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J Phys Chem B. 2013 Dec 27;117(51):16416-21. doi: 10.1021/jp409352z. Epub 2013 Dec 11.

Pseudo-rephasing and pseudo-free-induction-decay mechanism in two-color three-pulse photon echo of a binary system.

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Department of Chemistry, University of California , Berkeley, California 94720, United States.


We investigate the two-color three-pulse photon echo peak shift in a (left-right) binary system, where each component consists of a heterodimer. On the basis of the model, we find that the effect of the excitonic asymmetry between two components leads to an additional factor in the peak shift. A pseudo-rephasing and pseudo-free-induction-decay mechanism is proposed to explain the resultant negative peak shift, when the differences between the two left/right components have the opposite sign. In such a case, estimates of the electronic coupling strength via two- and one-color peak shift experiments lead to an underestimate of the coupling magnitude.

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