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The nonlinear optics of gigawatt power, 10 i m, 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 i m 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 i m, was realized by propagating 3 ps, 10 i m 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 i m pulses in GaAs was studied numerically by solving the Generalized Nonlinear Schri dinger 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 i m. 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.
A method and apparatus for achieving large susceptibilities and long interaction lengths in the generation of new wavelengths in the infrared spectral region. A process of resonantly enhanced four-wave mixing is employed, utilizing existing laser sources, such as the CO.sub. 2 laser, to irradiate a gaseous media. The gaseous media, comprising NH.sub. 3, CH.sub. 3 F, D.sub. 2, HCl, HF, CO, and H.sub. 2 or some combination thereof, are of particular interest since they are capable of providing high repetition rate operation at high flux densities where crystal damage problems become a limitation.
The editors have assembled a world-class group of contributors who address the questions the combustion diagnostic community faces. They are chemists who identify the species to be measured and the interfering substances that may be present; physicists, who push the limits of laser spectroscopy and laser devices and who conceive suitable measurement schemes; and engineers, who know combustion systems and processes. This book assists in providing guidance for the planning of combustion experiments, in judging research strategies and in conceiving new ideas for combustion research. It provides a snapshot of the available diagnostic methods and thier typical applications from the perspective of leading experts in the field.