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Title: Towards characterization of photo-excited electron transfer and catalysis in natural and artificial systems using XFELs

Abstract

The ultra-bright femtosecond X-ray pulses provided by X-ray Free Electron Lasers (XFELs) open capabilities for studying the structure and dynamics of a wide variety of biological and inorganic systems beyond what is possible at synchrotron sources. Although the chemistry and structure at the catalytic sites have been studied intensively in both biological and inorganic systems, a full understanding of the atomic-scale chemistry requires new approaches beyond the steady state X-ray crystallography and X-ray spectroscopy at cryogenic temperatures. Following the dynamic changes in the geometric and electronic structure at ambient conditions, while overcoming X-ray damage to the redox active catalytic center, is key for deriving reaction mechanisms. Such studies become possible by using the intense and ultra-short femtosecond X-ray pulses from an XFEL, where sample is probed before it is damaged. We have developed methodology for simultaneously collecting X-ray diffraction data and X-ray emission spectra, using an energy dispersive spectrometer, at ambient conditions, and used this approach to study the room temperature structure and intermediate states of the photosynthetic water oxidizing metallo-protein, photosystem II. Moreover, we have also used this setup to simultaneously collect the X-ray emission spectra from multiple metals to follow the ultrafast dynamics of light-induced charge transfer betweenmore » multiple metal sites. A Mn–Ti containing system was studied at an XFEL to demonstrate the efficacy and potential of this method.« less

Authors:
 [1];  [2];  [3];  [4];  [4];  [4];  [4];  [4];  [5];  [4];  [6];  [7];  [8];  [9];  [10];  [7];  [4];  [11];  [6];  [12] more »;  [2];  [4];  [2];  [4];  [10];  [7];  [9];  [6];  [5];  [13];  [9];  [4];  [4];  [8];  [14];  [15] « less
+ Show Author Affiliations
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Kyoto Univ. (Japan)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  5. North Carolina State Univ., Raleigh, NC (United States)
  6. RIKEN SPring-8 Center, Kouto (Japan); Tohoku Univ., Sendai (Japan)
  7. Tohoku Univ., Sendai (Japan)
  8. Humboldt Univ. of Berlin (Germany)
  9. Japan Synchrotron Radiation Research Institute (JASRI), Kouto (Japan)
  10. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  11. Umea Univ. (Sweden)
  12. Kyoto Univ. (Japan); RIKEN SPring-8 Center, Kouto (Japan)
  13. Center for High Pressure Science & Technology Advanced Research, Shanghai (China)
  14. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  15. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Tohoku Univ., Sendai (Japan)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1378998
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Faraday Discussions
Additional Journal Information:
Journal Volume: 194; Journal ID: ISSN 1359-6640
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Alonso-Mori, R., Asa, K., Bergmann, U., Brewster, A. S., Chatterjee, R., Cooper, J. K., Frei, H. M., Fuller, F. D., Goggins, E., Gul, S., Fukuzawa, H., Iablonskyi, D., Ibrahim, M., Katayama, T., Kroll, T., Kumagai, Y., McClure, B. A., Messinger, J., Motomura, K., Nagaya, K., Nishiyama, T., Saracini, C., Sato, Y., Sauter, N. K., Sokaras, D., Takanashi, T., Togashi, T., Ueda, K., Weare, W. W., Weng, T. -C., Yabashi, M., Yachandra, V. K., Young, I. D., Zouni, A., Kern, J. F., and Yano, J. Towards characterization of photo-excited electron transfer and catalysis in natural and artificial systems using XFELs. United States: N. p., 2016. Web. doi:10.1039/c6fd00084c.
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Alonso-Mori, R., Asa, K., Bergmann, U., Brewster, A. S., Chatterjee, R., Cooper, J. K., Frei, H. M., Fuller, F. D., Goggins, E., Gul, S., Fukuzawa, H., Iablonskyi, D., Ibrahim, M., Katayama, T., Kroll, T., Kumagai, Y., McClure, B. A., Messinger, J., Motomura, K., Nagaya, K., Nishiyama, T., Saracini, C., Sato, Y., Sauter, N. K., Sokaras, D., Takanashi, T., Togashi, T., Ueda, K., Weare, W. W., Weng, T. -C., Yabashi, M., Yachandra, V. K., Young, I. D., Zouni, A., Kern, J. F., & Yano, J. Towards characterization of photo-excited electron transfer and catalysis in natural and artificial systems using XFELs. United States. https://doi.org/10.1039/c6fd00084c
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Alonso-Mori, R., Asa, K., Bergmann, U., Brewster, A. S., Chatterjee, R., Cooper, J. K., Frei, H. M., Fuller, F. D., Goggins, E., Gul, S., Fukuzawa, H., Iablonskyi, D., Ibrahim, M., Katayama, T., Kroll, T., Kumagai, Y., McClure, B. A., Messinger, J., Motomura, K., Nagaya, K., Nishiyama, T., Saracini, C., Sato, Y., Sauter, N. K., Sokaras, D., Takanashi, T., Togashi, T., Ueda, K., Weare, W. W., Weng, T. -C., Yabashi, M., Yachandra, V. K., Young, I. D., Zouni, A., Kern, J. F., and Yano, J. Thu . "Towards characterization of photo-excited electron transfer and catalysis in natural and artificial systems using XFELs". United States. https://doi.org/10.1039/c6fd00084c. https://www.osti.gov/servlets/purl/1378998.
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@article{osti_1378998,
title = {Towards characterization of photo-excited electron transfer and catalysis in natural and artificial systems using XFELs},
author = {Alonso-Mori, R. and Asa, K. and Bergmann, U. and Brewster, A. S. and Chatterjee, R. and Cooper, J. K. and Frei, H. M. and Fuller, F. D. and Goggins, E. and Gul, S. and Fukuzawa, H. and Iablonskyi, D. and Ibrahim, M. and Katayama, T. and Kroll, T. and Kumagai, Y. and McClure, B. A. and Messinger, J. and Motomura, K. and Nagaya, K. and Nishiyama, T. and Saracini, C. and Sato, Y. and Sauter, N. K. and Sokaras, D. and Takanashi, T. and Togashi, T. and Ueda, K. and Weare, W. W. and Weng, T. -C. and Yabashi, M. and Yachandra, V. K. and Young, I. D. and Zouni, A. and Kern, J. F. and Yano, J.},
abstractNote = {The ultra-bright femtosecond X-ray pulses provided by X-ray Free Electron Lasers (XFELs) open capabilities for studying the structure and dynamics of a wide variety of biological and inorganic systems beyond what is possible at synchrotron sources. Although the chemistry and structure at the catalytic sites have been studied intensively in both biological and inorganic systems, a full understanding of the atomic-scale chemistry requires new approaches beyond the steady state X-ray crystallography and X-ray spectroscopy at cryogenic temperatures. Following the dynamic changes in the geometric and electronic structure at ambient conditions, while overcoming X-ray damage to the redox active catalytic center, is key for deriving reaction mechanisms. Such studies become possible by using the intense and ultra-short femtosecond X-ray pulses from an XFEL, where sample is probed before it is damaged. We have developed methodology for simultaneously collecting X-ray diffraction data and X-ray emission spectra, using an energy dispersive spectrometer, at ambient conditions, and used this approach to study the room temperature structure and intermediate states of the photosynthetic water oxidizing metallo-protein, photosystem II. Moreover, we have also used this setup to simultaneously collect the X-ray emission spectra from multiple metals to follow the ultrafast dynamics of light-induced charge transfer between multiple metal sites. A Mn–Ti containing system was studied at an XFEL to demonstrate the efficacy and potential of this method.},
doi = {10.1039/c6fd00084c},
journal = {Faraday Discussions},
number = ,
volume = 194,
place = {United States},
year = {Thu Jun 02 00:00:00 EDT 2016},
month = {Thu Jun 02 00:00:00 EDT 2016}
}
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    Works referencing / citing this record:

    Drop-on-demand sample delivery for studying biocatalysts in action at X-ray free-electron lasers
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