Studies of Magnetic Optical Activity in Raman Scattering


This thesis consists mainly of theoretical and experimental studies in Magnetic Raman Optical Activity (M.R.O.A.), although the main theoretical result also allows general deductions to be made about conventional vibrational Raman scattering. The main new experimental result presented in the thesis is the discovery of the phenomenon called Raman Electron Paramagnetic Resonance, which is a new category of vibrational M.R.O.A., involving scattering by degenerate ground state molecules. The main objective of the theoretical research was to apply the general magnetic optical activity expressions to explain the spectral features obtained for molecules exhibiting the effect. The main tool used for doing this was Irreducible Tensor Methods. The theoretical framework developed falls naturally into two parts, one for molecules having a non-degenerate ground state, and one for molecules having a degenerate ground state. For the former case, general formulae were obtained for the perturbed and unperturbed polarizability tensor patterns. These allow all the scattering parameters of interest to be calculated. They also allow very general deductions to be made about the form of the M.R.O.A. spectra for various classes of normal mode, along with information about the frequency dependence of M.R.O.A. General conclusions concerning the conditions under which non-degenerate molecules should exhibit signifigant M.R.O.A. are also deduced. For the latter, irreducible tensor methods were used to obtain general expressions for the polarizability tensor patterns. These show that all degenerate ground state molecules satisfying certain conditions should exhibit Raman E.P.R., and facilitate the calculation of detailed tensor patterns for specific molecules. These results are then applied to explain the form of the spectra of various types of molecule which have exhibited M.R.O.A

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This paper was published in Glasgow Theses Service.

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