Significant role of secondary electrons in the formation of a multi-body chemical species spur produced by water radiolysis

Abstract

Abstract Scientific insights into water photolysis and radiolysis are essential for estimating the direct and indirect effects of deoxyribonucleic acid (DNA) damage. Secondary electrons from radiolysis intricately associated with both effects. In our previous paper, we simulated the femtosecond (1 × 10− 15 s) dynamics of secondary electrons ejected by energy depositions of 11−19 eV into water via high-energy electron transport using a time-dependent simulation code. The results contribute to the understanding of simple “intra-spur” chemical reactions of tree-body chemical species (hydrated electrons, hydronium ion and OH radical) in subsequent chemical processes. Herein, we simulate the dynamics of the electrons ejected by energy depositions of 20−30 eV. The present results contribute to the understanding of complex “inter-spur” chemical reactions of the multi-body chemical species as well as for the formation of complex DNA damage with redox site and strand break on DNA. The simulation results present the earliest formation mechanism of an unclear multi-body chemical species spur when secondary electrons induce further ionisations or electronic excitations. The formation involves electron–water collisions, i.e. ionisation, electronic excitation, molecular excitation and elastic scattering. Our simulation results indicate that (1) most secondary electrons delocalise to ~ 12 nm, and multiple collisions are sometimes induced in a water molecule at 22 eV deposition energy. (2) The secondary electrons begin to induce diffuse band excitation of water around a few nm from the initial energy deposition site and delocalise to ~ 8 nm at deposition energies ~ 25 eV. (3) The secondary electron can cause one additional ionisation or electronic excitation at deposition energies > 30 eV, forming a multi-body chemical species spur. Thus, we propose that the type and density of chemical species produced by water radiolysis strongly depend on the deposition energy. From our results, we discuss formation of complex DNA damage.