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J Phys Chem A. 2008 May 8;112(18):4254-60. doi: 10.1021/jp7107889. Epub 2008 Apr 1.

Coherence quantum beats in two-dimensional electronic spectroscopy.

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Department of Chemistry and QB3 Institute, University of California, Berkeley and Physical Bioscience Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.


We study the coherence quantum beats in two-dimensional (2D) electronic spectroscopy of a coupled dimer system using a theoretical method based on a time-nonlocal quantum master equation and a recently proposed scheme for the evaluation of the third-order photon echo polarization [Gelin, M. F.; Egorova, D.; Domcek, W. J. Chem. Phys. 2005, 123, 164112]. The simulations show that the amplitude and peak shape beating in the 2D spectra is a result of the interplay between the rephasing and non-rephasing contributions to the 2D signals and can be used to elucidate the coherence dynamics in a multichromophoric system. In addition, the results suggest that the rephasing and non-rephasing 2D spectra contain complementary information, and a study of both of them could provide more dynamical information from 2D electronic spectroscopy.

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