Control of the nonlinear response of bulk GaAs induced by long-wavelength infrared pulses

The nonlinear optical response of GaAs is studied using extremely nonresonant 10 μm laser pulses with peak intensities greater than 2 GW/cm 2. We observe over an order of magnitude enhancement in the four-wave mixing efficiency by decreasing the CO 2 laser beat-wave frequency. This enhancement is attributed to currents of photoexcited unbound carriers modulated at the beat frequency, confirmed by measurements of nonlinear absorption at this long wavelength as well as a fully microscopic analysis of the excitation dynamics. Modeling of such nonperturbative semiconductor-laser interactions predicts that further decreasing the beat frequency can increase the nonlinear response and allow for its control over two orders of magnitude.