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The initial charge separation step in oxygenic photosynthesis

Author

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  • Yusuke Yoneda

    (University of California
    Lawrence Berkeley National Laboratory
    National Institute of Natural Sciences)

  • Eric A. Arsenault

    (University of California
    Lawrence Berkeley National Laboratory
    Kavli Energy Nanoscience Institute at Berkeley)

  • Shiun-Jr Yang

    (University of California
    Lawrence Berkeley National Laboratory)

  • Kaydren Orcutt

    (University of California
    Lawrence Berkeley National Laboratory)

  • Masakazu Iwai

    (Lawrence Berkeley National Laboratory
    University of California)

  • Graham R. Fleming

    (University of California
    Lawrence Berkeley National Laboratory
    Kavli Energy Nanoscience Institute at Berkeley)

Abstract

Photosystem II is crucial for life on Earth as it provides oxygen as a result of photoinduced electron transfer and water splitting reactions. The excited state dynamics of the photosystem II-reaction center (PSII-RC) has been a matter of vivid debate because the absorption spectra of the embedded chromophores significantly overlap and hence it is extremely difficult to distinguish transients. Here, we report the two-dimensional electronic-vibrational spectroscopic study of the PSII-RC. The simultaneous resolution along both the visible excitation and infrared detection axis is crucial in allowing for the character of the excitonic states and interplay between them to be clearly distinguished. In particular, this work demonstrates that the mixed exciton-charge transfer state, previously proposed to be responsible for the far-red light operation of photosynthesis, is characterized by the ChlD1+Phe radical pair and can be directly prepared upon photoexcitation. Further, we find that the initial electron acceptor in the PSII-RC is Phe, rather than PD1, regardless of excitation wavelength.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-29983-1
    DOI: 10.1038/s41467-022-29983-1
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    References listed on IDEAS

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    1. Yasufumi Umena & Keisuke Kawakami & Jian-Ren Shen & Nobuo Kamiya, 2011. "Crystal structure of oxygen-evolving photosystem II at a resolution of 1.9 Å," Nature, Nature, vol. 473(7345), pages 55-60, May.
    2. Elisabet Romero & Vladimir I. Novoderezhkin & Rienk van Grondelle, 2017. "Quantum design of photosynthesis for bio-inspired solar-energy conversion," Nature, Nature, vol. 543(7645), pages 355-365, March.
    3. 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.
    4. Bernhard Loll & Jan Kern & Wolfram Saenger & Athina Zouni & Jacek Biesiadka, 2005. "Towards complete cofactor arrangement in the 3.0 Å resolution structure of photosystem II," Nature, Nature, vol. 438(7070), pages 1040-1044, December.
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