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Mechanism enabling the observation of the formally optically-forbidden 2 A g - and 1 B u - states in resonance-Raman excitation profiles of spheroidene in KBr disc

Mechanism enabling the observation of the formally optically-forbidden 2 A g - and 1 B u - states in resonance-Raman excitation profiles of spheroiden

Mechanism enabling the observation of the formally optically-forbidden 2 A g - and 1 B u - states in resonance-Raman excitation profiles of spheroidene in KBr disc  
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An expression for the Albrecht A-term resonance-Raman excitation profiles (RREP) of a pigment dispersed in a KBr disc, in such a way that the pigment molecules aggregate in a microcrystal and the microcrystals are dispersed in the KBr disc, is formulated by taking into account the self-absorption of incident and scattered light and the distribution of microcrystals properly. Based on the resultant formula, simulations for the RREPs of spheroidene dispersed in KBr disc were carried out in the spectral region from 12,000 to 24,000cm−1. Fairly good agreement between the simulations and the observed RREPs was obtained for different concentrations of spheroidene. Mechanisms have been investigated which enable the observation of the formally optically-forbidden (very weakly allowed) 2Ag- and 1Bu- states of spheroidne in RREPs free from the contribution of the optically-allowed 1Bu+ state, and a two-step self-absorption mechanism is proposed.
Journal: Chemical Physics - CHEM PHYS , vol. 373, no. 1, pp. 145-152, 2010
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