Suppr超能文献

利用微观和宏观目标实验观测值对经典三位点刚性水模型进行多目标自动优化所获经验教训。

Lessons Learned from Multiobjective Automatic Optimizations of Classical Three-Site Rigid Water Models Using Microscopic and Macroscopic Target Experimental Observables.

作者信息

Perrone Mattia, Capelli Riccardo, Empereur-Mot Charly, Hassanali Ali, Pavan Giovanni M

机构信息

Department of Applied Science and Technology, Politecnico di Torino, Corso Duca degli Abruzzi 24, Torino I-10129, Italy.

Department of Biosciences, Università degli Studi di Milano, Via Celoria 26, Milano I-20133, Italy.

出版信息

J Chem Eng Data. 2023 Dec 5;68(12):3228-3241. doi: 10.1021/acs.jced.3c00538. eCollection 2023 Dec 14.

Abstract

The development of accurate water models is of primary importance for molecular simulations. Despite their intrinsic approximations, three-site rigid water models are still ubiquitously used to simulate a variety of molecular systems. Automatic optimization approaches have been recently used to iteratively refine three-site water models to fit macroscopic (average) thermodynamic properties, providing state-of-the-art three-site models that still present some deviations from the liquid water properties. Here, we show the results obtained by automatically optimizing three-site rigid water models to fit a combination of microscopic and macroscopic experimental observables. We use , a multiobjective particle-swarm-optimization algorithm, for training the models to reproduce the experimental radial distribution functions of liquid water at various temperatures (rich in microscopic-level information on, e.g., the local orientation and interactions of the water molecules). We systematically analyze the agreement of these models with experimental observables and the effect of adding macroscopic information to the training set. Our results demonstrate how adding microscopic-rich information in the training of water models allows one to achieve state-of-the-art accuracy in an efficient way. Limitations in the approach and in the approximated description of water in these three-site models are also discussed, providing a demonstrative case useful for the optimization of approximated molecular models, in general.

摘要

精确水模型的开发对于分子模拟至关重要。尽管存在固有的近似性,但三点刚性水模型仍被广泛用于模拟各种分子系统。最近,自动优化方法已被用于迭代优化三点水模型,以拟合宏观(平均)热力学性质,从而提供了仍与液态水性质存在一些偏差的先进三点模型。在此,我们展示了通过自动优化三点刚性水模型以拟合微观和宏观实验可观测量的组合所获得的结果。我们使用一种多目标粒子群优化算法来训练模型,以重现不同温度下液态水的实验径向分布函数(富含关于水分子局部取向和相互作用等微观层面的信息)。我们系统地分析了这些模型与实验可观测量的一致性以及向训练集添加宏观信息的效果。我们的结果表明,在水模型训练中添加丰富的微观信息能够以高效的方式实现先进的精度。我们还讨论了该方法以及这些三点模型中对水的近似描述的局限性,总体上为近似分子模型的优化提供了一个具有示范作用的案例。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6ae6/10726314/01bf25f06ed0/je3c00538_0001.jpg

文献AI研究员

20分钟写一篇综述,助力文献阅读效率提升50倍。

立即体验

用中文搜PubMed

大模型驱动的PubMed中文搜索引擎

马上搜索

文档翻译

学术文献翻译模型,支持多种主流文档格式。

立即体验