Nonadiabatic dynamics near metal surfaces with periodic drivings: A generalized surface hopping in Floquet representation

TL;DR

This paper develops a generalized surface hopping algorithm in Floquet space to study nonadiabatic dynamics of molecules near metal surfaces under strong, time-periodic laser drivings, enhancing understanding of light-matter interactions.

Contribution

It extends the previous surface hopping method to Floquet representation for open quantum systems with rapid periodic drivings.

Findings

Developed a Floquet-based surface hopping algorithm (FR-SH).

Applicable to molecules under strong periodic laser fields near metal surfaces.

Facilitates understanding of chemical processes in driven open quantum systems.

Abstract

With light-matter interaction extending into strong regime, as well as rapid development of laser technology, systems subjecting to a time-periodic perturbation are attracted broad attention. Floquet theorem and Floquet time-independent Hamiltonian are powerful theoretical framework to investigate the systems subjecting to time-periodic drivings. In this study, we extend the previous generalized SH algorithm near metal surface (J. Chem. Theory Comput. 2017, 13, 6, 2430-2439) to the Floquet space, and hence, we develop a generalized Floquet representation based surface hopping (FR-SH) algorithm. Here, we consider open quantum system with fast drivings. We expect that the present algorithm will be useful for understanding the chemical processes of molecules under time-periodic drivings near the metal surface.