期刊
STRUCTURAL DYNAMICS-US
卷 4, 期 5, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.4986627
关键词
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资金
- 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]
- National Institutes of Health (NIH) [GM110501, GM055302]
- Ruth L. Kirschstein National Research Service Award [5 F32 GM116423-02]
- Human Frontiers Science [RGP0063/2013 310]
- K&A Wallenberg foundation [2011.0055]
- Energimyndigheten [36648-1]
- Vetenskapsradet [2016-05183]
- Helmholtz Virtual Institute
- DOE Office of Biological and Environmental Research
- National Institutes of Health, National Institute of General Medical Sciences [P41GM103393]
- LCLS, Stanford University, through the Stanford Institute for Materials Energy Sciences (SIMES)
- Lawrence Berkeley National Laboratory (LBNL), University of Hamburg through the BMBF [FSP 301]
- Center for Free Electron Laser Science (CFEL)
- NIH [R01-GM102687A]
- NATIONAL INSTITUTE OF GENERAL MEDICAL SCIENCES [R37GM050781, F32GM116423, R01GM102687, R56GM055302, P41GM103393, R01GM055302, R01GM110501] Funding Source: NIH RePORTER
X-ray absorption spectroscopy at the L-edge of 3d transition metals provides unique information on the local metal charge and spin states by directly probing 3d-derived molecular orbitals through 2p-3d transitions. However, this soft x-ray technique has been rarely used at synchrotron facilities for mechanistic studies of metalloenzymes due to the difficulties of x-ray-induced sample damage and strong background signals from light elements that can dominate the low metal signal. Here, we combine femtosecond soft x-ray pulses from a free-electron laser with a novel x-ray fluorescence-yield spectrometer to overcome these difficulties. We present L-edge absorption spectra of inorganic high-valent Mn complexes (Mn similar to 6-15 mmol/l) with no visible effects of radiation damage. We also present the first L-edge absorption spectra of the oxygen evolving complex (Mn4CaO5) in Photosystem II (Mn < 1 mmol/l) at room temperature, measured under similar conditions. Our approach opens new ways to study metalloenzymes under functional conditions. (C) 2017 Author(s).
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