Ultrafast Energy Transfer in Excitonically Coupled Molecules Induced by a Nonlocal Peierls Phonon

The Journal of Physical Chemistry Letters
Hong-Guang DuanMichael Thorwart

Abstract

Molecular vibration can influence exciton transfer via either a local (intramolecular) Holstein or a nonlocal (intermolecular) Peierls mode. We show that a strong vibronic coupling to a nonlocal mode dramatically speeds up the transfer by opening an additional transfer channel. This Peierls channel is rooted in the formation of a conical intersection of the excitonic potential energy surfaces. For increasing Peierls coupling, the electronically coherent transfer for weak coupling turns into an incoherent transfer of a localized exciton through the intersection for strong coupling. The interpretation in terms of a conical intersection intuitively explains recent experiments of ultrafast energy transfer in photosynthetic and photovoltaic molecular systems.

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Citations

Sep 20, 2020·Science Advances·Hong-Guang DuanR J Dwayne Miller
Jun 24, 2019·The Journal of Chemical Physics·T Palm, P Nalbach
Nov 18, 2020·Nature Nanotechnology·Antonietta De SioChristoph Lienau
Aug 9, 2021·The Journal of Chemical Physics·Eric A ArsenaultGraham R Fleming

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