Title: Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations

Abstract

In ultrafast electron diffraction (UED) experiments, accurate retrieval of time-resolved structural parameters, such as atomic coordinates and thermal displacement parameters, requires an accurate scattering model. Unfortunately, kinematical models are often inaccurate even for relativistic electron probes, especially for dense, oriented single crystals where strong channeling and multiple scattering effects are present. This article introduces and demonstrates dynamical scattering models tailored for quantitative analysis of UED experiments performed on single-crystal films. As a case study, we examine ultrafast laser heating of single-crystal gold films. Comparison of kinematical and dynamical models reveals the strong effects of dynamical scattering within nm-scale films and their dependence on sample topography and probe kinetic energy. Applying to UED experiments on an 11 nm thick film using 750 keV electron probe pulses, the dynamical models provide a tenfold improvement over a comparable kinematical model in matching the measured UED patterns. Also, the retrieved lattice temperature rise is in very good agreement with predictions based on previously measured optical constants of gold, whereas fitting the Debye–Waller factor retrieves values that are more than three times lower. Altogether, these results show the importance of a dynamical scattering theory for quantitative analysis of UED and demonstrate models that can be practically appliedmore » to single-crystal materials and heterostructures.« less

Authors:

Durham, Daniel B.  ^[1];

• Search DOE PAGES for author "Durham, Daniel B."
• Search DOE PAGES for ORCID "0000-0002-5780-6852"

Ophus, Colin  ^[2];

• Search DOE PAGES for author "Ophus, Colin"
• Search DOE PAGES for ORCID "0000-0003-2348-8558"

Siddiqui, Khalid M.  ^[3];

• Search DOE PAGES for author "Siddiqui, Khalid M."
• Search DOE PAGES for ORCID "0000-0001-6640-2406"

Minor, Andrew M.  ^[1];

• Search DOE PAGES for author "Minor, Andrew M."
• Search DOE PAGES for ORCID "0000-0003-3606-8309"

Filippetto, Daniele  ^[4]

• Search DOE PAGES for author "Filippetto, Daniele"
• Search DOE PAGES for ORCID "0000-0001-5831-860X"

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1. University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
2. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
3. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Materials Sciences Division
4. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Accelerator Technology and Applied Physics Division

Publication Date:

Mon Dec 05 00:00:00 EST 2022

Research Org.:

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)

OSTI Identifier:

2278650

Alternate Identifier(s):

OSTI ID: 1902559

Grant/Contract Number:  

AC02-05CH11231; DMR 1548924

Resource Type:

Accepted Manuscript

Journal Name:

Structural Dynamics

Additional Journal Information:

Journal Volume: 9; Journal Issue: 6; Journal ID: ISSN 2329-7778

Publisher:

American Crystallographic Association/AIP

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE; Crystallography; Lattice dynamics; Bloch wave; Thin films; Ultrafast electron diffraction; Ultrafast lasers; Scattering problem; Scattering theory