Theoretical study of oxygenated (100) diamond surfaces in the presence of hydrogen

Quantum ab initio calculations and quantum semiempirical molecular-dynamics simulations were employed to study reconstructions of (100) diamond surfaces in the presence of hydrogen and oxygen. The results indicate that the energetically most favorable structures of oxygenated surfaces are those with chemisorbed hydroxyl groups. It was found that hydrogen bonds are formed among chemisorbed oxygenated species. The formation of these hydrogen bonds lowers the adlayer energy. A number of important vibrational modes characteristic of oxygenated diamond surfaces were identified. The analysis of surface vibrational spectra demonstrates the influence of the local environment on the position of vibrational modes and can be useful for interpretation of experimental data.