Abstract
AbstractTwo‐photon transition amplitudes, accounting for virtual double electric dipole–electric quadrupole (E1, E2) and electric dipole–magnetic dipole (E1, M1) transitions, are derived for isotropic molecular ensembles. The new‐type non‐resonant Raman scattering is shown to appear from the interfering emission fields generated by multipoles (electric dipole, electric quadrupole and magnetic dipole) induced on a scattering particle. The interference is found to affect strongly the angular distribution and polarization characteristics of the scattered radiation, damping the forward scattering while enhancing the backward scattering. When the excitation frequency approaches an absorption resonance, the interference features are shown to disappear from the Raman spectra. In the off‐resonance case, the Raman cross‐section equations for gases of linear and spherical (Td) molecules are elaborated in terms of the mixed electronic polarizabilities expressed via their invariants in the molecule‐fixed frame. Copyright © 2005 John Wiley & Sons, Ltd.
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