Radical-mediated Adsorption: Ozone Oxidation Of Passivated Silicon

摘要

We report first-principles molecular dynamics calculations on the initial oxidation of hydrogen-passiv-ated Si{001} by ozone (O_3). We observe an intriguing radical-mediated adsorption mechanism, archetypal of a class not reported in the literature so far. Singlet ozone abstracts one hydrogen atom to form a short-lived hydrotrioxy radical (HO_3), before dissociating into surface hydroxyl (-OH) and gas-phase O_2. Vibrational and electronic analysis of the hydrotrioxy species confirms the genuine radical nature of the reaction intermediate.