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Title: Vibronic phenomena and exciton–vibrational interference in two-dimensional spectra of molecular aggregates

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.
Authors:
;  [1] ;  [2] ;  [1]
  1. Department of Theoretical Physics, Faculty of Physics, Vilnius University, Sauletekio 9-III, 10222 Vilnius (Lithuania)
  2. (Lithuania)
Publication Date:
OSTI Identifier:
22255264
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 140; Journal Issue: 3; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; DIMERS; EXCITATION; INTERFERENCE; MOLECULES; SIGNALS; SIMULATION; SPECTRA; SPECTROSCOPY; TIME RESOLUTION