Aachener Verfahrenstechnik: Molecular Sciences and Transformations, Faculty of Mechanical Engineering, RWTH Aachen University, Schinkelstrasse 2, 52062 Aachen, Germany.
J Phys Chem A. 2012 May 10;116(18):4657-66. doi: 10.1021/jp3021886. Epub 2012 Apr 26.
We present a definition of intermolecular surface contact by applying weighted Voronoi tessellations to configurations of various organic liquids and water obtained from molecular dynamics simulations. This definition of surface contact is used to link the COSMO-RS model and molecular dynamics simulations. We demonstrate that additively weighted tessellation is the superior tessellation type to define intermolecular surface contact. Furthermore, we fit a set of weights for the elements C, H, O, N, F, and S for this tessellation type to obtain optimal agreement between the models. We use these radii to successfully predict contact statistics for compounds that were excluded from the fit and mixtures. The observed agreement between contact statistics from COSMO-RS and molecular dynamics simulations confirms the capability of the presented method to describe intermolecular contact. Furthermore, we observe that increasing polarity of the surfaces of the examined molecules leads to weaker agreement in the contact statistics. This is especially pronounced for pure water.
我们通过对各种有机液体和水的分子动力学模拟配置应用加权 Voronoi 镶嵌来提出分子间表面接触的定义。 该表面接触定义用于将 COSMO-RS 模型和分子动力学模拟联系起来。 我们证明，加和加权镶嵌是定义分子间表面接触的优越镶嵌类型。 此外，我们为该镶嵌类型的元素 C、H、O、N、F 和 S 拟合了一组权重，以获得模型之间的最佳一致性。 我们使用这些半径成功地预测了从拟合和混合物中排除的化合物的接触统计数据。 从 COSMO-RS 和分子动力学模拟得出的接触统计数据之间的一致性证实了所提出的方法在描述分子间接触方面的能力。 此外，我们观察到，被检查分子的表面极性增加会导致接触统计数据的一致性降低。 对于纯水来说，这种情况尤其明显。
