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The role of mixed vibronic Qy-Qx states in green light absorption of light-harvesting complex II

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  • Eric A. Arsenault

    (University of California
    Kavli Energy Nanoscience Institute at Berkeley
    Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory)

  • Yusuke Yoneda

    (University of California
    Kavli Energy Nanoscience Institute at Berkeley
    Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory)

  • Masakazu Iwai

    (Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory
    University of California)

  • Krishna K. Niyogi

    (Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory
    University of California
    University of California)

  • Graham R. Fleming

    (University of California
    Kavli Energy Nanoscience Institute at Berkeley
    Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory)

Abstract

The importance of green light for driving natural photosynthesis has long been underappreciated, however, under the presence of strong illumination, green light actually drives photosynthesis more efficiently than red light. This green light is absorbed by mixed vibronic Qy-Qx states, arising from chlorophyll (Chl)-Chl interactions, although almost nothing is known about these states. Here, we employ polarization-dependent two-dimensional electronic-vibrational spectroscopy to study the origin and dynamics of the mixed vibronic Qy-Qx states of light-harvesting complex II. We show the states in this region dominantly arise from Chl b and demonstrate how it is possible to distinguish between the degree of vibronic Qy versus Qx character. We find that the dynamics for states of predominately Chl b Qy versus Chl b Qx character are markedly different, as excitation persists for significantly longer in the Qx states and there is an oscillatory component to the Qx dynamics, which is discussed. Our findings demonstrate the central role of electronic-nuclear mixing in efficient light-harvesting and the different functionalities of Chl a and Chl b.

Suggested Citation

  • Eric A. Arsenault & Yusuke Yoneda & Masakazu Iwai & Krishna K. Niyogi & Graham R. Fleming, 2020. "The role of mixed vibronic Qy-Qx states in green light absorption of light-harvesting complex II," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-19800-y
    DOI: 10.1038/s41467-020-19800-y
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    Cited by:

    1. Vishal Kumar Jaiswal & Daniel Aranda Ruiz & Vasilis Petropoulos & Piotr Kabaciński & Francesco Montorsi & Lorenzo Uboldi & Simone Ugolini & Shaul Mukamel & Giulio Cerullo & Marco Garavelli & Fabrizio , 2024. "Sub-100-fs energy transfer in coenzyme NADH is a coherent process assisted by a charge-transfer state," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Yusuke Yoneda & Eric A. Arsenault & Shiun-Jr Yang & Kaydren Orcutt & Masakazu Iwai & Graham R. Fleming, 2022. "The initial charge separation step in oxygenic photosynthesis," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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