期刊
NATURE COMMUNICATIONS
卷 5, 期 -, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms5371
关键词
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资金
- NIH [GM055302, P41GM103393, GM095887, GM102520]
- Director, Office of Science, Office of Basic Energy Sciences (OBES), Division of Chemical Sciences, Geosciences and Biosciences (CSGB) of the Department of Energy (DOE) [DE-AC02-05CH11231]
- LBNL Laboratory Directed Research and Development
- Alexander von Humboldt Foundation
- European Union Seventh Framework Programme (FP7) [283745]
- Solar Fuels Strong Research Environment (Umea University)
- Artificial Leaf Project (K&A Wallenberg Foundation)
- Energimyndigheten
- VR
- DOE Office of Basic Energy Sciences, Chemical Sciences Division [DE-AC02-76SF00515]
- LCLS
- Human Frontiers Science Project Award [RPG005/2011]
- SLAC Laboratory Directed Research and Development Program
- DOE Office of Science [DE-AC02-05CH11231]
- DOE OBES
- National Center for Research Resources
- DOE Office of Biological and Environmental Research
The dioxygen we breathe is formed by light-induced oxidation of water in photosystem II. O-2 formation takes place at a catalytic manganese cluster within milliseconds after the photosystem II reaction centre is excited by three single-turnover flashes. Here we present combined X-ray emission spectra and diffraction data of 2-flash (2F) and 3-flash (3F) photosystem II samples, and of a transient 3F' state (250 mu s after the third flash), collected under functional conditions using an X-ray free electron laser. The spectra show that the initial O-O bond formation, coupled to Mn reduction, does not yet occur within 250 mu s after the third flash. Diffraction data of all states studied exhibit an anomalous scattering signal from Mn but show no significant structural changes at the present resolution of 4.5 angstrom. This study represents the initial frames in a molecular movie of the structural changes during the catalytic reaction in photosystem II.
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