Real-time observation of water radiolysis and hydrated electron formation induced by extreme-ultraviolet pulses

Abstract: The dominant pathway of radiation damage begins with the ionization of water. Thus far, however, the underlying primary processes could not be conclusively elucidated. Here, we directly study the earliest steps of extreme ultraviolet (XUV)–induced water radiolysis through one-photon excitation of large water clusters using time-resolved photoelectron imaging. Results are presented for H2O and D2O clusters using femtosecond pump pulses centered at 133 or 80 nm. In both excitation schemes, hydrogen or proton transfer is observed to yield a prehydrated electron within 30 to 60 fs, followed by its solvation in 0.3 to 1.0 ps and its decay through geminate recombination on a ∼10-ps time scale. These results are interpreted by comparison with detailed multiconfigurational non-adiabatic ab-initio molecular dynamics calculations. Our results provide the first comprehensive picture of the primary steps of radiation chemistry and radiation damage and demonstrate new approaches for their study with unprecedented time resolution

Location
Deutsche Nationalbibliothek Frankfurt am Main
Extent
Online-Ressource
Language
Englisch
Notes
Science advances. - 6, 3 (2020) , eaaz0385, ISSN: 2375-2548

Event
Veröffentlichung
(where)
Freiburg
(who)
Universität
(when)
2020
Creator
Svoboda, Vít
Michiels, Rupert Paul
LaForge, Aaron
Med, Jacub
Stienkemeier, Frank
Slavíček, Petr
Wörner, Hans Jakob
Contributor
Molekül- und Nanophysik

DOI
10.1126/sciadv.aaz0385
URN
urn:nbn:de:bsz:25-freidok-1715952
Rights
Open Access; Der Zugriff auf das Objekt ist unbeschränkt möglich.
Last update
25.03.2025, 1:56 PM CET

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Associated

Time of origin

  • 2020

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