Stabilization of AgI's polar surfaces by the aqueous environment, and its implications for ice formation.
Stabilization of AgI's polar surfaces by the aqueous environment, and its implications for ice formation.
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水环境对 AgI 极性表面的稳定性及其对冰形成的影响。
DOI：
10.1039/c9cp02193k
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发表时间：
2019
期刊：
影响因子：
--
通讯作者：
Sayer T
中科院分区：
文献类型：
--
作者：
Sayer T
碘化银是已知的最有效的无机冰成核颗粒之一，该特征通常归因于其基底Ag-（0001）和I-（000）表面与冰之间的优异晶格匹配。然而，该晶体终止是III型极性表面，并且其表面能因此随晶体尺寸发散，除非极性补偿机制占优势。在这项模拟研究中，我们研究了周围的水环境能够在多大程度上提供这种极性补偿。就其本身而言，我们发现，纯水是无法稳定的碘化银晶体在物理上合理的方式，和移动的电荷载体，如溶解的离子，是必不可少的。换句话说，邻近的溶解离子必须被认为是异质冰形成机制的一个组成部分。我们进行的模拟利用了模拟方法的最新进展，其中施加了适当的电场和电位移场。这项研究的一个有用的副产品是与常用的Yeh-Berkowitz方法进行直接比较。在这里，我们发现，幼稚的应用后者导致物理上不合理的结果，并大大影响了接触层中的H2O的结构。因此，我们希望这些结果是普遍的重要性，在水环境中的极性/带电表面的研究。
Silver iodide is one of the most potent inorganic ice nucleating particles known, a feature generally attributed to the excellent lattice match between its basal Ag-(0001) and I-(000) surfaces, and ice. This crystal termination, however, is a type-III polar surface, and its surface energy therefore diverges with crystal size unless a polarity compensation mechanism prevails. In this simulation study, we investigate to what extent the surrounding aqueous environment is able to provide such polarity compensation. On its own, we find that pure H2O is unable to stabilize the AgI crystal in a physically reasonable manner, and that mobile charge carriers such as dissolved ions, are essential. In other words, proximate dissolved ions must be considered an integral part of the heterogeneous ice formation mechanism. The simulations we perform utilize recent advances in simulation methodology in which appropriate electric and electric displacement fields are imposed. A useful by-product of this study is the direct comparison to the commonly used Yeh–Berkowitz method that this enables. Here we find that naive application of the latter leads to physically unreasonable results, and greatly influences the structure of H2O in the contact layer. We therefore expect these results to be of general importance to those studying polar/charged surfaces in aqueous environments.
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影响因子：
3.9
作者：
J. Uehara;K. Aramaki
通讯作者：
J. Uehara;K. Aramaki
DOI：
10.1063/1.5054843
发表时间：
2018-09
期刊：
The Journal of chemical physics
影响因子：
--
作者：
T. Sayer;M. Sprik;Chao Zhang
通讯作者：
T. Sayer;M. Sprik;Chao Zhang
影响因子：
1.7
作者：
F. Shimojo;M. Kobayashi
通讯作者：
M. Kobayashi
影响因子：
64.8
作者：
HEAD, RB
通讯作者：
HEAD, RB
影响因子：
4.4
作者：
Peter Wirnsberger;Domagoj Fijan;Andjela vSari'c;M. Neumann;C. Dellago;D. Frenkel
通讯作者：
D. Frenkel