The initial charge separation step in oxygenic photosynthesis

Yusuke Yoneda, Eric A. Arsenault, Shiun-Jr Yang, Kaydren Orcutt, Masakazu Iwai and Graham R. Fleming ()
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Yusuke Yoneda: University of California
Eric A. Arsenault: University of California
Shiun-Jr Yang: University of California
Kaydren Orcutt: University of California
Masakazu Iwai: Lawrence Berkeley National Laboratory
Graham R. Fleming: University of California

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-29983-1

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