Soft x-ray absorption spectroscopy of metalloproteins and high-valent metal-complexes at room temperature using free-electron lasers

Kubin, Markus; Kern, Jan; Gul, Sheraz; Kroll, Thomas; Chatterjee, Ruchira; Löchel, Heike; Fuller, Franklin D.; Sierra, Raymond G.; Quevedo, Wilson; Weniger, Christian; Rehanek, Jens; Firsov, Anatoly; Laksmono, Hartawan; Weninger, Clemens; Alonso-Mori, Roberto; Nordlund, Dennis L.; Lassalle-Kaiser, Benedikt; Glownia, James M.; Krzywinski, Jacek; Moeller, Stefan; Turner, Joshua J.; Minitti, Michael P.; Dakovski, Georgi L.; Koroidov, Sergey; Kawde, Anurag; Kanady, Jacob S.; Tsui, Emily Y.; Suseno, Sandy; Han, Zhiji; Hill, Ethan; Taguchi, Taketo; Borovik, Andrew S.; Agapie, Theodor; Messinger, Johannes; Erko, Alexei; Föhlisch, Alexander; Bergmann, Uwe; Mitzner, Rolf; Yachandra, Vittal K.; Yano, Junko; Wernet, Philippe

doi:10.1063/1.4986627

Title: Soft x-ray absorption spectroscopy of metalloproteins and high-valent metal-complexes at room temperature using free-electron lasers

Journal Article · Fri Sep 01 00:00:00 EDT 2017 · Structural Dynamics

DOI:https://doi.org/10.1063/1.4986627· OSTI ID:1416916

Kubin, Markus ^[1]; Kern, Jan ^[2]; Gul, Sheraz ^[3]; Kroll, Thomas ^[4]; Chatterjee, Ruchira ^[3]; Löchel, Heike ^[5]; Fuller, Franklin D. ^[3]; Sierra, Raymond G. ^[6]; Quevedo, Wilson ^[1]; Weniger, Christian ^[1]; Rehanek, Jens ^[5]; Firsov, Anatoly ^[5]; Laksmono, Hartawan ^[7]; Weninger, Clemens ^[8]; Alonso-Mori, Roberto ^[6]; Nordlund, Dennis L. ^[4]; Lassalle-Kaiser, Benedikt ^[9]; Glownia, James M. ^[6]; Krzywinski, Jacek ^[6]; Moeller, Stefan ^[6] more »

Helmholtz-Zentrum Berlin for Materials and Energy, Berlin (Germany). Inst. for Methods and Instrumentation for Synchrotron Radiation Research
SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource
Helmholtz-Zentrum Berlin for Materials and Energy, Berlin (Germany). Inst. for Nanometre Optics and Technology
SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford PULSE Inst.
SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source, Stanford PULSE Inst.
Synchrotron SOLEIL, St. Aubin (France)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford PULSE Inst.; Umea Univ. (Sweden). Inst. for Chemistry, Chemical Biological Center
Umea Univ. (Sweden). Inst. for Chemistry, Chemical Biological Center
California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering
Univ. of California, Irvine, CA (United States). Dept. of Chemistry
Umea Univ. (Sweden). Inst. of Chemistry, Centre for Biological Chemistry; Uppsala Univ. (Sweden). Dept. of Chemistry, Molecular Biomimetics
Helmholtz-Zentrum Berlin for Materials and Energy, Berlin (Germany). Inst. for Methods and Instrumentation for Synchrotron Radiation Research; Univ. of Potsdam (Germany). Inst. for Physics and Astronomy

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. But, 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 ~ 6-15 mmol/l) with no visible effects of radiation damage. We then present the first L-edge absorption spectra of the oxygen evolving complex (Mn ₄ CaO ₅ ) 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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1416916

Alternate ID(s):: OSTI ID: 1378120

Journal Information:: Structural Dynamics, Vol. 4, Issue 5; ISSN 2329-7778

Publisher:: American Crystallographic Association/AIPCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 23 works

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