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Suppression of X-ray-induced radiation damage to biomolecules in aqueous environments by immediate intermolecular decay of inner-shell vacancies

The predominant reason for the damaging power of high-energy radiation is multiple ionization of a molecule, either direct or via the decay of highly excited intermediates, as, e.g., in the case of X-ray irradiation. Consequently, the molecule is irreparably damaged by the subsequent fragmentation i...

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Main Authors: Hans, Andreas (Author) , Schmidt, Philipp (Author) , Küstner-Wetekam, Catmarna (Author) , Trinter, Florian (Author) , Deinert, Sascha (Author) , Bloß, Dana (Author) , Viehmann, Johannes H. (Author) , Schaf, Rebecca (Author) , Gerstel, Miriam (Author) , Saak, Clara M. (Author) , Buck, Jens (Author) , Klumpp, Stephan (Author) , Hartmann, Gregor (Author) , Cederbaum, Lorenz S. (Author) , Kryzhevoi, Nikolai V. (Author) , Knie, André (Author)
Format: Article (Journal)
Language:English
Published: July 23, 2021
In: The journal of physical chemistry letters
Year: 2021, Volume: 12, Issue: 30, Pages: 7146-7150
ISSN:1948-7185
DOI:10.1021/acs.jpclett.1c01879
Online Access:Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1021/acs.jpclett.1c01879
Verlag, lizenzpflichtig, Volltext: https://pubs.acs.org/doi/10.1021/acs.jpclett.1c01879
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Author Notes:Andreas Hans, Philipp Schmidt, Catmarna Küstner-Wetekam, Florian Trinter, Sascha Deinert, Dana Bloß, Johannes H. Viehmann, Rebecca Schaf, Miriam Gerstel, Clara M. Saak, Jens Buck, Stephan Klumpp, Gregor Hartmann, Lorenz S. Cederbaum, Nikolai V. Kryzhevoi, and André Knie
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Summary:The predominant reason for the damaging power of high-energy radiation is multiple ionization of a molecule, either direct or via the decay of highly excited intermediates, as, e.g., in the case of X-ray irradiation. Consequently, the molecule is irreparably damaged by the subsequent fragmentation in a Coulomb explosion. In an aqueous environment, however, it has been observed that irradiated molecules may be saved from fragmentation presumably by charge and energy dissipation mechanisms. Here, we show that the protective effect of the environment sets in even earlier than hitherto expected, namely immediately after single inner-shell ionization. By combining coincidence measurements of the fragmentation of X-ray-irradiated microsolvated pyrimidine molecules with theoretical calculations, we identify direct intermolecular electronic decay as the protective mechanism, outrunning the usually dominant Auger decay. Our results demonstrate that such processes play a key role in charge delocalization and have to be considered in investigations and models on high-energy radiation damage in realistic environments.
Item Description:Gesehen am 15.10.2021
Physical Description:Online Resource
ISSN:1948-7185
DOI:10.1021/acs.jpclett.1c01879

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