GEANT4-DNA simulation of temperature-dependent and pH-dependent yields of chemical radiolytic species

• Published in: Physics in medicine & biology 2023-06, Vol.68 (12), p.124002
• Main Authors: Bian, Jingyi, Duran, Juan, Shin, Wook-Geun, Ramos-Méndez, Jose, Sankey, Jack C, Childress, Lilian, Seuntjens, Jan, Enger, Shirin A
• Format: Article
• Language: English
• Subjects: Computer Simulation; DNA; GEANT4-DNA; Hydrogen-Ion Concentration; Linear Energy Transfer; Models, Chemical; Monte Carlo Method; Protons; radiation chemical yield; radiation chemistry; Temperature; Water; water radiolysis
• ISSN: 0031-9155; 1361-6560; 1361-6560
• DOI: 10.1088/1361-6560/acd90d

GEANT4-DNA can simulate radiation chemical yield ( -value) for radiolytic species such as the hydrated electron (eaq-) with the independent reaction times (IRT) method, however, only at room temperature and neutral pH. This work aims to modify the GEANT4-DNA source code to enable the calculation of -values for radiolytic species at different temperatures and pH values. In the GEANT4-DNA source code, values of chemical parameters such as reaction rate constant, diffusion coefficient, Onsager radius, and water density were replaced by corresponding temperature-dependent polynomials. The initial concentration of hydrogen ion (H )/hydronium ion (H O ) was scaled for a desired pH using the relationship pH = -log [H ]. To validate our modifications, two sets of simulations were performed. (A) A water cube with 1.0 km sides and a pH of 7 was irradiated with an isotropic electron source of 1 MeV. The end time was 1 s. The temperatures varied from 25 °C to 150 °C. (B) The same setup as (A) was used, however, the temperature was set to 25 °C while the pH varied from 5 to 9. The results were compared with published experimental and simulated work. The IRT method in GEANT4-DNA was successfully modified to simulate -values for radiolytic species at different temperatures and pH values. Our temperature-dependent results agreed with experimental data within 0.64%-9.79%, and with simulated data within 3.52%-12.47%. The pH-dependent results agreed well with experimental data within 0.52% to 3.19% except at a pH of 5 (15.99%) and with simulated data within 4.40%-5.53%. The uncertainties were below ±0.20%. Overall our results agreed better with experimental than simulation data. Modifications in the GEANT4-DNA code enabled the calculation of -values for radiolytic species at different temperatures and pH values.