Nondegenerate Nonlinear Refraction Research Articles

Dispersion of nondegenerate nonlinear refraction in semiconductors.

We use our recently developed beam-deflection technique to measure the dispersion of the nondegenerate nonlinear refraction (NLR) of direct-gap semiconductors. The magnitude and sign of the NLR coefficient n2(ωa; ωb) are determined over a broad spectral range for different values of nondegeneracy. In the extremely nondegenerate case, n2(ωa; ωb) is positively enhanced near the two-photon absorption (2PA) edge and is significantly larger than its degenerate counterpart, suggesting applications for nondegenerate all-optical switching. At higher photon energies within the 2PA regime, n2(ωa; ωb) switches sign to negative over a narrow wavelength range. This strong anomalous nonlinear dispersion provides large phase modulation of a femtosecond pulse with bandwidth centered near the zero-crossing frequency. The measured nondegenerate dispersion closely follows our earlier predictions based on nonlinear Kramers-Kronig relations [Sheik-Bahae et. al, IEEE J. Quant. Electron. 30, 249 (1994)].

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 680nm with pulse width of 10ps. 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.

Time-resolved Z-scan measurements of optical nonlinearities

We introduce a temporal delay in one beam of the two-color Z-scan apparatus, which measures nondegenerate nonlinear absorption and nondegenerate nonlinear refraction. This technique allows us to time resolve separately the sign and the magnitude of the nonlinear absorption and refraction at frequency ωp that are due to the presence of a strong excitation at frequency ωe. For example, in semiconductors we specifically measure the bound electronic, nondegenerate nonlinear refraction and nondegenerate two-photon absorption, as well as the two-photon-generated free-carrier refraction and absorption as functions of time. We demonstrate this technique on ZnSe, ZnS, and CS2, using picosecond pulses at 1.06 and 0.532 μm.