Ab initio real-time quantum dynamics of charge carriers in momentum space

Zhenfa Zheng; Yongliang Shi; Jin-Jian Zhou; Oleg V Prezhdo; Qijing Zheng; Jin Zhao

doi:10.1038/s43588-023-00456-9

Ab initio real-time quantum dynamics of charge carriers in momentum space

Nat Comput Sci. 2023 Jun;3(6):532-541. doi: 10.1038/s43588-023-00456-9. Epub 2023 Jun 1.

Authors

Zhenfa Zheng¹, Yongliang Shi^{2

3

4}, Jin-Jian Zhou⁵, Oleg V Prezhdo⁶, Qijing Zheng⁷, Jin Zhao^{8

9

10}

Affiliations

¹ Department of Physics, ICQD/Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, China.
² Department of Physics, ICQD/Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, China. sylcliff@xjtu.edu.cn.
³ Center for Spintonics and Quantum Systerms, State Key Laboratory for Mechanical Behavior of Materials, School of Materials Science and Engineering, Xi'an Jiaotong University, Xi'an, China. sylcliff@xjtu.edu.cn.
⁴ State Key Laboratory of Surface Physics and Department of Physics, Fudan University, Shanghai, China. sylcliff@xjtu.edu.cn.
⁵ School of Physics, Beijing Institute of Technology, Beijing, China.
⁶ Departments of Chemistry, Physics, and Astronomy, University of Southern California, Los Angeles, CA, USA.
⁷ Department of Physics, ICQD/Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, China. zqj@ustc.edu.cn.
⁸ Department of Physics, ICQD/Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, China. zhaojin@ustc.edu.cn.
⁹ Department of Physics and Astronomy, University of Pittsburgh, Pittsburgh, PA, USA. zhaojin@ustc.edu.cn.
¹⁰ Hefei National Laboratory, University of Science and Technology of China, Hefei, China. zhaojin@ustc.edu.cn.

PMID: 38177418
DOI: 10.1038/s43588-023-00456-9

Abstract

Application of the non-adiabatic molecular dynamics (NAMD) approach is limited to studying carrier dynamics in the momentum space, as a supercell is required to sample the phonon excitation and electron-phonon (e-ph) interaction at different momenta in a molecular dynamics simulation. Here we develop an ab initio approach for the real-time charge carrier quantum dynamics in the momentum space (NAMD_k) by directly introducing e-ph coupling into the Hamiltonian based on the harmonic approximation. The NAMD_k approach maintains the zero-point energy and includes memory effects of carrier dynamics. The application of NAMD_k to the hot carrier dynamics in graphene reveals the phonon-specific relaxation mechanism. An energy threshold of 0.2 eV-defined by two optical phonon modes-separates the hot electron relaxation into fast and slow regions with lifetimes of pico- and nanoseconds, respectively. The NAMD_k approach provides an effective tool to understand real-time carrier dynamics in the momentum space for different materials.

MeSH terms

Electrons*
Graphite*
Maintenance
Molecular Dynamics Simulation
Motion

Substances

Graphite