The Initial Charge Separation Step in Oxygenic Photosynthesis

Overview

Journal Nat Commun

Specialty Biology

Date 2022 Apr 28

PMID 35477708

Authors

Yusuke Yoneda

Eric A Arsenault

Shiun-Jr Yang

Kaydren Orcutt

Masakazu Iwai

Graham R Fleming

Affiliations

Soon will be listed here.

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 ChlPhe 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 P, regardless of excitation wavelength.

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