Observation of the fastest chemical processes in the radiolysis of water

Author:

Loh Z.-H.1ORCID,Doumy G.2ORCID,Arnold C.345ORCID,Kjellsson L.67ORCID,Southworth S. H.2ORCID,Al Haddad A.2,Kumagai Y.2ORCID,Tu M.-F.2ORCID,Ho P. J.2,March A. M.2ORCID,Schaller R. D.89ORCID,Bin Mohd Yusof M. S.1ORCID,Debnath T.1ORCID,Simon M.10,Welsch R.35ORCID,Inhester L.3ORCID,Khalili K.11ORCID,Nanda K.12ORCID,Krylov A. I.312ORCID,Moeller S.13,Coslovich G.13ORCID,Koralek J.13ORCID,Minitti M. P.13ORCID,Schlotter W. F.13ORCID,Rubensson J.-E.6ORCID,Santra R.345ORCID,Young L.214ORCID

Affiliation:

1. Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore.

2. Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA.

3. Center for Free-Electron Laser Science, DESY, Hamburg, Germany.

4. Department of Physics, Universität Hamburg, Hamburg, Germany.

5. Hamburg Centre for Ultrafast Imaging, Hamburg, Germany.

6. Department of Physics and Astronomy, Uppsala University, Uppsala, Sweden.

7. European XFEL GmbH, Schenefeld, Germany.

8. Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, USA.

9. Department of Chemistry, Northwestern University, Evanston, IL, USA.

10. Sorbonne Université and CNRS, Laboratoire de Chemie Physique-Matière et Rayonnement, LCPMR, F-750005 Paris, France.

11. Department of Energy Conversion and Storage, Technical University of Denmark, Roskilde, Denmark.

12. Department of Chemistry, University of Southern California, Los Angeles, CA, USA.

13. Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.

14. Department of Physics and James Franck Institute, University of Chicago, Chicago, IL, USA.

Abstract

The “hole” story of water ionization The direct observation of the cationic hole H 2 O + that is formed in liquid water after ionization has been a long-standing experimental challenge. Previous attempts using optical and ultraviolet techniques have failed to reveal its key spectroscopic signature during ultrafast transformation into a OH radical. Loh et al. address this gap by using intense, ultrafast x-ray pulses from an x-ray free electron laser at ∼530 electron volts. They found compelling evidence for the formation H 2 O + and its decay to an OH radical by a proton transfer mechanism and elucidated the other fastest–time scale steps in the early-time dynamics of ionized liquid water. Science , this issue p. 179

Funder

U.S. Department of Energy

H2020 European Research Council

Deutsche Forschungsgemeinschaft

National Science Foundation

Swedish Science Council

Singapore Ministry of Education

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

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