First-principles density-functional theory calculations in the generalized gradient
approximation were carried out in order to study the relative stabilities of oxygen
vacancies at the surface and sub-surface sites of anatase (101), TiO2(001) and
prototypical rutile (110) surfaces. The results indicated that these defects were
significantly more stable at sub-surface than at surface sites in the case of anatase
surfaces, whereas bridging oxygen sites were favoured for O vacancies at rutile (110) surfaces. Calculations of O-vacancy diffusion pathways at anatase (101)
surfaces showed that the energy barrier to diffusion from surface to sub-surface
sites was sufficiently low to ensure rapid equilibration of the vacancy distribution
at typical surface annealing temperatures. These results could explain why anatase
surfaces were found experimentally to have a significantly lower defect
concentration and/or to be more difficult to reduce than those of rutile.
Surface and Subsurface Oxygen Vacancies in Anatase TiO2 and Differences with
Rutile. H.Cheng, A.Selloni: Physical Review B, 2009, 79[9], 092101