Polaritons and Retarded Interactions in Nonlinear Optical Susceptibilities
In this paper we discuss the calculation of nonlinear optical susceptibilities in infinite crystals and in small molecular aggregates. In both cases, a systematic method is developed for treating the intermolecular interactions and the matter — field coupling. For the infinite crystal it is common to define the susceptibilities as the expansion coefficients of the polarization field in terms of the internal (Maxwell) electric field. This requires an analysis in which both the radiation field and the material variables are treated as degrees of freedom, which naturally leads to the introduction of polaritons: coupled field — matter eigenmodes. For molecular aggregates, it is more useful to define susceptibilities with respect to the external field, so that the problem may be analyzed in terms of material modes, such as excitons and biexcitons.
KeywordsTransition Dipole Moment Nonlinear Susceptibility Phase Conjugate Molecular Aggregate Nonlinear Optical Susceptibility
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