Dissociation of O2 at Al(111): The Role of Spin Selection Rules

TL;DR

This paper reveals that spin selection rules cause non-adiabatic behavior in O2 dissociation on Al(111), explaining discrepancies between experiments and calculations, and highlights the importance of considering spin effects and exchange-correlation accuracy.

Contribution

It introduces the role of spin selection rules in O2 dissociation on Al(111), addressing a key discrepancy in surface science modeling.

Findings

Spin selection rules cause non-adiabatic effects in O2/Al(111) interactions.

Current exchange-correlation functionals may be insufficient for accurate predictions.

The study explains experimental and theoretical discrepancies in O2 dissociation on Al(111).

Abstract

A most basic and puzzling enigma in surface science is the description of the dissociative adsorption of O2 at the (111) surface of Al. Already for the sticking curve alone, the disagreement between experiment and results of state-of-the-art first-principles calculations can hardly be more dramatic. In this paper we show that this is caused by hitherto unaccounted spin selection rules, which give rise to a highly non-adiabatic behavior in the O2/Al(111) interaction. We also discuss problems caused by the insufficient accuracy of present-day exchange-correlation functionals.