Competition between proton transfer and intermolecular Coulombic decay in water

Clemens Richter, Daniel Hollas, Clara-Magdalena Saak, Marko Förstel, Tsveta Miteva, Melanie Mucke, Olle Björneholm, Nicolas Sisourat, Petr Slavíček () and Uwe Hergenhahn ()
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Clemens Richter: Leibniz Institute of Surface Engineering (IOM)
Daniel Hollas: University of Chemistry and Technology Prague
Clara-Magdalena Saak: Uppsala University
Marko Förstel: Max Planck Institute for Plasma Physics
Tsveta Miteva: Sorbonne Université, CNRS
Melanie Mucke: Uppsala University
Olle Björneholm: Uppsala University
Nicolas Sisourat: Sorbonne Université, CNRS
Petr Slavíček: University of Chemistry and Technology Prague
Uwe Hergenhahn: Leibniz Institute of Surface Engineering (IOM)

Nature Communications, 2018, vol. 9, issue 1, 1-8

Abstract: Abstract Intermolecular Coulombic decay (ICD) is a ubiquitous relaxation channel of electronically excited states in weakly bound systems, ranging from dimers to liquids. As it is driven by electron correlation, it was assumed that it will dominate over more established energy loss mechanisms, for example fluorescence. Here, we use electron–electron coincidence spectroscopy to determine the efficiency of the ICD process after 2a1 ionization in water clusters. We show that this efficiency is surprisingly low for small water clusters and that it gradually increases to 40–50% for clusters with hundreds of water units. Ab initio molecular dynamics simulations reveal that proton transfer between neighboring water molecules proceeds on the same timescale as ICD and leads to a configuration in which the ICD channel is closed. This conclusion is further supported by experimental results from deuterated water. Combining experiment and theory, we infer an intrinsic ICD lifetime of 12–52 fs for small water clusters.

Date: 2018
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DOI: 10.1038/s41467-018-07501-6

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