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Vibronic phenomena and exciton-vibrational interference in two-dimensional spectra of molecular aggregates.
Journal of Chemical Physics 2014 January 22
A general theory of electronic excitations in aggregates of molecules coupled to intramolecular vibrations and the harmonic environment is developed for simulation of the third-order nonlinear spectroscopy signals. It is applied in studies of the time-resolved two-dimensional coherent spectra of four characteristic model systems: weakly/strongly vibronically coupled molecular dimers interacting with high/low frequency intramolecular vibrations. The results allow us to (i) classify and define the typical spectroscopic features of vibronically coupled molecules, (ii) separate the cases, when the long-lived quantum coherences due to vibrational lifetime borrowing should be expected, (iii) define when the complete exciton-vibrational mixing occurs, and (iv) when separation of excitonic and vibrational coherences is possible.
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