Dynamic mode decomposition of nonequilibrium electron-phonon dynamics: accelerating the first-principles real-time Boltzmann equation
Abstract
Nonequilibrium dynamics governed by electron–phonon (e-ph) interactions plays a key role in electronic devices and spectroscopies and is central to understanding electronic excitations in materials. The real-time Boltzmann transport equation (rt-BTE) with collision processes computed from first principles can describe the coupled dynamics of electrons and atomic vibrations (phonons). Yet, a bottleneck of these simulations is the calculation of e–ph scattering integrals on dense momentum grids at each time step. Here we show a data-driven approach based on dynamic mode decomposition (DMD) that can accelerate the time propagation of the rt-BTE and identify dominant electronic processes. We apply this approach to two case studies, high-field charge transport and ultrafast excited electron relaxation. In both cases, simulating only a short time window of ~10% of the dynamics suffices to predict the dynamics from initial excitation to steady state using DMD extrapolation. Analysis of the momentum-space modes extracted from DMD sheds light on the microscopic mechanisms governing electron relaxation to a steady state or equilibrium. The combination of accuracy and efficiency makes our DMD-based method a valuable tool for investigating ultrafast dynamics in a wide range of materials.
Copyright and License
© The Author(s) 2024. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.
Acknowledgement
This work was supported by the U.S. Department of Energy, Office of Science, Office of Advanced Scientific Computing Research, and Office of Basic Energy Sciences, Scientific Discovery through Advanced Computing (SciDAC) program under Award No. DESC0022088. The ultrafast carrier dynamics calculations are based on work performed within the Liquid Sunlight Alliance, which is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, and Fuels from Sunlight Hub under Award DE-SC0021266. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231.
Contributions
I.M., J. Yin, and J. Yao conducted the research work under the guidance of C.Y. and M.B. All authors contributed to writing the manuscript.
Data Availability
All the data supporting the results of this study are available upon reasonable request.
Code Availability
The PERTURBO code used in this work is open-source software and can be downloaded at https://perturbo-code.github.io.
Conflict of Interest
The authors declare no competing interests.
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Additional details
- United States Department of Energy
- DE-SC0022088
- United States Department of Energy
- DE-SC0021266
- United States Department of Energy
- DE-AC02-05CH11231