Density dependence of the yield of hydrated electrons in the low-LET radiolysis of supercritical water at 400 degrees C: influence of the geminate recombination of subexcitation-energy electrons prior to thermalization

作者：Meesungnoen Jintana; Sanguanmith Sunuchakan; Jay Gerin Jean Paul^*

来源：Physical Chemistry Chemical Physics, 2013, 15(39): 16450-16455.

DOI：10.1039/c3cp52630e

Monte Carlo simulations were used to calculate the yield of hydrated electrons (e(aq)(-)) in the low-linear energy transfer radiolysis of supercritical water at 400 degrees C as a function of water density over the range of similar to 0.15 to 0.6 g cm(-3). Very good agreement was found between our calculations and picosecond pulse radiolysis experimental data at similar to 60 ps and 1 ns at high density (%26gt;0.35 g cm(-3)). At densities lower than similar to 0.35 g cm(-3), our e(aq)(-) yields were lower than the experimental data, especially at similar to 60 ps. However, if we incorporated into the simulations a prompt geminate electroncation (H2O radical anion) recombination (prior thermalization of the electron) that decreased as the density decreased, our computed e(aq) yields at similar to 60 ps and 1 ns compared fairly well with the experimental data for the entire density range studied.

• 出版日期2013