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Investigation of OH ground-state energy transfer using picosecond IR-UV resonant four-wave-mixing spectroscopy

Settersten, Thomas B.

Two-color resonant four-wave-mixing spectroscopy (TC-RFWM) is used to investigate ground-state energy transfer of hydroxyl radical in atmospheric-pressure flames. Two amplified distributed-feedback dye lasers produce 50-ps, nearly transform-limited, infrared (IR) and ultraviolet pulses. The infrared pump laser is tuned to individual rovibrational transitions of OH X {sup 2}{pi}{sub 3/2} (v{prime}=1, N{prime}) {l_arrow} X {sup 2}{pi}{sub 3/2} (v{double_prime}=0, N{double_prime}), and the ultraviolet pulse probes either the directly pumped or collisionally populated intermediate levels via A{sup 2}{Sigma}{sup +} (v*=1, N*) {l_arrow} X{sup 2}{pi}{sub 3/2}(v{prime}=1, N{prime}). By time-delaying the probe pulse with respect to the pump pulse, and appropriately constraining the polarizations of each of the four fields taking part in the wave-mixing process, we are able to independently and unambiguously measure the moments of the rotational angular momentum distribution in single rotational levels of the ground state. We present measurements of population, alignment, and orientation decay in X {sup 2}{pi}{sub 3/2} for several flame conditions. These experiments provide data necessary for the development of accurate models for diagnostic techniques using saturating laser pulses.