Degenerate four-wave mixing measurements of high order nonlinearities in semiconductors

Degenerate four-wave mixing experiments on ZnSe and CdTe semiconductor samples with picosecond laser pulses at wavelengths below the bandgap are described. The authors identify the dominant nonlinearities in ZnSe and CdTe. They determine these to be fast third-order nonlinearities, due to the same processes which give rise to the effects of bound-electronic refraction and two-photon absorption, while higher order effects are due to free-carrier refraction. Measurements of the absolute magnitude of the combined third order susceptibilities are described. Studies of higher order effects due to free-carrier gratings are discussed. To obtain a quantitative measurement of the carrier induced nonlinearities, an expression for the diffraction efficiency of these carrier gratings was developed, and a value for the free-carrier refractive index coefficient in ZnSe was found. By measuring the angular dependence of the grating decay, the carrier diffusion coefficient was determined as a function of carrier density