Atomistic Calculation of Coulomb Interactions in Semiconductor Nanocrystals: Role of Surface Passivation and Composition Details

We report a theoretical investigation of electronic properties of semiconductor InAs and GaAs nanocrystals. Our calculation scheme starts with the single particle calculation using atomistic tight-binding model including spin-orbital interaction and d-orbitals. Then the exciton binding energies are calculated with screened Coulomb interaction. We study the role of surface passivation effects by varying value of surface passivation potential. We compare results obtained with dot center positioned on different lattice sites thus containing different number of anion and cations. We conclude that passivation of surface states affects significantly single particle energies and the value of electron-hole Coulomb attraction. Interestingly, due to limited screening, the short-range (on-site) contribution to the electron-hole Coulomb attraction plays significant role for small nanocrystals with radius smaller than 1 nm.