U.S. patent number 3,908,124 [Application Number 05/484,740] was granted by the patent office on 1975-09-23 for phase contrast in high resolution electron microscopy.
This patent grant is currently assigned to The United States of America as represented by the United States Energy. Invention is credited to Harald H. Rose.
United States Patent |
3,908,124 |
Rose |
September 23, 1975 |
Phase contrast in high resolution electron microscopy
Abstract
A device is provided for developing a phase contrast signal for
a scanning transmission electron microscope. The lens system of the
microscope is operated in a condition of defocus so that
predictable alternate concentric regions of high and low electron
density exist in the cone of illumination. Two phase detectors are
placed beneath the object inside the cone of illumination, with the
first detector having the form of a zone plate, each of its rings
covering alternate regions of either higher or lower electron
density. The second detector is so configured that it covers the
regions of electron density not covered by the first detector. Each
detector measures the number of electrons incident thereon and the
signal developed by the first detector is subtracted from the
signal developed by the record detector to provide a phase contrast
signal.
Inventors: |
Rose; Harald H. (Darmstadt,
DT) |
Assignee: |
The United States of America as
represented by the United States Energy (Washington,
DC)
|
Family
ID: |
23925410 |
Appl.
No.: |
05/484,740 |
Filed: |
July 1, 1974 |
Current U.S.
Class: |
250/311;
250/310 |
Current CPC
Class: |
H01J
37/244 (20130101); H01J 37/263 (20130101); H01J
2237/24465 (20130101); H01J 2237/24507 (20130101) |
Current International
Class: |
H01J
37/244 (20060101); H01J 37/26 (20060101); H01J
037/26 (); G01N 023/00 () |
Field of
Search: |
;250/305,306,307,309,310,311 |
References Cited
[Referenced By]
U.S. Patent Documents
Primary Examiner: Lawrence; James W.
Assistant Examiner: Grigsby; T. N.
Attorney, Agent or Firm: Carlson; Dean E. Churm; Arthur A.
Gottlieb; Paul A.
Government Interests
CONTRACTUAL ORIGIN OF THE INVENTION
The invention described herein was made in the course of, or under,
a contract with the UNITED STATES ATOMIC ENERGY COMMISSION.
Claims
The embodiments of the invention in which an exclusive property or
privilege is claimed and defined as follows:
1. In a scanning transmission electron microscope operating in a
condition of defocus such that there are within the cone of
illumination regions alternately of the quality of higher electron
density and of lower electron density, the alternate density
regions being caused by the interference within the cone of
illumination of electrons elastically scattered by the specimen
with electrons unscattered by the specimen, a device for developing
a phase contrast signal, comprising:
a first detector positioned within the cone of illumination, and
being of such radial configuration with respect to the optical axis
that electrons within all alternate regions of the cone of
illumination having one of the qualities of density are incident
thereon, said first detector being responsive to electrons incident
thereon to develop a first output signal representative of the
intensity thereof, a second detector positioned within the cone of
illumination and being of such configuration that electrons within
the cone of illumination not incident upon said first detector are
incident upon said second detector, said second detector being
responsive to electrons incident thereon to develop a second output
signal representative of the intensity thereof, a differencing
circuit coupled to said first and second detectors and responsive
to said first and second output signals therefrom to subtract said
first output signal from said second output signal and to develop a
phase contrast signal which is the subtraction of said first output
signal from said second output signal, and utilization means
coupled to said differencing circuit for utilizing said phase
contrast signal.
2. The device of claim 1 wherein said regions within the cone of
illumination of alternate electron density are concentric with the
cone of illumination, and wherein said first and second detectors
are concentric with said cone of illumination.
3. The device of claim 2 wherein the defocus length .DELTA.f of the
microscope is within 8 d.sup.2 /.lambda. of .DELTA.f = -C.sub.1
where d is the limit of resolution, .lambda. is the electron
wavelength and C.sub.1 is the first order coefficient of spherical
aberration.
4. The device of claim 3 wherein .DELTA. f = -C.sub.1.
5. The device of claim 4 wherein the microscope has a Seidel order
of n = 3 and an angle of illumination of
1.71(.lambda./C.sub.3).sup.1/4 radians, and wherein electrons
transmitted through the specimen and thereby directed between
approximately 0.92(.lambda./C.sub.3).sup.1/4 radians and
approximately 1.44(.lambda./C.sub.3).sup.1/4 radians with respect
to the optical axis are incident upon said first detector where
C.sub.3 is the third order coefficient of spherical aberration.
6. The device of claim 4 wherein the microscope has a Seidel order
of n = 5 and an angle of illumination of
1.87(.lambda./C.sub.5).sup.1/6 and wherein electrons transmitted
through the specimen and thereby directed between approximately
1.23(.lambda./C.sub.5).sup.1/6 radians and approximately
1.77(.lambda./C.sub.5).sup.1/6 radians with respect to the optical
axis are incident upon said first detector where C.sub.5 is the
fifth order coefficient of spherical aberration.
7. The device of claim 2 wherein said first detector includes a
zone plate having at least one ring and wherein said second
detector includes a disc so positioned that said first detector is
between said specimen and said second detector.
8. The device of claim 2 wherein said first detector includes a
zone plate having at least one ring and wherein said second
detector includes a zone plate having at least one ring.
Description
BACKGROUND OF THE INVENTION
The scanning transmission electron microscope has been operated
predominantly in the dark field mode using an annular detector to
collect scattered electrons falling outside the cone of
illumination, as described in U.S. Pat. No. 3,626,184. For
resolutions with the limit of resolution d .gtorsim. 2 A, the dark
field detector yields a high collection efficiency resulting in a
short scanning time and reduced dosage of electrons incident on the
specimen for each element of the reproduced image. The smaller the
dose to produce the image, the lower the radiation damage to the
specimen. However, as d is made smaller, more of the elastically
scattered electrons remain within the illumination cone, and fewer
of them fall onto the dark field detector. Thus, the amount of
information obtainable with the dark field detector decreases as
resolution increases.
Within the cone of illumination, a phase contrast image results
from an interference of unscattered electrons with elastically
scattered electrons. Detection of the phase contrast image or
interference pattern within the cone of illumination would provide
the information relative to elastically scattered electrons within
the cone of illumination necessary to allow increased resolution in
the scanning electron microscope without an unacceptable increase
in dosage.
It is therefore an object of this invention to provide an improved
detection system for a scanning electron microscope.
Another object of this invention is to provide a means for
obtaining information relative to elastically scattered electrons
obtaining information relative to elastically scattered electrons
in the cone of illumination.
Another object of this invention is to provide a means for
obtaining a phase contrast image within the cone of illumination
formed by interference between the unscattered electron wave and
the elastically scattered electron wave.
SUMMARY OF THE INVENTION
For the practice of this invention a device is provided for
developing in a scanning electron microscope a phase contrast
signal representative of the interference within the cone of
illumination of electrons elastically scattered by the specimen
with unscattered electrons. The microscope is operated in a
condition of defocus so that within and concentric with the cone of
illumination there will exist alternate regions of constructive and
destructive interference between the waves which will correspond to
regions of higher and lower electron density. A first detector is
placed within and concentric with the cone of illumination and has
the form of a zone plate covering alternate regions of higher or
lower electron density and is responsive to electrons incident
thereon to develop an output signal representative of the incident
electrons. A second detector is placed within and concentric with
the cone of illumination and is so configured that it detects and
develops an output signal representative of those regions of higher
or lower electron density undetected by the first detector. The
output signals are subtracted from each other to develop a phase
contrast signal.
BRIEF DESCRIPTION OF THE DRAWINGS
FIG. 1 is a drawing of a scanning transmission electron microscope
with the phase contrast detector;
FIG. 2 is a set of curves showing the sine of the phase
distribution over the cone of illumination;
FIG. 3 is a sectional view taken along line 3 -- 3 of FIG. 1;
FIG. 4 is a drawing of another embodiment of this invention;
FIG. 5 is a drawing of another embodiment of this invention;
and
FIGS. 6 and 7 are curves showing the phase contrast intensity as
related to defocus.
DETAILED DESCRIPTION OF THE EMBODIMENT
Referring to FIG. 1 there is shown a portion of the scanning
electron microscope, more particularly described in U.S. Pat. No.
3,626,184. The microscope includes an aperture 10 through which an
electron beam 12 is projected, an objective lens system 14 which
focuses electron beam 12 to as small a spot as possible at the
focus point 15 along the optical axis 16 of the lens system 14. The
angle .theta..sub.0 which defines the envelope of the focused beam
is called the illumination angle. The focused spot is scanned over
the area of specimen 20 to be examined in a manner similar to a TV
scan. Sweep generator 22 provides scanning voltages to a deflection
system in the microscope (represented by deflection plates 23 and
25). Voltages on the deflection plates act to move the electron
beam across the specimen in a desired manner.
Sweep voltages from sweep generator 22 are also applied to the
deflection plates of CRT 26 (represented by deflection plates 28
and 29). The sweep voltages applied to the CRT 26 are in
synchronism with the sweep voltages applied to the electron
microscope so that the electron beam in the CRT 26 traces a raster
on the face of the tube as the specimen 20 is scanned. Detection
system 31 placed beneath specimen 20 receives electrons transmitted
through the specimen. Signals which are developed by the various
types of detectors of the detector system 31 are applied to cathode
32 of CRT 26 to modulate the intensity of the electron beam in CRT
26 according to the electrons received by detector system 31. The
modulated electron beam forms a picture on the face of CRT 26
representative of the specimen being observed.
The electrons which reach the plane of detector 31 comprise three
components, those elastically scattered, those inelastically
scattered and unscattered electrons. Separation of information
relative to inelastically scattered electrons is obtained from
spectrometer 38, more particularly described in U.S. Pat. No.
3,191,028 and that of elastically scattered electrons falling
outside the cone of illumination 40 is obtained from dark field
detector 42, more particularly described in U.S. Pat. No.
3,626,184. The device herein disclosed deals with obtaining
information relative to elastically scattered electrons falling
within the cone of illumination 40.
Within the cone of illumination, a phase contrast image results
from an interference of the electron wave associated with electrons
elastically scattered by specimen 20 with the wave associated with
the unscattered electrons. The interference pattern arises because
the phase of the scattered wave is shifted with respect to the
unscattered wave. Additional phase shift in the cone of
illumination will be caused by any spherical aberration of lens
system 14 and any defocus in the microscope.
Defocus refers to a distance or defocus length .DELTA. f between
the specimen 20 and the focus point 15. If the microscope were in
focus, point 15 would generally coincide with specimen 20. It is
well known that phase shifts can be introduced between electrons in
the cone of illumination by operating the microscope in an
out-of-focus condition, that is with .DELTA.f less than 0, which
means that focus point 15 is before the specimen as shown in FIG.
1.
The spherical aberration of a lens system relates to imperfections
of the lens system causing failure of all the electrons of the
focused beam to converge to the same spot point 15. It is a
variable quantity depending upon the parameters of lens system 14.
Calculated approximations of the distribution of the beam about
point 15 associated with spherical aberration in the form of power
expansions are well known.
The phase contrast or interference pattern in the cone of
illumination will show up most prominently when the total phase
shift caused by the specimen, the defocus .DELTA.f and the
spherical aberration of lens system 14 approaches 0 of .pi. or
multiples thereof, which is the condition of maximum constructive
or destructive interference. We may approximate the phase shift
between elastically scattered and unscattered electrons caused by
the specimen as being 90.degree.. A constant phase shift of 0 or
.pi. over the entire illumination cone is never possible due to the
conservation of the number of electrons. However, concentric hollow
cones or regions within the cone of illumination with total phase
shift alternately being 0 or .pi. in each cone is allowable. This
is illustrated in FIG. 2 by the dashed phase distribution curve 50
which refers to the lower scale of FIG. 2. Curve 50 is the sin of
the ideal total phase shift .gamma., which is a step function,
where in FIG. 2, ##EQU1## c.sub.3 is the third order coefficient ot
spherical aberration and .THETA. is the angle with the optic axis
16. These hollow cones or regions of constructive and destructive
interference will also be hollow cones of higher and lower electron
density. It is known that by operating a microscope in an
out-of-focus condition, with .DELTA.f less than 0, an interference
pattern with regions approaching total phase shift of 0 or .pi. can
be achieved. For example, consider the distribution of total phase
shift when the defocus .DELTA.f = -C.sub.1 for a microscope
uncorrected for spherical aberration, that is one with a Seidel
order of n = 3, where C.sub.1 is the first order coefficient of
spherical aberration. The - sin of the total phase shift .gamma. is
shown by curve 51 which refers to the lower scale of FIG. 2. The
distribution of curve 51 provides a reasonable approximation of the
ideal distribution of the step function of curve 50.
To extract information out of the cone of illumination 40 where the
sin of the total phase shift approximates the step function as
illustrated by curve 51 of FIG. 2, two-phase contrast detectors are
placed beneath specimen 20 within the cone of illumination 40 as
shown in FIG. 1 and FIG. 3. The first detector 52 has the form of a
zone plate, each of its m rings generally covering all hollow cones
of either construction or destructive interference. For the phase
distribution illustrated by curve 51 of FIG. 2 only one such zone
plate ring 52 is required, i.e., m = 1, to cover the sole region of
lower density of this distribution. The second detector consists of
a detector in the form of a disc 53 covering the entire
illumination cone in the shadow of ring 52 covering those hollow
cones not covered by ring 52 which in this embodiment includes the
central and outer higher density regions. An alternate embodiment
is shown in FIG. 4 where the second detector is coplanar with ring
54 of the zone plate type first detector. Here the second detector
is also in the form of a zone plate with a central disc 55 and an
outer ring 56. The signals of the disc 55 and ring 56 are added
together to give the same signal as disc 53 of FIG. 1. A further
alternate embodiment is illustrated in FIG. 5 for detecting this
phase distribution. Here the second detector is a zone plate with a
disc 57 and ring 58 whose signals are added and the first detector
is a disc 59 covering the entire illumination cone. In this case,
rings 57 and 58 give the signal developed by disc 53 of FIG. 1 and
disc 59 gives the signal developed by zone plate 52 of FIG. 1.
Both detectors are intended to develop output signals corresponding
to the number of electrons incident thereon and may be, for
example, silicon surface barrier detectors. The signals of these
detectors are available simultaneously and can be conveniently
combined and applied to the cathode 32 of CRT 26 or only the signal
from one detector covering all regions of higher or lower electron
density may be used to vary the intensity of each element of the
raster scan. Best phase contrast is obtained by subtracting the
signal from one detector from the signal from the other detector
such as by means of a differencing circuit 60 to form a phase
contrast signal. Each scanned element of the specimen varies the
phase shift according to its own particular characteristics.
Because of the conservation of electrons, the variation in phase
shift which causes an increase in electron density in the hollow
cones of constructive interference must necessarily also result in
a decrease in the density in the hollow cones of destructive
interference and visa versa. By subtracting the two signals the
effect of each scanned element of the specimen on the resulting
phase contrast signal from differencing circuit 60 will be twice as
large as the effect on the signal from only one detector. This is
because the effect on phase contrast in each region or hollow cone
observed by each detector will be opposite in sign. The raster scan
of CRT 26 represents a comparison of intensities between each
element of the scan so that by doubling the effect of something
which varies the comparative intensity one will have made more
visibly evident the phase contrast effect.
The phase distribution obtained from a particular microscope lens
system operated in an out-of-focus condition is determined by the
spherical aberration characteristics of the lens system of the
microscope and in the actual value of .DELTA.f. The spherical
aberration of a lens system is quantitatively described by the
interrelated coefficients of spherical aberration denoted by C
which are readily obtainable and well known and appear in a power
expansion whose coefficients are C.sub.1, C.sub.3, C.sub.5, etc.
For a lens system in which no correction for spherical aberration
has been made, i.e., Seidel order n = 3, C.sub.3 dominates and all
of the outer power terms are negligible. For a microscope corrected
for third order aberration, i.e., Seidel order n = 5, C.sub.3,
C.sub.1 are the dominant coefficients which determine the phase
shift caused by the lens system. Generally, one can say that the
coefficients of spherical aberration which are dominant in
determining optimum phase are C.sub.1, . . . to
C.sub.2.sub..nu..sub.+1 where .nu. goes from 0 to (n-3)/2, where n
is the Seidel order which is limiting resolution. By variation of
the lens factors which effect these coefficients the phase
distribution is varied. Thus, for an uncorrected microscope, n = 3,
C.sub.1 is the only free parameter available for control over the
phase distribution, and for a microscope corrected for third order
aberrations, n = 5, C.sub.1 and C.sub.3 are free parameters. By
manipulation of the free parameters in the design and operation of
lens system 14 by well known means, it is possible to obtain
various usable phase distributions to approximate the ideal step
function distribution.
The actual values of .DELTA.f which provide adequate phase contrast
are illustrated in FIG. 6 and FIG. 7 which are curves showing the
relative relationship of .DELTA.f to the intensity G of the phase
contrast signal for an uncorrected microscope (n = 3) in FIG. 6 and
for a corrected microscope (n = 5) in FIG. 7. As shown by curves 70
and 71 of FIG. 6 and curves 72, 73 and 74 of FIG. 7 which are
curves of varying resolutions only three regions A, B and C exist
which contribute significantly to phase contrast. Regions B and C
are ones of phase contrast opposite in sign from region A. In each
case the central region A gives maximum contrast with its maxima
point D coinciding with .DELTA.f = - C.sub.1. The region of usable
values of .DELTA. f has been observed to be about 4 (d.sup.2
/.lambda.) on either side of point D for region A and about 8
(d.sup.2 /.lambda.) on either side of point D for regions A, B and
C where .lambda. is the electron wavelength and d is the limit of
resolution. The limit of resolution is a quantity which determines
the quality of the microscope. It is determined for an electron
microscope by using the well known method of Scherzer. Using
Scherzer's method for a microscope providing a phase contrast
signal as herein disclosed, d was determined to be, with n = 3, d
.apprxeq. 0.36(C.sub.3 .lambda..sup.3).sup.1/4 and with n = 5, d
.apprxeq. 0.31(C.sub.5 .lambda. .sup.5).sup.1/6. For a particular
microscope with n = 5 and with C.sub.5 .apprxeq. 15 cm, d is about
0.67 A for 100 kv electrons.
Generally, the microscopist is interested in reducing the radiation
applied to the specimen. Therefore, given the desired phase
distribution from the design of the lens system and from the value
of .DELTA.f, the best means for determining the optimum position
and dimensions for the detectors is to assume an acceptable fixed
signal to noise ratio for the phase contrast signal developed by
differencing circuit 60 and then minimizing the dose on the
specimen. The signal to noise ratio q is obtained by dividing the
noise contrast by the mean phase contrast and by well known
calculation procedures has been determined to be: ##EQU2## where
.alpha. is Sommerfeld's constant, .beta.c is the electron velocity,
Z is the atomic number of the atom being imaged, .sqroot.N is the
resulting noise which is identical to the statistical fluctuation
in the total number of electrons, N, incident on both detectors,
and G(O) is the value at the image point of G(R) which is the
intensity distribution of the phase contrast signal as a function
of R the effective radius of the image referred to the object
plane. G(R) is given by: ##EQU3## where .theta..sub.o is
illumination angle, m is the number of rings of the first detector,
.THETA. is the angle with respect to the optic axis defining the
cone of constructive or destruction interference covered by each
ring of the first detector, F is the atomic form factor, J.sub.o is
a Bessel function of zero order, the wavelength, .lambda. =
2.pi./k, .phi. is the angle subtending the vectors of
.theta.-.dwnarw. which are perpendicular to the optic axis and
.gamma. (.theta.) - .gamma. (.THETA.) is the additional phase shift
due to spherical aberration and defocus (the phase shift associated
with the specimen being assumed to be .pi./2) with ##EQU4## for
2.nu. + 1 = n the Seidel order, for .lambda. = 2 .pi./k the
wavelength of the electrons. Considering equation (1) for q, it is
apparent that for fixed, q, N, the dose, becomes smallest when G(O)
reaches its maximum. The problem may be simplified by approximation
of the atomic potential by a delta function, i.e. ##EQU5##
As stated previously, phase contrast will be most prominent when
the total phase shift approaches 0 to .pi. or multiples thereof.
Applying this to the maximization of G, this distribution occurs
when half of the incident electrons have an additional phase shift
due to spherical aberration and defocus of 0 or .pi. and the other
half an additional phase shift of .pi./2. Then the phase shift
between an arbitrary unscattered electron and a scattered electron
will be 0 or .pi./2 for certain hollow cones or regions of the cone
of illumination and .pi. or .pi./2 for the others. The total solid
angle of the cones yielding a constructive interference is equal to
that of cones with destructive interference. As stated before, the
ideal distribution of the phase shift can be approached in practice
in an uncorrected microscope with the ideal defocus, .DELTA.f =
-C.sub.1 which is the only free parameter available to vary the
phase distribution to desired levels. The other free parameters
determine the width of the first detector zone rings and do not
effect the actual phase shift. To approach the lowest dose for a
real microscope we maximize G with respect to the free parameters
.theta..sub.o, .THETA..sub..SIGMA. and C.sub.2.sub..nu..sub.+1. The
subscript o.sigma. runs from 1 to 2m, m being an integer indicating
the number of zone rings of detector 52. The subscript .nu. runs
from 0 to (n - 3)/2 where n is the Seidel order of that spherical
aberration which cannot be chosen arbitrarily and is limiting the
resolution. With the defocus equal to -C.sub.1, in an uncorrected
microscope then .DELTA.f .apprxeq. 1.44(C.sub.3 .lambda.).sup.1/2.
In this case the first phase contrast detector consists of a single
ring 52, i.e., m = 1, as shown in FIG. 1. The optimum angles of
this ring are .theta..sub.1 .apprxeq.
0.92(.lambda./C.sub.3).sup.1/4 radians, .theta..sub.2 .apprxeq.
1.44(.lambda./C.sub.3).sup.1/4 radians and the optimum illumination
angle is .theta..sub.o .apprxeq. 1.71(.lambda./C.sub.3).sup.1/4
radians. The areas of the second phase contrast detector which do
not lie in the shadow of the first detector 52 and which are
detected by the second detector's disc 54 are a central disc and an
outer ring.
In an microscope corrected for third order spherical aberration,
the coefficient C.sub.3 becomes an additional free parameter for
effecting the optimum phase contrast distribution. Optimum
operating conditions are approached if again we choose .DELTA.f
.apprxeq. -C.sub.1 so that C.sub.1 .apprxeq. +1.91(C.sub.5
.lambda..sup.2).sup.1/3, C.sub.3 = -3.2(C.sub.5.sup.2
.lambda.).sup.1/3. This is illustrated by curve 75 of FIG. 2 which
refers to the upper scale of FIG. 2. In the upper scale C.sub.5 is
the fifth order coefficient of spherical aberration. The optimum
configuration of the first detector is the same as in the case of
the uncorrected microscope, i.e. m = 1. Of course, the optimum
illumination and detector angles have changed. These optimized
angles are .theta..sub.1 .apprxeq. 1.23(.lambda./C.sub.5).sup.1/6
radians, .theta..sub.2 .apprxeq. 1.77(.lambda./c.sub.5).sup.1/6
radians and .theta..sub.o .apprxeq. 1.87(.lambda./C.sub.5).sup.1/6
radians.
In practice the signal developed by the phase contrast detector can
be combined with the dark field detector 42 signal and the signal
relating inelastically scattered electrons developed by the
spectrometer 38, by combining the signals together conveniently
with signal processor 76 and applying them to cathode 32. Note that
while it is not necessary to filter only the inelastically
scattered electrons from the cone of illumination with
spectrometer, improved detection is achieved if they are filtered
out before phase contrast detection as shown in FIG. 1, since they
would unnecessarily contribute to the intensity measured by the
detectors. Spectrometer 38 will bend the cone of illumination to
separate the lower energy inelastically scattered electrons,
however, since the elastically scattered and unscattered electrons
are of the same energy, the bending by spectrometer 38 will not
alter the relative distribution of elastically scattered and
unscattered electrons in the cone of illumination.
* * * * *