RESUMO
We develop an empirical tight binding approach for the modeling of the electronic states and optical properties of Si nanocrystals embedded in a SiO2 matrix. To simulate the wide band gap SiO2 matrix we use the virtual crystal approximation. The tight-binding parameters of the material with the diamond crystal lattice are fitted to the band structure of ß-cristobalite. This model of the SiO2 matrix allows us to reproduce the band structure of real Si nanocrystals embedded in a SiO2 matrix. In this model, we compute the absorption spectra of the system. The calculations are in an excellent agreement with experimental data. We find that an important part of the high-energy absorption is defined by the spatially indirect, but direct in k-space transitions between holes inside the nanocrystal and electrons in the matrix.
RESUMO
Increasing temperature is known to quench the excitonic emission of bulk silicon, which is due to thermally induced dissociation of excitons. Here, we demonstrate that the effect of temperature on the excitonic emission is reversed for quantum-confined silicon nanocrystals. Using laser-induced heating of silicon nanocrystals embedded in SiO2, we achieved a more than threefold (>300%) increase in the radiative (photon) emission rate. We theoretically modeled the observed enhancement in terms of the thermally stimulated effect, taking into account the massive phonon production under intense illumination. These results elucidate one more important advantage of silicon nanostructures, illustrating that their optical properties can be influenced by temperature. They also provide an important insight into the mechanisms of energy conversion and dissipation in ensembles of silicon nanocrystals in solid matrices. In practice, the radiative rate enhancement under strong continuous wave optical pumping is relevant for the possible application of silicon nanocrystals for spectral conversion layers in concentrator photovoltaics.