Real-time observation of water radiolysis and hydrated electron formation induced by extreme-ultraviolet pulses
Open Access
- 1 January 2020
- journal article
- research article
- Published by American Association for the Advancement of Science (AAAS) in Science Advances
- Vol. 6 (3), eaaz0385
- https://doi.org/10.1126/sciadv.aaz0385
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 similar to 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.Funding Information
- Carl-Zeiss-Stiftung
- Deutsche Forschungsgemeinschaft (DFG STI 125/19-1)
- Czech Science Foundation (18-23756S)
- ETH Zurich
- ERC starting Grant (#307270-ATTOSCOPE)
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