Disorder-Induced Quantum Beats in Two-Dimensional Spectra of Excitonically Coupled Molecules

Butkus, Vytautas; Dong, Hui; Fleming, Graham R.; Abramavicius, Darius; Valkunas, Leonas

doi:10.1021/acs.jpclett.5b02642

Disorder-Induced Quantum Beats in Two-Dimensional Spectra of Excitonically Coupled Molecules

Journal Article · Thu Jan 21 00:00:00 EST 2016 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.5b02642· OSTI ID:1379226

Butkus, Vytautas; Dong, Hui; Fleming, Graham R.; Abramavicius, Darius; Valkunas, Leonas

Here, a study is presented showing the conditions when long-lived electronic quantum coherences originating from recently proposed inhomogeneous broadening mechanism are enhanced and reflected in the two-dimensional electronic spectra of the excitonically coupled molecular dimer. We show that depending on the amount of inhomogeneous broadening, the excitonically coupled molecular system can establish long-lived electronic coherences, caused by a disordered subensemble, for which the dephasing due to static energy disorder becomes significantly reduced. On the basis of these considerations, we present explanations for why the electronic or vibrational coherences were or were not observed in a range of recent experiments.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1379226

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 2 Vol. 7; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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