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 structure and chemistry 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.
authors.affiliation: Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
authors.forename: R
authors.initials: R
authors.lastname: Alonso-Mori
authors.affiliation: Department of Physics, Graduate School of Science, Kyoto U., Kyoto, 606-8502, Japan.
authors.forename: K
authors.initials: K
authors.lastname: Asa
authors.affiliation: Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
authors.forename: U
authors.initials: U
authors.lastname: Bergmann
authors.affiliation: Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA. JFKern@lbl.gov JYano@lbl.gov.
authors.forename: A S
authors.initials: AS
authors.lastname: Brewster
authors.affiliation: Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA. JFKern@lbl.gov JYano@lbl.gov.
authors.forename: R
authors.initials: R
authors.lastname: Chatterjee
authors.affiliation: Joint Center for Artificial Photosynthesis (JCAP), Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA.
authors.forename: J K
authors.initials: JK
authors.lastname: Cooper
authors.affiliation: Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA. JFKern@lbl.gov JYano@lbl.gov.
authors.forename: H M
authors.initials: HM
authors.lastname: Frei
authors.affiliation: Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA. JFKern@lbl.gov JYano@lbl.gov.
authors.forename: F D
authors.initials: FD
authors.lastname: Fuller
authors.affiliation: Dept. of Chemistry, North Carolina State University, 2620 Yarborough Rd., Raleigh, NC 27695-8204, USA.
authors.forename: E
authors.initials: E
authors.lastname: Goggins
authors.affiliation: Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA. JFKern@lbl.gov JYano@lbl.gov.
authors.forename: S
authors.initials: S
authors.lastname: Gul
authors.affiliation: IMRAM, Tohoku U., Sendai 980-8577, Japan and RIKEN SPring-8 Center, Kouto, Sayo, Hyogo 679-5148, Japan.
authors.forename: H
authors.initials: H
authors.lastname: Fukuzawa
authors.affiliation: IMRAM, Tohoku U., Sendai 980-8577, Japan.
authors.forename: D
authors.initials: D
authors.lastname: Iablonskyi
authors.affiliation: Institut für Biologie, Humboldt-Universität zu Berlin, D-10099 Berlin, Germany.
authors.forename: M
authors.initials: M
authors.lastname: Ibrahim
authors.affiliation: Japan Synchrotron Radiation Research Institute (JASRI), SPring-8/SACLA, Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5198, Japan.
authors.forename: T
authors.initials: T
authors.lastname: Katayama
authors.affiliation: Stanford Synchrotron Radiation Lightsource (SSRL), SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
authors.forename: T
authors.initials: T
authors.lastname: Kroll
authors.affiliation: IMRAM, Tohoku U., Sendai 980-8577, Japan.
authors.forename: Y
authors.initials: Y
authors.lastname: Kumagai
authors.affiliation: Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA. JFKern@lbl.gov JYano@lbl.gov.
authors.forename: B A
authors.initials: BA
authors.lastname: McClure
authors.affiliation: Institutionen för Kemi, Kemiskt Biologiskt Centrum, Umeå Universitet, Umeå, Sweden.
authors.forename: J
authors.initials: J
authors.lastname: Messinger
authors.affiliation: IMRAM, Tohoku U., Sendai 980-8577, Japan and RIKEN SPring-8 Center, Kouto, Sayo, Hyogo 679-5148, Japan.
authors.forename: K
authors.initials: K
authors.lastname: Motomura
authors.affiliation: Department of Physics, Graduate School of Science, Kyoto U., Kyoto, 606-8502, Japan and RIKEN SPring-8 Center, Kouto, Sayo, Hyogo 679-5148, Japan.
authors.forename: K
authors.initials: K
authors.lastname: Nagaya
authors.affiliation: Department of Physics, Graduate School of Science, Kyoto U., Kyoto, 606-8502, Japan.
authors.forename: T
authors.initials: T
authors.lastname: Nishiyama
authors.affiliation: Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA. JFKern@lbl.gov JYano@lbl.gov.
authors.forename: C
authors.initials: C
authors.lastname: Saracini
authors.affiliation: Department of Physics, Graduate School of Science, Kyoto U., Kyoto, 606-8502, Japan.
authors.forename: Y
authors.initials: Y
authors.lastname: Sato
authors.affiliation: Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA. JFKern@lbl.gov JYano@lbl.gov.
authors.forename: N K
authors.initials: NK
authors.lastname: Sauter
authors.affiliation: Stanford Synchrotron Radiation Lightsource (SSRL), SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
authors.forename: D
authors.initials: D
authors.lastname: Sokaras
authors.affiliation: IMRAM, Tohoku U., Sendai 980-8577, Japan.
authors.forename: T
authors.initials: T
authors.lastname: Takanashi
authors.affiliation: Japan Synchrotron Radiation Research Institute (JASRI), SPring-8/SACLA, Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5198, Japan.
authors.forename: T
authors.initials: T
authors.lastname: Togashi
authors.affiliation: IMRAM, Tohoku U., Sendai 980-8577, Japan and RIKEN SPring-8 Center, Kouto, Sayo, Hyogo 679-5148, Japan.
authors.forename: K
authors.initials: K
authors.lastname: Ueda
authors.affiliation: Dept. of Chemistry, North Carolina State University, 2620 Yarborough Rd., Raleigh, NC 27695-8204, USA.
authors.forename: W W
authors.initials: WW
authors.lastname: Weare
authors.affiliation: Center for High Pressure Science & Technology Advanced Research, Shanghai, China.
authors.forename: T-C
authors.initials: TC
authors.lastname: Weng
authors.affiliation: Japan Synchrotron Radiation Research Institute (JASRI), SPring-8/SACLA, Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5198, Japan.
authors.forename: M
authors.initials: M
authors.lastname: Yabashi
authors.affiliation: Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA. JFKern@lbl.gov JYano@lbl.gov.
authors.forename: V K
authors.initials: VK
authors.lastname: Yachandra
authors.affiliation: Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA. JFKern@lbl.gov JYano@lbl.gov.
authors.forename: I D
authors.initials: ID
authors.lastname: Young
authors.affiliation: Institut für Biologie, Humboldt-Universität zu Berlin, D-10099 Berlin, Germany.
authors.forename: A
authors.initials: A
authors.lastname: Zouni
authors.affiliation: Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA and Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA. JFKern@lbl.gov JYano@lbl.gov.
authors.forename: J F
authors.initials: JF
authors.lastname: Kern
authors.affiliation: Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA. JFKern@lbl.gov JYano@lbl.gov and Joint Center for Artificial Photosynthesis (JCAP), Lawrence Berkeley National Laboratory, 1 Cyclotron Rd., Berkeley, CA 94720, USA and IMRAM, Tohoku U., Sendai 980-8577, Japan.
authors.forename: J
authors.initials: J
authors.lastname: Yano
mesh_terms: D002384:Catalysis; D018360:Crystallography, X-Ray; D004583:Electrons; D007834:Lasers; D014965:X-Rays