Strong light-matter interactions at metal surfaces are very relevant to a variety of chemical systems, including photo-induced chemical adsorption, photo-electrical catalysis, and polariton chemistry. However, such systems are challenging for theoretical study: the Born-Oppenheimer (BO) approximation fails to describe the nonadiabatic dynamics at metal surfaces, and perturbation theory is no longer valid for strong light-matter interactions. Here, we derived a Floquet electronic friction approach to describe the nonadiabatic dynamics at metal surfaces subjected to periodic driving by light. The Floquet electronic friction can be recast into a form in terms of Green’s functions. We show that the frictional tensor shows antisymmetric Berry force even at equilibrium. We further benchmarked our Floquet electronic friction dynamics against the Floquet surface hopping approach for one-level and two-level resonant systems near metal surfaces. We find that the strong light-matter interaction can strenuously affect the electron transfer rate at surfaces.

Floquet nonadiabatic dynamics: electron and energy transfer driven by light-matter interactions

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