Ab initio molecular dynamics study of crystal hydrates of HCl including path integral results
Ab initio molecular dynamics study of crystal hydrates of HCl including path integral results
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HCl 晶体水合物的从头算分子动力学研究，包括路径积分结果
DOI：
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发表时间：
1997
期刊：
影响因子：
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通讯作者：
M. Klein
中科院分区：
文献类型：
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作者：
T. T. Rosenvinge;M. Tuckerman;M. Klein
氯化氢的水合物是离子晶体，含有水合氢离子。据报道，一水化合物中的水合氢离子在与反转对称有关的两个可能位置之间具有统计上的无序性。利用基于密度泛函的Car-Parrinello技术，对氯化氢的一水合物、二水合物和三水合物进行了Abinitio分子动力学（MD）计算。模拟的目的是研究这些晶体中的质子无序性。通过路径积分MD模拟探讨了核量子效应的可能作用。结果表明，在一水化合物中提出的紊乱位点是动态不稳定的，因此不太可能是报道的紊乱的原因。不幸的是，由于二水合物的单位电池较大，导致模拟困难，因此获得的信息很少。核量子效应是表征三水合物中质子分布的重要手段。
The hydrates of hydrogen chloride are ionic crystals, which contain hydronium. The hydronium in the monohydrate has been reported to be statistically disordered between two possible sites related by inversion symmetry. Abinitio molecular dynamics (MD) calculations are presented for the mono-, di- and tri-hydrates of hydrogen chloride using the density functional based Car–Parrinello technique. The simulations were carried out with the goal of investigating proton disorder in these crystals. The possible role of nuclear quantum effects has been explored via path integral MD simulations. The results suggest that the proposed disordered sites in the monohydrate are dynamically unstable and therefore unlikely to be responsible for the reported disorder. Unfortunately, little information was obtained for the dihydrate because the large unit cell leads to difficulties in carrying out the simulations. Nuclear quantum effects are shown to be important for characterizing the proton distributions in the trihydrate.