Linear energy transfer dependence of transient yields in water irradiated by 150 keV – 500 MeV protons in the limit of low dose rates

FLASH radiotherapy is a new irradiation method in which large doses of ionizing radiation are delivered to tumors almost instantly (a few milliseconds), paradoxically sparing healthy tissue while preserving anti-tumor activity. Although this technique is primarily studied in the context of electron and photon therapies, proton delivery at high dose rates can also reduce the adverse side effects on normal cells. So far, no definitive mechanism has been proposed to explain the differences in the responses to radiation between tumor and normal tissues. Given that living cells and tissues consist mainly of water, we set out to study the effects of high dose rates on the radiolysis of water by protons in the energy range of 150 keV – 500 MeV (i.e., for linear energy transfer (LET) values between ∼72.2 and 0.23 keV/μm, respectively) using Monte Carlo simulations. To validate our methodology, however, we, first, report here the results of our calculations of the yields (G values) of the radiolytically produced species, namely the hydrated electron (e-aq ), •OH, H•, H2, and H2O2, for low dose rates. Overall, our simulations agree very well with the experiment. In the presence of oxygen, e-aq and H• atoms are rapidly converted into superoxide anion or hydroperoxyl radicals, with a well-defined maximum of G(HO2/O2-) at ∼1 μs. This maximum decreases substantially when going from low-LET 500 MeV to high-LET 150 keV irradiating protons. Differences in the geometry of the proton track structure with increasing LET readily explain this diminution in HO2/O2- radicals.The accepted manuscript in pdf format is listed with the files at the bottom of this page. The presentation of the authors' names and (or) special characters in the title of the manuscript may differ slightly between what is listed on this page and what is listed in the pdf file of the accepted manuscript; that in the pdf file of the accepted manuscript is what was submitted by the author

High-dose-rate effects in the radiolysis of water at elevated temperatures.

Monte Carlo track chemistry simulations were used to study the effects of high dose rates on the radical (e-aq, H•, and •OH) and molecular (H2 and H2O2) yields in the low linear energy transfer (LET) radiolysis of liquid water at elevated temperatures between 25–350 C. Our simulation model consisted of randomly irradiating water by single pulses of N incident protons of 300 MeV (LET ~ 0.3 keV/μm), which penetrate at the same time perpendicular to this water within the surface of a circle. The effect of dose rate was studied by varying N. Our simulations showed that, at any given temperature, the radical products decrease with increasing dose rate and, at the same time, the molecular products increase, resulting from an increase in the inter-track, radical-radical reactions. Using the kinetics of the decay of hydrated electrons at 25 and 350 C, we determined a critical time (τc) for each value of N, which corresponds to the “onset” of dose-rate effects. For our irradiation model, τc was inversely proportional to N for the two temperatures considered, with τc at 350 C being shifted by an order of magnitude to shorter times compared to its values at 25 C. Finally, the data obtained from the simulations for N = 2,000 generally agreed with the observation that during the track stage of the radiolysis, free radical yields increase, while molecular products decrease with increasing temperature from 25 to 350 C. The exceptions of e-aq and H2 to this general pattern are briefly discussed.The accepted manuscript in pdf format is listed with the files at the bottom of this page. The presentation of the authors' names and (or) special characters in the title of the manuscript may differ slightly between what is listed on this page and what is listed in the pdf file of the accepted manuscript; that in the pdf file of the accepted manuscript is what was submitted by the author

Characterizing the Early Acidic Response in Advanced Small Modular Reactors Cooled with High-Temperature, High-Pressure Water

Utilizing Monte Carlo multi-track chemistry simulations along with a cylindrical instantaneous pulse (Dirac) irradiation model, we assessed the initial acidic response in both subcritical and supercritical water under high radiation dose rates. This investigation spans a temperature range of 300 to 500 °C at a nominal pressure of 25 MPa, aligning with the operational conditions anticipated in proposed supercritical water (SCW)-cooled small modular reactors (SCW-SMRs). A pivotal finding from our study is the observation of a significant ‘acid spike’ effect, which shows a notable intensification in response to increasing radiation dose rates. Our results bring to light the potential risks posed by this acidity, which could potentially foster a corrosive environment and thereby increase the risk of accelerated material degradation in reactor components

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

(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”

Generation of ultrafast, transient, highly acidic pH spikes in the radiolysis of water at very high dose rates. Relevance for FLASH radiotherapy.

Monte Carlo multi-track chemistry simulations were carried out to study the effects of high dose rates on the transient yields of hydronium ions (H3OThe accepted manuscript in pdf format is listed with the files at the bottom of this page. The presentation of the authors' names and (or) special characters in the title of the manuscript may differ slightly between what is listed on this page and what is listed in the pdf file of the accepted manuscript; that in the pdf file of the accepted manuscript is what was submitted by the author

On the influence of electron mobilities on the yields of formation of positronium in liquids: New I3 measurements and Monte Carlo simulations

International audienceWe study the formation of positronium (Ps) at the end of the radiation tracks generated by the passage of energetic positrons in various liquids. We focus particularly on the possible influence of the thermal electron mobility μ(e⎯) on this process. To this end, we present a compilation of experimental data of the probability of ortho-Ps formation I3 and μ(e⎯) in 51 pure liquids at room temperature. We also present new measurements of I3 as a function of temperature for n-hexane, 2,2-dimethylbutane, tetramethylsilane, and tetramethylstannane from the melting point up to 294 K. Those results are compared to the variation of μ(e⎯) with temperature which can be found in the literature. Finally, we use Monte Carlo simulation techniques to perform a sensitivity study in which we evaluate the relative contributions of various physicochemical properties of the liquids (such as the mean thermalization distances of e+ and e⎯, their thermal mobilities, the dielectric constant, and the temperature) on the values of I3. A review of previous works on this question is also given

Scavenging of "dry" electrons prior to hydration by azide ions: Effect on the formation of H2 in the radiolysis of water by 60Co γ-rays and tritium β-electrons.

In this study, we use Monte Carlo track chemistry simulations to show that "dry" secondary electrons, precursors of the "hydrated" electron (eThe accepted manuscript in pdf format is listed with the files at the bottom of this page. The presentation of the authors' names and (or) special characters in the title of the manuscript may differ slightly between what is listed on this page and what is listed in the pdf file of the accepted manuscript; that in the pdf file of the accepted manuscript is what was submitted by the author