Ye Benjamin Bobin, Chen Shensheng, Wang Zhen-Gang
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, United States.
J Chem Theory Comput. 2024 Aug 13;20(15):6870-6880. doi: 10.1021/acs.jctc.4c00603. Epub 2024 Jul 16.
In recent years, molecular dynamics (MD) simulations have emerged as an essential tool for understanding the structure, dynamics, and phase behavior of charged soft matter systems. To explore phenomena across greater length and time scales in MD simulations, molecules are often coarse-grained for better computational performance. However, commonly used force fields represent particles as hard-core interaction centers with point charges, which often overemphasizes the packing effect and short-range electrostatics, especially in systems with bulky deformable organic molecules and systems with strong coarse-graining. This underscores the need for an efficient soft-core model to physically capture the effective interactions between coarse-grained particles. To this end, we implement a soft-core model uniting the Gaussian core model with smeared electrostatic interactions that is phenomenologically equivalent to recent theoretical models. We first parametrize it generically using water as the model solvent. Then, we benchmark its performance in the OpenMM toolkit for different boundary conditions to highlight a computational speedup of up to 34 × compared to commonly used force fields and existing implementations. Finally, we demonstrate its utility by investigating how boundary polarizability affects the adsorption behavior of a polyelectrolyte solution on perfectly conducting and nonmetal boundaries.
近年来,分子动力学(MD)模拟已成为理解带电软物质系统的结构、动力学和相行为的重要工具。为了在MD模拟中探索更大长度和时间尺度上的现象,分子通常会进行粗粒化处理以获得更好的计算性能。然而,常用的力场将粒子表示为带有点电荷的硬核相互作用中心,这往往过度强调了堆积效应和短程静电作用,特别是在含有大量可变形有机分子的系统以及具有强粗粒化的系统中。这凸显了需要一个有效的软核模型来物理地捕捉粗粒化粒子之间的有效相互作用。为此,我们实现了一个将高斯核模型与涂抹静电相互作用相结合的软核模型,该模型在现象学上等同于最近的理论模型。我们首先以水作为模型溶剂对其进行通用参数化。然后,我们在OpenMM工具包中针对不同边界条件对其性能进行基准测试,以突出与常用力场和现有实现相比高达34倍的计算加速。最后,我们通过研究边界极化率如何影响聚电解质溶液在理想导电和非金属边界上的吸附行为来证明其效用。