JOURNAL OF ELECTRON MICROSCOPY TECHNIQUE 13:40-50 (1989)

Techniques of Convergent Beam Electron Diffraction

R. VINCENT
Physics Department, Bristol University, Bristol BS8 1 TL, England

KEY WORDS Transmission electron microscopy, Commercial instruments, Crystal defects

ABSTRACT The techniques required to record standard convergent beam electron diffraction
patterns in an analytical electron microscope are discussed in detail, with emphasis on the design
of electron optics in commercial instruments. Practical comments are included on specimen
preparation, the influence of crystal defects, tilting to major zone axes, and alignment of the
instrument. The influence of parameters under experimental control such as probe size, acceler-
ating voltage, temperature, specimen thickness, and convergence angle is discussed in detail. Some
comments are included on the alignment and limitations of large angle patterns formed by a
defocused probe.
INTRODUCTION CBED patterns were obtained from specially adapted
Although the techniques of convergent beam elec- versions of older microscopes. However, none of these
tron diffraction (CBED) have been described in some conversions was,entirely satisfactory, even in skilled
detail by several investigators (Steeds, 1979; 1984; hands. Tilting experiments with a 10 nm probe are
Williams, 1984), our experience has shown that the regarded as routine today, but would be extremely
necessary transfer of practical skills is best effected by diEcult on an adapted instrument.
personal tuition. Nevertheless, some restatement of At this stage, the ideal specifications of an instru-
the essential instrumental and experimental parame- ment entirely suitable for CBED are discussed. Quite
ters controlling the quality of CBED patterns may be apart from electron optics, any microscope column that
convenient for the readers of other articles collected in contains significant levels of hydrocarbon vapour is
this journal. To record a sequence of CBED patterns guaranteed to produce rapid contamination whenever
with a high information content from a crystal with an a small probe is focused onto the specimen. Ideally, we
unknown structure is not an easy task. Even when the require some version of the design features pioneered
transmission microscope is entirely suitable for this by Philips in the EM400 series, which is an ion-pumped
type of diffraction, every film exposure represents column separated from the camera chamber by a
either a balance between competing factors or is chosen differentially pumped aperture, indium wire, or dry
to optimise the visibility of specific features within the O-ring vacuum seals, combined with an efficient anti-
pattern. The extension of CBED techniques to include contamination stage. Provided that specimens carry no
the large angle patterns invented by Tanaka is de- intrinsic contamination, continuous work with a 10 nm
scribed in some detail. The reader is referred to the probe should be possible. Routine precautions such as
other articles for a discussion of dynamic diffraction regularly cleaning specimen holders, never touching
and also the basic electron optics for CBED. However, holders with bare hands, and lubricating O-rings with
the relevant features are mentioned briefly here when a minimum of UHV-compatible grease are essential.
the choice of parameters under experimental control, Under these conditions, most specimens will not show
such as probe size, accelerating voltage, temperature, contamination in modern analytical electron micro-
specimen thickness, and convergence angle, is directly scopes (AEMs) for probe sizes larger than 10 nm.
involved. The paper is divided into four sections which However, electropolished foils often retain a layer of
inevitably overlap to some extent. These include in- mobile contaminants that may cause some problems.
strumentation, specimen preparation, experimental For nanometre probes, contamination should be ex-
technique, and large angle patterns. Examples of im- pected from a wide range of specimens. There are
perfect CBED patterns are collected in Figure 1 and several partial solutions to this problem, which are
are referenced within the text. discussed in the next section.
The design of flexible electron optics into the
INSTRUMENTATION condenser-objectivelenses surrounding the specimen is
critical for efficient CBED over a wide range of probe
To some degree, we may attribute the present avail- sizes and convergence angles. Even for a particular
ability of commercial microscopes ideal for CBED to manufacturer, the configuration of these lenses has
the wide acceptance over the past 15 years of energy
dispersive X-ray detectors as an essential tool for
microanalysis. Naturally, the electron optics and vac-
uum engineering required to form a small noncontam-
inating probe also provided the large convergence Received March 7, 1988;accepted in revised form May 6, 1988.
angle at the specimen not available in previous gener- Address reprint requests to R. Vincent, Physics Department, l‘yndall Avenue,
ations of microscopes. Of course, many of the initial Bristol University, Bristol BS8 lTL,England.

0 1989 ALAN R. LISS, INC.

 TECHNIQUES OF CBED
shown continuous evolution over the past few years. It
is not practical to describe every option that may be
encountered, but some comments on the Philips CM12
and CM30 (equivalent to the EM420 and EM4301 are
included here. In the standard microprobe mode used
for imaging, the probe size is controlled by the C1 lens
demagnification of the electron source. The excitation
of the condenser-objective lens above the specimen is
weak, and convergence angles, controlled by the C2
aperture size, are comparatively small. Typical aper-
ture diameters are 200, 100, and 50 pm, chosen to be
compatible with the usual range of Bragg angles be-
tween adjacent CBED discs. A much wider range of
apertures would be useful; if a fourth aperture is
available, as in the CM30, it is convenient to select a
small size (15 pm) suitable for large unit cells and also
for microdiffraction (see below).
It is essential that the angular field in the back focal
plane, which is limited by the geometry of the lower
objective pole piece, should be as large as possible.
Otherwise, higher order Laue zone (HOLZ) reflections
around major zone axes may not be transmitted down
the column. An ideal angular field is around 20",
although a lower cut-off (say 15") is not a serious
limitation in practice, provided that the shortest cam-
era length available is sufficient to record all reflec-
tions on film. The controls used to centre the diffraction
pattern on the screen should have sufficient range to
allow the details of HOLZ reflections to be visible
through binoculars. When measuring the spacing of
reciprocal lattice layers from HOLZ radii, it is impor-
tant to remember that diffraction patterns are imaged
in the back focal plane, with significant barrel distor-
tion at large scattering angles. By measuring the
HOLZ radii of a layer crystal in CBED patterns with
overlapping discs, a calibration curve relating the
measured and true radii can be produced (Steeds,
1981). The systematic error is quite important at large
angles (-15%). Equally significant, much larger er-
rors, dependant on the slope of the calibration curve,
can occur if interbranch extinction distances for the
projected potential are measured from the separation of
excess lines within a HOLZ reflection.
Another essential detail is that the C2 apertures
should show no evidence of charging because of con-
tamination, visible as distortions around the edge of
focused CBED discs (Fig. 1A). We have found that new
apertures are often less than ideal for CBED and that
the standard cleaning procedures produce no improve-
ment. It is simpler to test a new set of apertures and to
reject examples that are not imaged as perfect circular
discs at low voltages.
For some CBED experiments, the limited choice of
convergence angles controlled by the C2 apertures may
be a serious limitation. In conventional patterns the
maximum amount of information is recorded when the
discs are almost touching along the shortest reciprocal
lattice vector. In the previous generation of AEMs such
as the Philips EM400, this difficulty was overcome by
increasing the objective lens current to move continu-
ously from standard TEM mode toward the STEM
mode. If the specimen was kept a t the eucentric height,
imaging of the probe position was possible only by
41
examining the shadow image in CBED discs. Con-
versely, lowering the specimen away from the eucen-
tric position retained the option of direct specimen
imaging with a defocused probe. However, the most
recent Philips CM series and the JEOL FX models are
designed with a more symmetric lens configuration
around the specimen. In standard imaging mode the
upper lens is weakly excited. Probe sizes are controlled
entirely by the C1 lens demagnification of the source,
and the convergence angles are limited by the C2
aperture. In this microprobe mode, adjusting the spec-
imen height and/or the objective lens current does not
significantly change the convergence angle. In the
Philips CM series, switching to nanoprobe mode re-
verses the current through a separate coil in the upper
objective lens and increases the excitation of the upper
lens to a level similar to the lower objective lens. In this
symmetric Riecke-Ruska configuration, the upper ob-
jective behaves as a powerful final condenser with a
nine times increase in convergence angle relative to
the microprobe mode for a fixed C2 aperture. However,
an equivalent reduction of probe size is not achieved
because spherical aberration in the condenser-objective
limits the probe size to the disc of minimum confusion
unless the C2 aperture is reduced. The minimum probe
diameter for a given C1 demagnification of the source
is defined by accepting a similar contribution from the
lens aberration. Suitable combinations of C1 lens set-
tings and C2 aperture sizes are listed in the manual,
where the minimum probe size is 2 nm. However, probe
diameters of less than 5 nm are of limited use for
CBED. Quite apart from contamination and drift prob-
lems, the probe current is much reduced relative to
(say) a 10 nm probe in standard mode. In addition,
many CBED patterns are obtained from thick crystals
(>0.1 pm) in which the spreading of even an infinites-
imal beam incident on the top surface of a crystal
would limit the transverse spatial resolution to several
nanometres.
We have found that the nanoprobe setting has two
distinct advantages unlisted in the manufacturer's
manual. First, the large convergence angles limited
only by the largest C2 aperture are ideal for the
Tanaka mode diffraction patterns described in the final
section. Second, a simple modification of the lens
circuitry to give external control of the current through
the extra objective winding in both microprobe and
nanoprobe modes produces a continuous range of con-
vergence angles at the specimen (Greene and Eades,
1986). An equivalent result is achieved in the JEOL
FX series by a separate lens close to the specimen.
When examining the CBED patterns from an un-
known crystal, it is important to remember that weak
superlattice reflections and also diffuse streaking
caused by soft phonon modes or short range order are
easily overlooked. However, the well-known displace-
ment in position on the specimen for diffracted beams
caused by spherical aberration becomes unacceptably
large when a small selected area (SA) aperture is used
to record HOLZ reflections with plane wave illumina-
tion. A preferable method is to limit the area illumi-
nated on the specimen directly, either by using a
focused probe combined with the smallest possible C2
Figure 1
 TECHNIQUES' OF CBED
aperture (microdiffraction) or by slightly defocusing
the C2 lens away from crossover to form a parallel
beam with diameter limited by the C2 aperture. In
either case, there is no positional error on the specimen
for diffracted beams and HOLZ reflections are recorded
with no shadowing effect from the SA aperture.
The probe size in older microscopes such as the
Philips EM300 and JEOL lOOCX can be reduced to 0.2
pm when the C1 lens is fully excited, but the beam
convergence is limited to angles around five times too
small for fcc metals and tetrahedral semiconductors.
Nevertheless, some useful results can be obtained if
contamination is reduced by cleaning components, de-
greasing seals, and surrounding the specimen with an
eEcient anticontamination stage. In particular, the
ability to record the position and radius of HOLZ
reflections relative to the zero layer using microdif-
fraction can be an efficient method of exploring the
reciprocal lattice geometry of an unknown crystal in a
single CBED pattern, quite independent of symmetry
analysis, which requires precise alignment of the beam
parallel to the zone axis. The addition of a third
condenser or minilens to the EM300 reduces the probe
size t o 50 nm with an equivalent increase in conver-
gence angle. Although the electron optics in this mode
are suitable for CBED, the Contamination problem is
critical unless strict cleanliness is maintained in the
column, combined with the beam flooding technique
mentioned below.
In conventional AEMs, the electron source is usually
a tungsten filament, although a useful ipcrease in
brightness combined with a smaller effective source
size is obtained with a LaBs single crystal. At consid-
erable extra expense and difficulty, the beam may be
extracted from a field emission gun. All of these
sources are classified as incoherent when installed in a
standard AEM column if we use as a criterion the
absence of interference effects between overlapping
CBED discs.
Another important accessory for CBED is the facility
for continuous voltage variation between the usual
stepped settings. Fine control of the electron wave
vector is useful for direct measurement of small shifts
in HOLZ deficiency line intersections caused by lattice
parameter variations and also for exciting important
HOLZ reflections that may affect the whole pattern
symmetry. Likewise, direct control of the projected
crystal potential via y, the relativistic mass ratio is
essential for measurement of planar and zone axis
critical voltages (Matsuhata and Steeds, 1987).
To conclude this section, some comments on speci-
_ _ _ ~
Fig. 1. Examples of imperfect CBED patterns recorded at 120 kV.
Pattern A was obtained from the edge of a marcasite (FeS2) flake on
the [OOl] axis. The nonuniform intensity distribution within discs is
due to charging from contamination around the C2 aperture combined
with some departure from crossover in the specimen plane. A similar
problem is illustrated in B, taken on the [loll axis of a M3Bz boride
where the beam was not focused accurately onto the precipitate. The
dark bars in alternate reflections along the horizontal row are
distorted or absent. Internal strains often produce a similar effect. An
example of the displaced image of the BF disc produced by the
internal potential of a wedged particle is shown in C taken on the
<ll4>axis of a MC carbide. Similar contrast is just visible in B and
43
men holders are collected here. Obviously, only side-
entry holders offer sufficient access to a large cone of
tilt angles. For this reason, tilt-rotate holders with a
k60" tilt available in all directions are preferred to
double-tilt holders, which are limited to -1-45"on the
second tilt axis. In addition, the Philips rotation hold-
ers contain a specimen cup that is easily replaced by a
cheap brass version, ideal for mounting fragile or
magnetic specimens. This procedure is not practical
with the JEOL rotation holders, but an equally useful
conversion involves replacing the retaining circlip with
a threaded hexnut. The most useful accessory for
CBED is an efficient double-tilt specimen holder cooled
with liquid nitrogen. Cooling the specimen from 300K
to 100K not only eliminates contamination but also
reduces beam heating and radiation damage. Equally
important is the increase in the intensity and contrast
of HOLZ diffraction caused by the transfer of electrons
scattered through large angles from the thermal dif-
fuse background into Bragg reflections. Only crystals
with an unusually low or high Debye temperature fail
to show a considerable improvement in the range of
diffraction angles around the incident beam. Finally,
the goniometer should be in perfect condition, with the
preset horizontal adjustment exactly aligned. Other-
wise, no setting of the eucentric height control will
eliminate movement when tilting the specimen.
SPECIMEN PREPARATION
Comments are included here not only on the produc-
tion of specimens suitable for CBED but also on the
interpretation or avoidance of anomalous patterns that
may be attributed to the intrinsic nature of the speci-
men. First, the specimen preparation methods in gen-
eral use are each associated with specific advantages or
problems for CBED. For alloys, carbon extraction rep-
licas remove a representative sample of precipitate
phases over a large area. Both CBED and X-ray
analysis are comparatively simple in the absence of
interference from the matrix, even for 10 nm particles,
and contamination is rarely observed. The disadvan-
tage is that all topographic and epitaxial information
relating the particle to the matrix is lost. In the
corresponding electropolished or chemically etched
foils, the interphase boundaries between matrix grains
and precipitates are retained, but the quality of CBED
patterns may be degraded by unrelaxed strains across
interfaces (Fig. 1D). The simplest solution to this
problem is to concentrate on unstrained precipitates
partially attached around the edge of the foil. Electro-
polished foils often retain mobile contamination layers
D. The BF disc of D on the <111> axis of a y' precipitate in a nickel
superalloy shows slight departures from cubic symmetry in both the
projection and HOLZ contrast caused by unrelaxed strains from the
interface with the matrix. The Tanaka pattern in E from the <loo>
axis of GaAs is almost perfect except that the crystal is wedged with
thickness decreasing toward the top. A distinctly imperfect Tanaka
pattern is shown in F on the [loll axis of p-terphenyl where the
crystal is not only bent but also varies in thickness and shows signs of
beam damage. The dark arc toward the top right is due to imprecise
adjustment of both the SA aperture and C2 lens fine control (cf.
Fig. 5).
44 R.VINCENT
despite thorough washing and consequently show seri-
ous contamination with small focused probes. Cooling
the specimen eliminates this problem, but alternative
methods include gentle ion-cleaning or flooding the
specimen with an intense beam for several minutes,
which temporarily reduces the diffusion of contami-
nants.
Ion-thinned specimens, typically ceramics or semi-
conductors, never show contamination in clean micro-
scopes but some problems may be produced by ion
damage of surface layers. In thick crystals, the diffuse
background contributed by amorphous surface layers is
not noticeable, but the problem becomes quite severe if
patterns are required from thin crystals. A more insid-
ious effect that distorts the symmetry of CBED pat-
terns has been attributed to the dilation of subsurface
crystalline layers by embedded gas atoms, where
planes inclined to the surface are bent into S-shaped
curves (Preston, 1988).
If large transparent areas are not essential, crushed
particles often contain suitable edges free of contami-
nation, surface damage, and strain. As for lattice
imaging, particles are usually mounted in holey carbon
films, although a useful alternative is the Cu microgrid
(2,000 mesh), which is ideal for electron energy loss
spectra. In practice, the ideal flake with a small wedge
angle and free of debris and defects is often difficult to
find, and it is worth spending some time to select a
perfect example. Flakes always have poor thermal
contact with their support and care should be taken to
avoid excessive beam heating.
One of the most difficult specimens for CBED is a
polycrystalline evaporated film with small grain sizes
and uniform thickness. It is possible to obtain a set of
patterns from a single grain by working on a particle
protruding from the edge, but a simpler alternative for
exploratory work is to tilt the film and select grains
that are unusually dark in the bright-field (BF) image.
These grains are likely to be aligned close to major zone
axes.
The electron flux in a focused probe is sufficiently
high to produce damage within a second in all organic
crystals. The problem is less severe for ionic or hy-
drated crystals in which the structure is damaged
principally by beam heating combined with loss of
volatile species and diffusion of ions. For these crystals,
cooling to lOOK combined with medium voltages (say,
300 kV) may be sufficient to produce acceptable pat-
terns. This solution is less effective for molecular
crystals, but some results may be obtained by topolog-
ical symmetry analysis of large angle patterns formed
by a defocused beam (Fig. 1F) (Vincent, 1986).
The tilting of magnetic specimens always deflects
the beam and may bend the foil, but these effects are
less severe at medium voltages, especially if the vol-
ume of the specimen is reduced by avoiding jet-polished
discs. Likewise, insulating specimens can show severe
charging effects when large areas are illuminated, but
a small probe focused onto a thin edge may be quite
stable. Carbon coating and working at medium voltage
usually eliminates any serious problem.
It is important to recognize the influence of crystal
defects on the quality of CBED patterns used for
symmetry analysis. Point defects are not visible in the
image, but any CBED pattern that shows weak HOLZ
diffraction relative to the diffuse background may
contain static disorder if the Bragg contrast is not
improved by cooling. Typical examples include rapidly
quenched metals, MC carbides, and some oxides. The
nonuniform strain field associated with an extended
defect such as an isolated dislocation decays slowly
with distance and may influence the symmetry of
CBED patterns over large areas. Any strain field will
affect almost all reflections but often is most noticeable
in the projection contrast from zero layer reflections
around a zone axis, which are associated with short
interbranch extinction distances (Fig. lB,D). It is not
uncommon to record patterns in which the projection
symmetry is lower than the whole pattern symmetry,
including HOLZ reflections. This situation is forbidden
by the diffraction group tables and should be attributed
to some departure from the ideal geometry of a plane
parallel slab normal t o the beam enclosing a perfect
crystal.
Similar effects caused by inhomogeneous strain
fields are observed at many types of planar interfaces,
including surface oxide layers, dislocation arrays at
grain boundaries, and epitaxial interfaces. In addition,
thinning the specimen produces relaxation and planar
bending across any coherent interface that is not both
continuous and parallel to the surfaces. Examples
include the y-y' boundaries in nickel superalloys and
also transverse sections across semiconductor inter-
faces that are not lattice-matched.
A more subtle loss of symmetry is produced by
stacking faults in layer crystals. A heavily faulted
crystal is easily recognised because the reciprocal lat-
tice spots are streaked normal to the fault plane and so
the HOLZ reflections are expanded into broad rings. In
the limit that the reciprocal lattice becomes a set of
continuous rods, the distinction between zero and up-
per layer reflections is lost. However, the presence of a
single stacking fault is not easily recognised in a zone
axis pattern. The simplest test is to examine the
projection contrast in several systematic rows of reflec-
tions. If the dark-field (DF) rocking curve is not sym-
metric about the Bragg condition (s = 0),then the
crystal must contain planar faults (Tatlock and Steeds,
'73). In practice, the best way to avoid interference
from faults in layer crystals may be to focus on thin
flakes extended from the edge of the thicker areas.
EXPERIMENTAL TECHNIQUE
This discussion is divided into three sections, which
include some practical hints on tilting to major axes in
unknown crystals, followed by remarks on the lens
adjustments required to produce high quality CBED
patterns, and finally some comments on the strategy to
follow when the microscope is aligned and the crystal
zone axis is parallel to the beam.
In many ways, tilting the crystal onto a major zone
axis is the simplest step. As discussed by Steeds and
Vincent (19831, the examination of the whole pattern
and BF symmetry in CBED patterns on the major zone
axes that are parallel or orthogonal to the point group
symmetry elements is the most efficient procedure for
 TECHNIQUES OF CBED
determining the space group of a crystal. To find these
axes, we tilt the cystal through a large angular range,
select a strong Kikuchi band that is associated with a
closely spaced row of reflections and follow this band to
its intersection with a major zone axis. Obviously,
intermediate CBED patterns are checked for mirror
symmetry parallel to the Kikuchi band, and at the
major axis we require the whole pattern (WP), BF, and
DF symmetries to determine the diffraction group,
although the WP symmetry determined from HOLZ
reflections is usually sufficient when combined with
symmetries around other major axes.
In practice, it is unwise to use a small focused probe
when tilting the crystal. Apart from reducing the
brightness of the pattern, the risk of contamination is
increased with smaller probes. Likewise, a large con-
vergence angle may result in the overlap of CBED
discs, but the visibility of Kikuchi bands at large
scattering angles is improved. If a CBED pattern is
compared with the equivalent spot pattern produced by
a defocused beam, it is evident that the convergent
beam enhances the visibility of Kikuchi contrast. In
many specimens, exact control of the illuminated area
is not essential a t this stage. In some specimens, such
as particles in an extraction replica, slight defocusing
of the probe will produce a shadow image within the
CBED discs, allowing rotation and tilting to be com-
pleted entirely in reciprocal space, especially if an area
close to the rotation axis is selected. Otherwise, contin-
ual reference back to the real space image is recom-
mended. If a wide range of accelerating voltages is
available, the higher settings are more convenient for
tilting because penetration is improved and the Bragg
angles or Kikuchi band widths are reduced, with
improved definition of zone axes.
The most difficult skill to be acquired is the ability to
recognize the approach of a major axis even a t angles of
20" or 30" from the beam direction. Sometimes, the
reciprocal lattice planes normal to the axis are densely
populated with reflections, and the intersection of
these planes with the Ewald sphere produces arcs of
reflections curved toward the axis. Otherwise, we must
project the Kikuchi bands to some common intersection
beyond the viewing screen.
When a suitable axis has been selected, certain
adjustments of the microscope controls beyond the
usual alignment procedures are essential to record
standard CBED patterns. Initially, the eucentricity is
checked and then a suitable probe size is selected by
adjusting the C1 lens. At this stage, an intermediate
size, say 50 nm, is recommended. The probe is taken to
crossover with the C2 lens fine control, centred on the
screen, and the C2 astigmators are adjusted. If the
specimen is magnetic, the objective stigmators may
require further alignment. Next, the probe crossover,
by definition in the object plane of the objective lens
conjugate with the screen, is moved into the specimen
plane by adjusting both the objective current and the
C2 fine control. If the objective lens is not focused
exactly on the specimen, then we observe multiple
diffracted images of the probe that converge to a diffuse
halo and then to a single probe image as the objective
is adjusted. At this stage, a further slight adjustment of
45
the C2 lens fine control minimises the probe size on the
specimen. This method is both more accurate and
efficient than inserting an objective aperture, focusing
the image with a parallel beam and then setting the
probe to crossover on the specimen.
The probe is positioned on a suitable area, ideally
close to an edge and avoiding obvious defects, and the
microscope is switched to diffraction mode. Because of
lens interactions, some microscopes may show a small
shift of probe position and crossover setting when
switching between modes. For this reason, the final
positioning of the probe should be done on a slightly
defocused shadow image and then set to crossover in
diffraction mode. A useful test that crossover is set
exactly in the specimen plane is to check that there is
no evidence of a real space shadow when the probe is
moved across the edge (cf. Fig. 1A). Finally, a suitable
camera length is selected and the diffraction lens fine
control is adjusted to view the pattern exactly in the
back focal plane with sharp edges to CBED discs and
Kikuchi lines (Christenson and Eades, 1987). At the
camera length which includes the complete angular
field, the diffraction lens is adjusted to avoid shadows
or caustic images and to minimise the lens distortion at
large scattering angles. Ideally, this lens setting
should be reproducible and calibrated for measurement
of reciprocal lattice basis vectors and HOLZ radii. If the
beam is focused onto a small wedged particle, another
displaced image of the BF disc may be visible, resem-
bling the sun's corona when eclipsed by the moon (Fig.
1C). This contrast is attributed to electrons scattered
by the edge of the C2 aperture and subsequently
focused onto the specimen beyond the edge of the
particle. Except for these electrons, the entire CBED
pattern is displaced by the inner potential of the wedge
crystal, equivalent to a prism.
At this stage, decisions that affect the quality of the
final pattern are made. Usually, there is no single
combination of parameters that gives perfect visibility
of every feature in a single film exposure. It is standard
practice to record 10 or more exposures on a single axis
that is known to contain important information. The
first step is to select a C2 aperture that excludes
overlap of adjacent discs. In principle, the symmetry of
patterns is not affected by overlapping discs, but the
overall contrast is reduced and HOLZ reflections blend
into a continuous circle. Ideally, the discs should be
slightly separated, especially if HOLZ reflections are
an essential feature of the pattern. A useful prelimi-
nary step is t o insert the smallest C2 aperture to check
that weak reflections are not overlooked. To find the
WP and BF symmetry, the centre of the convergent
beam must be aligned exactly parallel to the zone axis.
Provided that the crystal has been tilted to within a
Bragg angle of the zone axis, it is simpler to complete
alignment by displacing the C2 aperture, equivalent to
tilting the beam. Of course, any adjustment of the C2
lens will displace the probe on the specimen if the C2
aperture is not centred. An equivalent method is to
adjust the angle of beam incidence with the DF tilt
controls.
Recognition of the exact pattern centre may be
simple if the BF disc includes interference rings or
46 R. VINCENT
similar contrast with an obvious centre. However,
many axes show uniform BF contrast, and the centre is
easily overlooked (cf. Fig. 1C). The problem becomes
severe for crystals with large projected unit cells where
the field of view is much reduced. Experience is the
best guide, but moving the C2 aperture over a wide
range can give some idea of the BF pattern extended
over a larger angular field. In some crystals, the BF
disc may be adjusted by reference to the zone centre as
defined by the common intersection area of Kikuchi
line pairs. Alternatively, the pattern may have to be
centred by comparing the projection contrast within
sets of discs. In the limit of large unit cells or thin
crystals, the discs may contain uniform intensities.
There is no guaranteed solution to this problem except
skill and persistence! In special cases, the Gjonnes-
Moodie dark bars parallel to the row of reciprocal
lattice vectors g in kinematically forbidden reflections
can be used as an accurate guide to the pattern centre,
at least in the direction perpendicular to g. Finally,
reducing the voltage increases the Bragg angles be-
tween discs and also reduces extinction distances.
Provided that absorbtion does not obscure the pattern,
some detail within the discs may become visible.
It is important to recognise and correct a t this stage
a common problem with the interpretation of CBED
patterns, where the projection symmetry around the
zone axis is reduced relative to the whole pattern
symmetry of HOLZ reflections. This absence of projec-
tion symmetry elements is contrary to any prediction of
the diffraction group tables and must be attributed to
inhomogeneous strain fields or bending of crystal
planes within the column illuminated by the probe.
Although any crystal distortion affects almost all re-
flections, this loss of symmetry is often most visible in
projection, where the contrast is dependent on short
interbranch extinction distances between Bloch waves.
If the symmetry andlor contrast changes unpredictably
with small movements of the probe within an area with
constant thickness, then some departure from the ideal
crystal geometry used to derive the diffraction groups
should be expected.
Even if individual crystal planes are not bent by the
strain fields from dislocations or an interface, the
averaging of orientations within the probe area always
reduces the pattern symmetry. It is essential that the
probe size should be smaller than the width of bend
contours in the image when viewed with plane wave
illumination. Likewise, any variation of crystal thick-
ness within the probe area reduces the projection
contrast and is likely to reduce the symmetry. How-
ever, any reduction of the probe beyond the size re-
quired to exclude imperfect areas of the crystal should
be avoided because exposure times beyond 30 sec or so
simply increase the risk of specimen drift or contami-
nation. A better alternative is to reduce exposure times
by increasing the emission to a high level.
The most important CBED pattern required on a
major zone axis with a large HOLZ radius is a high
quality image of the elastic contrast within HOLZ
reflections, obscured by the minimum diffuse back-
ground. Any pattern that shows only projection con-
trast or even a fuzzy HOLZ ring is of limited utility for
symmetry determination. The simplest parameter to
adjust for maximum HOLZ contrast is the specimen
thickness. Often, there is only a narrow thickness
window suitable for HOLZ diffraction. In thicker crys-
tals, the HOLZ ring is still visible but the elastic
contrast is reduced by the inelastic Kikuchi back-
ground, whereas thin crystals diffract too little inten-
sity into typical HOLZ reflections with long extinction
distances (- microns). If the contrast is too low, several
remedies are possible. An important step is to reduce
the convergence angle by inserting a smaller C2 aper-
ture. Although the field of view within CBED discs is
reduced, the inelastic intensity is still distributed over
the entire angular field, thereby improving the visibil-
ity of the HOLZ reflections. On an important zone axis,
microdiffraction patterns recorded with the smallest
C2 aperture are always useful both to deduce the
reciprocal lattice geometry from HOLZ reflections and
to check for the presence of weak superlattice reflec-
tions, possibly in separate HOLZ rings.
If the HOLZ contrast is still inadequate, reduction of
the accelerating voltage expands the angular radius of
HOLZ rings but reduces their radius R in reciprocal
space, where R cc k1’2 and k is the incident wave vector.
In effect, the structure factor for a HOLZ reflection
tends toward zero when the amplitude of thermal
vibrations approaches the planar spacing. Formally,
the Fourier components of the thermally smeared
crystal potential are multiplied by exp ( -Bs2), where s
= R/2 and B is an isotropic Debye-Waller factor. Then
the exponent s2 is directly proportional to k. Although
the majority of conventional CBED patterns are re-
corded a t 150 kV or less, there exists a lower limit on
the incident energy set by reduced penetration and the
enhanced inelastic background. For most crystals, a
further improvement in HOLZ diffraction is produced
by cooling the crystal to reduce the amplitude of atomic
vibrations. All of these measures may be necessary to
view the three-dimensional set of deficiency lines
within the BF disc where the contrast is reduced
relative to the excess lines in HOLZ reflections that
are viewed against a dark background. Provided that
some faint contrast from deficiency lines is visible in
the zero layer discs and the thickness is adjusted to
maximise the visibility, then a long camera length
pattern usually reveals a fine network of lines covering
both the BF disc and adjacent DF discs.
In crystals in which the point disorder is sufficient to
reduce the HOLZ contrast on all major axes, it is
necessary to test symmetry elements separately by
tilting along systematic rows. For superlattices, it may
be important to select orientations in which weak
symmetry-breaking reflections are strongly excited.
To establish the WP and BF symmetries with some
confidence requires experience. In crystals that are
bent, wedged, or contain a high defect density, many
patterns show clear evidence of broken symmetry.
Even for crystals that locally approximate the ideal
plane parallel slab, the existence of rough surfaces and
incomplete unit cells implies that no crystal gives
CBED patterns that are absolutely perfect in every
detail. If the deviations are very small and also differ
between patterns, then it is usually safe to overlook
 TECHNIQUES OF CBED 47
these details and to assign an “ideal” symmetry to the / \ hS.2cc / /
crystal. The logic behind this argument is based on
practical experience with hundreds of crystals in which
small atomic displacements known to exist from X-ray
work were always detected. Equally, examples are not
infrequent in which symmetry elements such as mir-
rors deduced from X-ray structure determinations have
proved to be clearly absent in CBED patterns.
Until now, we have considered the techniques re-
quired to determine the point group, but other simple
observations are sufficient to identify glide planes and
screw axes in the space group. If the microdiffraction
pattern formed with a small C2 aperture shows that
reflections present in the upper layers of the reciprocal
lattice are absent in the zero layer net, then there exist
glide planes normal to the zone axis with a correspond-
ing mirror in the point group. The analysis of three-
dimensional contrast within the two arms of the
Gjgnnes-Moodie dark cross for glide planes and screw
axes has been fully described by Tanaka et al. (1983).
One should always displace the C2 aperture away from
the zone axis setting to observe the second arm in the
dark cross a t the Bragg position perpendicular to g.
Alternatively, an expanded angular field of view is
available in DF Tanaka patterns. In crystals with large
projected cells, the line of absence may fill the disc, and
some reduction of the voltage and temperature may be
required to observe a clear dark line through the disc.
Similar measures are often essential to distinguish ~ . , .
glide planes from screw axes by examination of the +M A S 28-
three-dimensional contrast within arms of the dark Fig. 2. Schematic ray diagram excluding aberration for a speci-
cross. In practice, most lines of absence show only men illuminated by a defocused beam with finite diameter in the
two-dimensional or projection contrast, and a more object plane. Dashed lines indicate a diffracted beam. Parameters are
effective method to confirm the presence of a glide defined in the text.
plane in the space group is to check that the WP
symmetry includes a mirror parallel to g. Conversely,
any direction of beam incidence normal to a screw axis the Bragg angles between adjacent beams is an in-
should show perfect dark bars perpendicular to g crease of the area illuminated on the specimen to a
within the forbidden reflections. Dark bars are often circular patch, typically with a diameter not less than
observed in HOLZ reflections when the zone axis is 1 pm.
parallel to a glide plane. If tilting to other axes is not If the size of the probe in the object plane is ne-
practical, then some variation of the voltage may be glected, then the diameter of the area illuminated on
required to excite these reflections. the specimen a t height AS is given by the simple
expression 2a AS, where a is the convergence semian-
LARGE ANGLE DIFFRACTION PATTERNS gle of the beam. A more complete analysis, including
A wide range of alternative methods for the expan- aberrations, is given by Tanaka et al. (1980). For Bragg
sion or displacement of the angular field within the angles 20 between diffracted beams, the separation of
discs of CBED patterns have been described by Tanaka probe images in the image plane of the objective lens is
and coauthors and are illustrated in a recent publica- MAS 28, where M is the objective magnification. For a
tion (Tanaka and Terauchi, 1985). The ray diagram for SA aperture with diameter d, the minimum AS re-
the standard technique in which the angular field quired to transmit a single beam through the aperture
within a single BF or DF disc is expanded t o several is given by AS = d/M 20, and the beam diameter on the
degrees (Tanaka et al., 1980) is sketched in Figure 2 for specimen is equal to dcdM8. Setting 20 = 0.01 rad, (Y =
a probe with a finite diameter focused and imaged by 0.05 rad, d = 5 pm, and M = 40, the minimum
aberration-free lenses. As drawn here, the specimen is diameter is approximately 1 pm. In practice, the area
illuminated by a spherical wave converging to the illuminated is not reduced indefinitely by using a
beam crossover on a plane conjugate with the SA smaller SA aperture, because the minimum separation
aperture. By insertion of this aperture around one of of the probe images is limited by spherical aberration
the multiple diffracted images of the probe, only one of even for a point source. A lower limit on the diameter
the overlapping CBED discs is transmitted down the at the specimen is around 0.5 pm for crystals with
column and is imaged on the screen in diffraction small unit cells.
mode. In these Tanaka patterns, the price paid for Applications of these Tanaka patterns are described
expansion of the angular field beyond the limit set by elsewhere in this issue, but may be classified here into
48 R. VINCENT
Fig. 3. The dashed lines indicate ray paths for a perfect lens where
the angle of interception at the specimen is directly proportional to
distance from the optic axis. When spherical aberration is included
(continuous lines), the angle of interception is increased for marginal
rays, equivalent to pin-cushion distortion of the spatial images within
the CBED discs.
three categories. The first category is extension of
conventional space group analysis to radiation-
sensitive crystals in which the current density is re-
duced in a defocused probe (Vincent, 1986) and also t o
crystals in which the discs are too small to show useful
internal symmetry information in conventional CBED
patterns. Provided that the specimen has uniform
thickness within the illuminated area, bending of the
crystal distorts patterns, but topological symmetry is
retained. A second category includes the analysis of
multiple diffraction paths that contribute amplitude to
a reflection, visible as local perturbations of the DF
rocking curve around the Bragg position (Vincent,
1987). If the crystal has a uniform wedge profile, then
the real space information in large angle patterns (see
below) can be used t o advantage by arranging that the
thickness increases in a direction parallel to the dif-
fracting planes. Formally, these patterns are equiva-
lent to the standard images of a bent wedged crystal
illustrated in textbooks, except that the interpretation
is simpler because the radius of curvature in the
incident beam is both smaller and more uniform than
occurs naturally in bent foils.
The third and most general type of Tanaka pattern
occurs when a crystal defect of any type is illuminated
by the beam. Examples discussed by Cherns and Pre-
ston elsewhere in this journal include voids, disloca-
tions, stacking faults, and grain or interphase bound-
aries. Here, I discuss only the optics of the mapping
between the real space position of a column in the
specimen and the angular or reciprocal space position
Fig. 4. Ray paths in the image plane of the objective lens where
the SA aperture is positioned above the plane of the disc of least
confusion (cf. Fig. 5). Paraxial and marginal rays are transmitted, but
median rays are obstructed.
in the CBED disc. In Figure 2, the mapping is linear,
with spatial resolution equal to the probe size in the
object plane. In more detail, the crossover in the object
plane is equivalent to a cluster of parallel beams, each
with diameter equal to the probe size. The intensity
diffracted by any column with this diameter on the
specimen is focused to a point in the CBED disc. For an
aberration-free lens, a column a t distance r from the
optic axis, assumed to be a t the centre of the illumi-
nated area, is illuminated by a beam at an angle
directly proportional to r. For small a (-3'1, the map-
ping aberration of the imaging lens between the object
plane and back focal plane is negligible and the posi-
tion r' of the focused beam relative to the centre of the
CBED disc is proportional to r.
As illustrated in Figure 3, the inclusion of spherical
aberration in the condenser-objectivelenses inevitably
distorts this linear mapping, where the distortion re-
verses from barrel to pin-cushion type as the specimen
is raised from below to above the object plane. Usually
the distortion is not too severe except when AS is
deliberately minimised to confine variation of the
illuminated angle (2a) to within the area of a small
defect.
Below the condenser-objective lens, the combined
spherical aberrations usually limit the angular trans-
mission through the SA aperture to a semiangle p,
where p 5 a. The optimum position for the SA aperture
lies in the plane of the disc of least confusion. A slight
reduction of the C2 lens current effectively raises the
aperture above this level, expands the angular field,
 TECHNIQUES OF CBED
Fig. 5. Variation of the angular field in Tanaka patterns with
small increments in the C2 lens current. Relative to the optimum
but cuts off median rays, introducing an annular
shadow (Fig. 4).Conversely, a slight increase of the C2
current is equivalent to lowering the SA aperture
toward the gaussian image plane where marginal rays
are cut off and f3 reduced. The optimum setting is found
by adjusting the C2 current so that the annular shadow
is just invisible. If the disc of least confusion is set
equal to the SA aperture diameter d, then f3 is propor-
tional to d1'3, so that only a marginal improvement in
p is gained by increasing d from (say) 5 pm to 15 pm,
whereas the diameter of the area illuminated on the
specimen is linearly proportional to d (Vincent, 1986).
In practice, we have found that a 5 pm aperture
represents a suitable balance between these two fac-
tors, although a 15 pm aperture has been used to
maximise p and a 2 pm aperture to minimise the area
illuminated.
This section is concluded with some practical com-
ments on the production of Tanaka patterns on the
Philips EM430, although the principles should be ap-
plicable to other AEMs operated in nanoprobe mode. It
is usually preferable to operate at higher voltages,
especially if DF patterns from weak reflections in thick
crystals are required. With the microscope in the
standard microprobe mode, the largest C2 aperture is
inserted and centred, and a suitable C1 lens setting is
selected. The optimum spatial resolution is given with
C1 a t maximum excitation, but the intensity is reduced
and Bragg contrast may be obscured by defocused
Fresnel contrast from rough or contaminated surfaces.
Unless small defects are to be imaged, an intermediate
setting for C 1 is preferable.
The microscope is switched to nanoprobe mode and
the C2 lens current adjusted to the recommended range
(0.5-1.0 A), equivalent to a convergence angle, 2a of 6".
The specimen is moved away from the beam, the beam
tilts are adjusted to centre the illumination, and then
the objective lens is focused on the probe crossover
plane. Usually, the image does not show cylindrical
symmetry, but small balanced adjustments of the beam
tilts and shifts should correct this problem. Likewise,
49
setting (B), the SA aperture lies above and below the disc of least
confusion in (A) and (C), respectively.
some realignment of the C2 stigmators will be re-
quired. At the gaussian focal plane, the probe image
shows a peak a t the centre surrounded by a wide tail
caused by spherical aberration. Slight reduction of the
C2 current images the disc of least confusion. When the
specimen is moved to intercept the beam, multiple
overlapping images of the probe are observed if the
probe crossover is not exactly in the specimen plane. At
this stage, it is advisable to insert and centre the 5 pm
SA aperture and to increase the magnification to
around x 40,000. With the aperture removed, the spec-
imen height is reduced with the eucentric control until
the probe images are separated by distances at least
equal to the SA aperture diameter. If improved Bragg
contrast is required from a flat specimen with uniform
thickness, then increased separation of the probe im-
ages excludes some fraction of the diffuse scattering
between diffracted beams.
Usual practice is to reduce specimen height, al-
though raising the specimen does not appear to affect
the quality of patterns. Likewise, similar contrast is
obtained by keeping the specimen at eucentric height,
reducing the objective current and increasing the C2
current to retain images of the probe crossover. How-
ever, large values of A S increase the C2 current suffi-
ciently to reduce the convergence angle.
With the SA aperture inserted around the direct
beam, switch to diffraction mode, select a suitable
camera length, and adjust the diffraction fine focus
control to give a sharp image of the Bragg contrast. At
this stage, the aperture is not exactly centred. To
produce a pattern with cylindrical symmetry, always
use the shift controls because the SA aperture X-Y
mechanical drives are too coarse. Then the C2 current
is slightly reduced, adjusting the shift controls to
retain centring of the aperture. At some stage, an
annular shadow will appear, as described above (Fig.
5A). If this shadow is asymmetric or uneven, further
adjustment of both the C2 stigmators and shift controls
may be required. The shadow is most visible with the
specimen removed from the beam. Finally, the C 2
50
current is increased slightly to give uniform intensity
and the specimen is moved back into the beam. If DF
patterns are required, it is simpler to complete the BF
alignment first and then insert the aperture around
another probe image. Even if the specimen is nomi-
nally eucentric, tilting through large angles always
disturbs this alignment, which is extremely sensitive
to specimen height.
In older analytical microscopes such as the EM400,
removal of the C2 aperture in standard TEM mode
produces a beam with a large convergence angle.
Thereafter, alignment follows the steps described
above.
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