Structural, electronic and optical properties of tetrahedral SixGe47−x : H60 nanocrystals: A Density Functional study

The structural, cohesive, electronic and optical properties of mixed SiGe:H quantum dots are studied by Density Functional Theory (DFT) calculations on a representative ensemble of medium size nanoparticles of the form SixGe47−x : H60. The calculations have been performed in the framework of the hybrid non-local exchange-correlation functional of Becke, Lee, Parr and Yang (B3LYP). Besides the ground state DFT/B3LYP values we provide reliable result for the lowest spin and symmetry allowed electronic transition based on Time Dependent DFT (TDDFT/B3LYP) calculations. Our results show that the optical gap depends not only on the relative concentrations of silicon, germanium and hydrogen, but also on the relative position of the silicon and germanium shells relative to the surface of the nanocrystal. This is also true for the structural, cohesive and electronic properties allowing for possible electronic and optical gap engineering. Moreover, it is found that for the cases of nanoparticles with pure Ge or Si core, the optical properties are mainly determined by the Ge part of the nanoparticle, while silicon seem to act as a passivant.