Improving Force Field Accuracy by Training against Condensed-Phase Mixture Properties.
Improving Force Field Accuracy by Training against Condensed-Phase Mixture Properties.
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DOI：
10.1021/acs.jctc.1c01268
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发表时间：
2022-06-14
影响因子：
5.5
通讯作者：
Shirts, Michael R.
中科院分区：
文献类型：
--
作者：
Boothroyd, Simon;Madin, Owen C.;Mobley, David L.;Wang, Lee-Ping;Chodera, John D.;Shirts, Michael R.
开发一个足够精确的分子经典力场表示是实现分子模拟作为获得广泛的化学和生物现象的基本见解的途径的全部潜力的关键。然而，只有当模型准确地捕捉到系统中不同物种分子之间的复杂相互作用时，这才有可能实现。历史上，分子间范德华（vdW）相互作用主要是根据纯（单组分）体系的密度和蒸发焓进行训练的，偶尔使用水化自由能。在这项研究中，我们展示了包括二元混合物的物理性质数据如何更好地告知这些参数，在复杂的化学混合物中编码更多关于系统潜在物理的信息。为了证明这一点，我们针对二元液体混合物的混合密度和混合焓以及纯液体系统的蒸发密度和蒸发焓组成的训练集重新训练了一些描述OpenFF 1.0.0 （Parsley）固定电荷力场的vdW相互作用的Lennard-Jones参数，并评估了每种组合的性能。我们表明，针对混合物数据的再训练提高了力场重现混合物性质（包括溶剂化自由能）的能力，纠正了仅针对纯系统性质训练vdW相互作用时存在的一些系统误差。
Developing a sufficiently accurate classical force field representation of molecules is key to realizing the full potential of molecular simulation as a route to gaining fundamental insight into a broad spectrum of chemical and biological phenomena. This is only possible, however, if the many complex interactions between molecules of different species in the system are accurately captured by the model. Historically, the intermolecular van der Waals (vdW) interactions have primarily been trained against densities and enthalpies of vaporization of pure (single-component) systems, with occasional usage of hydration free energies. In this study, we demonstrate how including physical property data of binary mixtures can better inform these parameters, encoding more information about the underlying physics of the system in complex chemical mixtures. To demonstrate this, we re-train a select number of the Lennard-Jones parameters describing the vdW interactions of the OpenFF 1.0.0 (Parsley) fixed charge force field against training sets composed of densities and enthalpies of mixing for binary liquid mixtures as well as densities and enthalpies of vaporization of pure liquid systems, and assess the performance of each of these combinations. We show that retraining against the mixture data improves the force field’s ability to reproduce mixture properties, including solvation free energies, correcting some systematic errors that exist when training vdW interactions against properties of pure systems only.
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影响因子：
2.6
作者：
Alcalde, Rafael;Aparicio, Santiago;Leal, Jose M.
通讯作者：
Leal, Jose M.
影响因子：
2.6
作者：
Dai, Jianxing;Li, Xiaofeng;Sun, Huai
通讯作者：
Sun, Huai
影响因子：
3.5
作者：
Daoudi, Hadda;Kaci, Ahmed Ait;Tafat-Igoudjilene, Ouahiba
通讯作者：
Tafat-Igoudjilene, Ouahiba
影响因子：
3
作者：
BROOKS, BR;BRUCCOLERI, RE;KARPLUS, M
通讯作者：
KARPLUS, M
DOI：
10.1021/je034022n
发表时间：
2004-07-01
期刊：
JOURNAL OF CHEMICAL AND ENGINEERING DATA
影响因子：
--
作者：
George, J;Sastry, NV
通讯作者：
Sastry, NV