Coherence Quantum Beats in Two-Dimensional Electronic Spectroscopy | Zendy

YuanChung Cheng | Zendy; Graham R. Fleming | Zendy

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Coherence Quantum Beats in Two-Dimensional Electronic Spectroscopy

Author(s) -

YuanChung Cheng,

Graham R. Fleming

Publication year - 2008

Publication title -

the journal of physical chemistry a

Language(s) - English

Resource type - Journals

SCImago Journal Rank - 0.756

H-Index - 235

eISSN - 1520-5215

pISSN - 1089-5639

DOI - 10.1021/jp7107889

Subject(s) - coherence (philosophical gambling strategy) , spectroscopy , quantum , quantum master equation , chemistry , polarization (electrochemistry) , quantum beats , spectral line , quantum mechanics , photon , electron spectroscopy , amplitude , physics , atomic physics , molecular physics , master equation

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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