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Accurate description of nonadiabatic dynamics of molecules at metal surfacesinvolving electron transfer has been a longstanding challenge for theory. Here,we tackle this problem by first constructing high-dimensional neural networkdiabatic potentials including state crossings determined by constrained densityfunctional theory, then applying mixed quantum-classical surface hoppingsimulations to evolve coupled electron-nuclear motion. Our approach accuratelydescribes the nonadiabatic effects in CO scattering from Au(111) withoutempirical parameters and yields results agreeing well with experiments undervarious conditions for this benchmark system. We find that both adiabatic andnonadiabatic energy loss channels have important contributions to thevibrational relaxation of highly vibrationally excited CO(vi = 17), whereasrelaxation of low vibrationally excited states of CO(vi = 2) is weak anddominated by nonadiabatic energy loss. The presented approach paves the way foraccurate first-principles simulations of electron transfer mediatednonadiabatic dynamics at metal surfaces.

First-principles Nonadiabatic Dynamics of Molecules at Metal Surfaces with Vibrationally Coupled Electron Transfer