NON-MARKOVIAN THEORY OF COLLISIONAL DEPHASING IN NEAR RESONANCE LIGHT-SCATTERING

We present a general microscopic theory for near resonance light scattering (RLS) from collisionally perturbed atoms and molecules. The theory is based on the tetradic scattering formalism of Fano and Ben-Reuven. We perform a systematic density expansion and show that the four-time, many-body, dipole correlation functions necessary for the evaluation of the RLS cross section may be rigorously expressed (to lowest order in pressure) in terms of three single-particle, two-time, correlation functions, two of which are associated with the absorption and emission line broadening and the third is a cross correlation function. Our most general expressions are valid for an arbitrary value of the bath correlation time (relative to the broadening), and interpolate smoothly all the way from the static limit of inhomogenous broadening up to the reverse, the Markovian (homogenous) limit. The stochastic Gaussian model of Takagahara, Hanamura, and Kubo is obtained also as a special case of the present formulation. © 1979 American Institute of Physics.