Non-adiabatic molecular dynamics of carbon dioxide at metal surfaces

We investigate theoretically the collisions of carbon dioxide with gold surfaces at hyperthermal kinetic energies. We parameterize an accurate and computationally efficient system-specific tight-binding model to propagate molecular dynamics trajectories and sample over initial conditions, and incorporate the electron-hole pair excitations in the metal by an electronic friction model. We observe that the molecular electronic states interact along the trajectories of atomic motion and describe the non-adiabatic coupling at the state-averaged complete active space self-consistent field level. The theoretical model allows us to gain insight into the non-adiabatic molecular dynamics of carbon dioxide at metal surfaces.