Toward precise simulations of the coupled ultrafast dynamics of electrons and atomic vibrations in materials
- Creators
- Tong, Xiao
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Bernardi, Marco
Abstract
Ultrafast spectroscopies can access the dynamics of electrons and nuclei at short timescales, shedding light on nonequilibrium phenomena in materials. However, development of accurate calculations to interpret these experiments has lagged behind as widely adopted simulation schemes are limited to subpicosecond timescales or employ simplified interactions lacking quantitative accuracy. Here we show a precise approach to obtain the time-dependent populations of nonequilibrium electrons and atomic vibrations (phonons) up to tens of picoseconds, with a femtosecond time resolution. Combining first-principles electron-phonon and phonon-phonon interactions with a parallel numerical scheme to time-step the coupled electron and phonon Boltzmann equations, our method provides microscopic insight into scattering mechanisms in excited materials. Focusing on graphene as a case study, we demonstrate calculations of ultrafast electron and phonon dynamics, transient optical absorption, structural snapshots, and diffuse x-ray scattering. Our first-principles approach paves the way for quantitative atomistic simulations of ultrafast dynamics in materials.
Additional Information
© 2021 Published by the American Physical Society. Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Received 13 October 2020; accepted 6 April 2021; published 26 April 2021. The authors thank Jin-Jian Zhou for fruitful discussions. X.T. thanks the Resnick Sustainability Institute at the California Institute of Technology for fellowship support. This work was partially supported by the National Science Foundation under Grant No. DMR-1750613, which provided for theory development, and by the Department of Energy under Grant No. DE-SC0019166, which provided for numerical calculations and code development. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a US Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231.Attached Files
Published - PhysRevResearch.3.023072.pdf
Submitted - 2009.07958.pdf
Supplemental Material - S1.mov
Supplemental Material - Supplemental-Material.pdf
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Additional details
- Eprint ID
- 105784
- Resolver ID
- CaltechAUTHORS:20201005-102911333
- Resnick Sustainability Institute
- NSF
- DMR-1750613
- Department of Energy (DOE)
- DE-SC0019166
- Department of Energy (DOE)
- DE-AC02-05CH11231
- Created
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2020-10-05Created from EPrint's datestamp field
- Updated
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2021-04-28Created from EPrint's last_modified field
- Caltech groups
- Resnick Sustainability Institute