Optical properties of Si and Ge nanocrystals: Parameter-free calculations
Résumé
An overview is given on the electronic and optical properties of Si and Ge nanocrystals. We model freestanding Si and Ge nanocrystals passivated with H, with up to 363 group-IV atoms and 276 H and oxidized nanocrystals with additional silicon oxide shells, e.g. Si41(O60Si42)(O108Si64)H148. The results discussed are based on parameter-free calculations for relaxed atomic structures. The electronic states and the many-body effects are considered within the density-functional theory and the supercell method. Energy gaps are described within the Kohn–Sham independent-particle picture and within the independentquasiparticle picture, whereas electronic excitations are treated within the delta self-consistent method by pair excitation energies. The projector-augmented wave method allows the calculation of optical matrix elements, oscillator strengths, optical spectra, and radiative lifetimes. We discuss quantum confinement, structural relaxation, oxidation, and the role of defects in oxidized Si NCs.