TDHF-SOS treatments on linear and nonlinear optical properties of III-V semiconductor clusters (Ga3As3, Ga3Sb3, In3P3, In3As3, In3Sb3)

Abstract We employ an ab initio time-dependent Hartree–Fock (TDHF) formalism combined with sum-over-states (SOS) method to calculate the linear and nonlinear optical properties of direct semiconductor clusters. The obtained electronic absorption spectra predict a variety of the spectral shapes and peak positions and an increase of the second-order nonlinear optical response with an increase of V-group ionic radius in the title clusters. Charge transfers from the π bonding to π antibonding orbitals between III and V group atoms make a significant contribution to the second-order polarizability.