Feasibility of hydroxyl concentration measurements by laser-saturated fluorescence in high-pressure flames

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Abstract
A feasibility study has been performed on the application of laser-saturated fluoresence (LSF) to the measurement of OH concentration in high-pressure flames. Using a numerical model for the collisional dynamics of the OH molecule under nonuniform laser excitation, we have investigated the effect of pressure on the balanced cross-rate model and determined the sensitivity of the depopulation of the laser-coupled levels to the ratio of rate coefficients describing (1) electronic quenching of the vibrational levels for which υ″ > 0 and (2) vibrational relaxation from υ″ > 0 to υ″ = 0. At sufficiently high pressures in near-saturated conditions, the total population of the laser-coupled levels reaches an asymptotic value, which is insensitive to the degree of saturation. When the ratio of electronic quenching is vibrational relaxation is small and the rate coefficients for rotational transfer in the ground and excited electronic states are nearly the same, the balanced cross-rate model remains a good approximation for all pressures. When the above ratio is large, depopulation of the laser-coupled levels becomes significant at high pressures, and thus the balanced cross-rate model no longer holds. In these conditions, however, knowledge of the asymptotic value achieved by the laser-coupled levels could be used to correct the balanced cross-rate model and thus allow LSF measurements at sufficiently high pressures.