Rolf Mitzner, Jens Rehanek, Jan Kern, Sheraz Gul, Johan Hattne, Taketo Taguchi, Roberto Alonso-Mori, Rosalie Tran, Christian Weniger, Henning Schröder, Wilson Quevedo, Hartawan Laksmono, Raymond G. Sierra, Guangye Han, Benedikt Lassalle-Kaiser, Sergey Koroidov, Katharina Kubicek, Simon Schreck, Kristjan Kunnus, Maria Brzhezinskaya, Alexander Firsov, Michael P. Minitti, Joshua J. Turner, Stefan Möller, Nicholas K. Sauter, Michael J. Bogan, Dennis Nordlund, William F. Schlotter, Johannes Messinger, Andrew S. Borovik, Simone Techert, Frank M. F. de Groot, Alexander Föhlisch, Alexei Erko, Uwe Bergmann, Vittal K. Yachandra, Philippe Wernet, Junko Yano
- L-edge spectroscopy of 3d transition metals provides important electronic structure information and has been used in many fields. However, the use of this method for studying dilute aqueous systems, such as metalloenzymes, has not been prevalent because of severe radiation damage and the lack of suitable detection systems. Here we present spectra from a dilute Mn aqueous solution using a high-transmission zone-plate spectrometer at the Linac Coherent Light Source (LCLS). The spectrometer has been optimized for discriminating the Mn L-edge signal from the overwhelming 0 K-edge background that arises from water and protein itself, and the ultrashort LCLS X-ray pulses can outrun X-ray induced damage. We show that the deviations of the partial-fluorescence yield-detected spectra from the true absorption can be well modeled using the state-dependence of the fluorescence yield, and discuss implications for the application of our concept to biological samples.
MetadatenAuthor details: | Rolf MitznerORCiDGND, Jens Rehanek, Jan Kern, Sheraz Gul, Johan Hattne, Taketo Taguchi, Roberto Alonso-Mori, Rosalie Tran, Christian Weniger, Henning Schröder, Wilson Quevedo, Hartawan Laksmono, Raymond G. Sierra, Guangye Han, Benedikt Lassalle-Kaiser, Sergey Koroidov, Katharina Kubicek, Simon Schreck, Kristjan KunnusORCiD, Maria Brzhezinskaya, Alexander Firsov, Michael P. Minitti, Joshua J. Turner, Stefan Möller, Nicholas K. Sauter, Michael J. Bogan, Dennis Nordlund, William F. Schlotter, Johannes Messinger, Andrew S. Borovik, Simone Techert, Frank M. F. de Groot, Alexander FöhlischORCiDGND, Alexei Erko, Uwe Bergmann, Vittal K. Yachandra, Philippe Wernet, Junko Yano |
---|
DOI: | https://doi.org/10.1021/jz401837f |
---|
ISSN: | 1948-7185 |
---|
Title of parent work (English): | The journal of physical chemistry letters |
---|
Publisher: | American Chemical Society |
---|
Place of publishing: | Washington |
---|
Publication type: | Article |
---|
Language: | English |
---|
Year of first publication: | 2013 |
---|
Publication year: | 2013 |
---|
Release date: | 2017/03/26 |
---|
Volume: | 4 |
---|
Issue: | 21 |
---|
Number of pages: | 7 |
---|
First page: | 3641 |
---|
Last Page: | 3647 |
---|
Funding institution: | Office of Science, Office of Basic Energy Sciences (OBES), Division of
Chemical Sciences, Geosciences, and Biosciences (CSGB) of the Department
of Energy (DOE) [DE-AC02-050CH11231]; LBNL Laboratory Directed Research
and Development award; NIH [GM50781, GM055302]; Alexander von Humboldt
Foundation; Ruth L. Kirschstein National Research Service Award
[F32GM100595]; OBES; CSGB of the DOE [DE-AC02-76SF00515]; LCLS; SLAC
Laboratory Directed Research and Development award; Volkswagenstiftung
Peter Paul Ewald fellowship; Swedish Energy Agency (Energimyn-digheten);
K&A Wallenberg Foundation (Artificial Leaf Umea); Umea University (Solar
Fuels Umea); Stanford University through the Stanford Institute for
Materials Energy Sciences (SIMES); Lawrence Berkeley National Laboratory
(LBNL), University of Hamburg through the BMBF priority program [FSP
301]; Center for Free Electron Laser Science (CFEL); BMBF project "Next
generation instrumentation for ultrafast X-ray science at
accelerator-driven photon source" [05K12CB4]; Helmholtz Virtual
Institute "Dynamic Pathways in Multidimensional Landscapes"; European
Community [PCIG10-GA-2011-297905]; [SFB755-DFG] |
---|
Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
---|
Peer review: | Referiert |
---|