Density-functional model cluster studies of EPR g tensors of Fs+ centers on the surface of MgO

• Published in: The Journal of chemical physics 2006-01, Vol.124 (4), p.044708-044708
• Main Authors: Di Valentin, Cristiana, Neyman, Konstantin M, Risse, Thomas, Sterrer, Martin, Fischbach, Esther, Freund, Hans-Joachim, Nasluzov, Vladimir A, Pacchioni, Gianfranco, Rösch, Notker
• Format: Article
• Language: English
• ISSN: 0021-9606; 1089-7690
• DOI: 10.1063/1.2161190

We report g tensors of surface color centers, so-called F(s) (+) centers, of MgO calculated with two density-functional approaches using accurately embedded cluster models. In line with recent UHV measurements on single-crystalline MgO film, we determined only small g-tensor anisotropies and negative shifts Deltag identical with g-g(e) for all F(s) (+) sites considered, namely, (001)-terrace, step, edge, and corner sites. The g values are very sensitive to the local structure of the defect: relaxation reverses the sign of Deltag. However, accounting for the spin-orbit interaction either self-consistently or perturbatively yields very similar results. In addition to the values of the tensor components, their direction with respect to the surface was determined. In contrast to edges, significant deviations from ideal C(2v) symmetry were found for F(s) (+) centers at steps. Recent data on single-crystalline thin films are reevaluated in the light of these results.