Abstract

Exact non-singular effective polarizability operators are introduced that exhibit well defined time reversal and Hermiticity characteristics and can therefore be applied to all forms of (optically active) light scattering including resonance phenomena. Dual circular polarization (DCP) and dual linear polarization (DLP) Raman optical activity (ROA) observables are reformulated in terms of matrix elements of these generalized scattering operators. Employing the fundamental operator symmetry properties, Stokes and anti-Stokes ROA observables are shown to exhibit the same signs for the in-phase DCPI and out-of-phase DLPII modulation technique, and opposite signs for the out-of-phase DCPII and in-phase DLPI modulation approach for the case of diamagnetic chiral molecules.

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