Early and Transient Formation of Highly Acidic pH Spikes in Water Radiolysis under the Combined Effect of High Dose Rate and High Linear Energy Transfer

Abstract

(1) Background: Water radiolysis leads to the formation of hydronium ions H3O+ in less than 50 fs, resulting in the formation of transient acidic pH spikes in the irradiated water. The purpose of this study is to examine the time evolution of these spikes of acidity under irradiation conditions combining both high absorbed dose rate and high-LET radiation. (2) Methods: The early space–time history of the distributions of the various reactive species was obtained using our Monte Carlo multitrack chemistry simulation code IONLYS-IRT. To simulate different LETs, we used incident protons of varying energies as radiation sources. The “instantaneous pulse” (or Dirac) model was used to investigate the effect of dose rate. (3) Results: One major finding is that the combination of high dose rates and high LETs is clearly additive, with a very significant impact on the pH of the solution. For example, at 1 ns and for a dose rate of ~107 Gy/s, the pH drops from ~4.7 to 2.7 as the LET increases from ~0.3 to 60 keV/μm. (4) Conclusions: Confirming previous work, this purely radiation chemical study raises the question of the possible importance and role of these spikes of acidity in underpinning the physical chemistry and biology of the “FLASH effect”.

Keywords

• water radiolysis
• radiation dose rate
• linear energy transfer (LET)
• acidity (pH)
• Monte Carlo multitrack chemistry simulation
• radiation chemical yield (<i>G</i> value)