Proton-transfer mediated enhancement of nonlocal electronic relaxation processes in X-ray irradiated liquid water.
Proton-transfer mediated enhancement of nonlocal electronic relaxation processes in X-ray irradiated liquid water.
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质子转移介导的 X 射线照射液态水中非局域电子弛豫过程的增强
DOI：
10.1021/ja5117588
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发表时间：
2014
影响因子：
15
通讯作者：
Kryzhevoi N.V.
中科院分区：
文献类型：
--
作者：
Slavíček P;Winter B;Cederbaum L.S;Kryzhevoi N.V.
我们用从头算和量子动力学方法模拟了正常和重液态水的氧1s俄歇电子能谱。计算的光谱进行了分析，并与最近报道的实验数据进行了比较。暴露于电离X射线辐射的液态水中的电子弛豫比预期的要多样化和复杂得多，并且与孤立的水分子非常不同。液相中的核心水平离子化水分子，除了局部俄歇过程之外，还通过非局部能量和电荷转移（例如分子间库仑衰变和电子转移介导衰变（ETMD））来弛豫。我们评估这三类松弛过程的相对效率。对不同电子衰变模式相对效率的定量估计有助于确定电离X射线产生的各种反应物质的产率。在这里被认为是第一次在核心水平制度的ETMD过程中发现有一个令人惊讶的高效率。重要的是，我们发现，所有的非局域电子弛豫过程显着增强的核心离子化水和相邻分子之间的超快质子转移。
We have simulated the oxygen 1s Auger-electron spectra of normal and heavy liquid water usingab initioand quantum dynamical methods. The computed spectra are analyzed and compared to recently reported experimental data. The electronic relaxation in liquid water exposed to ionizing X-ray radiation is shown to be far more diverse and complex than anticipated and extremely different than for an isolated water molecule. A core-level ionized water molecule in the liquid phase, in addition to a local Auger process, relaxes through nonlocal energy and charge transfer, such as intermolecular Coulombic decay and electron-transfer mediated decay (ETMD). We evaluate the relative efficiencies for these three classes of relaxation processes. The quantitative estimates for the relative efficiencies of different electronic decay modes help determine yields of various reactive species produced by ionizing X-rays. The ETMD processes which are considered here for the first time in the core-level regime are found to have a surprisingly high efficiency. Importantly, we find that all nonlocal electronic relaxation processes are significantly enhanced by ultrafast proton transfer between the core-ionized water and neighboring molecules.
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控制共振螺旋钻过程中的衰变和破碎之间的相互作用
DOI：
--
发表时间：
1998
期刊：
影响因子：
--
作者：
E. Pahl;L. Cederbaum;H. Meyer;F. Tarantelli
通讯作者：
F. Tarantelli
液态水中电子激发过氧化氢的弛豫：来自俄歇电子发射的见解
DOI：
--
发表时间：
2013
期刊：
影响因子：
--
作者：
S. Thürmer;I. Unger;P. Slavíček;B. Winter
通讯作者：
B. Winter
影响因子：
2.8
作者：
Hjelte, I;Piancastelli, MN;Svensson, S
通讯作者：
Svensson, S
影响因子：
4.4
作者：
F. Tarantelli;A. Sgamellotti;L. Cederbaum
通讯作者：
F. Tarantelli;A. Sgamellotti;L. Cederbaum
影响因子：
3.4
作者：
Richard H. Henchman;Stuart J Cockram
通讯作者：
Richard H. Henchman;Stuart J Cockram