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


Ontology type: schema:ScholarlyArticle     


Article Info

DATE

2010-10

AUTHORS

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

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, has been performed in confined ionization spaces (nascent spurs). The calculated yield of hydrated electrons at early time, , 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 [ ..(non-independent pairs). A complete understanding of the G( 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 () 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. More... »

PAGES

121-135

References to SciGraph publications

Identifiers

URI

http://scigraph.springernature.com/pub.10.1140/epjd/e2010-00152-2

DOI

http://dx.doi.org/10.1140/epjd/e2010-00152-2

DIMENSIONS

https://app.dimensions.ai/details/publication/pub.1023286183


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