Coherence quantum beats in two-dimensional electronic spectroscopy.
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.
Cheng
Yuan-Chung
YC
Department of Chemistry and QB3 Institute, University of California, Berkeley and Physical Bioscience Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
Fleming
Graham R
GR
D019281:Dimerization; D004583:Electrons; D008956:Models, Chemical; D011789:Quantum Theory; D013057:Spectrum Analysis / Q000379:methods*; D013997:Time Factors