Abstract
We propose a temperature-dependent optimization procedure for the second-nearest neighbor (2NN) sp(3)s* tight-binding (TB) theory parameters to calculate the effects of strain, structure dimensions, and alloy composition on the band structure of heterostructure spherical core/shell quantum dots (QDs). We integrate the thermoelastic theory of solids with the 2NN sp(3)s* TB theory to calculate the strain, core and shell dimensions, and composition effects on the band structure of binary/ternary CdSe/Cd(Zn)S and ZnSe/Zn(Cd)S QDs at any temperature. We show that the 2NN sp(3)s* TB theory with optimized parameters greatly improves the prediction of the energy dispersion curve at and in the vicinity of L and X symmetry points. We further used the optimized 2NN sp(3)s* TB parameters to calculate the strain, core and shell dimensions, and composition effects on the nanocrystal bandgaps of binary/ternary CdSe/Cd(Zn)S and ZnSe/Zn(Cd)S core/shell QDs. We conclude that the 2NN sp(3)s* TB theory provides remarkable agreement with the measured nanocrystal bandgaps of CdSe/Cd(Zn)S and ZnSe/Zn(Cd)S QDs and accurately reproduces the energy dispersion curves of the electronic band structure at any temperature. We believe that the proposed optimization procedure makes the 2NN sp(3)s* TB theory reliable and accurate in the modeling of core/shell QDs for nanoscale devices.