Dynamics of Surface Processes: Impact of Adiabatic and Nonadiabatic Energy Dissipation

Dynamics of molecular interactions with solid surfaces, such as scattering, adsorption/desorption, diffusion, and reaction, are affected by energy dissipation at surfaces. Recent progress in experimental studies of surface dynamics has stimulated intense interest in theoretical investigation of microscopic mechanisms and pathways of energy transfer. This review summarizes recent developments in modeling such processes, emphasizing new understandings of electronically adiabatic and nonadiabatic energy dissipation mechanisms and dynamics in representative systems, using various theoretical methods. In particular, machine learning has been leveraged to represent high-dimensional adiabatic potential energy surfaces, electronic friction tensors, and effective multielectron diabatic Hamiltonians. When integrated with mixed quantum-classical dynamics methods, such as molecular dynamics with electronic friction and independent electron surface hopping, these first-principles-based simulations provided unprecedented insights into the roles played by adiabatic and nonadiabatic energy dissipation channels in surface dynamics and in-depth interpretation of experimental observations.