Raman scattering by molecules and macromolecules, arrayed in the electric field of an intense laser beam, is analyzed. Nonlinear changes in the intensity of light scattered by linear and symmetric-top molecules are calculated and expressed in terms of even-order generalized Langevin reorientation functions for all types of Raman-active vibrations. It is shown that the Raman line intensity can undergo an abatement or an enhancement as a result of reorientation, induced by laser radiation; the analysis of these changes in intensity provides additional information on the Raman polarizability tensor, particularly on the sign and magnitude of its anisotropy.
Ensemble averages (cos nν(t)) (n = 1, 2, 3, 4) are calculated for the two-dimensional Smoluchowski-Debye rotational diffusion model in the presence of a DC reorienting electric field. The time dependence of (cos nν(t)) is plotted for the special cases of (i) dipolar nonpolarizable molecules (p # 0), and (ii) nondipolar anisotropically polarizable molecules (p = 0) and rectangular reorienting pulses.
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