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  Intramolecular vibrations enhance the quantum efficiency of excitonic energy transfer

Duan, H.-G., Nalbach, P., Miller, R. J. D., & Thorwart, M. (2020). Intramolecular vibrations enhance the quantum efficiency of excitonic energy transfer. Photosynthesis Research, 144(2), 137-145. doi:10.1007/s11120-020-00742-x.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0006-4FBC-F Version Permalink: http://hdl.handle.net/21.11116/0000-0006-564F-2
Genre: Journal Article

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Duan2020_Article_IntramolecularVibrationsEnhanc.pdf (Publisher version), 2MB
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Duan2020_Article_IntramolecularVibrationsEnhanc.pdf
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This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder.
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https://dx.doi.org/10.1007/s11120-020-00742-x (Publisher version)
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 Creators:
Duan, H.-G.1, 2, 3, Author              
Nalbach, P.4, Author
Miller, R. J. D.2, 3, 5, Author              
Thorwart, M.1, 3, Author
Affiliations:
1I. Institut für Theoretische Physik, Universität Hamburg, ou_persistent22              
2Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
3The Hamburg Center for Ultrafast Imaging, ou_persistent22              
4Westfälische Hochschule, ou_persistent22              
5The Departments of Chemistry and Physics, University of Toronto, ou_persistent22              

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Free keywords: Excitation energy transfer, Vibronic coupling, Efficiency of exciton transfer
 Abstract: We study the impact of underdamped intramolecular vibrational modes on the efficiency of the excitation energy transfer in a dimer in which each state is coupled to its own underdamped vibrational mode and, in addition, to a continuous background of environmental modes. For this, we use the numerically exact hierarchy equation of motion approach. We determine the quantum yield and the transfer time in dependence of the vibronic coupling strength, and in dependence of the damping of the incoherent background. Moreover, we tune the vibrational frequencies out of resonance with the excitonic energy gap. We show that the quantum yield is enhanced by up to 10% when the vibrational frequency of the donor is larger than at the acceptor. The vibronic energy eigenstates of the acceptor acquire then an increased density of states, which leads to a higher occupation probability of the acceptor in thermal equilibrium. We can conclude that an underdamped vibrational mode which is weakly coupled to the dimer fuels a faster transfer of excitation energy, illustrating that long-lived vibrations can, in principle, enhance energy transfer, without involving long-lived electronic coherence.

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Language(s): eng - English
 Dates: 2019-12-262020-03-262020-04-182020-05
 Publication Status: Published in print
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1007/s11120-020-00742-x
 Degree: -

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Title: Photosynthesis Research
Source Genre: Journal
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Publ. Info: Hague : W. Junk
Pages: - Volume / Issue: 144 (2) Sequence Number: - Start / End Page: 137 - 145 Identifier: ISSN: 0166-8595
CoNE: https://pure.mpg.de/cone/journals/resource/954925482637