Phonon Scattering in

Transmission Electron Microscopy

Anjan Soumyanarayanan

Supervised by
Dr. Chris Boothroyd

Institute of Materials
Research & Engineering (IMRE)

29 June 2006

A log scale CBED pattern of a thick Si (111) sample Anjan Soumyanarayanan

C. Boothroyd, Invited Talk at Singapore-UK Materials Conference, 2005
 Outline

• Introduction to TEM

• Advances in Quantitative TEM

• The TEM Contrast Problem

• The Frozen Phonon Simulation Model

• Results and Current Work

• Conclusions and Future Work

Anjan Soumyanarayanan
 What is Microscopy?

• Rayleigh Criterion
λ
∆ rmin ≥
2

For light, ∆ rmin > 0 . 1µ m

• How do we ‘see smaller’?

Schematic of an Optical Microscope

Adelaide University Chemistry Dept

Anjan Soumyanarayanan
 Transmission Electron Microscopy

The IMRE Philips CM300 HRTEM Schematic of a Transmission

IMRE Corporate Communications Dept Electron Microscope

Anjan Soumyanarayanan
 How does a TEM work?

• Electrons are diffracted by planes of atoms

– A TEM image is a Fourier Transform of the diffraction pattern
– For a 200 kV microscope, λ ~ 0.025 Å
– Resolution limited by electron lensing constraints and spherical
aberration

• Used to study surfaces, interfaces and in-situ growth

Anjan Soumyanarayanan
 Advances in Quantitative HRTEM

A Graph showing the improvement in A Cs-Corrected HRTEM Image of SrTiO3

resolution of state-of-the-art TEMs with improved resolution and contrast
MRS Bulletin 31 (2006) MRS Bulletin 31 (2006)

Sub-angstrom Resolution
∆ rmin < 1Å
Anjan Soumyanarayanan
 Advances in Quantitative CBED

An Experimental CBED Pattern of a An Experimental CBED Pattern of Si(100)

thick Si(100) sample (Log Scale) (Log Scale)
Centre for Advanced Microscopy, Michigan State University

Anjan Soumyanarayanan
 Quantitative Image Matching

HRTEM Images of WNbO and Image Simulations

C. Boothroyd, Invited Talk at Singapore-UK Materials Conference, 2005

Contrast of experimental images is ~ 3 times lower than

that of the simulated images

THE CONTRAST PROBLEM IN TEM

Anjan Soumyanarayanan
 Atomic Vibrations in a Lattice
• Atoms in a crystal vibrate due
to thermal energy
Quantum Theory models vibrations
as phonons

• Phonons can scatter

A 3D view of a Silicon Crystal
Materials Science and Metallurgy Department
University of Cambridge
electrons off diffraction
maxima to give a thermal
diffuse background
Phonon Scattering (TDS) is more
intense for thicker samples

Anjan Soumyanarayanan
 TDS in Diffraction Patterns

An Elastic Simulation of the CBED An Experimental CBED Pattern of Si(100)

Pattern of Si(100) (Log Scale) (Log Scale)
C. Boothroyd, Invited Talk at Singapore-UK
Materials Conference, 2005

Anjan Soumyanarayanan
 The Frozen Phonon Simulation Model

• The lattice assumes a frozen configuration

for each single electron

• The Einstein Model of Phonon Dispersion

– The vibrations of all atoms are uncorrelated and Gaussian
– Atoms are independent Simple Harmonic Oscillators
– Mathematically elegant and computationally less intensive

Anjan Soumyanarayanan
Relating Back to the Contrast Problem

• Does the frozen phonon model give a ‘good enough’

match with experiment?

• Can the phonon background account for the anomalous

contrast?

• Compare the Phonon Contribution to CBED Patterns

with Simulations

Anjan Soumyanarayanan
 Comparing the CBED Patterns

An Experimental CBED Pattern of a Si(100) A Frozen Phonon Simulation of the CBED

with thickness 200 nm (Log Scale) Pattern of Si(100) with thickness 200
C. Boothroyd & M. Yeadon, Ultramicroscopy 96 (2003) 361 nm (Log Scale)

Anjan Soumyanarayanan
 Quantitative Comparisons
Bragg Spot Intensities Phonon Background

(a) 50 nm

(b) 200 nm

Section averages of the Bragg maxima and the phonon background for experimental
and simulated images of Si(100) at 200 kV with sample thicknesses (a) and (b)
Anjan Soumyanarayanan
 Quantitative Comparisons

Causes of Discrepancy
• Point spread of Bragg spots
• Atomic correlations

Comparisons are better at

higher angles where
phonon background
intensity is comparable to
Bragg spot intensity A comparison of the elastic and
diffuse scattering factors of a Silicon
atom against scattering angle
Z.L. Wang, Phil. Mag. B 79 (1999) 37

Studying the HOLZ Ring

Anjan Soumyanarayanan
 Studying the HOLZ Ring

• Quantitative comparisons
of the HOLZ:TDS ratio
and of the phonon
background

• This can lead to studying

the discrepancies in
image contrast to see if
phonon scattering can
account for it

An experimental CBED pattern for

Si (100) that includes the HOLZ ring
Anjan Soumyanarayanan
 Conclusions and Further Work

• For Si (100), lower angle matching of TDS background

improves at higher thicknesses
– Variations in the TDS background cannot be simulated
accurately within the Einstein Model

• Comparisons near the HOLZ ring could give a better

picture of the validity of the Einstein Model

• Studying other orientations of Si e.g. (111) and other

materials e.g. GaAs

Anjan Soumyanarayanan
 Challenges Imposed
• Guarding from Contamination and Beam Damage
– Improving the sample preparation technique and ‘treatment’

• Thickness Calibration Technique

– Large CA Fringe Spacing
– Filtered and Unfiltered Intensities

• Comparing Experimental Data with Simulations

– What to Compare?
– What is a good fit?

• TEM Instrumentation Techniques (Dr. Boothroyd)

– Obtaining a Low Camera Length (for high angle measurements)
– Sample Tilts and the Energy Filter

Anjan Soumyanarayanan
 Thank You!
Acknowledgements

Dr. Chris Boothroyd Supervisor

Ms Chow Shue Yin MSCL Lab In-Charge

Anjan Soumyanarayanan

Contact:
us-anjan@imre.a-star.edu.sg
Anjan Soumyanarayanan
anjan@mit.edu