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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.

Author information

1
Department of Chemistry and QB3 Institute, University of California, Berkeley and Physical Bioscience Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.

Abstract

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.

PMID:
18376878
DOI:
10.1021/jp7107889
[Indexed for MEDLINE]

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