Using periodic density functional theory, the structure and migration energies were
calculated for fluorine vacancies and interstitials in the bulk and at the stoichiometric bulk-truncated surface of these alkali-earth fluorides. A study was
then made of the adsorption of water and hydrogen, in both molecular and
dissociated form, at the ideal surface, and at neutral and charged vacancies in the
surface and sub-surface layers. The results demonstrated that molecular adsorption
was strongly favoured in nearly all cases. The migration paths and barriers were
also studied for the most probable configurations on the surfaces, and it was found
that water was highly mobile on the surface; even when adsorbed at defects. In
general, CaF2 and SrF2 exhibited a similar behaviour with respect to water, while
the adsorption energies and migration barriers for BaF2 were smaller.
Structure and Diffusion of Intrinsic Defects, Adsorbed Hydrogen, and Water
Molecules at the Surface of Alkali-Earth Fluorides Calculated Using Density
Functional Theory. A.S.Foster, T.Trevethan, A.L.Shluger: Physical Review B,
2009, 80[11], 115421