COHERENT RAMAN-SCATTERING WITH INCOHERENT-LIGHT FOR A MULTIPLY RESONANT MIXTURE - THEORY

The theory for coherent Raman scattering (CRS) with broadband incohere nt light is presented for a multiply resonant, multicomponent mixture of molecules that exhibits simultaneous multiple resonances with the f requencies of the driving fields. All possible pairwise hyperpolarizab ility contributions to the signal intensity are included in the theore tical treatment-(resonant-resonant, resonant-nonresonant, and nonreson ant-nonresonant correlations between chromophores) and it is shown how the different types of correlations manifest themselves as differentl y behaved components of the signal intensity. The Raman resonances are modeled as Lorentzians in the frequency domain, as is the spectral de nsity of the incoherent light. The analytic results for this multiply resonant mixture are presented and applied to a specific binary mixtur e. These analytic results will be used to recover frequencies and deph asing times in a series of experiments on multiply resonant mixtures. [S1050-2947(98)08702-2].