Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations
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...
| Main Authors: | , , , , |
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| Format: | Article |
| Language: | English |
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AIP Publishing LLC and ACA
2022-11-01
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| Series: | Structural Dynamics |
| Online Access: | http://dx.doi.org/10.1063/4.0000170 |
| _version_ | 1797947413285044224 |
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| author | Daniel B. Durham Colin Ophus Khalid M. Siddiqui Andrew M. Minor Daniele Filippetto |
| author_facet | Daniel B. Durham Colin Ophus Khalid M. Siddiqui Andrew M. Minor Daniele Filippetto |
| author_sort | Daniel B. Durham |
| collection | DOAJ |
| description | 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 applied to single-crystal materials and heterostructures. |
| first_indexed | 2024-04-10T21:27:23Z |
| format | Article |
| id | doaj.art-9b8c32dc91ed468da142c3b166676da2 |
| institution | Directory Open Access Journal |
| issn | 2329-7778 |
| language | English |
| last_indexed | 2024-04-10T21:27:23Z |
| publishDate | 2022-11-01 |
| publisher | AIP Publishing LLC and ACA |
| record_format | Article |
| series | Structural Dynamics |
| spelling | doaj.art-9b8c32dc91ed468da142c3b166676da22023-01-19T16:29:44ZengAIP Publishing LLC and ACAStructural Dynamics2329-77782022-11-0196064302064302-1210.1063/4.0000170Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulationsDaniel B. Durham0Colin Ophus1Khalid M. Siddiqui2Andrew M. Minor3Daniele Filippetto4 Department of Materials Science and Engineering, University of California, Berkeley, Berkeley, California 94720, USA National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA Department of Materials Science and Engineering, University of California, Berkeley, Berkeley, California 94720, USA Accelerator Technology and Applied Physics Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USAIn 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 applied to single-crystal materials and heterostructures.http://dx.doi.org/10.1063/4.0000170 |
| spellingShingle | Daniel B. Durham Colin Ophus Khalid M. Siddiqui Andrew M. Minor Daniele Filippetto Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations Structural Dynamics |
| title | Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations |
| title_full | Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations |
| title_fullStr | Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations |
| title_full_unstemmed | Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations |
| title_short | Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations |
| title_sort | accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single crystal films using dynamical scattering simulations |
| url | http://dx.doi.org/10.1063/4.0000170 |
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