Modeling water using multipole response tensors fitted to the monomer geometry.

IF 3.1 2区 化学 Q3 CHEMISTRY, PHYSICAL
Jonatan Öström, Lars G M Pettersson
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引用次数: 0

Abstract

The water molecule's electronic Cartesian multipole moment and polarizability tensors have been fitted with Gaussian process regression to the internal coordinates and are used to evaluate accurate electrostatic, induction, and dispersion energy components between flexible molecules. The model yields a handful of damping and scaling parameters that were adjusted for the energy components to agree with 2-body symmetry-adapted perturbation theory decomposition and then fine-tuned in order for the total energy to agree with CCSD(T) for small clusters. We present a simple algorithm for rotating symmetric Cartesian tensors and employ a dispersion potential based on multipole polarizabilities. At short range, the 2- and 3-body potential energy was corrected to CCSD(T) accuracy using Gaussian approximation potentials. The radial distribution function and self-diffusion coefficient obtained with molecular dynamics simulations agree well with experiments.

用适合单体几何的多极响应张量模拟水。
利用高斯过程回归将水分子的电子笛卡尔多极矩和极化张量拟合到内部坐标,并用于精确计算柔性分子之间的静电、感应和色散能量分量。该模型产生了一些阻尼和缩放参数,这些参数经过调整,使能量成分符合二体对称性摄动理论分解,然后进行微调,使总能量符合小簇的CCSD(T)。我们提出了一个旋转对称笛卡尔张量的简单算法,并采用了基于多极极化率的色散势。在近距离内,利用高斯近似势能将二体和三体势能修正为CCSD(T)精度。分子动力学模拟得到的径向分布函数和自扩散系数与实验结果吻合较好。
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来源期刊
Journal of Chemical Physics
Journal of Chemical Physics 物理-物理:原子、分子和化学物理
CiteScore
7.40
自引率
15.90%
发文量
1615
审稿时长
2 months
期刊介绍: The Journal of Chemical Physics publishes quantitative and rigorous science of long-lasting value in methods and applications of chemical physics. The Journal also publishes brief Communications of significant new findings, Perspectives on the latest advances in the field, and Special Topic issues. The Journal focuses on innovative research in experimental and theoretical areas of chemical physics, including spectroscopy, dynamics, kinetics, statistical mechanics, and quantum mechanics. In addition, topical areas such as polymers, soft matter, materials, surfaces/interfaces, and systems of biological relevance are of increasing importance. Topical coverage includes: Theoretical Methods and Algorithms Advanced Experimental Techniques Atoms, Molecules, and Clusters Liquids, Glasses, and Crystals Surfaces, Interfaces, and Materials Polymers and Soft Matter Biological Molecules and Networks.
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