Charge Scaling Manifesto: A Way of Reconciling the Inherently Macroscopic and Microscopic Natures of Molecular Simulations
Charge Scaling Manifesto: A Way of Reconciling the Inherently Macroscopic and Microscopic Natures of Molecular Simulations
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DOI：
10.1021/acs.jpclett.9b02652
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发表时间：
2019-12-05
影响因子：
5.7
通讯作者：
Jungwirth, Pavel
中科院分区：
文献类型：
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作者：
Kirby, Brian J.;Jungwirth, Pavel
在生物相关的水溶液中，如涉及盐离子、蛋白质、核酸或磷脂膜的水溶液中，电子极化效应在带电物种的相互作用中起着重要的作用。无论是从力场参数化的角度来看，还是从模拟的实际性能来看，在分子模拟中显式包含电子极化都是乏味的。因此，绝大多数生物分子模拟是使用不可极化力场进行的，这可能会导致离子配对被严重高估等伪影，特别是当涉及多价离子时。在这里，我们表明，这些问题中的许多可以通过电荷重新标度以平均场的方式包括电子极化来补救，而不需要额外的计算成本。我们还奠定了这种方法的坚实的物理基础，并从这个角度协调了不可极化力场的微观和宏观性质。
Electronic polarization effects play an important role in the interactions of charged species in biologically relevant aqueous solutions, such as those involving salt ions, proteins, nucleic acids, or phospholipid membranes. Explicit inclusion of electronic polarization in molecular modeling is tedious both from the point of view of force field parametrization and actual performance of the simulations. Therefore, the vast majority of biomolecular simulations is performed using nonpolarizable force fields, which can lead to artifacts such as dramatically overestimated ion pairing, particularly when polyvalent ions are involved. Here, we show that many of these issues can be remedied without extra computational costs by including electronic polarization in a mean field way via charge rescaling. We also lay the solid physical foundations of this approach and reconcile from this perspective the microscopic versus macroscopic natures of nonpolarizable force fields.