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Title: Imaging phonon dynamics with ultrafast electron microscopy: Kinematical and dynamical simulations

Abstract

Ultrafast x-ray and electron scattering techniques have proven to be useful for probing the transient elastic lattice deformations associated with photoexcited coherent acoustic phonons. Indeed, femtosecond electron imaging using an ultrafast electron microscope (UEM) has been used to directly image the influence of nanoscale structural and morphological discontinuities on the emergence, propagation, dispersion, and decay behaviors in a variety of materials. Here, we describe our progress toward the development of methods ultimately aimed at quantifying acoustic-phonon properties from real-space UEM images via conventional image simulation methods extended to the associated strain-wave lattice deformation symmetries and extents. Using a model system consisting of pristine single-crystal Ge and a single, symmetric Lamb-type guided-wave mode, we calculate the transient strain profiles excited in a wedge specimen and then apply both kinematical- and dynamical-scattering methods to simulate the resulting UEM bright-field images. While measurable contrast strengths arising from the phonon wavetrains are found for optimally oriented specimens using both approaches, incorporation of dynamical scattering effects via a multi-slice method returns better qualitative agreement with experimental observations. Contrast strengths arising solely from phonon-induced local lattice deformations are increased by nearly an order of magnitude when incorporating multiple electron scattering effects. We also explicitly demonstrate themore » effects of changes in global specimen orientation on the observed contrast strength, and we discuss the implications for increasing the sophistication of the model with respect to quantification of phonon properties from UEM images.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of Minnesota, Minneapolis, MN (United States)
Publication Date:
Research Org.:
Univ. of Minnesota, Minneapolis, MN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1625003
Alternate Identifier(s):
OSTI ID: 1615381; OSTI ID: 1662024
Grant/Contract Number:  
SC0018204
Resource Type:
Accepted Manuscript
Journal Name:
Structural Dynamics
Additional Journal Information:
Journal Volume: 7; Journal Issue: 2; Journal ID: ISSN 2329-7778
Publisher:
American Crystallographic Association/AIP
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; Chemistry; Physics; Ultrafast X-rays; Electron microscopy; Computer simulation; Crystal lattices; Waveguides; Photoexcitations; Phonons; Lamb waves; Fourier analysis; Electron scattering; 36 MATERIALS SCIENCE

Citation Formats

Du, Daniel X., and Flannigan, David J. Imaging phonon dynamics with ultrafast electron microscopy: Kinematical and dynamical simulations. United States: N. p., 2020. Web. https://doi.org/10.1063/1.5144682.
Du, Daniel X., & Flannigan, David J. Imaging phonon dynamics with ultrafast electron microscopy: Kinematical and dynamical simulations. United States. https://doi.org/10.1063/1.5144682
Du, Daniel X., and Flannigan, David J. Sun . "Imaging phonon dynamics with ultrafast electron microscopy: Kinematical and dynamical simulations". United States. https://doi.org/10.1063/1.5144682. https://www.osti.gov/servlets/purl/1625003.
@article{osti_1625003,
title = {Imaging phonon dynamics with ultrafast electron microscopy: Kinematical and dynamical simulations},
author = {Du, Daniel X. and Flannigan, David J.},
abstractNote = {Ultrafast x-ray and electron scattering techniques have proven to be useful for probing the transient elastic lattice deformations associated with photoexcited coherent acoustic phonons. Indeed, femtosecond electron imaging using an ultrafast electron microscope (UEM) has been used to directly image the influence of nanoscale structural and morphological discontinuities on the emergence, propagation, dispersion, and decay behaviors in a variety of materials. Here, we describe our progress toward the development of methods ultimately aimed at quantifying acoustic-phonon properties from real-space UEM images via conventional image simulation methods extended to the associated strain-wave lattice deformation symmetries and extents. Using a model system consisting of pristine single-crystal Ge and a single, symmetric Lamb-type guided-wave mode, we calculate the transient strain profiles excited in a wedge specimen and then apply both kinematical- and dynamical-scattering methods to simulate the resulting UEM bright-field images. While measurable contrast strengths arising from the phonon wavetrains are found for optimally oriented specimens using both approaches, incorporation of dynamical scattering effects via a multi-slice method returns better qualitative agreement with experimental observations. Contrast strengths arising solely from phonon-induced local lattice deformations are increased by nearly an order of magnitude when incorporating multiple electron scattering effects. We also explicitly demonstrate the effects of changes in global specimen orientation on the observed contrast strength, and we discuss the implications for increasing the sophistication of the model with respect to quantification of phonon properties from UEM images.},
doi = {10.1063/1.5144682},
journal = {Structural Dynamics},
number = 2,
volume = 7,
place = {United States},
year = {2020},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
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Figures / Tables:

FIG. 1 FIG. 1: Depiction of the transient structural distortion and the resulting quantitative strain for the first-order symmetric Lamb mode (S1) in a photoexcited wedge specimen. (a) A wireframe, cross-sectional side view of the wedge. The wedges shown are before (left) and after (right) fs photoexcitation (i.e., t < to andmore » t > to, respectively, where to is when the peak of the Gaussian excitation pulse arrives at the specimen). The common regions in the dashed rectangles highlight the resulting distortion following photoexcitation. The distortion of the wireframe is greatly exaggerated for illustrative purposes. (b) The percent strain spatial profile in the x and y directions [according to the coordinate system in (a)] for the dilatational symmetry (blue and red, respectively) along the top surface of the wedge for t > to [green in panel (a)], in addition to the xy shear component (black). (c) The percent strain spatial profile in the x and y directions for the dilatational symmetry (blue and red, respectively) through the width of the wedge for t > to [purple in panel (a)], in addition to the xy shear component. The percent strain in panels (b) and (c) is on the order of the calculated strains arising from the S1 Lamb mode (see below).« less

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Works referenced in this record:

Quasi-ballistic thermal transport from nanoscale interfaces observed using ultrafast coherent soft X-ray beams
journal, November 2009

  • Siemens, Mark E.; Li, Qing; Yang, Ronggui
  • Nature Materials, Vol. 9, Issue 1
  • DOI: 10.1038/nmat2568

4D Electron Microscopy: Principles and Applications
journal, August 2012

  • Flannigan, David J.; Zewail, Ahmed H.
  • Accounts of Chemical Research, Vol. 45, Issue 10
  • DOI: 10.1021/ar3001684

Design and implementation of a fs-resolved transmission electron microscope based on thermionic gun technology
journal, September 2013


Observation of the Acoustoelectric Effect
journal, June 1957


4D ultrafast electron microscopy: Imaging of atomic motions, acoustic resonances, and moiré fringe dynamics
journal, December 2009


Ultralow Thermal Conductivity in Disordered, Layered WSe2 Crystals
journal, January 2007


Ultrafast lattice response of photoexcited thin films studied by X-ray diffraction
journal, November 2014

  • Schick, Daniel; Herzog, Marc; Bojahr, André
  • Structural Dynamics, Vol. 1, Issue 6
  • DOI: 10.1063/1.4901228

Time-Resolved X-Ray Diffraction from Coherent Phonons during a Laser-Induced Phase Transition
journal, January 2000


Observation of Anisotropic Strain-Wave Dynamics and Few-Layer Dephasing in MoS 2 with Ultrafast Electron Microscopy
journal, September 2019


Picosecond acoustic phonon pulse generation in nickel and chromium
journal, May 2003


Kikuchi ultrafast nanodiffraction in four-dimensional electron microscopy
journal, January 2011

  • Yurtsever, A.; Zewail, A. H.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 8
  • DOI: 10.1073/pnas.1018733108

Probing Impulsive Strain Propagation with X-Ray Pulses
journal, April 2001


Optical Generation and Characterization of Acoustic Waves in Thin Films: Fundamentals and Applications
journal, August 2000


Diffraction contrast as a sensitive indicator of femtosecond sub-nanoscale motion in ultrafast transmission electron microscopy
conference, September 2013

  • Cremons, Daniel R.; Schliep, Karl B.; Flannigan, David J.
  • SPIE Optical Engineering + Applications, SPIE Proceedings
  • DOI: 10.1117/12.2023145

Debye–Waller Factors and Absorptive Scattering Factors of Elemental Crystals
journal, May 1996

  • Peng, L. -M.; Ren, G.; Dudarev, S. L.
  • Acta Crystallographica Section A Foundations of Crystallography, Vol. 52, Issue 3
  • DOI: 10.1107/S010876739600089X

Nanomechanical Motions of Cantilevers: Direct Imaging in Real Space and Time with 4D Electron Microscopy
journal, February 2009

  • Flannigan, David J.; Samartzis, Peter C.; Yurtsever, Aycan
  • Nano Letters, Vol. 9, Issue 2
  • DOI: 10.1021/nl803770e

Acoustic mode with time-dependent phase velocity in photoexcited semiconductors
journal, November 1991

  • Hu, Ben Yu-Kuang; Stanton, Christopher J.; Wilkins, John W.
  • Physical Review B, Vol. 44, Issue 20
  • DOI: 10.1103/PhysRevB.44.11067

Photon-induced near-field electron microscopy
journal, December 2009

  • Barwick, Brett; Flannigan, David J.; Zewail, Ahmed H.
  • Nature, Vol. 462, Issue 7275
  • DOI: 10.1038/nature08662

Observing (non)linear lattice dynamics in graphite by ultrafast Kikuchi diffraction
journal, March 2014

  • Liang, W.; Vanacore, G. M.; Zewail, A. H.
  • Proceedings of the National Academy of Sciences, Vol. 111, Issue 15
  • DOI: 10.1073/pnas.1404101111

Transient Strain Driven by a Dense Electron-Hole Plasma
journal, October 2003


Evaluation of photo-induced shear strain in monoclinic VTe 2 by ultrafast electron diffraction
journal, August 2018

  • Nakamura, Asuka; Shimojima, Takahiro; Matsuura, Masatoshi
  • Applied Physics Express, Vol. 11, Issue 9
  • DOI: 10.7567/APEX.11.092601

Imaging surface acoustic wave dynamics in semiconducting polymers by scanning ultrafast electron microscopy
journal, January 2018


Four-dimensional ultrafast electron microscopy
journal, May 2005

  • Lobastov, V. A.; Srinivasan, R.; Zewail, A. H.
  • Proceedings of the National Academy of Sciences, Vol. 102, Issue 20
  • DOI: 10.1073/pnas.0502607102

Second Harmonic Generation of Nanoscale Phonon Wave Packets
journal, November 2015


Defect-mediated phonon dynamics in TaS 2 and WSe 2
journal, July 2017

  • Cremons, Daniel R.; Plemmons, Dayne A.; Flannigan, David J.
  • Structural Dynamics, Vol. 4, Issue 4
  • DOI: 10.1063/1.4982817

Four-Dimensional Electron Microscopy
journal, April 2010


Picosecond phase-velocity dispersion of hypersonic phonons imaged with ultrafast electron microscopy
journal, December 2017


Femtosecond mega-electron-volt electron microdiffraction
journal, January 2018


Dynamic diffraction effects and coherent breathing oscillations in ultrafast electron diffraction in layered 1 T -TaSeTe
journal, July 2017

  • Wei, Linlin; Sun, Shuaishuai; Guo, Cong
  • Structural Dynamics, Vol. 4, Issue 4
  • DOI: 10.1063/1.4979643

Ultrafast core-loss spectroscopy in four-dimensional electron microscopy
journal, March 2015

  • van der Veen, Renske M.; Penfold, Thomas J.; Zewail, Ahmed H.
  • Structural Dynamics, Vol. 2, Issue 2
  • DOI: 10.1063/1.4916897

Spatiotemporal Evolution of Coherent Elastic Strain Waves in a Single MoS 2 Flake
journal, May 2017


Diffraction of Quantum Dots Reveals Nanoscale Ultrafast Energy Localization
journal, August 2014

  • Vanacore, Giovanni M.; Hu, Jianbo; Liang, Wenxi
  • Nano Letters, Vol. 14, Issue 11
  • DOI: 10.1021/nl502293a

Surface generation and detection of phonons by picosecond light pulses
journal, September 1986


Femtosecond single-electron diffraction
journal, May 2014

  • Lahme, S.; Kealhofer, C.; Krausz, F.
  • Structural Dynamics, Vol. 1, Issue 3
  • DOI: 10.1063/1.4884937

Acoustoelectric Effect in n -Type Germanium
journal, April 1959

  • Weinreich, Gabriel; Sanders, T. M.; White, Harry G.
  • Physical Review, Vol. 114, Issue 1
  • DOI: 10.1103/PhysRev.114.33

Nanoscale diffractive probing of strain dynamics in ultrafast transmission electron microscopy
journal, January 2018

  • Feist, Armin; Rubiano da Silva, Nara; Liang, Wenxi
  • Structural Dynamics, Vol. 5, Issue 1
  • DOI: 10.1063/1.5009822

Ultrafast Electron Microscopy Visualizes Acoustic Vibrations of Plasmonic Nanorods at the Interfaces
journal, August 2019


Ultrafast electron optics: Propagation dynamics of femtosecond electron packets
journal, August 2002

  • Siwick, Bradley J.; Dwyer, Jason R.; Jordan, Robert E.
  • Journal of Applied Physics, Vol. 92, Issue 3
  • DOI: 10.1063/1.1487437

Simulations of weak-beam diffraction contrast images of dislocation loops by the many-beam Schaeublin–Stadelmann equations
journal, July 2018


Sources of error in Debye–Waller-effect measurements relevant to studies of photoinduced structural dynamics
journal, January 2019


The Acousto-Electric Effect
journal, March 1953


Acoustodynamic Effects in Semiconductors
journal, October 1956


Direct in situ thermometry: Variations in reciprocal-lattice vectors and challenges with the Debye–Waller effect
journal, February 2016


Excitation of longitudinal and transverse coherent acoustic phonons in nanometer free-standing films of (001) Si
journal, March 2009


Structural dynamics of surfaces by ultrafast electron crystallography: Experimental and multiple scattering theory
journal, December 2011

  • Schäfer, Sascha; Liang, Wenxi; Zewail, Ahmed H.
  • The Journal of Chemical Physics, Vol. 135, Issue 21
  • DOI: 10.1063/1.3663963

Advances in applications of time-domain Brillouin scattering for nanoscale imaging
journal, September 2018

  • Gusev, Vitalyi E.; Ruello, Pascal
  • Applied Physics Reviews, Vol. 5, Issue 3
  • DOI: 10.1063/1.5017241

Measurement of the Electronic Grüneisen Constant Using Femtosecond Electron Diffraction
journal, January 2006


Simulations of weak-beam diffraction contrast images of dislocation loops by the many-beam Howie–Basinski equations
journal, October 2006


Generation and detection of picosecond acoustic pulses in thin metal films
journal, March 1987

  • Eesley, Gary L.; Clemens, Bruce M.; Paddock, Carolyn A.
  • Applied Physics Letters, Vol. 50, Issue 12
  • DOI: 10.1063/1.98077

Coherent Zone-Folded Longitudinal Acoustic Phonons in Semiconductor Superlattices: Excitation and Detection
journal, February 1999


Tracking picosecond strain pulses in heterostructures that exhibit giant magnetostriction
journal, March 2019

  • Zeuschner, S. P.; Parpiiev, T.; Pezeril, T.
  • Structural Dynamics, Vol. 6, Issue 2
  • DOI: 10.1063/1.5084140

Observation of large multiple scattering effects in ultrafast electron diffraction on monocrystalline silicon
journal, February 2018


Characterization of fast photoelectron packets in weak and strong laser fields in ultrafast electron microscopy
journal, November 2014


Coherent Acoustic Phonon Oscillations in Semiconductor Multiple Quantum Wells with Piezoelectric Fields
journal, January 2000


Structural dynamics of nanoscale gold by ultrafast electron crystallography
journal, October 2011


Ultrafast electron energy-loss spectroscopy in transmission electron microscopy
journal, July 2018

  • Pomarico, Enrico; Kim, Ye-Jin; García de Abajo, F. Javier
  • MRS Bulletin, Vol. 43, Issue 7
  • DOI: 10.1557/mrs.2018.148

Picosecond photoexcitation of acoustic waves in locally canted gold films
journal, February 2008

  • Pezeril, T.; Leon, F.; Chateigner, D.
  • Applied Physics Letters, Vol. 92, Issue 6
  • DOI: 10.1063/1.2841823

4D Electron Tomography
journal, June 2010


Nonchaotic Nonlinear Motion Visualized in Complex Nanostructures by Stereographic 4D Electron Microscopy
journal, August 2010

  • Kwon, Oh-Hoon; Park, Hyun Soon; Baskin, J. Spencer
  • Nano Letters, Vol. 10, Issue 8
  • DOI: 10.1021/nl102141t

Defect effects on spatiotemporal evolution of photoinduced martensitic transition in MnNiSn
journal, September 2018

  • Zhang, Ming; Li, Zi-An; Tian, Huanfang
  • Applied Physics Letters, Vol. 113, Issue 13
  • DOI: 10.1063/1.5047080

The Elastic Constants of Germanium Single Crystals
journal, April 1950


Picosecond acoustic response of a laser-heated gold-film studied with time-resolved x-ray diffraction
journal, May 2011

  • Nicoul, Matthieu; Shymanovich, Uladzimir; Tarasevitch, Alexander
  • Applied Physics Letters, Vol. 98, Issue 19
  • DOI: 10.1063/1.3584864

4D Nanoscale Diffraction Observed by Convergent-Beam Ultrafast Electron Microscopy
journal, October 2009


A method for simulating electron microscope dislocation images
journal, May 1993


Transition from piezoelectric to deformation potential mechanism of hypersound photogeneration in n -doped GaAs semiconductors
journal, March 2011

  • Babilotte, P.; Ruello, P.; Pezeril, T.
  • Journal of Applied Physics, Vol. 109, Issue 6
  • DOI: 10.1063/1.3552912

Ultrafast Kikuchi Diffraction: Nanoscale Stress–Strain Dynamics of Wave-Guiding Structures
journal, June 2012

  • Yurtsever, Aycan; Schaefer, Sascha; Zewail, Ahmed H.
  • Nano Letters, Vol. 12, Issue 7
  • DOI: 10.1021/nl301644t

Atomic-scale imaging of ultrafast materials dynamics
journal, July 2018

  • Flannigan, David J.; Lindenberg, Aaron M.
  • MRS Bulletin, Vol. 43, Issue 7
  • DOI: 10.1557/mrs.2018.146

Transmission Electron Microscopy Image Contrast of Disclination Defects in Crystals (Computer Simulation)
journal, June 2002


On the validity of the column approximation in electron microscopy
journal, October 1967


Anharmonic Lattice Dynamics in Germanium Measured with Ultrafast X-Ray Diffraction
journal, July 2000


Probing Structural and Electronic Dynamics with Ultrafast Electron Microscopy
journal, April 2015


Physical mechanisms of coherent acoustic phonons generation by ultrafast laser action
journal, February 2015


Electron atomic scattering factors and scattering potentials of crystals
journal, December 1999


Ultrafast atomic-scale visualization of acoustic phonons generated by optically excited quantum dots
journal, July 2017

  • Vanacore, Giovanni M.; Hu, Jianbo; Liang, Wenxi
  • Structural Dynamics, Vol. 4, Issue 4
  • DOI: 10.1063/1.4998009

Full Spatiotemporal Control of Laser-Excited Periodic Surface Deformations
journal, August 2019


Valley Acoustoelectric Effect
journal, June 2019


Four-Dimensional Ultrafast Electron Microscopy: Insights into an Emerging Technique
journal, December 2016

  • Adhikari, Aniruddha; Eliason, Jeffrey K.; Sun, Jingya
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 1
  • DOI: 10.1021/acsami.6b12301

Coherent phonon emission in the supersonic expansion of photoexcited electron-hole plasma in Ge
journal, June 2000


Femtosecond electron imaging of defect-modulated phonon dynamics
journal, April 2016

  • Cremons, Daniel R.; Plemmons, Dayne A.; Flannigan, David J.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms11230

Ultrafast Three-Dimensional Imaging of Lattice Dynamics in Individual Gold Nanocrystals
journal, May 2013


Coherent Phonon Generation and Detection by Picosecond Light Pulses
journal, September 1984


Picosecond–milliångström lattice dynamics measured by ultrafast X-ray diffraction
journal, March 1999

  • Rose-Petruck, Christoph; Jimenez, Ralph; Guo, Ting
  • Nature, Vol. 398, Issue 6725
  • DOI: 10.1038/18631

Ultrafast electron microscopy: Instrument response from the single-electron to high bunch-charge regimes
journal, September 2017


Imaging Intra- and Interparticle Acousto-plasmonic Vibrational Dynamics with Ultrafast Electron Microscopy
journal, October 2016


EELS femtosecond resolved in 4D ultrafast electron microscopy
journal, January 2009


udkm1Dsim—A simulation toolkit for 1D ultrafast dynamics in condensed matter
journal, February 2014


Ultrafast structural and electronic dynamics of the metallic phase in a layered manganite
journal, December 2013

  • Piazza, L.; Ma, C.; Yang, H. X.
  • Structural Dynamics, Vol. 1, Issue 1
  • DOI: 10.1063/1.4835116

Ultrafast electron crystallography of monolayer adsorbates on clean surfaces: Structural dynamics
journal, July 2012


    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.