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We study the gas-surface dynamics of O2 at Ag(111) with the particularobjective to unravel whether electronic non-adiabatic effects are contributingto the experimentally established inertness of the surface with respect tooxygen uptake. We employ a first-principles divide and conquer approach basedon an extensive density-functional theory mapping of the adiabatic potentialenergy surface (PES) along the six O2 molecular degrees of freedom. Neuralnetworks are subsequently used to interpolate this grid data to a continuousrepresentation. The low computational cost with which forces are available fromthis PES representation allows then for a sufficiently large number ofmolecular dynamics trajectories to quantitatively determine the very lowinitial dissociative sticking coefficient at this surface. Already theseadiabatic calculations yield dissociation probabilities close to the scatteredexperimental data. Our analysis shows that this low reactivity is governed bylarge energy barriers in excess of 1.1 eV very close to the surface.Unfortunately, these adiabatic PES characteristics render the dissociativesticking a rather insensitive quantity with respect to a potential spin orcharge non-adiabaticity in the O2-Ag(111) interaction. We correspondinglyattribute the remaining deviations between the computed and measureddissociation probabilities primarily to unresolved experimental issues withrespect to surface imperfections.

Non-adiabatic effects during the dissociative adsorption of O2 at Ag(111)? A first-principles divide and conquer study