Abstract
The resonance Raman (RR) spectrum of C60 has been studied in benzene and carbon disulfide using eight excitation wavelengths between 406.7 and 647.1 nm. Raman excitation profile calculations have been performed on the five most intense RR bands; the Hg(1), Ag(1), Gg(4), Hg(7), and Ag(2) vibrational modes. Two main scattering mechanisms predominate, Herzberg−Teller (HT) B-term scattering and nonadiabatic D-term scattering. This is the first observation of rare D-term scattering in a system without a metal. The requirement of a Jahn−Teller distortion of the excited state, produced upon population of the degenerate T1u LUMO, is essentially negated by solvent distortion of the symmetry of C60. While the Ih point group is a good descriptor for the 10 fundamental Raman modes of C60, the slight reduction in the high symmetry of the molecule, due to solvent and 13C effects, activates at least 6 of the remaining 36 Raman-silent modes. At resonance with the HOMO−LUMO transition of C60, or its vibronic sideband, the...
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