Département de Médecine Nucléaire et Radiobiologie, Faculté de Médecine et des Sciences de la Santé, Université de Sherbrooke, 3001, 12ème Avenue Nord, Sherbrooke, Québec J1H 5N4, Canada.
Phys Chem Chem Phys. 2013 Oct 21;15(39):16450-5. doi: 10.1039/c3cp52630e. Epub 2013 Sep 2.
Monte Carlo simulations were used to calculate the yield of hydrated electrons (eaq(-)) in the low-linear energy transfer radiolysis of supercritical water at 400 °C as a function of water density over the range of ~0.15 to 0.6 g cm(-3). Very good agreement was found between our calculations and picosecond pulse radiolysis experimental data at ~60 ps and 1 ns at high density (>0.35 g cm(-3)). At densities lower than ~0.35 g cm(-3), our eaq(-) yields were lower than the experimental data, especially at ~60 ps. However, if we incorporated into the simulations a prompt geminate electron-cation (H2O˙(+)) recombination (prior thermalization of the electron) that decreased as the density decreased, our computed eaq(-) yields at ~60 ps and 1 ns compared fairly well with the experimental data for the entire density range studied.
采用蒙特卡罗模拟方法，计算了 400°C 超临界水中低线性能量转移辐射分解作用下水合电子（eaq(-)）的产额随水密度的变化，水密度范围约为 0.15 至 0.6 g cm(-3)。在高密度（>0.35 g cm(-3)）时，我们的计算结果与皮秒脉冲辐射分解实验数据在约 60 ps 和 1 ns 处非常吻合。在密度低于约 0.35 g cm(-3)时，我们的 eaq(-)产额低于实验数据，特别是在约 60 ps 时。然而，如果我们在模拟中加入一个快速的复合电子-阳离子（H2O˙(+)）复合（电子的先预热），随着密度的降低而降低，那么我们在约 60 ps 和 1 ns 时计算的 eaq(-)产额与整个研究密度范围内的实验数据相比相当吻合。
