研究目的
To reveal the mechanism of water oxidation by analyzing structures of PSII in the S1, S2, and S3 states using x-ray free-electron laser serial crystallography.
研究成果
The structural changes observed in the O4 channel provide insights into the timing of proton release and a way to prevent the backflow of the released proton. Insertion of O6 occurs in the S2-to-S3 transition, providing an oxyl/oxo species in the S3 state. The structure and O=O bond formation mechanism revealed here should serve as an important blueprint for rational design of artificial catalysts capable of oxidizing water by visible light.
研究不足
The resolution of the S3-state structure was limited, which made the chemical entity of the oxo intermediates not identified unambiguously.
1：Experimental Design and Method Selection:
Fixed-target serial femtosecond crystallography (SFX) at cryogenic temperatures was used to analyze PSII structures in the S1, S2, and S3 states.
2：Sample Selection and Data Sources:
Microcrystals of PSII from the thermophilic cyanobacterium Thermosynechococcus vulcanus were used.
3：List of Experimental Equipment and Materials:
X-ray free-electron laser (XFEL) at SACLA, laser system for sample preparation, and beamline operation setup.
4：Experimental Procedures and Operational Workflow:
Single-shot diffraction images were collected in a fixed-target data collection manner at a cryogenic temperature.
5：Data Analysis Methods:
Structural changes were analyzed using isomorphous difference Fourier maps and Fobs – Fcalc difference Fourier maps.
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