Acta mater. Vol. 46, No. 10, pp.

3605±3617, 1998
# 1998 Acta Metallurgica Inc.
Published by Elsevier Science Ltd. All rights reserved
Printed in Great Britain
PII: S1359-6454(98)00024-X 1359-6454/98 $19.00 + 0.00

NON-LINEAR DEFORMATION MECHANISMS DURING

NANOINDENTATION
D. F. BAHR{, D. E. KRAMER and W. W. GERBERICH
Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, MN 55455,
U.S.A.

(Received 22 September 1997; accepted in revised form 29 December 1997)

AbstractÐExperiments involving the indentation of single crystals of both tungsten and an iron alloy show
that the observed yield phenomena can be predicted using a superdislocation model driven by the change
in shear stress between the elastically and fully plastic loading conditions. A low density of dislocation mul-
tiplication sites is required to support elastic loading which approaches applied shear stresses on the order
of the theoretical shear strength of the material. Oxide ®lm thickness and crystal orientation are examined
as parameters in controlling the yield phenomena. A model based on activation of dislocation multipli-
cation sources is suggested to explain the initiation of the yield point during indentation and the overall
load±depth relationship during indentation. # 1998 Acta Metallurgica Inc.

1. INTRODUCTION high, with only minimal evidence of plastic defor-

The ability of a metal to sustain extremely high
shear stresses was initially observed by Gane and
Bowden [1]. The process of bringing a tungsten car-
bide tip into contact with an electropolished and
annealed gold surface was observed in a scanning
electron microscope while the load on the tip was
monitored. For very low loads no indentation was
observed upon removing the tip from the surface.
Upon reaching some critical load, the tip rapidly
penetrated into the sample, leaving an impression
of the indentation on the gold surface. This was a
signi®cantly di€erent phenomena than had been
suggested by Hertz in 1882 [2]. Rather than observ-
ing a transition from elastic to plastic deformation
at applied shear stresses which meet either the
Tresca or von Mises yield criteria, the authors
suggest that the stresses being applied to the gold
sample approach the theoretical shear strength of
the material, even though it is likely that the stress
®eld around the indenter will encounter a dislo-
cation prior to the onset of plasticity.
Pethica and Tabor [3] applied a load to a clean
tungsten tip in contact with a nickel (111) surface in
an ultra high vacuum environment while monitor-
ing the electrical resistance between the tip and sur-
face. The nickel had been annealed, sputtered to
remove contaminants, and then annealed again to
remove surface damage from the sputtering process.
When an oxide was grown on the nickel to thick-
nesses of greater than 50 AÊ loading was largely elas-
tic while the electrical resistance remained extremely
{Present address: Mechanical and Materials
Engineering, Washington State University, Pullman, WA
99164-2920, U.S.A.
3605
mation. However, past some critical load the resist-
ance between the tip and sample dropped
dramatically, with continued loading suggestive of
largely plastic deformation.
These two sets of experiments have been the basis
for further discussion regarding the onset of plas-
ticity during indentation. With the development of
indenters which continuously monitor both the load
and depth of penetration of a tip into a sample
further examples of this phenomena have been
observed. Sudden excursions in depth at low loads
during nanoindentation have been observed in elec-
tropolished nickel (at depths of about 5 nm) [4],
sputtered aluminum ®lms which had been annealed
(at depths less than 10 nm) [5], and electropolished
single crystal of tungsten [6]. These excursions were
ascribed to oxide ®lm failure in the case of the
nickel and aluminum and to the onset of plasticity
in the case of tungsten.
Pethica and Oliver determined that there is purely
elastic contact between a diamond tip and a sap-
phire surface for very low loads [7]. The authors
utilized Hertzian contact mechanics to estimate the
shear stress under the indenter tip, and found that
it approached the theoretical shear stress of the ma-
terial. The authors also measured the contact resist-
ance between a tungsten tip and an aluminum
sample in air while making an indentation. The sud-
den jump in the depth which occurs at depths of
approximately 10 nm during nanoindentation is
suggested to be indicative of the oxide ®lm break-
ing. However, there remained a very high resistance
between the sample and tip until depths approach-
ing 250 nm, whereupon the electrical resistance
between the tip and sample dropped by several
3606 BAHR et al.: NANOINDENTATION
orders of magnitude. They use this result to demon-
strate that oxide ®lm fracture and extensive plastic
deformation may occur prior to a electrical resist-
ance drop between the tip and sample, thus making
a resistance drop a poor measure of tip±sample
contact.
Page et al. [8] studied the deformation of ceramic
crystals using nanoindentation techniques coupled
with scanning electron microscopy (SEM) and
transmission electron microscopy (TEM). By ima-
ging the structure of indentations into sapphire and
silicon carbide using SEM and TEM, the authors
®nd no residual impression when the load±depth
curve from the indentation data shows no residual
depth upon unloading. TEM observations of
indents past this ``pop-in'' show dislocation loop
structures have developed underneath the indenta-
tion. The authors also mention that the observed
displacement during pop-in will be an upper bound
to the product of the number of dislocation loops
and the Burgers vector.
A study of the e€ects of the passivating ®lm on
the loading behavior of an iron-3 weight percent
silicon (Fe±3%Si) single crystal was carried out by
Venkataraman et al. [9]. In this study, it was shown
that electropolished Fe±3%Si has the same general
behavior as tungsten, exhibiting elastic loading at
low loads followed by a sudden excursion in the
load±depth curve. By adding a drop of HCl to dis-
solve the passive ®lm, it was shown that removing
the oxide ®lm on Fe±3%Si removes the ability to
support elastic loading. When the liquid evaporated
and the sample repassivated, the ability to sustain
elastic loading and the subsequent excursion was
recovered. A subsequent study has shown that some
of the conclusions drawn regarding softening of ma-
terial without the passive ®lm were actually caused
by metal dissolution [10].
The lack of plasticity prior to the excursion, fol-
lowed by the sudden penetration of the indenter
may correspond to either the oxide breaking or dis-
location nucleation. Two schools of thought pre-
sently exist regarding the mechanism occurring
during this excursion. It was suggested by
Gerberich et al. [11] that dislocations actually were
generated prior to the excursion, and that the
excursion is indicative of the failure of a passive
oxide ®lm on the surface. This model requires dislo-
cation loops to nucleate upon loading, move under
the indenter tip, cross slip to planes leading back to
the free surface, and then break through the oxide
and escape to the free surface. There is direct evi-
dence using TEM that dislocations do cross slip
under an indenter tip and travel back to the surface
in Fe±3%Si [12, 13]. In addition, atomic force mi-
croscopy (AFM) and scanning tunneling mi-
croscopy (STM) have been used to measure the
amount of pile up around indenter in Fe±3%Si [14],
silicon [15], and tungsten and molybdenum [16]. In
all cases, material is found to be piled up around
the indentation. This pile up corroborates the TEM
observations of cross slip of dislocations from
underneath the indenter tip back to the free surface.
The pile up in single crystal tungsten also follows
crystallographic directions, with slip observed in the
h111i direction, most likely on the {112} planes [16].
Further investigations by Gerberich et al. [17] pro-
vide some evidence of dislocation nucleation at very
low loads, and then an excursion at larger loads
corresponding to dislocations cross slipping back to
the free surface and breaking the oxide. This model
relates the load and depth at which the excursion
begins and ends to the shear strength of the ma-
terial.
The second school of thought regarding the
nature of these loading excursions attributes the
excursion to only dislocation nucleation, and that
the oxide breaking is not the controlling factor in
the process. Mann and Pethica [18, 19] suggested
that the kinetic energy of the tip (based on the
approach velocity of the tip prior to contact) as it
impacts a surface can alter the loads at which
excursions occur in GaAs and tungsten. Asif and
Pethica [20] have shown that it is likely that there is
no mobile dislocation density prior to the excursion
using a continuous sti€ness measurement. After the
excursion the sti€ness of the contact increases while
held at a constant maximum load (suggesting that
the indenter is plastically deforming the sample
with time), while before the excursion a hold at
constant load shows no change in sti€ness
(suggesting no plastic deformation during the hold).
There is additional evidence of dislocation nuclea-
tion on gold coated with a self assembled mono-
layer of an organic thiol solution, where an oxide
®lm is not expected, using an interfacial force
microscope, which does not show large excursions,
but instead shows small deviations from the
expected loading pattern [21].
The di€erence between this concept and the pre-
vious models of Gerberich et al. [11, 17] is the
assumption that dislocations are not nucleated until
the excursion, and that all loading prior to the
excursion is purely elastic deformation of the ma-
terial. It should be noted that Mann and Pethica
have attributed the loading excursion in tungsten to
only dislocation processes due to the observation
that when immersed in dilute HCl there is still an
excursion [18, 22]. The authors claim that immer-
sion in HCl will remove the oxide ®lm (in a manner
similar to the experiment regarding HCl and Fe±
3%Si [9]), and since there is still an excursion on
the samples immersed in HCl the phenomena can-
not be controlled by the presence of an oxide.
However, since tungsten has very low corrosion
rates in dilute HCl [23], it is possible that the oxide
has not been removed during immersion in dilute
HCl. If this is the case, the authors suggestion that
the oxide has been removed is incorrect, and the
 BAHR et al.: NANOINDENTATION
question of the role of the passive ®lm on the oxide
®lm breakthrough is still open to debate.
To further examine the mechanisms related to the
onset of permanent deformation during indentation,
two sets of experiments have been carried out.
First, the e€ects of the thickness of an oxide ®lm
grown on a metal on the excursions during indenta-
tion will be examined. Second, by altering the crys-
tal orientation and dislocation density in a sample,
the e€ects related to dislocation multiplication and
motion will be explored.
2. EXPERIMENTAL METHODS
Based on the prior work concerning yield
phenomena in metals during indentation, the ma-
terials used for this study consist of Fe±3%Si single
crystals and tungsten single crystals. The Fe±3%Si
was cut so that the h100i direction was normal to
the sample surface. Fe±3%Si samples were cut to
various shapes and thicknesses, all approximately
1 cm square with thicknesses between 300 mm and
4 mm. Samples were mechanically polished to 600
grit, and then electropolished in 95% acetic acid
5% perchloric acid at room temperature with 40±
60 V using a stainless steel cathode. After electro-
polishing, the samples were annealed in air for 1 h
between 100 and 3508C. After annealing, oxide
thickness was measured using ellipsometry.
A tungsten single crystal was cut into pieces
oriented in the h100i, h110i, and h111i directions.
Samples were then polished to a 0.3 mm ®nish, and
then electropolished in a mixture of 10 g NaOH,
100 ml H20, and 100 ml glycerol at 20 V with a
stainless steel cathode. To utilize the same crystal
for indentations, the samples were indented at var-
ious stages of oxidation. Initial testing was carried
out on the electropolished surface. The tungsten
was oxidized at 2508C for 2 h, tested again, oxidized
for 6 more hours at 2508C, indented again, and
®nally oxidized for another 24 h (for a total of
32 h) and the surface was tested again. A fourth
sample was oxidized at 5008C for 21 h and then
tested. A second set of tungsten samples in all three
orientations were mechanically polished to a
0.05 mm ®nish, and then treated to the same oxi-
dation and testing schedule as the electropolished
samples. Final oxide thicknesses were measured
using either ellipsometry or depth pro®ling during
X-ray photoelectron spectroscopy (XPS), and corre-
spond closely to that predicted by other
researchers [24]. The electropolished surface the
oxide thickness determined by XPS was less than
1 nm.
Indentations were made using either a
Nanoindenter II [25] or a Hysitron Triboscope [26],
which is an indentation attachment to an atomic
force microscope (AFM). In the Nanoindenter, the
tip approached the sample at a rate of 10 nm/s,
whereas in the Hysitron system the tip is in contact
3607
with the sample prior to the indent. In the
Nanoindenter, indentation rates were at either
30 mN/s or 300 mN/s, and loads between 400 mN
and 120 mN were applied. In the Hysitron loading
rates were between 100 and 1000 mN/s. The tips
used were di€erent in each system, with the tip used
in the Hysitron system being a three sided pyramid
with a tip radius of approximately 70 nm and an
included angle of about 90 degrees. The tip in the
Nanoinstruments system was a Berkovich tip with a
tip radius of approximately 400 nm.
3. RESULTS
3.1. Yield phenomena during indentation
An indentation into an electropolished tungsten
h100i crystal which exhibits the yield point phenom-
ena is shown in Fig. 1. The excursion corresponds
to the sudden jump in depth during loading; which
for this indentation occurs at approximately
900 mN. Purely elastic loading is shown in Fig. 2 for
the tungsten h100i surface. We will de®ne this as
elastic loading since there are two ways of verifying
that there is no residual plastic deformation. First,
the load±depth curve unloads on top of the loading
curve (within the noise of the system), suggesting
no permanent deformation. A second method to
verify the lack of permanent deformation is that an
AFM image of the area of similar indentations
using the Hysitron attachment shows no evidence
of a cavity. However, it should be noted that is it
possible that a few dislocations are moved during
this procedure which retreat during unloading, in a
manner analogous to dislocation damping [27].
Since any plastic deformation of this type will likely
be smaller than the depths which can be clearly
resolved using this equipment, the loading will con-
tinue to be dominated by elastic deformation, and
Fig. 1. Load±depth curve of an indentation into the h100i
face of a tungsten single crystal. The initial elastic portion
of the curve is compared with elastic contact theory.
3608 BAHR et al.: NANOINDENTATION
Fig. 2. Elastic loading of a h100i tungsten surface. There is
no evidence of residual plastic deformation, the loading
and unloading curves overlap.
thus will be described as elastic. This initial loading
can be modeled as the elastic loading of two spheri-
cal elastic bodies, where the load is related to the
displacement between remote points in the bodies
by [28]
4 p
P ˆ E* Rd3 , …1†
3
where P is the load, R the radius of the indenter tip
if the sample is planar, d is the depth of pen-
etration, and E* is the reduced Young's modulus of
the sample and indenter, given by
1 1 ÿ 21 1 ÿ 22
ˆ ‡ : …2†
E* E1 E2
This ignores any oxide ®lm on the material.
However, since the modulus of the ®lm and sub-
strate are within factors of two for both Fe and W,
and the contact radius of the impression is most
likely at least an order or magnitude greater than
the ®lm thickness, the assumption of ignoring the
oxide ®lm in the elastic deformation analysis seems
reasonable. Elastic loading modeled by equation (1)
is shown in Fig. 1, using R = 400 nm and
E* = 322 GPa.
After the excursion, the loading continues in an
elastic±plastic manner. The shape of the load depth
curve is related to the tip geometry, the plastic ¯ow
behavior of the material, and the elastic properties
of the material. The load±depth behavior after the
excursion will be referred to as the geometrically
necessary loading curve. Other researchers have
proposed using this geometrically necessary loading
curve to extract the material properties of coated
systems [29]. The material ¯ows in a geometrically
similar expanding plastic zone during geometrically
necessary loading, i.e. the shape of the plastic zone
around the indentation does not change, only the
extent of deformation increases.
This geometrically necessary loading curve is
unrelated to the load at which an excursion during
loading occurs. Figure 3 shows three indentations
into an electropolished tungsten h111i crystal. The
load at which the excursion occurs can easily vary
by up to a factor of 3, as shown in Fig. 3, but after
the excursion the loading curves follow the same
geometrically necessary curve. This supports the
concept that the geometrically necessary loading
curve is de®ned by the material properties of plastic
¯ow and elastic deformation.
The yield behavior of the tungsten surfaces at
times exhibited ``staircase'' yielding, similar to the
loading discontinuities which have been previously
observed on gold single crystals [30]. In this case,
the sample loaded elastically, yielded, but did not
reach the geometrically necessary curve. After the
initial yield point, the sample continues to load elas-
tically, yields again, and repeats this process until
the geometrically necessary curve is reached. Note
that the loading steps after the initial yield point
are not an o€set of the Hertzian curve. This is due
to the tip penetrating to larger depths, which results
in an e€ectively larger radius of curvature at the
tip. This type of phenomena may be due to limited
slip systems in this particular orientation. Figure 4
illustrates the type of loading behavior which can
occur in the h111i crystals. The other orientations
of tungsten which were tested also sporadically
exhibited this type of behavior. Only the h111i face
consistently exhibited the staircase phenomena.
Mechanically polished surfaces did not exhibit
the yield point phenomena in any of the orien-
tations tested in this study. The geometrically
necessary loading curves of the mechanically
polished surfaces are consistently above the electro-
Fig. 3. Indentations in which the initial yield point varies,
yet the remaining elastic±plastic loading curves are identi-
cal. This behavior is suggestive of a geometrically necess-
ary loading curve for a given sample de®ned by both the
elastic and plastic properties of the material and the shape
of the indenter tip. Included is the prediction of the load-
ing curve based on combining equations (1) and (12).
 BAHR et al.: NANOINDENTATION
Fig. 4. ``Staircase'' yielding phenomena, observed during
indentation of a tungsten h111i surface.
polished curves after the yield point, this is shown
in Fig. 5 for the h100i samples. In addition, the cal-
culated hardness [7] of the mechanically polished
surfaces was consistently higher than that of the
electropolished surfaces. Since the modulus of the
tungsten should not be altered appreciably by the
presence of dislocations, it is not surprising that if
the load needed to reach a given depth is greater in
the mechanically polished samples than the electro-
polished samples the calculated hardness is also
greater. That is, the ¯ow stress which controls the
geometrically necessary loading curves is increased
by the dislocations introduced during mechanical
polishing.
Fig. 5. Comparison between indentations into mechani-
cally polished and electropolished tungsten with the same
thickness oxide. The mechanically polished surfaces do not
exhibit initial elastic loading. The hardness of the
mechanically polished surface is higher than the hardness
of the electropolished crystal after the yield point.
3609
3.2. Oxide thickness e€ects on yield
It has been previously shown that a native oxide
or passive ®lm in solution on Fe±3%Si can have a
dramatic e€ect on the load at which the yield excur-
sion occurs [9, 10]. The e€ect of oxide thickness on
the load at which the excursion occurs in electropol-
ished tungsten is shown in Fig. 6. For the h100i
orientation, no signi®cant variation in the yield
load is observed after the initial oxidation. For the
h110i and h111i orientations, there is no clear e€ect
of oxide thickness variation on the load at which
the ®rst excursion occurs. Qualitatively, fewer
indents exhibited the ``staircase'' yield phenomena
after oxidation, but the phenomena did still occur.
When thermal oxides are grown at higher tem-
peratures to greater thicknesses (approaching 50±
100 nm) a di€erent behavior occurs. In this case,
permanent plastic deformation occurs at the lowest
loads applied in this study. No evidence of a yield
phenomena after purely elastic loading is observed.
However, a discontinuity in the loading curve
appears at loads approaching 20±50 mN in the elec-
tropolished sample which was oxidized at 5008C.
Once again, the mechanically polished surface
which was oxidized at 5008C did not exhibit any
discontinuities in the load depth curve up to loads
reaching 120 mN.
Figure 7 presents both load±depth curves and
AFM images of indentations in the electropolished
sample with the thick oxide showing concentric and
radial cracks running on the surface of the sample,
as shown in Fig. 7(A). Note that the radial cracks
correspond to the crystal symmetry, and not the
geometry of the tip. AFM images of indents
unloaded prior to this excursion, such as the AFM
image in Fig. 7(C) still show residual impressions,
but do not have any evidence of cracking. Images
Fig. 6. E€ect of oxide thickness on the load at which the
initial excursion occurs for three orientations of tungsten
crystals. Except for the initial oxidation of the h100i sur-
face there is no clear e€ect of oxide thickness on the load
at yield for this range of oxide thicknesses.
3610 BAHR et al.: NANOINDENTATION

Fig. 7. (caption opposite).

 BAHR et al.: NANOINDENTATION 3611

of indents unloaded immediately after the excursion

do not have cracking to the extent of samples
loaded past the excursion, but do have a slight
amount of cracking on the surface, as shown in
Fig. 7(E). It is therefore likely that the cracking
observed around the indentations may begin at the
excursion, but continues to grow steadily as the
sample is loaded past the excursion.
The tungsten yield behavior with oxide thickness
is very di€erent than that predicted by Gerberich et
al. [17] in Fe±3%Si. In the iron alloy, thicker oxides
lead to an increase in the load at which the excur-
sion occurred, as shown in Fig. 8. The oxide thick-
ness in Fe±3%Si dramatically a€ects the load at
which the excursion occurs. These tests were made
on samples which had been prepared by electropol-
ishing followed by thermal oxidation. Each oxide
thickness was achieved by altering the thermal oxi- Fig. 8. E€ect of oxide thickness on the load at which the
dation temperature, with oxidation occurring for initial excursion occurs for Fe±3%Si single crystals. The
load at yield increases with increasing oxide thickness.
1 h. The temperatures ranged between 100 and
3508C. In addition, samples which were only elec-
mechanically polished, it will be assumed that the
tropolished were also tested (corresponding to the
excursion is linked to the low dislocation density of
lowest oxide thickness). Indentations were carried
the electropolished surface. The facts that the load-
out using the Hysitron indentation system. The
ing and unloading curves prior to this excursion lie
di€erence between the behavior of the oxide ®lm on
on top of each other, and that no residual im-
tungsten and Fe±3%Si will be discussed in the next
pression of an indentation has been observed prior
section.
to the excursion suggests that the loading is elastic.
For elastic loading of a sphere onto a ¯at surface,
the maximum pressure under an indentation, pm,
4. DISCUSSION
can be given by [28]
4.1. Shear stress driven excursions 3P
pm ˆ , …3†
Two distinct phenomena were observed on the 2pa2
electropolished and oxidized surfaces. First, on the
where P is again the load, and a is the radius of
samples with thin (less than 20 nm) oxides, the
contact between the tip and the sample. Since the
loading behavior observed was elastic up until some
load, depth, and contact radius are related during
point, whereupon a rapid excursion in the depth at
loading, the maximum pressure can also be de®ned
constant load occurred, corresponding to the onset
as
of plastic deformation. The second phenomenon,
 
which also has a displacement excursion at higher 6E*2 1=3 1=3
loads, occurred on the samples with a thick oxide. pm ˆ P , …4†
p3 R2
In this case, however, the sample exhibited perma-
nent plastic deformation at low loads. At some where R and E* are the same as previously de®ned.
higher load there was a rapid excursion in the The maximum shear stress, tmax, under a spherical
depth at constant load. These two types of loading elastic contact is given by
excursions will not be treated as the same type of tmax ˆ 0:31pm …5†
event, since the one yield point corresponds to the
onset of plastic deformation while the other exhibits and is located underneath the indenter tip at a
plastic deformation prior to the excursion. depth of 0.48 a (which is in general much deeper
Consider the yield point which occurs on electro- than the metal/oxide interface). The shear stress
polished samples with a thin oxide. Since this yield ®eld does not drop o€ that rapidly, and there is a
point does not occur on samples which are region under the indenter tip extending to approxi-

Fig. 7. AFM images of impressions from indentations into the tungsten crystal with the 60 nm oxide
and corresponding load±depth curves. (A) Indent to 120 mN. Note the concentric and radial cracks,
which correspond to crystallographic orientations and not the geometry of the indenter. (B) Load±
depth curve for (A). An excursion occurred at approximately 30 mN. (C) Indent to 25 mN, with clear
permanent deformation. (D) The corresponding load±depth curve shows no excursion, but did show
permanent plastic deformation. (E) Indent to 35 mN. Very little evidence of cracking is observed
around the indentation. (F) The load±depth curve for (E), showing a clear excursion.
3612 BAHR et al.: NANOINDENTATION
mately 2a which has an applied shear stress of ap-
proximately 0.25 pm.
If the excursions are driven by the shear stress
underneath an indenter tip, then it should be poss-
ible to relate the plastic ¯ow characteristics to the
excursion. As will be shown, this allows prediction
of the entire load±depth curve. It has been
suggested [8, 11] that the number of dislocations
generated underneath an indenter tip is related to
the excursion length. The generation of dislocations
must be able to accommodate the displacement of
the tip. Since some of the dislocation loops will
cross slip back to the free surface, and others will
act as shielding dislocation [13], let us say that
some fraction of the dislocations will participate in
accommodating the displacement of the tip. The re-
lationship between the number of dislocations parti-
cipating in the event and the excursion is then given
by
1 dex
Nˆ …6†
b b
where N is the number of dislocation loops, 1/b is
the fraction of dislocations that go toward accom-
modating the tip displacement, b is the Burgers vec-
tor of the dislocation, and dex is the length of the
excursion. We will assume that, to ®rst order, half of
the total dislocations generated will participate in
direct motion of the indenter tip. The motion of ma-
terial to accommodate the displacement of the tip
can be modeled as a ``superdislocation'' an average
distance r from the indenter tip on a plane at an
angle y from the indentation direction after a
change in shear stress, Dt, has been applied. This
suggests that the super dislocation may be de®ned
by [11]
Dtr tan y
N1 , …7†
Gb
where N is the number of dislocations in the
``superdislocation'' and G is the shear modulus of
the material. By combining equations (6) and (7),
the excursion length can be determined as a func-
tion of the change in shear stress and the superdis-
location position, given by
Dtr tan y
dex ˆ b : …8†
G stress, the excursion length as a function of load at
After an excursion the loading follows a geometri-
cally necessary load±depth curve. This curve,
assuming a constant elastic modulus for a given
sample, will be dependent on the ¯ow stress of the
material. Traditional de®nitions of hardness as
either three times the tensile yield strength or three
times the ¯ow stress at a given strain (usually con-
sidered to be approximately 8% strain) [31] re¯ect
this idea. For a ®rst order approximation, it will be
assumed that the hardness of the sample is constant
after the excursion, and that the maximum shear
stress which can be supported after plastic yielding
has occurred is equivalent to the bulk shear ¯ow
stress of the material. It should be noted that
assuming the hardness to be constant after an
excursion, irrespective of load, implies that there is
no indentation size e€ect. The maximum change in
shear stress over the load excursion is then just the
di€erence between the maximum shear stress under
an elastic contact [equations (4) and (5)] and the
bulk characteristic ¯ow stress of the material, tf.
This is given by
 
6E*2 1=3 1=3
Dt ˆ 0:31 3 2 P ÿ tf : …9†
p R
This would be the maximum change in shear stress,
The actual shear stress which is applied to a given
slip plane would be reduced if the maximum
applied elastic shear stress was at a di€erent orien-
tation than the slip plane. Therefore, equation (9)
will be considered an upper bound for the change
in shear stress.
It has been shown [14] that a force balance of
Johnson's elastic±plastic indentation model can be
used to model the plastic zone, c, as a function of
the load applied and tensile yield strength, sys, to
an indenter for large indentations. This model,
given by
s
3P
cˆ …10†
2psys
is valid for large indentations [32]. Using this model
as a ®rst order approximation of the plastic zone
size after the indentation allows us to approximate
the plastic zone radius based on the load applied to
the indenter tip after yielding. If the plastic zone
radius is known, then the super dislocation position
(the position from the indenter tip at which half of
the dislocations have moved further than and half
have moved less than that point) can be approxi-
mated as
c
r1 : …11†
4
By combining equations (8)±(11), and using the von
Mises criteria to approximate p the tensile yield
strength in equation (10) as 3 times the shear ¯ow
which the excursion occurs at is given by
s  
tan y 3 6E*2 1=3 5=6 ÿ1=2
dex ˆb p 0:31 3 2 P tf
4G 2 3p p R

ÿ P 1=2 tf1=2 : …12†
as long as the load at which the excursion began is
the same as the load at which the excursion ends.
In a load controlled test instrument, this is very
close to the actual situation (where the load will
increase by a few micronewtons between sampled
 BAHR et al.: NANOINDENTATION
data points), and the load at the excursion can be
used for both the starting and ending load. Also
note that equation (12) assumes that the arrest of
the excursion is the geometrically necessary load
depth curve, and therefore cannot be used during
``staircase'' yielding. It should be noted that this
behavior does not rely on the end of the excursion
remaining in the spherical region of the tip. The
only constraint is that the elastic portion of the
loading curve can be described by loading a spheri-
cal tip.
The ®nal quantity needed to predict the excursion
length is the ¯ow stress of the tungsten, which can
be determined experimentally by examining the
stress±strain curve. Under a compression test, the
resulting true stress±true strain curve is shown in
Fig. 9. The crystal fractured at the end of the test,
so strains past 1.6% could not be recorded. As seen
in this ®gure, the 0.2% o€set yield strength is only
310 MPa, but the crystal has a very large strain
hardening coecient, 0.45. This strain hardening
coecient allows the ¯ow stress at 8% strain to be
calculated; it would be approximately 1400 MPa. If
the approximation is made that hardness is 3 times
the ¯ow stress at 8% strain, the hardness of the
crystal would be 4.2 GPa. The measured hardness
of the crystal at depths between 100 and 500 nm is
between 3 and 7 GPa. This would correspond to a
shear ¯ow stress of 1800 MPa as an upper bound,
and a shear ¯ow stress of 1175 MPa as a lower
bound.
The excursion length can now be predicted using
equation (12). Figure 10 shows the relationship
Fig. 9. True stress±true strain ¯ow curve for tungsten single crystal in the h100i orientation.
3613
between the excursion length and the load at which
the excursion occurred in the tungsten h100i crystal
which was oxidized for a total of 2 and 32 h. Also
shown here is the prediction of equation (12). The
¯ow stresses used are the upper and lower bounds,
along with the ¯ow stress from the point at which
the stress±strain test ended due to sample fracture.
It is important to note that the tip radius and the
¯ow stress are not ®tting parameters of the
equation, but are independently determined from
other experiments and observations. The ¯ow angle
is chosen according to the active slip systems
observed by TEM for an indentation into another
b.c.c. metal, the Fe±3%Si single crystal [13].
To verify that this theory holds for very low
loads, similar measurements were made for the ex-
periments performed in the Hysitron system using
Fe±3%Si single crystals. In this case, the reduced
modulus of the system is 191 GPa and the radius of
curvature of the indenter tip is approximately
70 nm. The shear ¯ow stress of the material was
not measured on this speci®c sample p due to size
constraints, but will be taken as 1/ 3 of the pre-
viously measured tensile yield strength of a similar
crystal [33], e€ectively assuming the material to be
elastic±perfectly plastic. Figure 11 compares the
measured relationships between the excursion length
and the load at yield and the prediction of
equation (12). It appears that equation (12) pro-
duces a reasonable approximation to the data for
loads above 100 mN. Below this range the limited
sensitivity of the instrument and possible inaccura-
cies in the radius of the tip may make accurate
3614 BAHR et al.: NANOINDENTATION
Fig. 10. Comparison between excursion distance and the
load at which the excursion occurred. The experimentally
measured values for two oxide thicknesses on h100i tung-
sten crystals are compared to the theoretical model pre-
sented in equation (12).
measurements of the excursion length dicult,
which would account for the discrepancies between
the measured data and the theory. Alternatively,
the assumptions made in the model regarding a
hemispherical plastic zone (when it is actually
shaped according to crystallographic orientation)
and average dislocation spacing may become
increasingly invalid at these very small defor-
mations.
The correspondence between the model and the
data suggests that the model is a possible expla-
nation for the mechanisms which control the
motion of the tip during the rapid yield phenomena.
This model does not address the issue of nucleation,
only of propagation of the plastic zone between
elastic and plastic loading. However, it seems likely
Fig. 11. Comparison between excursion distance and the
load at which the excursion occurred at very low loads in
Fe±3%Si. Several oxide thicknesses are included in these
data, along with the prediction using the model in
equation (12).
that the yield phenomena is controlled by the di€er-
ences in shear stresses between the elastically loaded
sample and the indent after plastic deformation.
4.2. Predictive capabilities of the theory to the load-
ing curve
If the elastic portion of the loading curve is
described by elastic contact mechanics, and the
excursion distance can be predicted based on the
load at which the excursion occurs, then it should
be possible to predict the load depth curve for a
material which exhibits a loading excursion. The
displacement based on elastic loading can be deter-
mined by solving equation (1) for the displacement
as a function of load. If the excursion length
[equation (12)] is then added to this displacement,
the resulting load±depth relationship should
describe the ending points of the excursion. In turn,
the ending points of the excursion de®ne the geome-
trically necessary loading curve. The prediction for
tungsten is shown in Fig. 3 using a tip radius of
400 nm and a shear ¯ow stress of 400 MPa, and
compares favorably with the experimental data. The
di€erence between the experimental data and the
prediction is based on the increasingly inaccurate
description of elastic loading based on equation (1).
At higher loads the tip appears to act as if it were
blunter than 400 nm (the elastic curve is ``deeper''
than the actual experimental data). As the tip
radius a€ects both equations (1) and (12), the
resulting sum of the two will be limited in accuracy
to the range of elastic loading which can be
described by equation (1). Since the approximation
of a sphere is just that, an approximation, it is
expected that a more complete description of the
elastic loading of a tip of an arbitrary pro®le into a
planar surface would describe both the elastic load-
ing and resulting geometrically necessary loading
curve. For instance, a parabaloid of revolution may
be a better description of the indenter tip once the
initial spherical portion is passed (as the tips are
actually three sided pyramids). However, since the
stresses that develop underneath the tip are more
complicated than for the spherical case, a full treat-
ment of that case is beyond the scope of the present
work.
4.3. Nucleation of plasticity
The propagation of a rapidly expanding plastic
zone does not provide signi®cant insight into the
mechanism which is responsible for the nucleation
of the plastic zone. For this we note several exper-
iments which may add to the understanding of the
plasticity nucleation phenomena. First, our working
de®nition of plasticity will be the motion of dislo-
cations to permanent positions so as to induce shape
change. Two types of behavior fall into the category
of non-plastic deformation during indentation. The
®rst is simply elastic deformation of the sample.
The second is a more theoretical argument, and can
 BAHR et al.: NANOINDENTATION
be described as the motion of dislocations con-
strained to one slip plane under the indenter tip.
This has been previously suggested by Gerberich et
al. [17] to occur prior to the yield point, and that
the yield point only occurs when these limited
mobility dislocations cross slip to the free surface
and fracture the oxide ®lm.
Consider the theoretical shear strength of the
tungsten used in this study. One method of estimat-
ing the theoretical shear strength of a material is to
divide the shear modulus of the material by 2p. For
tungsten, the shear stress required for dislocation
nucleation is approximately 26 GPa. If the radius of
the indenter tip is known, then the load required to
reach the theoretical shear strength of the material
can be determined by combining equations (4) and
(5) in a manner similar to that described by Page et
al. [8]. For the indenter used in this study, with a
tip radius of approximately 400 nm, the load which
would cause dislocation nucleation is about 4.5 mN.
For the indent with the highest load at which the
excursion occurred, 6.3 mN for h100i tungsten oxi-
dized for 32 h, the maximum shear stress is
28.6 GPa. As only seven out of 143 indents which
produced loading excursions occurred above
4.5 mN (and only one was above 5 mN) the theor-
etical shear strength estimation seems reasonable.
Therefore, it appears that the upper load limit
which can be reached prior to permanent defor-
mation is the theoretical shear strength of the ma-
terial. Variations in the load at which the
excursions occur based on crystal orientation di€er-
ences (see Fig. 6) also suggest that the critical
resolved shear stress under the indenter is a factor.
One point which should be noted regarding yield
in metals under indentation is the observation that
under high pressures the compressive yield strength
of many b.c.c. metals will increase over the yield
strength measured at ambient conditions [34, 35].
However, this strengthening e€ect tends to increase
compressive yield strengths only by factors of two
at pressures in the 100 GPa regime. Thus, it is unli-
kely that the lack of permanent plastic deformation
is due only to pressure strengthening.
The experimental observations in this study and
others [22] have found that mechanically polished
surfaces do not exhibit the yield point phenomena.
Since mechanically polished surfaces will have high
densities of dislocations and dislocation sources, it
seems likely that the lack of a yield point is associ-
ated with the presence of dislocation sources. In ad-
dition, growing a thermal oxide on mechanically
polished tungsten does not generate the yield point
phenomena. Therefore, we may discount the possi-
bility that the rapid yield phenomena is indicative
of only the oxide ®lm breaking. This is not meant
to suggest that the oxide ®lm does not fracture
during loading a mechanically polished sample,
only that there is not a sudden and singular fracture
event in the oxide.
3615
Elastic loading in Fe±3%Si has been shown to be
associated with the presence of an electrochemically
grown passive ®lm [10]. When the passive ®lm is
removed, the ability to sustain elastic loading is
removed. The results for Fe±3%Si in this study do
show that the load at which the excursion occurs
increases with increasing oxide ®lm thickness.
However, it is dicult to ascribe the results on the
electropolished tungsten to the deformation and
fracture of an oxide less than 1 nm thick. In ad-
dition, altering the indentation with respect to crys-
tal orientation will change the resolved shear
stresses underneath the indenter, but not dramati-
cally alter the oxide characteristics. It is therefore
reasonable to suggest that the di€erences observed
between the three tungsten crystals may be due to
dislocation based phenomena and not the oxide
®lm. The oxide ®lm appears to have an a€ect on
the yield phenomena, but is not responsible for the
yield phenomena. Other studies have identi®ed
loading excursions on gold surfaces (which should
be oxide free) [21, 29], lending further support to
the concept that the excursions are indicative of dis-
location multiplication and not oxide ®lm fracture.
These experimental observations and calculations
suggest a possible model for the mechanisms and
processes occurring during indentation which lead
to the yield point phenomena. When a tip
approaches a surface the initial contact must be on
an atomic scale. If sources for dislocation multipli-
cation are present (or created during the contact as
suggested by Mann and Pethica [19]), a load on the
tip will cause dislocation loops to multiply and
expand to some distance away from the indenter.
As the dislocation loops travel away from the tip,
the tip will penetrate the sample and continue to
plastically and elastically deform the material
around and underneath the loaded region.
However, if during the initial contact the tip does
not encounter or generate sources for dislocation
multiplication, elastic loading can occur. Clearly,
the likelihood of the stress ®eld under the tip acti-
vating a source for dislocation multiplication will
decrease as the dislocation density of the material is
decreased. An oxide ®lm may well act to reduce the
likelihood of the stress ®eld under the tip activating
a dislocation source by one of two methods based
on the assumption that dislocations are not gener-
ated in the oxide, but at the interface between the
®lm and substrate. First, the oxide ®lm can act to
slightly distribute the load around the indenter tip,
lowering the stresses applied to the metal. In ad-
dition, this would act to move the indenter tip away
from the metal, so that for a dislocation source
®xed in the metal the tip must reach a higher load
to bring the stress ®eld under the tip into contact
with the source. A second method by which the
oxide may act to increase the likelihood of elastic
loading is due to image forces applied to dislo-
cations. It has been shown that an oxide ®lm on a
3616 BAHR et al.: NANOINDENTATION
bulk soft metal tends to increase the yield strength
of the metal [36]. An elastically sti€er oxide than
metal will tend to repel free dislocations in the
metal away from the oxide/metal interface. We
begin by assuming that the dislocation source is the
intersection of a single dislocation limited to one
slip plane with two immobile dislocations. Moving
this dislocation further from the surface of the
oxide will require a higher load to generate a stress
®eld large enough to move this dislocation. This
would be the case for the Fe±3%Si, where the
oxide is sti€er than the metal. However, in the case
of the tungsten, it is possible that any image forces
would either be negligible or allow dislocations to
be slightly closer to the free surface (the modulus
measured by indentation of a thick tungsten
oxide is approximately 250 GPa, lower than the
410 GPa of tungsten metal). In this case, the load
needed to nucleate a source would remain relatively
constant.
A model such as this explains the behavior
observed on samples which exhibited ``staircase''
yielding. If loading the tip activates a source and
several dislocations are generated this can accom-
modate the displacement of the tip. However, once
some plastic deformation has occurred the tip is no
longer in elastic contact with the sample. Therefore,
the stress driving the dislocations drops dramati-
cally. If this stress is low enough, the sample again
will elastically load until a shear stress is reached
which is high enough to activate the same or
another dislocation source. The reason that this
process becomes less likely when very high mean
pressures are generated is that after the ®rst dislo-
cation avalanche is initiated so many dislocations
are created that the sample has a larger number of
sources which will continue to accommodate plastic
deformation. Thus, the staircase phenomena is lim-
ited to cases where a source is activated and only a
few dislocations are emitted. This may also be simi-
lar to the concept of mechanical damping due to
dislocation motion, where pinned dislocations can
bow under stress prior to creating a dislocation
source [37].
It should be noted that the concept of initiating a
source is not a contradiction to previous results,
particularly the work of Asif and Pethica [22]. In
their case the sample is loaded and held at a con-
stant load prior to the excursion while the sti€ness
of the system is monitored. They observe no creep
in elastically loaded samples. However, since the
stress ®eld under an elastic contact drops away
from the contact area, it is very possible that a
single dislocation could move outward from the
indenter tip during the hold. If this dislocation did
not meet a source, it would quickly arrest due to
the decreasing stress ®eld. Since the dislocation vel-
ocity depends on the applied shear stress through
an exponential or power-law relationship, it is likely
that this would drop to negligible values and no
creep would be observed [38]. However, in mechani-
cally polished tungsten where a source is likely to
be in the stress ®eld under the indenter tip, the
small reduction in shear stress at a given position
due to an increased contact area may not be su-
cient to stop the source from multiplying dislo-
cations. As dislocations multiply and move outward
(until they stop due to the reduction in applied
shear stress with distance from the contact), they
will allow some motion of the indenter, and creep
will occur.
5. SUMMARY AND CONCLUSIONS
Continuous depth sensing indentation has been
used to study yielding phenomena during the initial
stages of indentation. The excursion associated with
the onset of plasticity has been examined as a func-
tion of crystal orientation, oxide ®lm thickness, and
dislocation density in tungsten, and as a function of
oxide ®lm thickness in an Fe±3%Si single crystal.
The load at which the excursion occurs varied with
crystal orientation, with the h100i face supporting
the highest loads prior to yield. Oxide ®lm thickness
does not dramatically alter the load at which the
excursion occurs in tungsten except for an initial
oxidation of the h100i face. Iron, on the other
hand, shows a trend of increasing load at excursion
with increasing oxide ®lm thickness. The shear
stress under the indenter tip is less than or equal to
the theoretical shear strength of the material being
indented.
A model has been suggested to detail the pro-
cesses which occur during the yield phenomena
observed in small scale indentations. Based on a
superdislocation model driven by the change in
shear stress from the elastically loaded condition to
the fully plastic indent, the excursion length can be
predicted as a function of the load at which the
excursion occurs. The model closely corresponds to
the experimental data for both tungsten and iron,
but is only valid when the shear stress under elastic
loading is much greater than the ¯ow stress of the
material. When the shear stress prior to yield is
only slightly higher than the ¯ow stress a phenom-
ena referred to as ``staircase'' yielding occurs.
The experimental evidence suggests that the
nucleation of permanent plastic deformation is con-
trolled by the presence of favorably aligned sources
for dislocation multiplication, and not by oxide
fracture. Mechanically polished samples do not
exhibit the ability to sustain large elastic stresses,
whereas electropolished samples with low dislo-
cation density surfaces can support shear stresses
approaching the theoretical shear strength of the
material. However, this does not preclude dislo-
cation motion prior to the excursion if the motion
is restricted to a few dislocations on limited slip
planes with no favorable sources for multiplication
available.
 BAHR et al.: NANOINDENTATION
AcknowledgementsÐThe authors wish to thank N. R.
Moody of Sandia National Laboratories for helpful dis-
cussions and the use of the Nanoindenter II. This work
was supported by the Oce of Naval Research under
grants N00014-95-10539 and N00014-91-J-1998.
Additionally, the authors would like to gratefully acknowl-
edge the discussions and information provided by J. B.
Pethica of Oxford University and A. B. Mann of Johns
Hopkins University.
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