Demerdash Omar, Yap Eng-Hui, Head-Gordon Teresa
Department of Chemistry.
Annu Rev Phys Chem. 2014;65:149-74. doi: 10.1146/annurev-physchem-040412-110040. Epub 2013 Dec 9.
Computational modeling at the atomistic and mesoscopic levels has undergone dramatic development in the past 10 years to meet the challenge of adequately accounting for the many-body nature of intermolecular interactions. At the heart of this challenge is the ability to identify the strengths and specific limitations of pairwise-additive interactions, to improve classical models to explicitly account for many-body effects, and consequently to enhance their ability to describe a wider range of reference data and build confidence in their predictive capacity. However, the corresponding computational cost of these advanced classical models increases significantly enough that statistical convergence of condensed phase observables becomes more difficult to achieve. Here we review a hierarchy of potential energy surface models used in molecular simulations for systems with many degrees of freedom that best meet the trade-off between accuracy and computational speed in order to define a sweet spot for a given scientific problem of interest.
在过去十年中，为应对充分考虑分子间相互作用多体性质这一挑战，原子尺度和介观尺度的计算建模取得了显著进展。这一挑战的核心在于能够识别成对加和相互作用的强度和特定局限性，改进经典模型以明确考虑多体效应，从而增强其描述更广泛参考数据的能力，并增强对其预测能力的信心。然而，这些先进经典模型相应的计算成本大幅增加，以至于凝聚相可观测量的统计收敛变得更难实现。在此，我们回顾了用于具有多个自由度系统的分子模拟中的势能面模型层次结构，这些模型在准确性和计算速度之间达到了最佳平衡，以便为给定的感兴趣科学问题确定一个最佳点。
