Measurements of dynamics of nondegenerate optical nonlinearity in ZnS with pulses from optical parameter generation

We expand the degenerate PO pump-probe technique to nondegenerate field and use it to investigate optical nonlinear dynamics in ZnS single crystal. Excited by 532-nm laser pulses with 21-ps duration, the temporal response of nondegenerate nonlinear absorption and nondegenerate nonlinear refraction are probed by laser pulses from optical parameter generation (OPG) at 600 and 680 nm with pulse width of 10 ps. Based on the theory of free-carrier optical nonlinearity, we study the pure free-carrier refraction in ZnS. By numerically fitting based on the nondegenerate pump-probe theory, the nondegenerate two-photon absorption coefficient, the free-carrier lifetime, the free-carrier absorptive cross section and refractive coefficient at both probe wavelengths are determined respectively. The dispersion of the free-carrier refractive coefficients is discussed.