Elucidating linear and nonlinear optical properties of defect chalcopyrite compounds ZnX2Te4 (X=Al, Ga, In) from electronic transitions

Abstract

We presented a theoretical study of electronic band structure of three compounds ZnAl2Te4, ZnGa2Te4 and ZnIn2Te4 using pseudo potential method within density functional theory. Calculated band structures show that all band gaps are direct with at Γ with values of 1.639eV for ZnAl2Te4, 1.026eV for ZnGa2Te4and 0.836eV ZnIn2Te4. The linear properties based on dielectric function and non-linear optical properties based on second harmonic generation (SHG) were computed. The origin of four critical points (peaks) determined from the second derivative of the imaginary part of the dielectric function is elucidated. The use of individual k-points and individual combination of valence and conduction bands dependent matrix of the dielectric function and the nonlinear optical susceptibility allowed to a precise determination of inter band optical transitions. Indeed, inter-band analysis shows the high intensity of non-linear effect compared to linear effect. Moreover, non-linear inter-band optical transitions involve lower valence bands and higher conduction bands.