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A few concepts in TEM and STEM explained

Martin Ek
March 19, 2013

1 Introduction
This is a collection of short, qualitative explanations of key concepts in TEM and
STEM. Most of them are beyond what you need to know in the undergraduate
courses, but it can be very useful to have some understanding of the underlying con-
cept rather than to just accept them. They are also quite difficult to explain on the
fly during the labs.1

For TEM:

Section 2 on Fresnel fringes. We use these to gauge the defocus in TEM images,
but what are they?

Section 3 on diffraction. In order to understand what is happening when we


tilt crystals in the TEM we need to go a little beyond Braggs law.

Section 4 on high resolution imaging. Here the importance of knowing the


imaging conditions is discussed briefly.

For STEM:

Section 5 on the Ronchigram. Sometimes described as looking like a boiling


brain, but the wierd name hides a not-too-difficult concept.

1 This document can be found at: www.polymat.lth.se/staff/MartinE/TEMconcepts.pdf

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Underfocus Focus Overfocus

Figure 1: Fresnel fringes at different defocus for an indentation in a glass plate (the
image is formed by light rather than electrons). Photons passing through the inden-
tation will experience a phase change compared to the ones passing through the full
glass plate. In a similar fashion there is a phase difference between electrons passing
through a carbon film compared to ones passing through vacuum.

2 Fresnel fringes
Fresnel fringes show up along edges when we look at something out of focus using a
coherent illumination. This is the case for the edge between the carbon film and vac-
uum, your sample and the carbon film (or vacuum), or aperture edges in the TEM to
give a few examples. What you need to know is that the appearence of fringes indi-
cate that the object you are looking at is out of focus: dark fringes indicate overfocus
and you need to reduce the strength of the objective lens (or lower the sample), bright
fringes indicate underfocus and you need to increase the strength of the objective lens
(or raise the sample). Figure 1 shows Fresnel fringes in an underfocused, in focus, and
overfocused light image of an indentation in a glass plate.2 This section will discuss
why these fringes appear, in some detail for the simpler case of an opaque object (like
an aperture) and very briefly for the much more difficult case of a transparent phase
object (like the carbon film).
Figure 2 shows the imaging geometry for an out-of-focus object.3 There is a fixed
image plane (which we observe), an object plane from which the image is formed, and
the actual object. If we set the strength of the objective lens just right the object plane
and the actual object will coincide, and we will form an in-focus image. In this case
an opaque object should give a sharp transition from bright (in the vacuum where
the electrons pass unimpeded) to dark (where the electrons hit the object and are
excluded from the image). If the object is instead a transparent phase object, which
only changes the phase of the electron wave and not its amplitude, the in-focus image
would be completely uniform as we can only observe the amplitude.
To get the electron wave in the object plane (which is what we will image) we need
2 From Experimental High-Resolution Electron Microscopy by John C. H. Spence.
3 Most of this material is adapted from www.rodenburg.org

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Objective lens
Image plane
Actual object Object plane (fixed)

Fringes!

Figure 2: Image formation of a defocused object. The object plane which we image
in the fixed image plane is below the actual object (overfocused). To get the electron
wave at the object plane we propagate the wave from the actual object a distance f .

to propagate the electron wave from the object a distance f (which is the defocus).
To illustrate the concept lets consider what happens if we image vacuum as in figure
3 (a): in this case the object electron wave has uniform amplitude and phase. To
see what the electron wave is in a certain point furhter down the microscope column
(remember figure 2) we draw paths to this point from every part of the object. The
wave in this point is then the sum of the object wave with a phase change (represented
by the angle of the arrows) proportional to the distance from the object wave to the
point. The parts of the object directly above the point will get roughly the same
phase and add, but the areas further away in the object will contribute less as they
rapidly become out of phase. Adding these arrows from the entire object produces
the (Cornu) spiral shown in figure 3. We then get the total amplitude by connecting
the two end-points of the spiral. As this is the same for every point in the propagated
wave we have uniform intensity.
If we now insert an opaque edge in the object some parts of the object electron
wave will no longer contribute to the propagated wave. Think of this as shielding
some of the paths we drew in (a) so that the arrows from these parts no longer
contribute to the sum. This truncates the spiral as shown in (b) and (c). If the
truncation removes primarily the parts that had the opposite phase of the straight
path this actually increases the amplitude as shown in (c). Of course it is also possible
to remove mainy in-phase paths and thereby decrease the amplitude, as shown in (b).
This produces the oscillating behaviour which far away from the edge will converge
to the vacuum intensity. These are the Fresnel fringes!4
4 For a lecture on this, see: vega.org.uk/video/subseries/8

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(a) No edge (b) A distance away from the edge (c) Close to the edge

de
itu
pl
m
la
ta
To

Dark fringe
Bright fringe
Image intensity

Vacuum Object

Figure 3: Illustation of how a summation of the contribution of all points in the


object yield the wave at a certain distance below the object: with a plane wave object
without an edge(a), an object with an opaque edge some distance away (b), and close
to the opaque edge (c). In the last case we actually get higher intensity in the image
than if we had just imaged vacuum since the out-of-phase contributions are removed.

In the above description you might have noticed that the direction of propagation
of the object wave will make no difference: the fringes will be identical in over- and
underfocus. This is the case for fringes from an opaque edge in the object. An edge
from a phase object on the other hand changes the phase of the electron wave, which
can either add or subtract to the phase change of the propagation. Figure 4 illustrates
how this effects the propagated wave. This simplified picture shows that close to the
edge in the underfocused case there are more in-phase contributions which will result
in a higher amplitude (bright fringe). Conversely, in the overfocus case these contri-
butions are more out-of-phase and reduce the amplitude, which roughly explains the
different appearence of the fringes around your sample with defocus in the TEM.
The Fresnel fringes themselves can be analysed to give information about the
sample, but mostly they are used as a simple gauge of defocus. What you need to
remember from this section is only that if the outermost fringe is dark the image is
overfocused (reduce objective lens strength or lower sample), if instead it is bright
the image is underfocused (increase objective lens strength or raise sample). However
at the exact focus, phase objects are invisible. Since your sample likely (hopefully)

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Underfocus
Object

Overfocus

Figure 4: Propagation of an electron wave up (underfocus) and down (overfocus)


from a phase object. Notice the effect on the phase of the blue arrow which originates
from the region with the phase object.

is a phase object we usually record the images with a slight underfocus, but his is
discussed in more detail in section 4.

3 Diffraction in TEM
First, lets start with Braggs law as illustrated in figure 5 (a).5 In ordet to get intensity
at spot G the rays reaching this point should be in phase, that is the path difference
(marked with orange) should be a multiple of the wavelength . This requirement
describes Braggs law:

2d sin B = n
If we instead look at this in reciprocal space as in (b) we have an incomming wave-
vector kI with the same direction as before, but with a length of 1/. The diffracted
wave-vector kD has the same direction as the diffracted beam, with a length also
equal to 1/. The scattering-vector K is then the difference between the two and has
a length:
1
K = kD kI = 2 sin

According to this model we have diffraction if K corresponds to an actual recip-
rocal disctance between planes in the crystal, that is if |K| = 1/d . If you insert this
definition of K into the formula above it produces Braggs law. To be a bit more
precise we should say that in order to get diffraction K = g where g is the reciprocal
5 Material adapted from ch. 11 and 12 in Williams & Carter

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~ which is the reciprocal of the vector between the planes in the
lattice vector OG,
crystal. In figure 5 notice how g has to fall on a circle (sphere in 3D) with radius
|kI | = 1/ in order to result in diffraction. This is the Ewald sphere and it shows
where the Bragg conditions are fulfilled.

(a) Real space (b) Reciprocal space

B |k I| = |k D| = 1

d kD
kI

2B
G
G K
O O

Figure 5: (a) illustration of Braggs law. When the (orange) path difference between
the two rays is a multiple of the wavelength there is constructive interference and we
see a diffraction spot at G. Some rays will always go straight through and form O,
the orgigin of the diffraction pattern. (b) shows the exact same diffraction geometry
from a reciprocal perspective. Notice how the difference between the incomming
and diffracted wave always end up on a circle independent of the angle : this is the
Ewald sphere.

We can now have a look at an actual crystal containing many planes and construct
~ In figure 6 (a) a very
a reciprocal lattice which shows the location of all possible OG.
simple real space lattice of (green) atoms is shown from the side with the electrons
comming from the top (imagine it extending infinitely to the left and right). The
corresponding reciprocal lattice with the origin O and a series of G are shown in (b)
(imagine it extending infinitely in all directions). Since 0.002 nm the Ewald
sphere is very large compared to |g| as typical plane spacings are on the order of 0.2
nm. As you can see the sphere only intersects O (which it always will) and not any of
the G shown, although it comes close enough for diffraction to occur.
For small crystals the Bragg condition does not need to perfectly satisfied in order
to result in diffraction. This can be justified by looking at Braggs law which is derived
from only two planes: if the angle is close to, but not exactly equal to, the Bragg angle
the two rays will be almost in phase and therefore produce some intensity. Rather
than describing discrete diffraction spots, Braggs law gives a smooth variation with

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the highest intensity at the Bragg angle (where the rays are completely in-phase) to 0
intensity (where the rays are completely out-of-phase). Only for an infinite lattice do
we get actual point-like spots. In this sense the diffraction laws are relaxed when
there are only a few planes present, which is the case in at least one direction for a
thin TEM sample.

(a) Real space (b) Reciprocal space kI

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b b*
a a*
-
10 O 10 20 30 40

Figure 6: Illustration of a real space lattice of atoms (a) viewed from the side, and the
corresponding reciprocal lattice (b) with lattice points corresponding to planes. The
crystal in (a) should be imagined to stretch infinitely to the left and right (and also
into and out of the paper), while the reciprocal lattice extends infinitely in all direc-
tion. The large Ewald sphere in (b) shows for which planes the diffraction conditions
(almost) fulfil the Bragg condition.

Looking closer at figure 6 (b) we can see that the incident wave-vector kI is in
this case comming down perpendicular to the reciprocal lattice-vector a . This means
that the normals of these planes are perpendicular, and the planes themselves parallel,
to the incomming electrons. Again this means that none of theses planes satisfy the
Bragg condition, but since the Bragg angle is very small (since is small, and the
Ewald sphere large) and the crystal is thin we still get diffraction. Since these G are in
the same plane as O and perpendicular to kI they are in the so called zero-order Laue
zone (ZOLZ). Further out where the curvature of the Ewald sphere brings it closer
to G one layer up along b we also get diffraction, and these are in the first-order
Laue zone (FOLZ). Even further away from O the sphere will intersect a layer 2b
up, and so on. The key thing to remember is that often in an electron diffraction
pattern we have a set of spots around O which are formed from planes parallel to
the electron beam, surrounded by rings of spots corresponding to where the Ewald
sphere intersects the higher layers in the reciprocal lattice.
How are the concepts of reciprocal lattices and Ewald spheres used practically at
the TEM? For imaging we often want to view the sample from a certain direction

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(a) Perpendicular (b) Tilted
kI kI
Side view

O
O

ZOLZ
Top view

O O

FOLZ

Figure 7: Illustration of the formation of a diffraction pattern with a crystal having


planes parallel to the viewing direction (a) and slightly tilted (b). The topmost images
show how the Ewald sphere intersects the reciprocal lattice from from a side view.
The bottom images illustrate the same from a top view, which also correspond to the
appearence of the diffraction pattern on the screen. Only the layers along 2b are
shown for clarity.

and the diffraction pattern allows us to see the sample orientation. In high resolution
TEM in particular we want the atoms to line-up into columns, which is the same
as saying that we want to have many planes of atoms parallel to the electron beam.
Figure 7 illustrates the appearence of a diffraction pattern as the crystal is tilted. The
first case corresponds to the same conditions as in figure 6 and we can see a series
of spots from the parallel planes in the ZOLZ surrounded by a ring of FOLZ spots
(which might not be visible for crystals with small unit cells). Only the different b
layers are shown in order to remove some clutter from the illustration: just assume
that there are plenty of possible G in each layer which can be excited where the Ewald
sphere intersects. When the crystal is tilted the diffraction pattern will no longer be
symmetric arround O, but will have more intensity in one direction. Also, the rings
of spots outside the ZOLZ will get a crescent like appearence. Orienting a crystal
into a good direction for high resolution imaging involves recognising these patterns
and trying to make them round and symmetrical around O by tilting.
If we look at a crystal with |a|  |b| then |a |  |b | since |a | = 1/ |a|. From
figure 6 we can see that looking perpendicular to a we expect many spots in the
ZOLZ (since there are many G to interesect) and a long spacing between the ZOLZ
and the FOLZ (since the distance between the layers in b is large). If we instead look
perpendicular to b we should expect fewer spots with larger spacings in the ZOLZ
singe the planes parallel to the beam have small spacings. On the other hand now the

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short a deetermines where the higher order zones appear and as a result they will be
closer to O.

4 High resolution imaging in TEM


For high resolution imaging in TEM the change in phase of the electron wave as
it passes through a very thin sample is used. If the sample is properly oriented so
that we view along colums of atoms (i.e. parallel to planes of atoms) there will be
a phase difference between the electron which have experienced the attractive force
of the atomic nuclei, and the electrons passing between the atoms. The phase of
the electron wave therefor contains information about the location of the atomic
columns, and potentially some information about the chemistry as heavier nuclei
will have a stronger effect than a lighter ones. In the same way a thicker specimen
will give a different phase shift compared to a thin one.
It is not possible to directly detect the phase however, and we need to transfer the
phase information into amplitude variations in the electron wave hitting the detector.
We do this by allowing the objective lens to add a further phase shift to the parts of
the electron wave that have been scattered by the atomic columns, thereby generating
an interference pattern between these electrons and the unaffected electrons which
have passed straight through the sample. The phase shifts caused by the objective
lens are mainly determined by three parameters: the electron wavelength (related to
the accelerating voltage) which determines to what angle the atomic columns scatter
the electrons, the spherical aberration (Cs ) which is an unavoidable lens imperfection
for round magnetic lenses, and the defocus (f ) which we can control by changing
the strength of the objective lens. In practice we use defocus to compensate for
the spherical aberration by recording images with a slight underfocus in a way that
allows as much phase information as possible to be reliably transfered into amplitude
variations.
To show the effect of electron wavelength (and spherical aberration), crystal thick-
ness, and defocus simulated images of NaNb13 O33 are shown in figure 8, 9 and 10.
NaNb13 O33 has a flat unit cell with angles of almost 90 and for the simulations
and the polyhedra-models we are looking down the short axis. In these axamples we
will mainly see Nb atoms (in the centre of the octahedra), but sometimes also Na
(situated in the channels between the octahedra and illustrated by a purple dot) and
O (on the corners of the octahedra). There are many different Nb-Nb spacing in this
structure as there are both octahedra sharing only corners and octahedra sharing ei-
ther two or four edges. This gives plenty of detail in the images which can be affected
by the microscope parameters.

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(a) 120 kV Cs= 2.2 mm (b) 200 kV Cs= 1.0 mm (c) 300 kV Cs= 0.6 mm

Libra 120, W-filament JEOL 2010, LaB6 JEOL 3000F, FEG

Figure 8: (a) This 120 kV TEM cannot resolve the edge sharing octahedra. (b) a
200 kV TEM with a LaB6 filament resolves all the Nb columns. (c) This microscope
corresponds to the JEOL 3000F here in Lund. All Nb atoms are resolved and even
the O columns start to appear as faint grey spots.

(a) t= 1.2 (b) 3.5 (c) 6.5 nm

Figure 9: Illustration of the effect of increasing thickness on images simulated for


a 3000F. Only for a crystal 1.2 nm (about 3 unit cells) thick is the image directly
interpretable in terms of dark atom positions and bright voids. For greater thicknesses
the contrast starts to revert and the O columns become more prominent.

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(a) f= -30 (b) -42 (c) -54 nm

Figure 10: The effect of varying the defocus around its optimal value of -42 nm
(b) on the 3000F. The optimum value is determined by the accelerating voltage and
the spherical aberration. These focus changes represent less than one click on the
course focus knob. Notice how in (c) the contrast has reverted to show bright atoms.

From this we can conclude that it is very important for the interpretation of
high resolution TEM images to know the settings that were used to acquire them.
It is always a good idea to try to match the images with simulations, but beware:
simulated images tend to have much more contrast than experimental images so the
comparison is not always straight forward.

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5 The Ronchigram
The Ronchigram might seem very complicated from the description in the STEM
manual, but as you can see in the ray diagram in figure 11 the underlying principles
are not too difficult. The most important concept here is that at exact focus only a
single point on the sample is illuminated and as a consequence magnified to cover the
entire image: the point is infinitely magnified. When the Ronchigram is defocused
the image is more recogniseable as a simple projection of the sample.
Overfocused Focused Underfocused
Illumination
Sample
Image

Infinite magnification!

Figure 11: The Ronchigram: a shadow image of an object formed by a convergent


illumination. The illustrations show how the image would appear for different defoci
with a perfect lens.

In the previous illustration the illumination was focused perfectly to a single spot.
This is not the case in a real microscope where we have a considerable spherical
aberration, which causes high angle rays to be deflected more than rays which have
a smaller angle to the optical axis. Each ray will therefore be focused to different
points depending on their angle to the optical axis. The Ronchigram will no longer
be either a projected shadow image or an infinitely magnified point, but something
in between. A real Ronchigram of an amorphous carbon film is shown in figure 12
(a). The amorphous film has an even speckled (dotty) pattern which is imaged
differently in different parts of the underfocused Ronchigram.
The ray paths in get a bit more complicated with spherical aberration as seen in
(b), but we can break them down into three cases as in figure 12 (c). The central part
of the Ronchigram comes from rays with low angles which are underfocused. These
form a normal shadow image in the centre (c1). The rays with higher angles are
focused on the sample and form images with infinite magnification. Two rays from
oposite sides of the optical axis, but with equal angles, will magnify a single point on
the sample to the outer parts of the Ronchigram, which will stretch into a ring with

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(a) Underfocused Ronchigram with Cs (c) The zones in the Ronchigram Underfocused image

1 2 3
(Ring of) Infinite radial magnification

(b) Ray diagram


(Ring of) Infinite angular magnification

Probe Amorphous carbon Image

Figure 12: (a) Underfocused Ronchigram with spherical aberration, (Cs ). Three
zones (1-3) show different types of images, which are formed according to (c).

infinite angular magnification (c3). Two rays on the same side of the optical axis, but
with slightly different angles, will coincide on a ring on the sample. In the image
the points on this ring will be stretched radially to form an area with infinite radial
magnification (c2).6
This explains what we see in the Ronchigram, but how is this useful to us? First
of all the Ronchigram tells us the focus. In a focused Ronchigram the central shadow
image dissapears and is replaced by an area of infinite magnification. This also helps
us to select the aperture: ideally we want only rays passing through a single point
on the sample to form our probe. This is not the case for the rays in the ring of
infinte radial magnification, and we select an aperture which excludes these and only
contains the central part of the Ronchigram. If there is astigmatism present the
Ronchigram will no longer be round, but instead oval (as there is different defocus in
different directions). Using the stigmator coils in the microscope we can compensate
for this and correct the Ronchigram until it is round.

6 Adapted from slides by Alan J. Craven

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