Nonadiabatic dynamics near metal surfaces under Floquet engineering: Floquet electronic friction vs Floquet surface hopping

Abstract

In the previous study Wang and Dou [J. Chem. Phys. 158, 224109 (2023)], we have derived a Floquet classical master equation (FCME) to treat nonadiabatic dynamics near metal surfaces under Floquet engineering. We have also proposed a trajectory surface hopping algorithm to solve the FCME. In this study, we map the FCME into a Floquet Fokker–Planck equation in the limit of fast Floquet driving and fast electron motion as compared to nuclear motion. The Fokker–Planck equation is then being solved using Langevin dynamics with explicit friction and random force from the nonadiabatic effects of hybridized electrons and Floquet states. We benchmark the Floquet electronic friction dynamics against Floquet quantum master equation and Floquet surface hopping. We find that Floquet driving results in a violation of the second fluctuation–dissipation theorem, which further gives rise to heating effects.