Nonadiabatic molecular dynamics simulation with external field
Abstract
Nonadiabatic molecular dynamics simulations with classical path approximation (CPA-NAMD) cannot simulate the carrier dynamics under an external field. We develop CPA-NAMD-extF, a first-principles density-matrix framework for calculating field-driven electronic responses along precomputed finite-temperature ionic trajectories. The method combines explicit external-field coupling with self-consistent updates of electronic density while retaining the computational efficiency of the classical-path approximation. Benchmarks against regular TDDFT methods show close agreement for time-dependent dipoles, finite-field currents, and linear optical responses. Applications to the linear absorption spectrum of crystalline and amorphous SiO2 demonstrate its capability to large and structurally complex systems. This method is also applied to the 2D hybrid perovskite (BA)2CsPb2Br7. Finite-temperature calculations show that the second-order opto-current response is strongly affected by structural fluctuations. Real-space DC current density further reveals pronounced Br-centered vortex currents, and its microscopic origin is investigated.
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BibTeX
@misc{li2026nonadiabatic,
title = {{Nonadiabatic molecular dynamics simulation with external field}},
author = {Chengji Li and Fan Zheng},
howpublished = {arXiv},
year = {2026},
month = nov,
doi = {10.48550/arxiv.2611.02606},
eprint = {2611.02606},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2611.02606},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Nonadiabatic molecular dynamics simulation with external field
AU - Chengji Li
AU - Fan Zheng
PY - 2026
DA - 2026/11/02
PB - arXiv
DO - 10.48550/arxiv.2611.02606
UR - https://arxiv.org/abs/2611.02606
AB - Nonadiabatic molecular dynamics simulations with classical path approximation (CPA-NAMD) cannot simulate the carrier dynamics under an external field. We develop CPA-NAMD-extF, a first-principles density-matrix framework for calculating field-driven electronic responses along precomputed finite-temperature ionic trajectories. The method combines explicit external-field coupling with self-consistent updates of electronic density while retaining the computational efficiency of the classical-path approximation. Benchmarks against regular TDDFT methods show close agreement for time-dependent dipoles, finite-field currents, and linear optical responses. Applications to the linear absorption spectrum of crystalline and amorphous SiO_2 demonstrate its capability to large and structurally complex systems. This method is also applied to the 2D hybrid perovskite (BA)_2CsPb_2Br_7. Finite-temperature calculations show that the second-order opto-current response is strongly affected by structural fluctuations. Real-space DC current density further reveals pronounced Br-centered vortex currents, and its microscopic origin is investigated.
ER -