An improved static corrugation model

Abstract

Accurately describing surface temperature effects for the dissociation of H₂ on Cu(111) remains challenging. While Ab initio Molecular Dynamics (AIMD), the current state-of-the-art method for modelling such systems, can produce accurate results, it is computationally very expensive to use for extensive testing of, for example, density functionals. A chemically accurate static corrugation model for H₂ and D₂ on Cu(111) dissociation was made by introducing effective three-body interactions as well as an H₂-bond dependence and fitting the model to density functional theory energies for 15 113 different configurations. Reaction probabilities and rovibrational (in)elastic scattering probabilities were computed and compared to experiments and other calculations. Theoretical and experimental results are in good agreement, except for the reaction of (v = 0, J = 0) H₂ where both AIMD and the newly developed static corrugation model, both based on the same underlying density functional, predict a similar deviation from the experiment.