Pseudo-Rephasing and Pseudo-Free-Induction-Decay Mechanism in Two-Color Three-Pulse Photon Echo of a Binary System

Dong, Huafeng; Ryu, Ian Seungwan; Fleming, Graham R.

doi:10.1021/jp409352z

Cited by 1 publication

(2 citation statements)

References 30 publications

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“…Since the 2CCPE is homodyne detected, a beating pattern with the frequency of the exciton energy gap is not observed. However, the nuclear DoF interference 32 and the asymmetry of two branches 29 may provide an oscillating modulation of the decay signal. 10 This effect is beyond the main scope of the paper and will be discussed elsewhere.…”

Section: Resultsmentioning

confidence: 99%

“…However, the bRC is far more complicated than a dimer. For example, the asymmetry between two branches will bring interference, 29 and the inclusion of the special pair will result in a complex exciton level structure. The full model of bRC will thus inevitably complicate the physical mechanism of the disorder-induced long-lived coherence presented.…”

Section: Modelmentioning

confidence: 99%

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Inhomogeneous Broadening Induced Long-Lived Integrated Two-Color Coherence Photon Echo Signal

Dong

Fleming

2014

J. Phys. Chem. B

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Recent observations of the long-lasting nonlinear signals in a variety of light-harvesting complexes have initiated an active debate on the origin of long-lived coherence in the biological systems. In this work we show that disorder of site energy can induce a long-lived electronic coherence between two chromophores in a strongly coupled dimer system, in addition to the ensemble dephasing effect. This phenomenon is physically explained as the correlated fluctuation of excitons with the equal delocalization on two sites, when the site-energy distributions overlap to give resonance. Using the integrated two-color coherence photon echo signal as an example, we show that the coherence in such a system exhibits a biexponential decay with a slow component with a lifetime of hundreds of femtoseconds and a rapid component with a lifetime of tens of femtoseconds. The current result provides a possible microscopic basis for the electronic coherence to be the origin of the long-lived coherence signals to be considered along with other recently proposed mechanisms.

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Section: Resultsmentioning

confidence: 99%

Section: Modelmentioning

confidence: 99%