Observation of the fastest chemical processes in the radiolysis of water

Z-H Loh; G Doumy; C Arnold; L Kjellsson; S H Southworth; A Al Haddad; Y Kumagai; M-F Tu; P J Ho; A M March; R D Schaller; M S Bin Mohd Yusof; T Debnath; M Simon; R Welsch; L Inhester; K Khalili; K Nanda; A I Krylov; S Moeller; G Coslovich; J Koralek; M P Minitti; W F Schlotter; J-E Rubensson; R Santra; L Young

doi:10.1126/science.aaz4740

Observation of the fastest chemical processes in the radiolysis of water

Science. 2020 Jan 10;367(6474):179-182. doi: 10.1126/science.aaz4740.

Authors

Z-H Loh¹, G Doumy², C Arnold^{3

4

5}, L Kjellsson^{6

7}, S H Southworth², A Al Haddad², Y Kumagai², M-F Tu², P J Ho², A M March², R D Schaller^{8

9}, M S Bin Mohd Yusof¹⁰, T Debnath¹⁰, M Simon¹¹, R Welsch^{3

5}, L Inhester³, K Khalili¹², K Nanda¹³, A I Krylov^{3

13}, S Moeller¹⁴, G Coslovich¹⁴, J Koralek¹⁴, M P Minitti¹⁴, W F Schlotter¹⁴, J-E Rubensson⁶, R Santra^{15

4

5}, L Young^{16

17}

Affiliations

¹ Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore. [email protected] [email protected] [email protected].
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 Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore.
¹¹ Sorbonne Université and CNRS, Laboratoire de Chemie Physique-Matière et Rayonnement, LCPMR, F-750005 Paris, France.
¹² Department of Energy Conversion and Storage, Technical University of Denmark, Roskilde, Denmark.
¹³ Department of Chemistry, University of Southern California, Los Angeles, CA, USA.
¹⁴ Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
¹⁵ Center for Free-Electron Laser Science, DESY, Hamburg, Germany. [email protected] [email protected] [email protected].
¹⁶ Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA. [email protected] [email protected] [email protected].
¹⁷ Department of Physics and James Franck Institute, University of Chicago, Chicago, IL, USA.

PMID: 31919219
DOI: 10.1126/science.aaz4740

Abstract

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, H₂O⁺, 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 (H₂O⁺/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.

Publication types

Research Support, U.S. Gov't, Non-P.H.S.
Research Support, Non-U.S. Gov't

Grants and funding

ERC_/European Research Council/International