THEORY OF COHERENT RAMAN-SCATTERING WITH QUASI-CW NOISY LIGHT FOR A GENERAL LINE-SHAPE FUNCTION

The theory of electronically nonresonant coherent Raman scattering (CR S) with quasi-cw noisy light (I-(2) CRS) is developed for a general ma terial response. The (Raman) resonant-resonant and resonant-nonresonan t hyperpolarizability contributions to the 1(2) CRS signal are interfe rometrically separable. It is found that, in general, the interferomet ric decay of each of these terms exposes the Raman line shape function in a different manner. Only for a Lorentzian line is their decay iden tical. Thus, in principle, I-(2) CRS provides a new way to explore the line shape function that is analytically distinct from frequency doma in and time domain methods. By way of illustration, the general theory is applied to three common line shapes: Lorentzian (as in the origina l I-(2) CRS theory), Gaussian, and Voigt. The results are shown to be consistent with the principles of factorized time correlation diagram analysis. (C) 1997 American Institute of Physics.