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Research Article

Energy-dispersive X-ray emission spectroscopy using an X-ray free-electron laser in a shot-by-shot mode

Roberto Alonso-Mori, Jan Kern, Richard J. Gildea, Dimosthenis Sokaras, Tsu-Chien Weng, Benedikt Lassalle-Kaiser, Rosalie Tran, Johan Hattne, Hartawan Laksmono, Julia Hellmich, Carina Glöckner, Nathaniel Echols, Raymond G. Sierra, Donald W. Schafer, Jonas Sellberg, Christopher Kenney, Ryan Herbst, Jack Pines, Philip Hart, Sven Herrmann, Ralf W. Grosse-Kunstleve, Matthew J. Latimer, Alan R. Fry, Marc M. Messerschmidt, Alan Miahnahri, M. Marvin Seibert, Petrus H. Zwart, William E. White, Paul D. Adams, Michael J. Bogan, Sébastien Boutet, Garth J. Williams, Athina Zouni, Johannes Messinger, Pieter Glatzel, Nicholas K. Sauter, Vittal K. Yachandra, Junko Yano, and Uwe Bergmann
PNAS first published November 5, 2012; https://doi.org/10.1073/pnas.1211384109
Roberto Alonso-Mori
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Jan Kern
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
bPhysical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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Richard J. Gildea
bPhysical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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Dimosthenis Sokaras
cStanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Tsu-Chien Weng
cStanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Benedikt Lassalle-Kaiser
bPhysical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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Rosalie Tran
bPhysical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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Johan Hattne
bPhysical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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Hartawan Laksmono
dPULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Julia Hellmich
eMax-Volmer-Laboratorium für Biophysikalische Chemie, Technische Universität, D-10623 Berlin, Germany;
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Carina Glöckner
eMax-Volmer-Laboratorium für Biophysikalische Chemie, Technische Universität, D-10623 Berlin, Germany;
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Nathaniel Echols
bPhysical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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Raymond G. Sierra
dPULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Donald W. Schafer
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Jonas Sellberg
cStanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
fDepartment of Physics, AlbaNova, Stockholm University, S-106 91 Stockholm, Sweden;
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Christopher Kenney
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
cStanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Ryan Herbst
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
cStanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Jack Pines
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
cStanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Philip Hart
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
cStanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Sven Herrmann
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
cStanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Ralf W. Grosse-Kunstleve
bPhysical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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Matthew J. Latimer
cStanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Alan R. Fry
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Marc M. Messerschmidt
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Alan Miahnahri
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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M. Marvin Seibert
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Petrus H. Zwart
bPhysical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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William E. White
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Paul D. Adams
bPhysical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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Michael J. Bogan
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
eMax-Volmer-Laboratorium für Biophysikalische Chemie, Technische Universität, D-10623 Berlin, Germany;
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Sébastien Boutet
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Garth J. Williams
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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Athina Zouni
eMax-Volmer-Laboratorium für Biophysikalische Chemie, Technische Universität, D-10623 Berlin, Germany;
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Johannes Messinger
gInstitutionen för Kemi, Kemiskt Biologiskt Centrum, Umeå Universitet, Umeå, Sweden; and
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Pieter Glatzel
hEuropean Synchrotron Radiation Facility, F-38043 Grenoble Cedex, France
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Nicholas K. Sauter
bPhysical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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Vittal K. Yachandra
bPhysical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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  • For correspondence: bergmann@slac.stanford.edu vkyachandra@lbl.gov JYano@lbl.gov
Junko Yano
bPhysical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720;
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  • For correspondence: bergmann@slac.stanford.edu vkyachandra@lbl.gov JYano@lbl.gov
Uwe Bergmann
aLinac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025;
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  • For correspondence: bergmann@slac.stanford.edu vkyachandra@lbl.gov JYano@lbl.gov
  1. Edited by Harry B. Gray, California Institute of Technology, Pasadena, CA, and approved October 16, 2012 (received for review July 7, 2012)

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Abstract

The ultrabright femtosecond X-ray pulses provided by X-ray free-electron lasers open capabilities for studying the structure and dynamics of a wide variety of systems beyond what is possible with synchrotron sources. Recently, this “probe-before-destroy” approach has been demonstrated for atomic structure determination by serial X-ray diffraction of microcrystals. There has been the question whether a similar approach can be extended to probe the local electronic structure by X-ray spectroscopy. To address this, we have carried out femtosecond X-ray emission spectroscopy (XES) at the Linac Coherent Light Source using redox-active Mn complexes. XES probes the charge and spin states as well as the ligand environment, critical for understanding the functional role of redox-active metal sites. Kβ1,3 XES spectra of MnII and Mn2III,IV complexes at room temperature were collected using a wavelength dispersive spectrometer and femtosecond X-ray pulses with an individual dose of up to >100 MGy. The spectra were found in agreement with undamaged spectra collected at low dose using synchrotron radiation. Our results demonstrate that the intact electronic structure of redox active transition metal compounds in different oxidation states can be characterized with this shot-by-shot method. This opens the door for studying the chemical dynamics of metal catalytic sites by following reactions under functional conditions. The technique can be combined with X-ray diffraction to simultaneously obtain the geometric structure of the overall protein and the local chemistry of active metal sites and is expected to prove valuable for understanding the mechanism of important metalloproteins, such as photosystem II.

  • energy-dispersive XES
  • Kβ emission lines
  • femtosecond x-ray spectroscopy

Footnotes

  • ↵1To whom correspondence may be addressed. E-mail: bergmann{at}slac.stanford.edu, vkyachandra{at}lbl.gov, or JYano{at}lbl.gov.
  • Author contributions: R.A.-M., J.K., V.K.Y., J.Y., and U.B. designed research; R.A.-M., J.K., D.S., T.-C.W., B.L.-K., R.T., J. Hattne, H.L., J. Hellmich, C.G., N.E., R.G.S., D.W.S., J.S., A.R.F., M.M.M., M.M.S., M.J.B., S.B., G.J.W., A.Z., J.M., P.G., N.K.S., V.K.Y., J.Y., and U.B. performed research; J.K., R.J.G., J. Hattne, J. Hellmich, C.G., N.E., C.K., R.H., J.P., P.H., S.H., M.J.L., A.M., W.E.W., P.D.A., M.J.B., A.Z., N.K.S., V.K.Y., and J.Y. contributed new reagents/analytic tools; R.A.-M., J.K., R.J.G., J. Hattne, N.E., R.W.G.-K., P.H.Z., and N.K.S. analyzed data; and R.A.-M., J.K., D.S., J.M., V.K.Y., J.Y., and U.B. wrote the paper.

  • The authors declare no conflict of interest.

  • This article is a PNAS Direct Submission.

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Shot-by-shot energy-dispersive XES using an XFEL
Roberto Alonso-Mori, Jan Kern, Richard J. Gildea, Dimosthenis Sokaras, Tsu-Chien Weng, Benedikt Lassalle-Kaiser, Rosalie Tran, Johan Hattne, Hartawan Laksmono, Julia Hellmich, Carina Glöckner, Nathaniel Echols, Raymond G. Sierra, Donald W. Schafer, Jonas Sellberg, Christopher Kenney, Ryan Herbst, Jack Pines, Philip Hart, Sven Herrmann, Ralf W. Grosse-Kunstleve, Matthew J. Latimer, Alan R. Fry, Marc M. Messerschmidt, Alan Miahnahri, M. Marvin Seibert, Petrus H. Zwart, William E. White, Paul D. Adams, Michael J. Bogan, Sébastien Boutet, Garth J. Williams, Athina Zouni, Johannes Messinger, Pieter Glatzel, Nicholas K. Sauter, Vittal K. Yachandra, Junko Yano, Uwe Bergmann
Proceedings of the National Academy of Sciences Nov 2012, 201211384; DOI: 10.1073/pnas.1211384109

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Shot-by-shot energy-dispersive XES using an XFEL
Roberto Alonso-Mori, Jan Kern, Richard J. Gildea, Dimosthenis Sokaras, Tsu-Chien Weng, Benedikt Lassalle-Kaiser, Rosalie Tran, Johan Hattne, Hartawan Laksmono, Julia Hellmich, Carina Glöckner, Nathaniel Echols, Raymond G. Sierra, Donald W. Schafer, Jonas Sellberg, Christopher Kenney, Ryan Herbst, Jack Pines, Philip Hart, Sven Herrmann, Ralf W. Grosse-Kunstleve, Matthew J. Latimer, Alan R. Fry, Marc M. Messerschmidt, Alan Miahnahri, M. Marvin Seibert, Petrus H. Zwart, William E. White, Paul D. Adams, Michael J. Bogan, Sébastien Boutet, Garth J. Williams, Athina Zouni, Johannes Messinger, Pieter Glatzel, Nicholas K. Sauter, Vittal K. Yachandra, Junko Yano, Uwe Bergmann
Proceedings of the National Academy of Sciences Nov 2012, 201211384; DOI: 10.1073/pnas.1211384109
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