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Toward precise simulations of the coupled ultrafast dynamics of electrons and atomic vibrations in materials

Tong, Xiao and Bernardi, Marco (2021) Toward precise simulations of the coupled ultrafast dynamics of electrons and atomic vibrations in materials. Physical Review Research, 3 (2). Art. No. 023072. ISSN 2643-1564. doi:10.1103/PhysRevResearch.3.023072.

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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.

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Bernardi, Marco0000-0001-7289-9666
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.
Group:Resnick Sustainability Institute
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Resnick Sustainability InstituteUNSPECIFIED
Department of Energy (DOE)DE-SC0019166
Department of Energy (DOE)DE-AC02-05CH11231
Issue or Number:2
Record Number:CaltechAUTHORS:20201005-102911333
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:105784
Deposited By: Tony Diaz
Deposited On:05 Oct 2020 17:50
Last Modified:28 Apr 2021 18:00

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