather simple for rocks ( 13.2), it has not been the
case for C/C composites and ceramics ( 13.3 and 13.4). More elaborated
acquisition procedures are required there. Development and testing of those
procedures will be possible only if the collaboration between users and beamline
staff continues.

Acknowledgement
All the micro-tomography data has been acquired at the ESRF (European
Synchrotron Radiation Facility, Grenoble, France) on the ID 19 beamline. 3D
* CM3D is a thematic research group from Bordeaux (Caracterisation et Modelisation 3D de 1'evolution
des milieux poreux reels. Contact: bernard@icmcb.u-bordeaux.fr).

Modelling of porous materials evolution

191

reconstructions have been performed using VOLUMIC, a code developed by


CREATIS (UMR5515, CNRS-INSA Lyon).

13.6. References
[BER 95] BERNARD D., "Using the Volume Averaging Technique to Perform the
First Change of Scale for Natural Random Porous Media", Adv. Methods for
Groundwater Pollution Control, Gambolati & Verri Eds., p. 9-24, Springer
Verlag, New York, 1995.
[CLO 96] CLOETENS P., BARRETT R., BARUCHEL J., GUIGAY J., SCHLENKER
M., "Phase Objects in Synchrotron Radiation Hard-X-ray Imaging", J. Phys. D :
Appl. Phys., vol 29, p. 133-146, 1996.
[COB 61] COBLE R.L., "Sintering Crystalline Solids. I. Intermediate and Final State
Diffusion Models", J. Appl. Phys., vol. 32, p. 787-792, 1961.
[HEI 94] HEINTZ J.M., SUDRE O., LANGE F.F., "Instability of Polycrystalline
Bridges than Span Cracks in Powder Films Densified on a Substrate", J. Am.
Ceram. Soc., vol. 77 [3], p. 787-91, 1994.
[LAN 89] LANGE F.F., "Powder Processing Science and Technology for Increased
reliability", J. Am. Ceram. Soc., vol. 72 [1], p. 3-16, 1989.
[LEE 98] LEE S-B., STOCK S.R., BUTTS M.D., STARR T.L., BREUNIG T.M.,
KINNEY J.H., "Pore Ggeometry in Woven Fiber Structures: 0/90 Plain-Weave
Cloth Lay-up Preform", J. Mater. Res., vol 13(5), p. 1209-1217, 1998.
[LET 94] LETULLIER P., Ph.D. thesis, n1247, University Bordeaux I, 1994.
[NAS 99] NASLAIN R., "Key Engineering Materials", CSJ Series - Publications of
the Ceramic Society of Japan vol. 164-165, Switzerland, Trans Tech Pub., p. 38, 1999.
[HAZ 95], HAZLETT R.D., "Simulation of Capillary-Dominated Displacements in
Microtomographic Images of Reservoir Rocks", Transport in Porous Media, vol
20(1-2), p. 21, 1995.
[QUI 93] QUINTARD M., WHITAKER S., "Transport in Ordered and Disordered
Porous Media: Volume-Averaged Equations, Closure Problems, and
Comparison with Experiment", Chem. Eng. Sci., vol 48, p. 2537, 1993.
[POT 97] POTDEVIN J-L., HASSOUTA L., "Bilan de matiere des processus
d'illitisation et de surcroissance de quartz dans un reservoir petrolier du champ
d'Ellon (zone Alwyn, Mer du Nord)", Bull. Soc. Geol. France, vol 168 (2), p.
219-229, 1997.
[POU 96] POUTET J., MANZONI D., HAGE-CHEHADE F., JACQUIN C.G.,
BOUTECA M.J., THOVERT J-F., ADLER P.M., "The Effective Mechanical
Properties of Reconstructed Porous Media", Int. J. Rock. Mech. Min. Sci. &
Geomech. Abstr., vol 33(4), p. 409-415, 1996.
[VIG 95] VIGNOLES G.L., "Modelling Binary, Knudsen, and Transition Regime
Diffusion inside Complex Porous Media", J. de Physique IV, vol 65(1), p. 159166, 1995.

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[WHI 99] WHITAKER S., The Method of Volume Averaging : Theory and
Applications of Transport in Porous Media, Theories and Applications of
Transport in Porous Media, V. 13, Kluwer Acad. Pub., Dordrecht, 1999.

Chapitre 14

Study of damage during superplastic


deformation

Superplastic deformation of some industrial alloys can induce damage, leading to


premature fracture. This damage by cavitation is generally divided in three main
steps: nucleation of the cavities, their growth and finally coalescence between
cavities. Up to now, this latter point has been poorly documented due to a difficulty
to get reliable data with conventional techniques of 2D characterisation of damage.
In this work, high resolution X-ray micro-tomography is used as a technique of
quantification of the population of cavities due to the ability to obtain 3D
information and a particular attention is given to the coalescence process. In the case
of a superplastically deformed Al-Mg alloy, it is shown that coalescence occurs in a
large strain interval and that just before fracture, most cavities are connected
together. A parameter is proposed to quantify the coalescence process.

14.1. Introduction to damage in superplasticity


Superplasticity is frequently defined as the ability for a polycrystalline material
deformed at high temperature, to reach elongations to fracture at least one order
larger than those obtained in conventional plasticity. Elongations larger than 1000 %
may be obtained in the case of metallic alloys. A sample of aluminium alloy
deformed in superplastic tensile conditions is presented in figure 14.1.
Superplasticity requires both specific experimental (temperature and strain rate)
and microstructural conditions. It is associated to the predominance of grain
boundary sliding (GBS) as the main mechanism of deformation. The movement of
grains during superplastic deformation is illustrated by figure 14.2, which displays a

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X-ray tomography in material science

SEM micrograph of a Pb-Sn alloy of which a marker line was drawn on the polished
surface before testing [DUP 97]. After deformation, the marker line inside the grains
is not significantly modified whereas gaps are detected through the grain boundaries,
which indicates that movements of grains are predominant.

Figure 14.1. Example of an aluminium alloy deformed in superplastic conditions

In consequence, superplastic properties are promoted by a reduction of the mean


grain size of the material. For metallic alloys, grain sizes of about 10 microns are
generally needed to exhibit superplasticity at strain rates compatible with industrial
processes. From a rheological point of view, superplastic deformation occurs under
very moderate flow stresses (typically less than 10 MPa) and is associated with a
large plastic stability resulting from the high value of the strain rate sensitivity
parameter m, deduced from the conventional viscoplastic law between the flow
stress a and the strain rate e :

m
a = Ke

[1]

Superplastic forming (SPF) is to day an industrial forming process to produce


components with complex shapes. It concerns particularly titanium and aluminium
and major applications have been developed in the aeronautical industry.
However, in the case of single-phase materials, like aluminium alloys,
superplastic deformation induces damage through the microstructure, leading to
premature fracture but also to a reduction of service properties of the alloy after
SPF. Such damage can be observed on figure 14.3, which shows a SEM micrograph
of a superplastically deformed aluminium-magnesium alloy [LAR 98].
To day, industrial SPF overcomes this difficulty by forming components under
superimposed pressure, which inhibits the damage process but increases the cost and
limits the maximum size of the components to be shaped. In consequence, a way for
the promotion of SPF in the future, is the ability to superplastically form aluminium
alloys under atmospheric pressure. Previous works have demonstrated that some

Study of damage during superplastic deformation

195

benefits in terms on damage sensitivity can already be obtained by appropriate heat


treatments before testing [BLA 96]. Nevertheless, a better understanding of the
damage process in superplastic conditions appears as a key parameter for the future
development of SPF.

Figure 14.2. SEM micrograph showing


the predominance ofGBS in superplasticity

Figure 14.3. Example of strain-induced


cavitation when an aluminium alloy is
superplastically deformed

The damage process induced by superplastic deformation is usually divided in


three main steps: nucleation of the cavities, growth and coalescence leading to
fracture.
Cavity nucleation is attributed to microcracking or vacancy agglomeration and is
mainly located at triple junctions or near intergranular particles through the alloy
[RAJ 77], as a result of stress concentrations generated by GBS.
Cavity growth is generally interpreted thanks to models initially developed for
materials deforming in creep conditions [RIC 69, HAN 76, CHO 86]. For small cavities,
diffusion is expected to contribute predominantly to cavity growth whereas for
larger cavities, it is considered that growth is controlled by plastic deformation of
the matrix surrounding the cavity. In this case, the variation with strain 8 of the
volume V of a cavity is given by [HAN 76]:
V = V0 exp(r|ge)

[2]

with V0 a constant and r|g the cavity growth parameter. Some expressions of the
parameter r)g have been proposed in the past, in particular as a function of the
rheology of the matrix [PIL 85]. However, it must be underlined that, since these
models of cavity growth were initially developed for alloys deforming in creep
conditions, they do not take into account GBS, although it is the predominant
mechanism of deformation in superplasticity.

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X-ray tomography in material science

Despite its crucial link with fracture, the coalescence process between growing
cavities has been poorly documented [STO 83, STO 84]. Very limited experimental
data have been reported and few models were proposed. Moreover, these models are
generally based on very strong hypotheses about the spatial distribution of the
cavities through the microstructure and the criteria of coalescence. In particular, they
assume that the cavities are randomly distributed through the microstructure and that
all the cavities have a spherical shape and the same diameter. Lastly, coalescence is
supposed to occur only when cavities impinge.
It is expected that such assumptions are not experimentally satisfied. As already
mentionned, many cavities are preferentially nucleated near grain boundary
particles, which are not randomly distributed through the microstrucutre. Moreover,
the shapes of large cavities after superplastic deformation can be very irregular, as it
is illustrated by figure 14.4, which shows an optical micrograph of the fracture zone
for a superplastically deformed aluminium alloy. This irregularity of the shape of the
cavities is attributed to GBS, which is the main mechanism of deformation in
superplasticity.
Experimental data about strain-induced damage in superplastic conditions are
frequently quantified from the variation with strain of the cavity volume fraction Cv.
Figure 14.5 displays such a variation of Cv with s in the case of superplastic
deformation of Al-Mg alloy. The cavity volume fraction continuously increases with
strain and after a period of apparent incubation in which the level of cavitation
remains limited (less than 1 %), a sharp increase is obtained and the cavity volume
fraction, when fracture occurs, is generally high in the case of superplastic alloys,
typically more than 10 %.

Figure 4. Optical micrograph of the


fracture zone after superplastic
deformation of an Al-Li alloy

Figure 14.5. Variation with strain of cavity


volume fraction Cv during superplastic
deformation of an Al-Mg alloy

Study of damage during superplastic deformation

197

The variation with strain of Cy is frequently rationalised according to:


Cv = Cvo exp(Tiapps)

[3]

where CVo is a constant and r\app the apparent parameter of cavitation sensitivity. The
logarithm of experimental values of Cv is plotted as a function of strain and in most
cases, a straight line can be roughly obtained in a relatively large strain interval,
which allows the measurement of a slope r|app.
The corresponding value of r)app is then compared to those deduced from the
cavity growth models. Indeed, these models predict also an exponential variation of
the volume of the cavity with strain under two main assumptions : firstly, growth is
controlled by plastic deformation of the matrix which surrounds the cavity;
secondly, the number of cavities is roughly constant in the corresponding strain
interval.
The differences between such predictions and r)app are frequently discussed in
detail and sometimes interpreted in terms of continuous nucleation of cavities during
deformation.
Despite the fact that these assumptions (in particular the constancy of the number
of cavities per unit volume in a large strain interval) appear very questionable, it is
difficult to draw conclusions with data deduced from conventional 2D techniques of
characterisation.

14.2. Usual techniques of characterisation


Two techniques of characterisation are generally used to quantify strain-induced
cavitation in superplasticity: variation of relative density of the alloy and
quantitative metallography from polished sections. Both techniques have some
notable disadvantages.
Density variation measurements are relatively easy to perform and allow
detection of low cavity volume fraction, typically less than 0.01 %, but the
measurements appear doubtful for large cavity volume fraction. Indeed, for such
levels of cavitation, some cavities may connect with the outer surfaces of the
specimen and artificially modify the results, leading to an apparent slackening of the
cavitation increase with strain. Moreover, some precautions must be taken to
systematically check the possible variation of density of the alloy during an heat
treatment similar to that undergone by the sample during high temperature
deformation [VAR 89]. Finally, this technique is a global one since only Cv can be
measured whereas no data about the population of the cavities (number, size...) are
available.

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X-ray tomography in material science

By quantitative metallography, such data about the population of cavities can be


obtained but it requires to polish the surfaces to observe, which can modify the
apparent size and shape of the cavities, particularly in the case of aluminium alloys.
Moreover, as already mentioned, irregular shapes of cavities can be detected in
superplastically deformed alloys, as shown in figure 14.4. In such conditions, the
study of cavity coalescence from two-dimensional data appears very hazardous.
From these remarks, it appears very interesting to use a technique of threedimensional (3D) characterisation of the population of cavities in a superplastically
deformed alloy. In consequence, high resolution X-ray micro-tomography seems to
be a very promising technique since it can provide three-dimensional images of the
bulk of materials [HIR 95, BUF 99].

14.3. Experimental procedure


Tomography experiments were carried out at the ID 19 beamline of the
European Synchrotron Radiation Facility (ESRF). ID 19 is devoted to highresolution imaging. The beam energy was 17.5 keV. The samples were set on a
goniometer allowing a precise positioning of the sample. A scan of the samples
consisting of the recording of 800 two-dimensional radiographs was performed
during a 180 rotation around the vertical axis. Those radiographs were recorded on
a 1024 x 1024 CCD camera developed at ESRF [LAB 96]. The average exposure time
for a radiograph was 0.3 s and the whole scan lasted about 10 minutes. The pixel
size of the camera was 2x2 (irn2. The detector was set 3 mm behind the sample. For
each sample, the investigated volume was approximately 0.6 x 0.6 x 0.6 mm3,
knowing that for large strains, the final thickness of the sheet after SPF in industrial
conditions, may be less than 1 mm. In a first step of characterisation, only cavities
with a volume larger than 10 voxels were taken into account. It is the reason why the
interpretation of the results deduced from X-ray micro-tomography were focused on
the coalescence process, in order to deal with relatively large cavities.
The studied material was an aluminium-magnesium alloy (Al - 4.2Mg - 0.7Mn 0.2Fe - 0.1 Cr, wt %). The alloy was provided in the form of sheets of 2.5-mm
thickness. The mean grain size was about 10 urn. The superplastic properties of this
alloy have been investigated in detail [MAR 99] and the cavitation behaviour in
superplastic conditions was studied by deforming the alloy at 525C and 10"4 s"1 at
different strains. In these conditions of deformation, the elongation to fracture was
about 400 %. Density variation measurements were performed on a micro-weighing
machine allowing detection of relative density variation close to 0.005 % and limited
quantitative metallography on polished sections were also carried out on SEM
micrographs.

Study of damage during superplastic deformation

199

14.4. X-ray micro-tomography results


Figure 14.6 shows a 2D section of the superplastically deformed alloy, deduced
from X-ray micro-tomography data. Well-contrasted sections are obtained, resulting
from the difference of X-ray attenuation between the cavities (in dark) and the
aluminium alloy.

Figure 6. 2D section showing good contrast


between cavities and the aluminium alloy.

Figure 7. Comparison of the variations


with strain of Cv between X-ray microtomography and density variation
measurements

Figure 14.7 compares the variations with strain of the cavity volume fractions
deduced from density variation measurements and from X-ray micro-tomography. A
good correlation between the results obtained by these two independent techniques
is found. It confirms the validity of X-ray micro-tomography as a fruitful technique
of quantification of strain-induced cavitation in superplastic alloys.
Moreover, this technique allows to get information about the population of
cavities as illustrated by figure 14.8, which displays the reconstructed image of the
spatial distribution of the cavities after an elongation of about 170 %. This condition
corresponds to a mean cavity volume fraction of about 1 %. For this elongation,
most cavities are isolated through the microstructure, although some connections
between cavities can be detected.

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X-ray tomography in material science

Figure 14.8. Reconstructed image of the population of cavities after


an elongation of about 170% (Cv 1 %)

14.5. Quantification of the coalescence process


As already mentioned, the increase with strain of the cavity volume fraction is
frequently described according relation [3]. A value of the parameter r|app is thus
estimated and compared to those predicted by the cavity growth models. In the case
of the investigated alloy, a value of r|app close to 5 was obtained which is agreement
with previous works (IWA 91, FRI 96). Nevertheless, this value is significantly larger
than the values predicted by cavity growth models (typically close to 2 in this case).
This difference is generally attributed to continuous nucleation of cavities during
strain, resulting in an apparent increase of the value of r\. To confirm this
interpretation, the variation with strain of the number of cavities nA per unit area is
frequently determined from SEM micrographs. This work was carried out in the
case of the studied alloy [LAR 98] and an increase of nA with strain was obtained in
the investigated strain interval.
From the 3D data obtained in tomography, it is also possible to estimate the
variation with strain of the apparent number of cavities par unit area for a given
family of planes (as it is shown in figure 14.6). This estimation has been performed
in the case of the investigated alloy and an increase of this apparent number of
cavities per unit area is obtained whatever the planes of observation. Consequently,
these results have confirmed those deduced from SEM micrographs, even if, for a
given strain, the values of nA may depend on the technique of characterisation: nA is
lower in the case of the tomography results, which can be attributed to the fact that
small cavities (i.e. equivalent diameter smaller than 5 urn) have not be taken into
account in the treatment of the X-ray tomography data.

Study of damage during superplastic deformation

201

However, as already mentioned, when strain is increased, the cavities become very
irregular and consequently, the interpretation of the associated variation of nA may
be delicate. It appears more reliable to study the variation with strain of the number
of cavities nv per unit volume.
Figure 14.9 shows the variation with elongation of the number nv of detected
cavities per unit volume. Between elongations from 200 % to more than 400 %, a
continuous decrease of nv is obtained, which points out the extent of the coalescence
process. The data obtained for an elongation close to 150 % has to be considered
with caution since it must be kept in mind that only cavities with a volume larger
than 10 voxels were taken into account in the procedure of counting. It means that
an apparent increase of ny with strain can be partially attributed to cavity growth.

Figure 14.9. Variation with elongation of the number of cavities per mm

From the results presented in figure 14.9, it can be concluded that the effects of
strain on the variation of nv and nA (deduced from SEM observations or from X-ray
micro-tomography data) are contrary. These differences between the dependencies
on strain of nv and nA confirm the fact that a the usual interpretation of the cavitation
processes from 2D characterisations is very hazardous.
The variation with strain of the number of cavities per unit volume is a first
approach to quantify the coalescence process. However, this parameter gives only
limited indications about the mechanism of coalescence. A way to get additional
data is to follow the variation with testing conditions of the largest cavity in the
investigated volume, since it may give indication about the extent of connection
between cavities through the microstructure. In this view, figure 14.10 displays a 3D
observation of the largest cavity obtained after an elongation of about 400 % for
which Cv is about 14.5 %. It can be seen in figure 10 that the largest cavity admits a
very irregular shape and extends beyond the studied volume. Moreover, this cavity

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X-ray tomography in material science

corresponds to about 75 % of the total cavity volume fraction, which indicates that
most cavities have connected together.
From this conclusion, a coalescence parameter CP can be defined, according to:
CP =

volume of the largest cavity

-x 100
total volume of cavities

Figure 14.10. Reconstructed image of the largest cavity through the


microstructure after an elongation of about 400 %

Figure 14.11 shows the variation with strain of the coalescence parameter CP.
The value of this parameter remains limited up to a strain of about 1.2 and then
sharply increases. This strain corresponds, for the associated conditions of
deformation (525C and 10"4 s"1) to a value of Cv close to 5 %.
These results confirm the importance of the coalescence process during
superplastic deformation since they point out that coalescence occurs in a large
domain of strain. It must be kept in mind that between 8 1.2 (i.e. an elongation
230 %) and fracture, which is obtained after an elongation 400 %), the mean
cavity volume fraction Cv increases roughly from 5 % to 15 %. Consequently, it
indicates that coalescence takes place not only in a large strain interval but also in a
large domain of Cv.

Study of damage during superplastic deformation

203

Moreover, from figures 14.9 and 14.11, it seems that two domains of coalescence
may be identified. In a first step (for strains between 1.0 and 1.3), a significant
reduction of nv is obtained whereas the value of the coalescence parameter remains
low. It means that a large number of cavities coalesce but that the volume of the
largest cavity through the volume remains comparable to the mean cavity volume of
the cavities. It is expected that this step of coalescence is associated to a nonuniform spatial distribution of cavities. Indeed, as already mentioned, cavity
nucleation takes place preferentially near intergranular particles which are not
uniformly dispersed in the alloy, as a result of the thermomechanical process
undergone by the material. Indeed, previous work has shown that, as a result of the
thermomechanical process undergone by the material, some stringers of second
phase particles are present in the studied alloy [LAR 98]. In a second step (when 8 >
1.3), the value of CP increases sharply. It indicates that a large fraction of cavities
connect together, leading to one cavity which concentrates the coalescence process.

Figure 14.11. Variation with strain of the coalescence parameter .CP

Complementary data are nevertheless required before any definite conclusion


about the relevance of these two steps of the coalescence process.

14.6. Conclusions
High resolution X-ray micro-tomography appears as a very promising technique
to characterise cavitation induced by superplastic deformation of industrial alloys. It
confirms the difficulty to interpret experimental information deduced from
conventional 2D quantitative metallography. In the case of an Al-Mg alloy, the
coalescence process has been preferentially investigated since it is concerned with
large cavities.

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X-ray tomography in material science

Despite a quite limited number of experiments, significant results have been


obtained. Coalescence occurs in a large strain interval, which means that the
frequently used assumption that the number of cavities remains roughly constant
during deformation is not valid. Just before fracture, most cavities are connected
together. A parameter CP was proposed to quantify the degree of connection of the
cavities in the superplastically deformed alloy and the variation with strain of CP
suggests a coalescence process in two steps.
Additional experiments are however needed to establish a reliable quantitative
correlation between CP and the experimental conditions of testing of superplastic
alloys.

14.7. References
[BLA 96] BLANDIN J.J., HONG B., VARLOTEAUX A., SUERY M., L'ESPERANCE G.,
Acta Mater., vol. 44, p. 2317-2326, 1996.
[BUF99JBUFFIERE J.Y., MAIRE E., CLOETENS P., LORMAND G., FOUGERES R., Acta
Mater., vol. 47, p. 1613, 1999.
[CHO 86] CHOKSHI A.H., J. Mater. Sc., vol. 21, p. 2073, 1986.
[DUP 97]DUPUY L., DEA INP Grenoble, 1997.
[FRI 96] FRIEDMAN P.A., GHOSH A.K., Metall. Mater. Trans., vol. 27A, p. 3827,
1996.
[HAN 76] HANCOCK J.W., Metal Sc., vol. 10, p. 319, 1976.
[HIR 95] HlRANO T., USAMI K., TANAKA Y., MASUDA C., J. Mater. Res., vol. 10, p.

381, 1995.
[rwA91]IWASAKi H., HIGASHI K., TANIMURA S., KOMATUBARA T., HAYAMI S.,
Proc. of Int. Conf. on Superplasticity of Advanced Materials (ICSAM), p. 447,
1991.
[LAB 96]LABICHE C., SEGURA-PUCHADES J., VAN BRUSSEL D., MOY J.P., ESRF

Newsletter, vol. 25, p. 42, 1996.


[LAR 98]LARIVIERE D., DEA INP Grenoble, 1998.
[MAR 99] MARTIN C.F., Thesis INP Grenoble, 1999.
[PIL 85] PILLING J., RIDLEY N., Res. Mechanica, vol. 23, p. 31, 1985.
[RAJ 77] RAJ R., Acta Metall., vol. 25, p. 995, 1977.
[RIC 69] RICE J.R., TRACEY D.M., J. Mech. Phys. Solids, vol. 17, p. 201, 1969.
[STO 83] STOWELLMJ., Metal. Sc., vol. 17, p. 1, 1983.
[STO 84] STOWELL M.J., LIVESEY D.W., RIDLEY N., Acta Metall., vol. 32, p. 35,
1984.
[VAR 89] VARLOTEAUX A., BLANDIN J.J., SUERY M., Mater. Sc. Tech., vol. 5, p.
1109, 1989.

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