Molecular theory of optical polarization and light scattering in dielectric fluids. II. Extensions and applications

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Abstract
A microscopic theory of light scattering developed in a previous publication, which incorporates all intermolecular-force effects, is here extended and applied to specific experimental situations. The consistency between the molecular theory and macroscopic theories of light scattering is established. The formal theory is then elaborated to include explicitly the contributions of higher-multipole hyperpolarizabilities, and of nonlinear effects of the external field. The many-body hyperpolarizabilities are expanded in terms of the corresponding single-particle operators and intermolecular forces. Three specific applications of this formalism are considered: (a) collision-induced forbidden Raman scattering in which higher-multipole polarizabilities are shown to partake; (b) collision-induced second-harmonic generation (SHG) by fluids of centrosymmetric molecules; and (c) SHG by atomic fluids. The latter process is shown to contain direct information on the three-particle correlation function.