Hydration Structure of Na + and K + Ions in Solution Predicted by Data-Driven Many-Body Potentials
Hydration Structure of Na + and K + Ions in Solution Predicted by Data-Driven Many-Body Potentials
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数据驱动的多体势预测溶液中 Na 和 K 离子的水合结构
DOI：
10.1021/acs.jpcb.2c05674
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Paesani, Francesco
中科院分区：
文献类型：
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作者：
Zhuang, Debbie;Riera, Marc;Zhou, Ruihan;Deary, Alexander;Paesani, Francesco
Na+和K+离子在溶液中的水合结构进行了系统的研究，逐步包括多体相互作用的更准确的表示使用的分子模型的层次结构。我们发现，一个传统的经验成对加性力场，通常用于生物分子模拟是无法重现扩展的X射线吸收精细结构（EXAFS）光谱的两种离子。与此相反，逐步列入严格来自多体膨胀的能量的多体效应允许MB-nrg势能函数（PEFs），以实现几乎定量的协议与实验EXAFS光谱，从而使发展的分子水平的图片的水合结构的Na+和K+在溶液中。由于MB-nrg PEFs已经被证明可以准确地描述气相中小离子-水簇的异构平衡和振动光谱，因此本研究表明，MB-nrg PEFs有效地代表了长期寻求的模型，能够正确地预测从气相到液相的离子水溶液体系的性质，迄今为止仍然难以捉摸。
The hydration structure of Na+and K+ions in solution is systematically investigated using a hierarchy of molecular models that progressively include more accurate representations of many-body interactions. We found that a conventional empirical pairwise additive force field that is commonly used in biomolecular simulations is unable to reproduce the extended X-ray absorption fine structure (EXAFS) spectra for both ions. In contrast, progressive inclusion of many-body effects rigorously derived from the many-body expansion of the energy allows the MB-nrg potential energy functions (PEFs) to achieve nearly quantitative agreement with the experimental EXAFS spectra, thus enabling the development of a molecular-level picture of the hydration structure of both Na+and K+in solution. Since the MB-nrg PEFs have already been shown to accurately describe isomeric equilibria and vibrational spectra of small ion–water clusters in the gas phase, the present study demonstrates that the MB-nrg PEFs effectively represent the long-sought-after models able to correctly predict the properties of ionic aqueous systems from the gas to the liquid phase, which has so far remained elusive.