CO2 dissociative sticking on Cu(110)

Abstract

In this work, we perform quasi-classical trajectory calculations using an artificial neural network potential parameterized from ab initio calculations, to investigate the dynamics of CO2 interacting with Cu(110). The obtained dependencies of the molecular and dissociative adsorption probabilities on the initial translational energy of the molecules and surface temperature are in good (qualitative) agreement with available supersonic molecular beam experiments. We also investigate the influence of impact energy and surface temperature on the final state of the dissociation products, and we find that above ∼2.5 eV and close to or above room temperature, CO2 dissociation induces strong surface distortions, including final structures involving Cu adatoms. The creation of Cu vacancy–adatom pairs is stimulated by the presence of both COads and Oads, which interact strongly with the Cu adatoms and even give rise to unexpected (O–Cu–CO)ads linear moieties anchored to the surface by the dissociated O atom and involving a Cu adatom almost detached from the surface. These surface distortions produced by dissociation products of high-energy CO2 molecules at and above room temperature might explain recent experiments that have found saturation oxygen coverage for high energy molecules, larger than for slow molecules.