Observation of the fastest chemical processes in the radiolysis of water.

Autor: Loh ZH; Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore. zhiheng@ntu.edu.sg robin.santra@cfel.de young@anl.gov., Doumy G; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA., Arnold C; Center for Free-Electron Laser Science, DESY, Hamburg, Germany.; Department of Physics, Universität Hamburg, Hamburg, Germany.; Hamburg Centre for Ultrafast Imaging, Hamburg, Germany., Kjellsson L; Department of Physics and Astronomy, Uppsala University, Uppsala, Sweden.; European XFEL GmbH, Schenefeld, Germany., Southworth SH; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA., Al Haddad A; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA., Kumagai Y; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA., Tu MF; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA., Ho PJ; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA., March AM; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA., Schaller RD; Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, USA.; Department of Chemistry, Northwestern University, Evanston, IL, USA., Bin Mohd Yusof MS; Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore., Debnath T; Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore., Simon M; Sorbonne Université and CNRS, Laboratoire de Chemie Physique-Matière et Rayonnement, LCPMR, F-750005 Paris, France., Welsch R; Center for Free-Electron Laser Science, DESY, Hamburg, Germany.; Hamburg Centre for Ultrafast Imaging, Hamburg, Germany., Inhester L; Center for Free-Electron Laser Science, DESY, Hamburg, Germany., Khalili K; Department of Energy Conversion and Storage, Technical University of Denmark, Roskilde, Denmark., Nanda K; Department of Chemistry, University of Southern California, Los Angeles, CA, USA., Krylov AI; Center for Free-Electron Laser Science, DESY, Hamburg, Germany.; Department of Chemistry, University of Southern California, Los Angeles, CA, USA., Moeller S; Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Coslovich G; Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Koralek J; Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Minitti MP; Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Schlotter WF; Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA., Rubensson JE; Department of Physics and Astronomy, Uppsala University, Uppsala, Sweden., Santra R; Center for Free-Electron Laser Science, DESY, Hamburg, Germany. zhiheng@ntu.edu.sg robin.santra@cfel.de young@anl.gov.; Department of Physics, Universität Hamburg, Hamburg, Germany.; Hamburg Centre for Ultrafast Imaging, Hamburg, Germany., Young L; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA. zhiheng@ntu.edu.sg robin.santra@cfel.de young@anl.gov.; Department of Physics and James Franck Institute, University of Chicago, Chicago, IL, USA.
Jazyk: angličtina
Zdroj: Science (New York, N.Y.) [Science] 2020 Jan 10; Vol. 367 (6474), pp. 179-182.
DOI: 10.1126/science.aaz4740
Abstrakt: Elementary processes associated with ionization of liquid water provide a framework for understanding radiation-matter interactions in chemistry and biology. Although numerous studies have been conducted on the dynamics of the hydrated electron, its partner arising from ionization of liquid water, H 2 O + , remains elusive. We used tunable femtosecond soft x-ray pulses from an x-ray free electron laser to reveal the dynamics of the valence hole created by strong-field ionization and to track the primary proton transfer reaction giving rise to the formation of OH. The isolated resonance associated with the valence hole (H 2 O + /OH) enabled straightforward detection. Molecular dynamics simulations revealed that the x-ray spectra are sensitive to structural dynamics at the ionization site. We found signatures of hydrated-electron dynamics in the x-ray spectrum.
(Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.)
Databáze: MEDLINE
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