Nonimpact unified theory of four-wave mixing and two-photon processes

A microscopic correlation-function theory for coherent, parametric, four-photon processes (four-wave mixing) and for single-absorber two-photon processes (two-photon absorption, Raman, and fluorescence spectra) is developed. Both types of experimental observables are expressed in terms of four-point correlation functions of the dipole operator. The latter are then evaluated semiclassically or within the factorization approximation in which they are expressed in terms of ordinary single-photon line-shape functions. The common results of the Bloch equations are shown to be the outcome of two successive approximations: the factorization approximation and the impact limit whereby the single-photon line-shape functions are taken to be Lorentzian. Effects of fluctuations in the radiation fields are easily incorporated within the present approach.