Multi-Scale Modelling of the Gamma Radiolysis of Nitrate Solutions

Research output: Contribution to journalArticle

  • Authors:
  • Gregory Horne
  • Thomas Donoclift
  • Howard E. Sims
  • Robin M. Orr
  • Simon Pimblott


A multi-scale modelling approach has been developed for the extended timescale long-term radiolysis of aqueous systems. The approach uses a combination of stochastic track structure and track chemistry as well as deterministic homogeneous chemistry techniques and involves four key stages; radiation track structure simulation, the subsequent physicochemical processes, nonhomogeneous diffusion-reaction kinetic evolution, and homogeneous bulk chemistry modelling. The first three components model the physical and chemical evolution of an isolated radiation chemical track and provide radiolysis yields, within the extremely low dose isolated track paradigm, as the input parameters for a bulk deterministic chemistry model. This approach to radiation chemical modelling has been tested by comparison with the experimentally observed yield of nitrite from the gamma radiolysis of sodium nitrate solutions. This is a complex radiation chemical system which is strongly dependent on secondary reaction processes. The concentration of nitrite is not just dependent upon the evolution of radiation track chemistry and the scavenging of the hydrated electron and its precursors, but also on the subsequent reactions of the products of these scavenging reactions with other water radiolysis products. Without the inclusion of intra-track chemistry, the deterministic component of the multi-scale model is unable to correctly predict experimental data, highlighting the importance of intra-track radiation chemistry in the chemical evolution of the irradiated system.

Bibliographical metadata

Original languageEnglish
Pages (from-to)11781-11789
Number of pages9
JournalThe Journal of Physical Chemistry Part B
Issue number45
Early online date25 Oct 2016
StatePublished - 17 Nov 2016