Time-correlation functions for new cross-multipole field fluctuations in binary light scattering by unlike polar molecules

Abstract

2014 Le formalisme des tenseurs multipolaires Cartésiens est appliqué à l'analyse d'un nouveau mécanisme de diffusion de la lumière, dû à l'interférence des variations des polarisabilités moléculaires linéaires et non linéaires induites par les fluctuations temporelles des champs multipolaires électriques. Des formules générales sont proposées pour les fonctions de corrélation temporelles de diffusion isotrope et anisotrope, où entrent les multipolarités de rang arbitraire. Ces formules sont appliquées aux approximations quadrupolaire, octupolaire et hexadécapolaire de molécules à symétrie axiale, tétraédrique et octaédrique. Abstract. 2014 Multipole Cartesian tensor formalism is applied to analyse a new mechanism of light scattering due to the interference of changes in linear and nonlinear molecular polarizabilities induced by space-time fluctuations of multipole electric fields. General formulae are derived for the binary time-correlation functions of isotropic and anisotropic scattering involving multipolarities of arbitrary rank and are applied to the quadrupole, octupole and hexadecapole approximations of simple axially, tetrahedrally and octahedrally symmetric molecules.

Quantum-statistical theory of Raman scattering processes

“…We shall analyze, in particular, cross-fluctuations (cross-correlations) in quadratures and in photocount statistics between different radiation modes. The theory of coherent light scattering within the consistent multipole tensor formalism, developed by Kielich [117] (see also Refs. [27,58,60]) was successfully applied to disclose a novel cross-fluctuation mechanism.…”