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High energy radiation femtochemistry of water molecules: early electron-radical pairs processes

  • Topical issue on Molecular level assessments of radiation biodamage
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Abstract

The damages triggered by ionizing radiation on chemical and biological targets depend on the survival probability of radicals produced in clusters of ionization-excitation events. In this paper, we report on femtolysis (FEMTOsecond radioLYSIS) of pure liquid water using an innovative laser produced high-energy, ultra-short electron bunches in the 2.5-15 MeV range and high energy radiation femtochemistry (HERF) measurements. The short-time monitoring of a primary reducing radical, hydrated electron e\(^{-}_{aq}\), has been performed in confined ionization spaces (nascent spurs). The calculated yield of hydrated electrons at early time, \(G({\rm e}^{-}_{aq})_{ET}\), is estimated to be 6.5 ± 0.5 (number/100 eV) at t ~ 5 ps after the ultrafast energy deposition. This estimated value is high compare to (i) the available data of previous works that used scavenging techniques; (ii) the predictions of stochastic water radiolysis modelling for which the initial behaviour of hydrated electron is investigated in the framework of a classical diffusion regime of independent pairs. The HERF developments give new insights into the early ubiquitous radical escape probability in nascent aqueous spurs and emphasize the importance of short-lived solvent bridged electron-radical complexes [\({\rm H}_{3}{\rm O}^{+...}\)  \({\rm e}_{aq}^{-}\) ..\({\rm OH}]_{n{\rm H}_2{\rm O}}\) (non-independent pairs). A complete understanding of the G(\({\rm e}^{-}_{aq})_{ET}\) value needs to account for quantum aspects of 1s-like trapped electron ground state and neoformed prototropic radicals that govern ultra-fast recombination processes within these non-independent pair configurations. Femtolysis data emphasize that within a time-dependent non-diffusion regime, spatio-temporal correlations between hydrated electron and nearest neighbours OH radical or hydrated proton (\({\rm H}_{3}{\rm O}^{+}\)) would assist ultrafast anisotropic 1D recombination within solvent bridged electron-radical complexes. The emerging HERF domain would provide guidance for understanding of ultrashort-lived sub-structure of tracks and stimulate future semi-quantum simulations on prethermal radical reactions.

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  1. Laboratoire d’Optique Appliquée, CNRS UMR 7639, École Polytechnique ParisTech – ENSTA ParisTech, 91761, Palaiseau Cedex, France

    Y. A. Gauduel, Y. Glinec, J.-P. Rousseau, F. Burgy & V. Malka

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Gauduel, Y., Glinec, Y., Rousseau, JP. et al. High energy radiation femtochemistry of water molecules: early electron-radical pairs processes. Eur. Phys. J. D 60, 121–135 (2010). https://doi.org/10.1140/epjd/e2010-00152-2

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