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  Does electronic coherence enhance anticorrelated pigment vibrations under realistic conditions?

Duan, H.-G., Thorwart, M., & Miller, R. J. D. (2019). Does electronic coherence enhance anticorrelated pigment vibrations under realistic conditions? The Journal of Chemical Physics, 151(11): 114115. doi:10.1063/1.5119248.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0004-D683-6 Version Permalink: http://hdl.handle.net/21.11116/0000-0004-D684-5
Genre: Journal Article

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https://dx.doi.org/10.1063/1.5119248 (Publisher version)
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 Creators:
Duan, H.-G.1, 2, 3, Author              
Thorwart, M.2, 3, Author
Miller, R. J. D.1, 3, 4, Author              
Affiliations:
1Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
2I. Institut für Theoretische Physik, Universität Hamburg, ou_persistent22              
3The Hamburg Center for Ultrafast Imaging, ou_persistent22              
4The Departments of Chemistry and Physics, University of Toronto, ou_persistent22              

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 Abstract: The light-harvesting efficiency of a photoactive molecular complex is largely determined by the properties of its electronic quantum states. Those, in turn, are influenced by molecular vibrational states of the nuclear degrees of freedom. Here, we reexamine two recently formulated concepts that a coherent vibronic coupling between molecular states would either extend the electronic coherence lifetime or enhance the amplitude of the anticorrelated vibrational mode at longer times. For this, we study a vibronically coupled dimer and calculate the nonlinear two-dimensional (2D) electronic spectra that directly reveal electronic coherence. The time scale of electronic coherence is initially extracted by measuring the antidiagonal bandwidth of the central peak in the 2D spectrum at zero waiting time. Based on the residual analysis, we identify small-amplitude long-lived oscillations in the cross-peaks, which, however, are solely due to groundstate vibrational coherence, regardless of having resonant or off-resonant conditions. Our studies neither show an enhancement of the electronic quantum coherence nor an enhancement of the anticorrelated vibrational mode by the vibronic coupling under ambient conditions.

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Language(s): eng - English
 Dates: 2019-07-112019-08-302019-09-202019-09-21
 Publication Status: Published in print
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 Rev. Method: Peer
 Identifiers: DOI: 10.1063/1.5119248
arXiv: 1904.04033
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Project name : We acknowledge financial support by the Max Planck Society and the Hamburg Centre for Ultrafast Imaging (CUI) within the German Excellence Initiative supported by the Deutsche Forschungsgemeinschaft.
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Title: The Journal of Chemical Physics
  Other : J. Chem. Phys.
Source Genre: Journal
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Publ. Info: Woodbury, N.Y. : American Institute of Physics
Pages: - Volume / Issue: 151 (11) Sequence Number: 114115 Start / End Page: - Identifier: ISSN: 0021-9606
CoNE: https://pure.mpg.de/cone/journals/resource/954922836226