Ionic-charge dependence of the intermolecular coulombic decay time scale for aqueous ions probed by the core-hole clock.

Ionic-charge dependence of the intermolecular coulombic decay time scale for aqueous ions probed by the core-hole clock.
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核心孔时钟探测的水离子的分子间库仑衰变时间尺度的离子电荷依赖性。

DOI:
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发表时间:
2011
影响因子:
15
通讯作者:
O. Björneholm
O. Björneholm
中科院分区:
化学1区
文献类型:
--
作者:
W. Pokapanich;N. Kryzhevoi;N. Ottosson;S. Svensson;L. Cederbaum;G. Öhrwall;O. Björneholm

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用俄歇电子能谱结合理论计算研究了Ca(2+)水溶液中Ca 2p核心空穴的衰变。除了本地化的两个洞的最终状态的钙离子,起源于一个正常的俄歇过程,我们已经进一步确定了最终状态的钙离子和它的水环境之间的离域和产生的核心水平的分子间库仑衰变(ICD)过程。应用核孔时钟方法,测定了Ca(2+)水溶液中2p核孔的核级ICD时标为33 ± 1fs。将该时间常数与水溶液中K(+)、Na(+)、Mg(2+)和Al(3+)离子的时间常数进行比较,发现相差1至2个数量级。这种大的变化的核心水平ICD过程的特征时间尺度的定性解释不同的内部衰变机制,在不同的离子,以及不同的离子溶剂的距离和相互作用。
Auger electron spectroscopy combined with theoretical calculations has been applied to investigate the decay of the Ca 2p core hole of aqueous Ca(2+). Beyond the localized two-hole final states on the calcium ion, originating from a normal Auger process, we have further identified the final states delocalized between the calcium ion and its water surroundings and produced by core level intermolecular Coulombic decay (ICD) processes. By applying the core-hole clock method, the time scale of the core level ICD was determined to be 33 ± 1 fs for the 2p core hole of the aqueous Ca(2+). The comparison of this time constant to those associated with the aqueous K(+), Na(+), Mg(2+), and Al(3+) ions reveals differences of 1 and up to 2 orders of magnitude. Such large variations in the characteristic time scales of the core level ICD processes is qualitatively explained by different internal decay mechanisms in different ions as well as by different ion-solvent distances and interactions.
DOI: 10.1038/nphys1500
发表时间: 2010-02-01
期刊: NATURE PHYSICS
影响因子: 19.6
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发表时间: 2003-05-23
影响因子: 8.6
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