A new approach for simulating inhomogeneous chemical kinetics

Journal Article · 27 August 2023 · Scientific Reports

DOI: https://doi.org/10.1038/s41598-023-39741-y · OSTI ID:1997064

Bradshaw, Georgia; O’Leary, Mel; Purser, Arthur S. F.; Villagomez-Bernabe, Balder; Wyett, Cyrus; Currell, Frederick; Webb, Marcus

Abstract In this paper, inhomogeneous chemical kinetics are simulated by describing the concentrations of interacting chemical species by a linear expansion of basis functions in such a manner that the coupled reaction and diffusion processes are propagated through time efficiently by tailor-made numerical methods. The approach is illustrated through modelling $$$$\alpha$$$$ $\alpha$ - and $$$$\gamma$$$$ $\gamma$ -radiolysis in thin layers of water and at their solid interfaces from the start of the chemical phase until equilibrium was established. The method’s efficiency is such that hundreds of such systems can be modelled in a few hours using a single core of a typical laptop, allowing the investigation of the effects of the underlying parameter space. Illustrative calculations showing the effects of changing dose-rate and water-layer thickness are presented. Other simulations are presented which show the approach’s capability to solve problems with spherical symmetry (an approximation to an isolated radiolytic spur), where the hollowing out of an initial Gaussian distribution is observed, in line with previous calculations. These illustrative simulations show the generality and the computational efficiency of this approach to solving reaction-diffusion problems. Furthermore, these example simulations illustrate the method’s suitability for simulating solid-fluid interfaces, which have received a lot of experimental attention in contrast to the lack of computational studies.

• Research Organization: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
• Sponsoring Organization: USDOE
• Grant/Contract Number: 89233218CNA000001
• OSTI ID: 1997064
• Journal Information: Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 13; ISSN 2045-2322
• Publisher: Nature Publishing GroupCopyright Statement
• Country of Publication: United Kingdom
• Language: English