Cation substitution effects on structural, electronic and optical properties of nonlinear optical AgGa(SxSe1-x)(2) crystals

Abstract

The structural, electronic and optical properties of tetragonal nonlinear optical (NLO) crystals, AgGa(SxSe1-x)(2) (x = 0.0, 0.25, 0.5, 0.75, and 1.0), were investigated theoretically and experimentally. The results obtained indicated that the electronic bandgaps, optical properties and bulk moduli of these compounds were linearly dependent on the substitution concentration of cations. From partial density of state analysis, it was found that the electronic states near the band edges of AgGa(SxSe1-x)(2) were a simple proportional mixture of the atomic orbitals of sulfur and selenium. A cell-volume effect was proposed as the major cause of the linear dependence of material properties on the substitution concentration. It was calculated that the second-order NLO susceptibilities were scaled with the cubic power of bandgap, although a minor deviation existed. This deviation arose from the optical transition moment products.