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Radiation damage by extensive local water ionization from two-step electron-transfer-mediated decay of solvated ions

Gopakumar, G. (author)
Uppsala universitet,Uppsala University,Institutionen för fysik och astronomi,Lund Univ, MAX Lab 4, Lund, Sweden.
Unger, I. (author)
Uppsala universitet,Uppsala University,German Electron Synchrotron (DESY),Institutionen för fysik och astronomi,DESY, FS BIG, Hamburg, Germany.
Slavíček, P. (author)
University of Chemistry and Technology, Prague,Univ Chem & Technol, Dept Phys Chem, Prague, Czech Republic.
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Hergenhahn, U. (author)
Fritz Haber Institute of the Max Planck Society
Öhrwall, G. (author)
Lund University,Lunds universitet,MAX IV-laboratoriet,MAX IV Laboratory
Malerz, S. (author)
Fritz Haber Institute of the Max Planck Society,Fritz Haber Inst Max Planck Gesell, Berlin, Germany.
Céolin, D. (author)
Synchrotron SOLEIL, LOrme Merisiers, Paris, France.
Trinter, F. (author)
Goethe University,Fritz Haber Institute of the Max Planck Society,Fritz Haber Inst Max Planck Gesell, Berlin, Germany.;Goethe Univ Frankfurt Main, Inst Kernphys, Frankfurt, Germany.
Winter, B. (author)
Fritz Haber Institute of the Max Planck Society,Fritz Haber Inst Max Planck Gesell, Berlin, Germany.
Wilkinson, I. (author)
Helmholtz-Zentrum Berlin für Materialien und Energie GmbH,Helmholtz Zentrum Berlin Mat & Energie, Inst Elect Struct Dynam, Berlin, Germany.
Caleman, Carl (author)
Uppsala universitet,Uppsala University,German Electron Synchrotron (DESY),Institutionen för fysik och astronomi,DESY, Ctr Free Elect Laser Sci, Hamburg, Germany.
Muchová, E. (author)
University of Chemistry and Technology, Prague,Univ Chem & Technol, Dept Phys Chem, Prague, Czech Republic.
Björneholm, Olle (author)
Uppsala universitet,Uppsala University,Institutionen för fysik och astronomi
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 (creator_code:org_t)
Nature Publishing Group, 2023
2023
English 7 s.
In: Nature Chemistry. - : Nature Publishing Group. - 1755-4330 .- 1755-4349. ; 15:10, s. 1408-1414
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  • Journal article (peer-reviewed)
Abstract Subject headings
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  • Biomolecular radiation damage is largely mediated by radicals and low-energy electrons formed by water ionization rather than by direct ionization of biomolecules. It was speculated that such an extensive, localized water ionization can be caused by ultrafast processes following excitation by core-level ionization of hydrated metal ions. In this model, ions relax via a cascade of local Auger–Meitner and, importantly, non-local charge- and energy-transfer processes involving the water environment. Here, we experimentally and theoretically show that, for solvated paradigmatic intermediate-mass Al3+ ions, electronic relaxation involves two sequential solute–solvent electron transfer-mediated decay processes. The electron transfer-mediated decay steps correspond to sequential relaxation from Al5+ to Al3+ accompanied by formation of four ionized water molecules and two low-energy electrons. Such charge multiplication and the generated highly reactive species are expected to initiate cascades of radical reactions. [Figure not available: see fulltext.]

Subject headings

NATURVETENSKAP  -- Kemi -- Fysikalisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Physical Chemistry (hsv//eng)

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