化学平衡自由能微扰计算的视角
Perspective on Free-Energy Perturbation Calculations for Chemical Equilibria.
作者信息
Jorgensen William L, Thomas Laura L
机构信息
Department of Chemistry, Yale University, New Haven, Connecticut 06520-8107.
出版信息
J Chem Theory Comput. 2008 May 9;4(6):869-876. doi: 10.1021/ct800011m.
Abstract
An overview is provided on the computation of free energy changes in solution using perturbation theory, overlap sampling, and related approximate methods. As a specific application, extensive results are provided for free energies of hydration of substituted benzenes using the OPLS-AA force field in explicit TIP4P water. For a similar amount of computer time, the double-wide sampling and overlap sampling methods yield very similar results in the free-energy perturbation calculations. With standard protocols, the average statistical uncertainty in computed differences in free energies of hydration is 0.1 - 0.2 kcal/mol. Application of the power-series expansion in the Peierls equation was also tested. Use of the first-order term is generally reliable, while inclusion of the slowly-convergent, second-order fluctuation term causes deterioration in the results for strongly hydrogen-bonded solutes.
摘要
本文概述了使用微扰理论、重叠抽样及相关近似方法计算溶液中自由能变化的方法。作为一个具体应用，本文给出了在显式TIP4P水中使用OPLS-AA力场计算取代苯水合自由能的大量结果。在自由能微扰计算中，对于相同的计算机运行时间，双宽抽样和重叠抽样方法得到的结果非常相似。按照标准协议，计算得到的水合自由能差异的平均统计不确定度为0.1 - 0.2 kcal/mol。本文还测试了在Peierls方程中幂级数展开的应用。使用一阶项通常是可靠的，而包含收敛缓慢的二阶涨落项会导致强氢键溶质的计算结果变差。
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