Theory of Intercollisional Interference Effects. I. Induced Absorption in a Lorentz Gas

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Abstract
A general kinetic theory of intercollisional interference effects in induced infrared spectra is developed, in which the correlations between all the collisions in the collision sequence of a molecule are taken into account, but the effect of the ternary and higher-order collisions is neglected. The resulting series expression for the line-shape function is explicitly summed for a Lorentz gas. From this general theory expressions are derived for the depth of the intercollisional dip and the shape of the intercollisional spectrum assuming that the pair dipole moment and the intermolecular force are exponential functions with slightly different ranges. The extension of the theory to take into account the frequency dependence of the intracollisional spectrum, and the resulting inadequacy of the neglect of ternary collisions, are discussed.

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