论文标题
由物理正规化:图形神经网络参数性电位以描述分子间相互作用
Regularized by Physics: Graph Neural Network Parametrized Potentials for the Description of Intermolecular Interactions
论文作者
论文摘要
对于许多感兴趣的系统,使用电子结构方法对使用电子结构方法进行明确描述的模拟仍然不可行。结果,诸如力场(FF)之类的经验方法已成为模拟大型和复杂分子系统的建立工具。但是,FF的参数化很耗时,传统上主要基于实验数据,这对于许多功能组而言都是稀缺的。因此,近年来,越来越多的努力自动化了FF参数化,并朝着FF拟合量子机械参考参考证据的转变。在这里,我们提出了一种参数化分子间相互作用的替代策略,该策略利用机器学习和基于梯度的优化,同时保留基于物理学的功能形式。可以将此策略视为现有FF参数化方法的概括。在提出的方法中,图形神经网络与自动分化一起使用,以将有力动机的模型参数为潜在能量表面,从而实现了完全自动化和化学空间中的广泛适用性。结果,获得了高度精确的FF模型,该模型保留了经典FF的计算效率,可解释性和鲁棒性。为了展示所提出的方法的潜力,固定电荷模型和可极化模型都被参数化以进行分子间相互作用,并应用于包括二聚体分离曲线和凝聚相凝度系统的各种系统。
Simulations with an explicit description of intermolecular forces using electronic structure methods are still not feasible for many systems of interest. As a result, empirical methods such as force fields (FF) have become an established tool for the simulation of large and complex molecular systems. However, the parametrization of FF is time consuming and has traditionally been based largely on experimental data, which is scarce for many functional groups. Recent years have therefore seen increasing efforts to automatize FF parametrization and a move towards FF fitted against quantum-mechanical reference data. Here, we propose an alternative strategy to parametrize intermolecular interactions, which makes use of machine learning and gradient-descent based optimization while retaining a functional form founded in physics. This strategy can be viewed as generalization of existing FF parametrization methods. In the proposed approach, graph neural networks are used in conjunction with automatic differentiation to parametrize physically motivated models to potential-energy surfaces, enabling full automatization and broad applicability in chemical space. As a result, highly accurate FF models are obtained which retain the computational efficiency, interpretability and robustness of classical FF. To showcase the potential of the proposed method, both a fixed-charge model and a polarizable model are parametrized for intermolecular interactions and applied to a wide range of systems including dimer dissociation curves and condensed-phase systems.