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

Alonso-Mori, Roberto; Kern, Jan; Gildea, Richard J.; Sokaras, Dimosthenis; Weng, Tsu -Chien; Lassalle-Kaiser, Benedikt; Tran, Rosalie; Hattne, Johan; Laksmono, Hartawan; Hellmich, Julia; Glockner, Carina; Echols, Nathaniel; Sierra, Raymond G.; Schafer, Donald W.; Sellberg, Jonas; Kenney, Christopher; Herbst, Ryan; Pines, Jack; Hart, Philip; Herrmann, Sven; Grosse-Kunstleve, Ralf W.; Latimer, Matthew J.; Fry, Alan R.; Messerschmidt, Marc M.; Miahnahri, Alan; Seibert, M. Marvin; Zwart, Petrus H.; White, William E.; Adams, Paul D.; Bogan, Michael J.; Boutet, Sebastien; Williams, Garth J.; Zouni, Athina; Messinger, Johannes; Glatzel, Pieter; Sauter, Nicholas K.; Yachandra, Vittal K.; Yano, Junko; Bergmann, Uwe

doi:10.1073/pnas.1211384109

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

Journal Article · Mon Nov 05 00:00:00 EST 2012 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1211384109· OSTI ID:1132324

Alonso-Mori, Roberto ^[1]; Kern, Jan ^[2]; Gildea, Richard J. ^[3]; Sokaras, Dimosthenis ^[1]; Weng, Tsu -Chien ^[1]; Lassalle-Kaiser, Benedikt ^[3]; Tran, Rosalie ^[3]; Hattne, Johan ^[3]; Laksmono, Hartawan ^[1]; Hellmich, Julia ^[4]; Glockner, Carina ^[4]; Echols, Nathaniel ^[3]; Sierra, Raymond G. ^[1]; Schafer, Donald W. ^[1]; Sellberg, Jonas ^[5]; Kenney, Christopher ^[1]; Herbst, Ryan ^[1]; Pines, Jack ^[1]; Hart, Philip ^[1]; Herrmann, Sven ^[1] more »

SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Technische Univ. Berlin (Germany)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Stockholm Univ., Stockholm (Sweden)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Technische Univ. Berlin (Germany)
Umea Univ., Umea (Sweden)
European Synchrotron Radiation Facility, Grenoble Cedex (France)

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. Kβ_1,3 XES spectra of Mn^II and Mn₂^III,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. Furthermore, 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.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1132324

Report Number(s):: SLAC-REPRINT--2014-130

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 47 Vol. 109; ISSN 0027-8424

Publisher:: National Academy of Sciences, Washington, DC (United States)Copyright Statement

Country of Publication:: United States

Language:: English

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