Strong anisotropic interaction controls unusual sticking and scattering of CO at Ru(0001)

TL;DR

This study uses molecular dynamics simulations to reveal that strong rotational anisotropy in CO-Ru(0001) interactions explains unusual sticking and scattering behaviors observed experimentally, with implications for surface reaction mechanisms.

Contribution

It introduces a detailed first-principles-based simulation approach that uncovers the role of anisotropic interactions in CO scattering and sticking on Ru(0001).

Findings

Unusual sticking occurs despite strong CO binding.

Narrow angular scattering distributions are explained by anisotropic interactions.

Implications for precursor states in CO desorption and scattering.

Abstract

Complete sticking at low incidence energies and broad angular scattering distributions at higher energies are often observed in molecular beam experiments on gas-surface systems which feature a deep chemisorption well and lack early reaction barriers. Although CO binds strongly on Ru(0001), scattering is characterized by rather narrow angular distributions and sticking is incomplete even at low incidence energies. We perform molecular dynamics simulations, accounting for phononic (and electronic) energy loss channels, on a potential energy surface based on first principles electronic structure calculations that reproduce the molecular beam experiments. We demonstrate that the mentioned unusual behavior is a consequence of a very strong rotational anisotropy in the molecule-surface interaction potential. Beyond the interpretation of scattering phenomena, we also discuss implications of our results for the recently proposed role of a precursor state for the desorption and scattering of CO from ruthenium.