Theory of correlation measurements of resonance light scattering

A. P. Kazantsev, Vladimir S. Smirnov, V. P. Sokolov

Pavel A Apanasevich

Edward R. Pike, John B. Abbiss

A. A. Villaeys, Karl F. Freed

The authors present a weak light field, scattering theoretical description of the intensity autocorrelation function for the scattered light from a many-atom (molecule) system. The theory considers both resonant and near-resonant scattering for atoms with many sublevels in both the ground and electronically excited states, and it incorporates the effects of the finite coherence time of the incident radiation. The theory is derived using incident two-photon wave packets with spatial dispersion among the target atoms. Purely anti-bunching contributions arise from single-atom-two-photon scattering and from successive two-atom-two-photon scattering events. However, there are interleaved two-atom-two-photon scattering processes which provide purely bunching contributions since both atoms may be scattering at the same time. Path length differences in the successive two-atom scatterings can also induce some bunching character to the correlation function. The dependence of the risetime and decay of the intensity correlation function upon the atomic excited state lifetimes and the coherence time of the incident light emphasises the correlation between photons which have been coherently and/or incoherently scattered.

Shaul Mukamel

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.

A. A. Villaeys