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Progress in AberrationCorrected Transmission

Electron Microscopy
Jason R. Albia
2004-62574
PhD MSE

Project Submitted to MSE 285 under Dr. Alberto V. Amorsolo, Jr.

Image:http://media.wiley.com/product_data/cov
erImage300/10/04705185/0470518510.jpg

Brief Introduction of Report


Since the invention of electron microscopes, there had
been numerous efforts to increase its resolution limit in
order to maximize its potential particularly in
characterization of material properties. This document
aims to provide a brief report on the history and recent
researches on the aberration correctors that reduces the
intrinsic spherical and chromatic aberrations in electron
lenses used in electron microscopes particularly in
Transmission Electron Microscope (TEM).

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Outline
I. Basic Information on TEM
II. Spherical and Chromatic Aberration
III. Aberration Correctors
A. Convetional Correctors
1. Octupole / Quadropole Assembly
2. Hexapole Assembly
3. Advanced Hexapole Assembly
B. Future Correctors
4. STM Cc Correctors
5. Hexapole Aplanat Corrector
6. Cc/Cs corrector for TEAM

IV. Future Outlook

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I. Transmission Electron Microscope (TEM)


Basic Information
invented by invented in 1933 by Max Knoll
and Ernst Ruska at the Technical College in
Berlin
microscopy technique in which beam of
electrons is transmitted through an ultrathin specimen
capable of producing real images or
crystallographic information (i.e., diffraction
pattern and Kikuchi lines) of specimen

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The
first
practical
TEM,
originally installed at IG FarbenWerke and now on display at
the Deutsches Museum in
Munich, Germany

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I. Transmission Electron Microscope (TEM)


Basic Information
has three basic components
1. Illumination System
-consist of electron guns and electron lenses
-can be operated in two principal modes
(convergent beam for imaging and microanalysis or
parallel beam for diffraction)

2. Objective Lens/Stage System

-heart of TEM where beam-specimen interaction


takes place
-where the beam is manipulated for STEM imaging

3. Imaging System

-uses several lenses to magnify the image or


diffraction pattern produced by object
-focuses the image on the viewing screen

Basic layout of Transmission


Electron Microscope.
(http://www.wikiwand.com/en/Transmission_electron_mi
croscopy)

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I. Transmission Electron Microscope (TEM)


Basic Information
provides better resolution than scanning
electron microscope (SEM)
highest resolution reached in phase
contrast mode is around 0.5 (0.050
nm)* (half the size of hydrogen atom)
this resolution is less than the practical
limitations or achievable resolution of the
TEM which about in the order of electron
wavelength =3.7 2.0 pm for typical 100300 keV accelerating potential

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The
first
practical
TEM,
originally installed at IG FarbenWerke and now on display at
the Deutsches Museum in
Munich, Germany

UP Diliman, PH

I. Transmission Electron Microscope (TEM)


Improving Resolution:
Unfortunately, the resolution limit of the TEM is not
dictated by electron wavelength () but by the intrinsic
imperfection of electron lenses
These imperfections are called spherical and chromatic
aberrations.
Resolution therefore can be improved by reducing these
aberrations using auxiliary lenses called aberration
correctors.

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II. Spherical and Chromatic Aberrations


Background
In 1947, Otto Scherzer proposed the limit of attainable resolution of
electron microscope.
Scherzer Theorem:
Spherical aberration and axial chromatic aberration are
unavoidable for static rotationally symmetric electron lenses
free of space charges.

It follows then that to design an aberration-free objective lens, one has


to deviate from Scherzer Theorem by either:
1. using of multipole system or time varying field, or
2. placing a charge at the back focal plane
The second method is not possible if one does not want to disturb
electron path.
The first method has been recognized as possibilities to correct
aberrations.
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II. Spherical and Chromatic Aberrations


TIMELINE
There had been considerable attempts to improve lens system of electron
microscope to reduced aberrations.
Year

Development

1950s

First attempts by Seeliger (1951) and Moellenstedt (1956) in


Germany

1960s

Deltrap (1964) and Hardy (1967) started building aberration


corrected system in Cavendish, UK

1980S

Crewe (1982) compensate aberration in scanning TEM


Hely (1982) proof of principle that spherical and chromatic
aberration can be minimized
attempt to reduced aberration for low voltage scanning electron
microscope (LVSEM) for biological sample

1990s

first aberration correction system with an improvement of


resolution from 5.6 nm down to 1.8 nm (Zach & Haider, 1995)
in LVSEM

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II. Spherical and Chromatic Aberrations


TIMELINE
There had been considerable attempts to improve lens system of electron
microscope to reduced aberrations.
Year

Development

1990s

Rose (1990) proposed a new hexapole correction system for


such an electron microscope (EM), which would allow the
imaging of a fairly large object area at a resolution around 0.1
nm.
Haider (1997) breakthrough in correcting aberration in highresolution electron microscope
Krivanek (1997) proof of principle was demonstrated for
compensation of the spherical aberration for probe-forming
system

2003

Krivanek (2003) breakthrough in resolution was achieved with a


quadropole-octupole corrector. Since then, compensation of
spherical aberration has stimulated several groups to exploit
benefits of such improved high-resolution electron microscope.

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II. Spherical and Chromatic Aberrations


Lens Aberrations
well known from optics, also play a role
in electron microscopy.
not unique to the magnetic lenses used
in electron microscopes, but rather a
fundamental problem of optical systems.
Spherical Aberration, Cs
Rays entering a round lens system away
from the optical axis are refracted more
strongly than those entering close to the
optical axis.

Chromatic Aberration, Cc
Rays with different wavelengths enter a
round lens resulting in the rays
diffracting differently depending on their
wavelength.

The shorter the focal length, the smaller the spherical


aberration coefficient and hence smaller amount of
blur.

The smaller the energy width of the electron source


and/or the better the stability of the high voltage
(the lens), the smaller the chromatic spread and
hence smaller chromatic aberration.
Images: https://physics.aps.org/articles/v2/85

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II. Spherical and Chromatic Aberrations


Point Resolution Limit (Rp)

R p ~ Cs 4
1

Cs coefficient of spherical aberration


electron wavelength
Effects of Spherically Aberrated Lens
Rays passing at a high angle to the optic
axis are brought to a focus closer to the
lens than the rays passing along or at a
small angle to the optic axis.
incorrectly focused rays produce a
smearing in the image, represented in the
illustration by the enlarged blue disk.

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In a standard electron lens with spherical aberration, rays at


different angles to the optic axis are brought to a focus at
different points. (b) The effect of correcting the spherical
aberration is to bring all rays into focus at the same point.
The small blue area on the right of the lens represents the
aberration disc.

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III. Aberration Correctors


Spherical and Chromatic Aberrations are reduced using aberration
correctors.
Correctors use multipole lenses that are capable of generating a negative
value of Cs and thus can cancel the positive Cs of the round lens. The net
effect is the elimination / reduction of Cs .
Rays scattered at high angles to the optic axis are brought to the correct
focus, and the point resolution limit is extended.
There are several types of aberration correctors
Conventional Correctors
Future Correctors
Octupole / Quadropole Assembly
STM Cc Correctors
Hexapole Assembly
Hexapole Aplanat Corrector
Advanced Hexapole Assembly
Cc/Cs corrector for TEAM

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Conventional Correctors
1. Octupole / Quadropole Assembly
2. Hexapole Assembly
3. Advanced Hexapole Assembly

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III. Aberration Correctors


1. Octupole / Quadropole Assemby
Corrector uses 4 quadropoles and 3
octupoles
quadropoles are made from 1 separate
poles
weak dipoles, quadropoles and sextupoles
of arbitrary orientation and weak B-type can
be excited in each quadropoles stage
octupoles are made from just 8 poles and
are optimized for maximum strength but also
contain weak auxiliary dipoles and
quadropoles

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Schematic drawing of Cs corrected STEM


using quadropole-octupole coupling.

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III. Aberration Correctors


1. Octupole / Quadropole Assemby

Improvements:
Demonstrate that the Cs corrector can make
spherical aberration adjustable while adding
only 0.2 mm chromatic aberration

autotuning software tune up all aberrations up


to third order with high degree of precision
Resolution limit enhanced from
(uncorrected) down to 0.8 (corrected)

Actual Cscorrected VG HB 501 STEM


using quadropole-octupole coupling.

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III. Aberration Correctors


1. Octupole / Quadropole Assemby
Probe Size

The current in the probe is given by:

d (d 2aber d 2 source)0.5
The aberration determined probe size

d aber 0.4Cs 4
1

B is the gun brightness


is the half angle of the optimum
illumination

For Cs-limited system and


5

d aber 0.4C5
1

I B 2d 2 source 2 / 4

For Cs-corrected one. Here, Cs=1.33mm,


=3.7 pm and C5=10 cm (for corrected m
microscope).
Dellby et al. Journal of Electron Microscopy 50(3): 177-185 (2001)
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III. Aberration Correctors


1. Octupole / Quadropole Assemby

Other Advantages:
Optimum use of a flat (corrected) aberration function
Insensitivity to field aberration
Immunity to resolution lost due to chromatic aberration
Improved resolution
Increased beam current

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III. Aberration Correctors


1. Octupole / Quadropole Assemby

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III. Aberration Correctors


1. Octupole / Quadropole Assemby

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III. Aberration Correctors


1. Octupole / Quadropole Assemby

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III. Aberration Correctors


2. Hexapole Assembly
The first successful development of a corrector to
compensate the spherical aberration of the objective
lens of a 200 kV TEM was a hexapole correction system.
It is based on a pair of strong hexapoles and two
transfer round-lens doublets which reduces the fourthorder aberration from previous design
Additional transfer lens doublet is incorporated to
avoid introduction or increase of off-axial aberration

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Aberration Correctors
2. Hexapole Assembly
The first successful development of a corrector to
compensate the spherical aberration of the objective
lens of a 200 kV TEM was a hexapole correction system.
Thus, the design consists of two modules:
Upper Module double transfer lens and additional
image deflectors and stigmator
Lower Module - two multipole stages to generate
the strong hexapole fields (HP), two transfer
lenses (TL) and a final adapter lens (ADL)

transfer lens doublet in the upper part matches the


coma-free plane of the objective lens with that of the
hexapole corrector.

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Aberration Correctors
2. Hexapole Assembly
The first successful development of a corrector to
compensate the spherical aberration of the
objective lens of a 200 kV TEM was a hexapole
correction system.
coma-free plane of the objective lens is situated very
close to its back focal plane; without the transfer
system, off-axial third-order coma and fifth-order
spherical aberration C5 would be too large to achieve a
substantial improvement in high resolution.
This arrangement has the advantage that all secondorder aberration rays vanish identically outside the
corrector.
Today, this system forms the basis for all available
hexapole correctors.
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Aberration Correctors
2. Hexapole Assembly

Diffractograms from the (a) uncorrected and (b) nearly corrected TEM state. In (a), the
black rings at the 0.19 nm spacing and other rings beyond (at smaller spacings) indicate
undesirable contrast reversals, a direct consequence of Cs. In (b), the contrast is continuous
well beyond 0.19 nm. (The visible fringes are a device used to distinguish genuine signal
from mere noise.) The dotted circle corresponds to a 10% signal transfer at 0.12 nm.
(Reprinted with permission from17. 2004 JEOL.)
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III. Aberration Correctors


2. Hexapole Assembly
A fully corrected lens assembly produces a tableau of identical diffractograms, whereas the same
assembly set to a Cs of 0.1 mm produces diffractograms whose character depends on the incident
beam direction, as shown in below.

Two Zemlin tableau. (Left) All diffractograms are identical indicating full correction
of the lens aberrations, including Cs. (Right) An imposed Cs of 0.1 mm is revealed in
the outer diffractograms as an induced change in focus and astigmatism. The outer
tilt is 18 mrad.

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III. Aberration Correctors


2. Hexapole Assembly
Improvements:
higher-order aberrations remain rather stable
Images of ceramic specimens can now reveal light elements in the
structures and even measure the occupancy of oxygen atoms in
individual columns.
Small particles can be investigated more satisfactorily now that the
contrast of the supporting amorphous layer can be minimized
Reduced probe size resulting in a higher resolution STEM image, or
an increased condenser aperture size leading to better signal levels for
microanalysis.

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III. Aberration Correctors


3. Advanced Hexapole Corrector
In 2004, the Transmission Electron Aberration-corrected Microscope
(TEAM) Project (TEAM 2005) set the goal of 50 pm resolution in STEM
and TEM.
To achieve this goal, redesign of conventional hexapole corrector is
necessary.
This is done by introducing an advanced hexapole corrector also called as
D-COR.
D-COR reduces the intrinsic sixfold astigmatism A5 introduced by the
corrector and to offer the possibility to compensate for the fourth-order
parasitic aberrations by appropriate alignment tools.

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III. Aberration Correctors


3. Advanced Hexapole Corrector
Improvements
D-COR-type push the STEM d50 probe size down to 50pm and to increase
the probe current without loss of spatial resolution for an acceleration
voltage of 200 or 300 kV.

Ronchigram of an amorphous layer


with an outer border showing a
semi-aperture of 80 mrad. The
aberration-free area extends in this
case to about 60 mrad.

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III. Aberration Correctors


3. Advanced Hexapole Corrector
Improvements
D-COR-type push the STEM d50 probe size down to 50pm and to increase
the probe current without loss of spatial resolution for an acceleration
voltage of 200 or 300 kV.
Annular dark field (ADF) image of
Ge (112) which clearly shows the
dumbbell structure in 112
orientation. In the line scan
shown at the right side, one can
easily discriminate between the
individual atom columns showing
a spacing of 0.82 . The
histogram indicates the welladapted black level and gain of
the ADF signal.
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Future Correctors
4. STM Cc Correctors
5. Hexapole Aplanat Corrector
6. Cc/Cs corrector for TEAM

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III. Aberration Correctors


4. STM Cc Correctors
The motivation is to exploit full advantage of the advanced hexapole STEM
corrector
Done by combining corrector with a cold field emitter or high-brightness
Schottky Field Emission Gun monochromator
Or to combine the performance of the D-COR with Cc-correction
capability to compensate simultaneously within one corrector the spherical
and chromatic aberrations.
The lateral resolution is only dependent on the product of energy with E
and the chromatic aberration coefficient
This design maintain the angular intensity with an increased aperture thus
high current beam can be obtained

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III. Aberration Correctors


4. STM Cc Correctors
The attainable STEM d50 probe size with an assumed virtual source size of 25nm for
an illumination angle of 25 and 40 mrad and for three different energy lengths is
shown in below.
Plots of calculated electron probe shapes
for various parameters of a Cs-corrected
300 kV STEM. The Cs value is 5m; the
energy width E is 0.7 eV; the illumination
cone is (a) 25 mrad and (bd) 40 mrad;
and the energy length is (b) 1.7 eV mm, (c)
0.8 eVmm and (d) 0.1 eV mm. Other
parameters: (a) Cc =2.4 mm, dFWHM =46.16
pm, d30 =41.26 pm, d50 =61.96 pm, d59 =
75.32 pm; (b) Cc =2.4 mm, dFWHM =36.08
pm, d30 =47.53 pm, d50 =81.36 pm, d59
=101.28 pm; (c) Cc =1.2 mm, dFWHM =33.74
pm, d30 =32.76 pm, d50 =49.97 pm, d59
=60.60 pm; and (d) Cc = 0.1 mm, dFWHM
=32.21 pm, d30 =25.48 pm, d50 =36.44 pm,
d59 =42.11 pm.

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III. Aberration Correctors


4. STM Cc Correctors
Improvements
a resolution in the sub-ngstrm region can be achieved
sharpened electron probe by using monochromator
high density electron probe can be positioned onto single
atomic column which is advantages for analytical
purposes
The requirement for a resolution below 1 in the STEM
using Cc-corrected is still ongoing project.

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III. Aberration Correctors


5. Hexapole Aplanat Corrector
aplanatic means an optical system that is free from
spherical aberration and off-axial coma
This can be done by using transfer lens systems to avoid
fifth order aberration that arises from a combination of
aberration from objective lens and corrector
Transfer lens system also allows imaging of the coma-free
plane of the objective lens into the coma-free plane of the
corrector.
However, magnetic lenses still introduces anisotropic offaxial coma thus, optical system should be called semiaplanat
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III. Aberration Correctors


5. Hexapole Aplanat Corrector
hexapole semi-aplanats consisting of a magnetic round lens and a
hexapole doublet are commercially available options for both the
TEM and the STEM
Optimized and stable current drivers and high voltage supplies,
monochromators have dramatically improved the limit of resoultion.
Large apertures is the remaining anistropic part of the off-axial coma
seriously limit the field of view that can be imaged
Hence, one needs an advanced hexapole corrector that is also capable
of eliminating the anisotropic part of the off-axial coma
Combining this corrector with a magnetic objective lens results in a
true aplanatic system

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III. Aberration Correctors


5. Hexapole Aplanat Corrector

The set-up of the quadrupoles of a Cs/Cc corrector as used for an


LVSEM and which, in principle, could also be used for a highresolution probe-forming system. The axial rays are focused at the
specimen plane although the energy is varied by 10 per cent.

In order to generate the required azimuthal offaxis coma, the hexapole fields have to be rotated
with respect to each other around the optical
axis (as shown in the figure above).

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Layout of a minimal aplanatic hexapole corrector.


This system only consists of three hexapole
elements and two transfer lens doublets. The
hexapole elements have to be oriented around the
optical axis with respect to each other.

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III. Aberration Correctors


5. Cc/Cs corrector for TEAM
To optimize resolution of electron microscope, intrinsic spherical
and chromatic aberration should be reduced.
This is only possible with the consequence that other imaging
modes, e.g. in situ or Lorentz microscopy suffer from this
optimization.
No improvement for these imaging modes could be gain by
correcting spherical aberration alone.

Real breakthrough in electron microscopes if chromatic aberration


could be reduced in all imaging modes.
An initiative was done by Gibson (2000) to reduced chromatic
aberration in imaging a 50 pm lateral resolution.
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III. Aberration Correctors


5. Cc/Cs corrector for TEAM
This task also entails a need for a
large field of view which will
require the compensation of the
off-axial coma to achieve a
aberration-free imaging of the
entire image.
This is possible is introducing a
new Cc/Cs corrector with precise
electron optical component and
stable power supplies

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The prototype of this achroplanator


has been designed and constructed,
and it has been built into a Titan.

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III. Aberration Correctors


5. Cc/Cs corrector for TEAM
The apochromat consisting of 10
quadrupole
elements
that
can
compensate Cs, Cc, and the off-axial
coma B3 of the objective lens was
designed.
This system allows aberration-free
imaging at a resolution of 50 pm at 200
and 300 kV and a very large field of
view.
The prototype of this achroplanator
has been designed and constructed,
and it has been built into a Titan.
The C-COR which has an overall
corrector length of 83 cm.
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III. Aberration Correctors


5. Cc/Cs corrector for TEAM
C-COR is in operation and has already
proved
its
capability to fully
compensate the chromatic aberration
of the objective lens for the main
acceleration steps in the range from 80
up.
The measurement of the chromatic
aberration shows almost no change of
defocus even for a very large variation
of energy of 1000 eV.

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The prototype of this achroplanator


has been designed and constructed,
and it has been built into a Titan.
The C-COR which has an overall
corrector length of 83 cm.
UP Diliman, PH

III. Aberration Correctors


5. Cc/Cs corrector for TEAM
Measurement of chromatic aberration with Cc/Cs corrector TEAM is
practically resulted to no change in focusing.

Measurement of the induced defocus when the energy is varied over a large range from
1500 to +1500 eV. For a large range of energy of almost 1000 eV, there is no noticeable
change of focus which indicates a very small Cc.

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III. Aberration Correctors


5. Cc/Cs corrector for TEAM

An extended Zemlin tableau of (a) an only Cs-corrected TEM and (b) a Cc/Cs-corrected TEM. In
the case of the correction of Cc, the contrast of the Thon rings is not damped for the images
taken with a tilted beam, whereas for the Cs-only correction this damping in the tilt direction
is clearly visible. The tilt of the beam is in both cases 35 mrad.

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IV. Future Outlook


There are still on-going researches in various fields that aim to develop
new corrector systems to further reduced the effect of spherical and
chromatic aberrations that is applicable to various imaging modes such
as Lorentz microscopy, in situ, and cryo-microscopy of electron
microscopes. Some of these projects are:

1. for high-resolution analytical purposes, a Cc and Cs-corrected probe


corrector for a TEM/STEM;
2. an aplanatic correction system for a very large field of view;
3. TEAM corrector for TEM.

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Journal References
1. M. Haider, P. Hartel, H. Mller, S. Uhlemann and J. Zach, Phil. Trans. R.
Soc. A (2009) 367, 36653682.
2. C. Hetherington. MaterialsToday December 2004 Issue. ISSN:1369
7021 Elsevier Ltd 2004
3. N. Dellby, O. Krivanek, P Nellist, P. Batson, and A. Lupini. Journal of
Electron Microscopy 50(3): 177-185 (2001)
4. I. Maclaren, Q. Ramasse. International Materials Reviews Vol 59 No.
3 (2014).
5. B. Freitag, S. Kujawa, P.M. Mul, J. Ringnalda, P.C. Tiemeijer.
Ultramicroscopy 102 (2005) 209214
6. M. Haider, H. Rose, S. Uhlemann, E. Schwan, B. Kabius, K. Urban.
Ultramicroscopy 75 (1998) 53-60.
7. C. Kisielowski; et al. (2008). Microscopy Microanalysis 14: 469477

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