Intermolecular Coulombic decay in liquid water competes with proton transfer and non-adiabatic relaxation

Pengju Zhang (), Joel Trester, Jakub Dubský, Přemysl Kolorenč, Petr Slavíček () and Hans Jakob Wörner ()
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Pengju Zhang: Chinese Academy of Sciences
Joel Trester: ETH Zürich
Jakub Dubský: University of Chemistry and Technology
Přemysl Kolorenč: Institute of Theoretical Physics
Petr Slavíček: University of Chemistry and Technology
Hans Jakob Wörner: ETH Zürich

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract Despite decades of research, our understanding of radiation damage in aqueous systems remains limited. The recent discovery of Intermolecular Coulombic Decay (ICD) following inner-valence ionization of liquid water raises interesting questions about its efficiency as a major source of low-energy electrons responsible for radiation damage. To investigate, we performed electron-electron coincidence measurements on liquid H2O and D2O using a monochromatized high-harmonic-generation light source, detecting ICD electrons in coincidence with photoelectrons from the 2a1 shell. We find that the ICD efficiency γ is below unity in both liquids and that γ(H2O)/γ(D2O) = 0.86 ± 0.03. Ab initio calculations reveal that ICD competes with proton transfer and non-adiabatic relaxation, which can close the ICD channel. A multi-scale stochastic model incorporating solvent effects reproduces these efficiencies. Our combined experimental and theoretical results suggest that the higher ICD efficiency in D2O arises from slower proton transfer and non-adiabatic transitions, highlighting the crucial role of nuclear motion in liquid-phase ICD and advancing the understanding of radiation damage.

Date: 2025
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DOI: 10.1038/s41467-025-61912-w

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