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We report reflection anisotropy spectroscopy (RAS) measurements of the oxidized (001) surface of a type IIb natural diamond. These measurements were made possible due to recent developments in diamond surface preparation. We compare RAS results from the hydrogenated, clean and oxidized C(001) surface and demonstrate that RAS is sensitive to the structural transition of the surface from the 2 × 1 reconstruction of the clean surface to the 1 × 1 reconstruction of the oxidized surface.

We compare the results of ab initio calculations with measured reflection anisotropy spectra and show that strongly bound surface-state excitons occur on the clean diamond (100) surface. These excitons are found to have a binding energy close to 1 eV, the strongest ever observed at a semiconductor surface. Important electron-hole interaction effects on the line shape of the optical transitions above the surface-state gap are also found.