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Characterizing heterogeneous dynamics at hydrated electrode surfaces

机译:表征水合电极表面的异质动力学

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In models of Pt 111 and Pt 100 surfaces in water, motions of molecules in the first hydration layer are spatially and temporally correlated. To interpret these collective motions, we apply quantitative measures of dynamic heterogeneity that are standard tools for considering glassy systems. Specifically, we carry out an analysis in terms of mobility fields and distributions of persistence times and exchange times. In so doing, we show that dynamics in these systems is facilitated by transient disorder in frustrated two-dimensional hydrogen bonding networks. The frustration is the result of unfavorable geometry imposed by strong metal-water bonding. The geometry depends upon the structure of the underlying metal surface. Dynamic heterogeneity of water on the Pt 111 surface is therefore qualitatively different than that for water on the Pt 100 surface. In both cases, statistics of this ad-layer dynamic heterogeneity responds asymmetrically to applied voltage.
机译:在水中的Pt 111和Pt 100表面模型中,第一水化层中分子的运动在空间和时间上是相关的。为了解释这些集体运动,我们应用了动态异质性的定量度量,这是考虑玻璃系统的标准工具。具体来说,我们根据迁移率字段以及持续时间和交换时间的分布进行分析。这样做,我们表明在受挫的二维氢键网络中,瞬态无序促进了这些系统的动力学。挫败是由于强大的金属与水之间的键合造成几何形状不利的结果。几何形状取决于下层金属表面的结构。因此,Pt 111表面上水的动态异质性与Pt 100表面上水的动态异质性在质量上是不同的。在这两种情况下,此广告层动态异质性的统计信息均不对称地响应施加的电压。

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