Abstract
The technique of irreducible tensor operators is used to obtain an accurate expression for the macroscopic cubic susceptibility tensor of a homogeneous isotropic medium formed by randomly oriented molecules (liquids and gases). The result is expressed in terms of the invariants of the molecular hyperpolarizability tensor. Purely rotational and vibrational-rotational molecular transitions are considered. The conditions for maximum intensity of the coherent active Raman (anti-Stokes) spectroscopy (CARS) signal are determined for a finely dispersed medium (crystalline powder). A separate analysis is made of CARS of a noncentrosymmetric crystal powder in which suppression of the cascade process by the quadratic nonlinearity is possible. The first experimental observation of an ARS signal from a finely dispersed sample is reported.
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