Calcium, conformational selection, and redox-active tyrosine YZ in the photosynthetic oxygen-evolving cluster

Proceedings of the National Academy of Sciences of the United States of America
Zhanjun GuoBridgette A Barry

Abstract

In Photosystem II (PSII), YZ (Tyr161D1) participates in radical transfer between the chlorophyll donor and the Mn4CaO5 cluster. Under flashing illumination, the metal cluster cycles among five Sn states, and oxygen is evolved from water. The essential YZ is transiently oxidized and reduced on each flash in a proton-coupled electron transfer (PCET) reaction. Calcium is required for function. Of reconstituted divalent ions, only strontium restores oxygen evolution. YZ is predicted to hydrogen bond to calcium-bound water and to His190D1 in PSII structures. Here, we report a vibrational spectroscopic study of YZ radical and singlet in the presence of the metal cluster. The S2 state is trapped by illumination at 190 K; flash illumination then generates the S2YZ radical. Using reaction-induced FTIR spectroscopy and divalent ion depletion/substitution, we identify calcium-sensitive tyrosyl radical and tyrosine singlet bands in the S2 state. In calcium-containing PSII, two CO stretching bands are detected at 1,503 and 1,478 cm-1 These bands are assigned to two different radical conformers in calcium-containing PSII. At pH 6.0, the 1,503-cm-1 band shifts to 1,507 cm-1 in strontium-containing PSII, and the band is reduced in intensity in...Continue Reading

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Mar 7, 2013·The Journal of Physical Chemistry Letters·Brandon C Polander, Bridgette A Barry

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Citations

Jun 18, 2020·Frontiers in Plant Science·Tabassum HussainXiaojing Liu
Jan 13, 2021·Photosynthesis Research·Emmanuel OdellaAna L Moore
Aug 8, 2019·Journal of the American Chemical Society·Emmanuel OdellaAna L Moore

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