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)].