Department of Chemistry, School of Physical Sciences, The University of Adelaide, Adelaide, South Australia 5005, Australia.
J Chem Phys. 2022 May 14;156(18):184118. doi: 10.1063/5.0085006.
We derive a systematic and general method for parameterizing coarse-grained molecular models consisting of anisotropic particles from fine-grained (e.g., all-atom) models for condensed-phase molecular dynamics simulations. The method, which we call anisotropic force-matching coarse-graining (AFM-CG), is based on rigorous statistical mechanical principles, enforcing consistency between the coarse-grained and fine-grained phase-space distributions to derive equations for the coarse-grained forces, torques, masses, and moments of inertia in terms of properties of a condensed-phase fine-grained system. We verify the accuracy and efficiency of the method by coarse-graining liquid-state systems of two different anisotropic organic molecules, benzene and perylene, and show that the parameterized coarse-grained models more accurately describe properties of these systems than previous anisotropic coarse-grained models parameterized using other methods that do not account for finite-temperature and many-body effects on the condensed-phase coarse-grained interactions. The AFM-CG method will be useful for developing accurate and efficient dynamical simulation models of condensed-phase systems of molecules consisting of large, rigid, anisotropic fragments, such as liquid crystals, organic semiconductors, and nucleic acids.
我们从凝聚相分子动力学模拟的细粒度(例如全原子)模型中推导出一种系统而通用的方法,用于参数化由各向异性粒子组成的粗粒度分子模型。该方法称为各向异性力匹配粗粒化(AFM-CG),它基于严格的统计力学原理,在粗粒化和细粒化相空间分布之间保持一致性,从而推导出粗粒化力、扭矩、质量和转动惯量的方程,这些方程涉及凝聚相细粒系统的性质。我们通过对两种不同各向异性有机分子苯和并五苯的液体系统进行粗粒化来验证该方法的准确性和效率,并表明参数化的粗粒化模型比以前使用其他方法参数化的各向异性粗粒化模型更准确地描述了这些系统的性质,这些方法没有考虑到凝聚相粗粒化相互作用的有限温度和多体效应。AFM-CG 方法将有助于开发由大的、刚性的、各向异性片段组成的凝聚相分子系统的准确和高效动力学模拟模型,例如液晶、有机半导体和核酸。