Four-Wave Mixing of Gigawatt Power, Long-Wave Infrared Radiation in Gases and Semiconductor

The nonlinear optics of gigawatt power, 10 microm, 3 and 200 ps long pulses propagating in gases and semiconductors has been studied experimentally and numerically. In this work, the development of a high-repetition rate, picosecond, CO2 laser system has enabled experiments using peak intensities in the range of 1--10 GW/cm2, approximately one thousand times greater than previous nonlinear optics experiments in the long-wave infrared (LWIR) spectral region.;The first measurements of the nonlinear refractive index of the atomic and molecular gases Kr, Xe, N2, O2 and the air at a wavelength near 10 microm were accomplished by studying the four-wave mixing (FWM) of dual-wavelength, 200 ps CO2 laser pulses. These measurements indicate that the nonlinearities of the diatomic molecules N2, O2 and the air are dominated by the molecular contribution to the nonlinear refractive index.;Supercontinuum (SC) generation covering the infrared spectral range, from 2--20 microm, was realized by propagating 3 ps, 10 microm pulses in an approximately 7 cm long, Cr-doped GaAs crystal. Temporal measurements of the SC radiation show that pulse splitting accompanies the generation of such broadband light in GaAs. The propagation of 3 ps, 10 microm pulses in GaAs was studied numerically by solving the Generalized Nonlinear Schrodinger Equation (GNLSE). These simulations, combined with analytic estimates, were used to determine that stimulated Raman scattering combined with a modulational instability caused by the propagation of intense LWIR radiation in the negative group velocity dispersion region of GaAs are responsible for the SC generation process.;The multiple FWM of a 106 GHz, 200 ps CO2 laser beat-wave propagating in GaAs was used to generate a broadband FWM spectrum that was compressed by the negative group velocity dispersion of GaAs and NaCl crystals to form trains of high-power, picosecond pulses at a wavelength near 10 microm. Experimental FWM spectra obtained using 165 and 882 GHz beat-waves revealed an unexpected and rapid decrease in the FWM yield that was not predicted by the GNLSE model that accounts for third-order nonlinearities alone. These results suggest that the effective nonlinear refractive index of GaAs, having formidable second- and third-order susceptibilities, may be altered by quadratic nonlinearities.