Mixed quantum-classical equilibrium in global flux surface hopping.
作者： Andrew E. Sifain , Linjun Wang , Oleg V. Prezhdo
DOI: 10.1063/1.4922162
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摘要: Global flux surface hopping (GFSH) generalizes fewest switches (FSSH)—one of the most popular approaches to nonadiabatic molecular dynamics—for processes exhibiting superexchange. We show that GFSH satisfies detailed balance and leads thermodynamic equilibrium with accuracy similar FSSH. This feature is particularly important when studying electron-vibrational relaxation phonon-assisted transport. By dynamics in a three-level quantum system coupled classical atom contact bath, we demonstrate both FSSH achieve Boltzmann state populations. Thermal attained significantly faster GFSH, since it accurately represents superexchange process. converges closer averages than exhibits smaller statistical errors.
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