Modeling Molecular Interactions in Water: From Pairwise to Many-Body Potential Energy Functions.
Modeling Molecular Interactions in Water: From Pairwise to Many-Body Potential Energy Functions.
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DOI：
10.1021/acs.chemrev.5b00644
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发表时间：
2016-07-13
期刊：
影响因子：
62.1
通讯作者：
Paesani F
中科院分区：
文献类型：
--
作者：
Cisneros GA;Wikfeldt KT;Ojamäe L;Lu J;Xu Y;Torabifard H;Bartók AP;Csányi G;Molinero V;Paesani F
从第一次对水进行计算机模拟到现在已经过去了近50年，从那时起，人们提出了大量的分子模型来阐明水在不同相中的独特行为。在这篇文章中，我们回顾了最近的进展，旨在正确地代表多体效应的分析势能函数的发展。从相互作用能的多体展开开始，具体重点是建立在近似层次结构上的不同类别的势能函数，以及它们准确再现从最先进的电子结构计算和实验测量获得的参考数据的能力。我们表明，最近的势能函数，其中包括明确的两体和三体效应的短程表示沿着与物理上正确的描述多体效应在所有距离，预测水的性质，从气体到凝聚相前所未有的准确性，从而为人们长期寻求的能够描述水在不同条件和不同环境下的行为的“通用模型”打开了大门。
Almost 50 years have passed from the first computer simulations of water, and a large number of molecular models have been proposed since then to elucidate the unique behavior of water across different phases. In this article, we review the recent progress in the development of analytical potential energy functions that aim at correctly representing many-body effects. Starting from the many-body expansion of the interaction energy, specific focus is on different classes of potential energy functions built upon a hierarchy of approximations and on their ability to accurately reproduce reference data obtained from state-of-the-art electronic structure calculations and experimental measurements. We show that most recent potential energy functions, which include explicit short-range representations of two-body and three-body effects along with a physically correct description of many-body effects at all distances, predict the properties of water from the gas to the condensed phase with unprecedented accuracy, thus opening the door to the long-sought “universal model” capable of describing the behavior of water under different conditions and in different environments.