Radiolysis of liquid water: An attempt to reconcile Monte-Carlo calculations with new experimental hydrated electron yield data at early times
Radiolysis of liquid water: An attempt to reconcile Monte-Carlo calculations with new experimental hydrated electron yield data at early times
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液态水的辐射分解：早期尝试将蒙特卡罗计算与新的实验水合电子产率数据相协调
DOI：
10.1139/v02-173
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发表时间：
2002
影响因子：
1.1
通讯作者：
S. Mankhetkorn
中科院分区：
文献类型：
--
作者：
Y. Muroya;J. Meesungnoen;J. Jay;A. Filali‐Mouhim;T. Goulet;Y. Katsumura;S. Mankhetkorn
本文对我们的蒙特-卡罗模拟液态水在低线性能量转移（LET ~ 0.3 keV µ m 1）辐射作用下的辐解进行了重新检验，试图使我们的模拟结果与最近修订的早期实验水合电子（eaq）产额数据相一致。亚激发电子的热化距离、热化前电子与水母体阳离子的复合截面以及水分子振动激发态解离衰变中不同竞争机制的分支比被作为可调参数。使用全局拟合程序，我们一直无法找到一组值为这些参数，以同时重现（i）修订的eaq产额4.0 ± 0.2分子每100 eV在“时间零”（即，减少了约20%，比迄今为止接受的值4.8分子每100 eV），（ii）新测量的eaq衰变动力学曲线从100 eV。
A re-examination of our Monte-Carlo modeling of the radiolysis of liquid water by low linear-energy-transfer (LET ~ 0.3 keV µm1) radiation is undertaken herein in an attempt to reconcile the results of our simulation code with recently revised experimental hydrated electron (eaq) yield data at early times. The thermalization distance of subexcitation electrons, the recombination cross section of the electrons with their water parent cations prior to thermalization, and the branching ratios of the different competing mechanisms in the dissociative decay of vibrationally excited states of water molecules were taken as adjustable parameters in our simulations. Using a global-fit procedure, we have been unable to find a set of values for those parameters to simultaneously reproduce (i) the revised eaq yield of 4.0 ± 0.2 molecules per 100 eV at "time zero" (that is, a reduction of ~20% over the hitherto accepted value of 4.8 molecules per 100 eV), (ii) the newly measured eaq decay kinetic profile from 100 ...