Polarizable Drude Model with s-Type Gaussian or Slater Charge Density for General Molecular Mechanics Force Fields,Journal of Chemical Theory and Computation

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Polarizable Drude Model with s-Type Gaussian or Slater Charge Density for General Molecular Mechanics Force Fields
Journal of Chemical Theory and Computation ( IF 5.7 ) Pub Date : 2018-10-03 00:00:00 , DOI: 10.1021/acs.jctc.8b00430
Mohammad Mehdi Ghahremanpour ₁ , Paul J. van Maaren ₁ , Carl Caleman _{2,

3} , Geoffrey R. Hutchison ₄ , David van der Spoel ₁

Affiliation

Gas-phase electric properties of molecules can be computed routinely using wave function methods or density functional theory (DFT). However, these methods remain computationally expensive for high-throughput screening of the vast chemical space of virtual compounds. Therefore, empirical force fields are a more practical choice in many cases, particularly since force field methods allow one to routinely predict the physicochemical properties in the condensed phases. This work presents Drude polarizable models, to increase the physical realism in empirical force fields, where the core particle is treated as a point charge and the Drude particle is treated either as a 1s-Gaussian or a ns-Slater (n = 1, 2, 3) charge density. Systematic parametrization to large high-quality quantum chemistry data obtained from the open access Alexandria Library (https://doi.org/10.5281/zenodo.1004711) ensures the transferability of these parameters. The dipole moments and isotropic polarizabilities of the isolated molecules predicted by the proposed Drude models are in agreement with experiment with accuracy similar to DFT calculations at the B3LYP/aug-cc-pVTZ level of theory. The results show that the inclusion of explicit polarization into the models reduces the root-mean-square deviation with respect to DFT calculations of the predicted dipole moments of 152 dimers and clusters by more than 50%. Finally, we show that the accuracy of the electrostatic interaction energy of the water dimers can be improved systematically by the introduction of polarizable smeared charges as a model for charge penetration.

中文翻译：

具有一般分子力学力场的s型高斯或斯拉特电荷密度的可极化Drude模型

分子的气相电特性可以使用波动函数法或密度泛函理论（DFT）进行常规计算。然而，这些方法对于虚拟化合物的广阔化学空间的高通量筛选在计算上仍然昂贵。因此，经验力场在许多情况下是更实际的选择，特别是因为力场方法允许人们常规地预测凝聚相的理化性质。这项工作提出了Drude可极化模型，以提高经验力场中的物理真实性，其中将核心粒子视为点电荷，将Drude粒子视为1 s-高斯或ns- Slater（n= 1，2，3）电荷密度。从开放存取亚历山大图书馆（https://doi.org/10.5281/zenodo.1004711）获得的大量高质量量子化学数据的系统参数化确保了这些参数的可传递性。由提议的Drude模型预测的分离分子的偶极矩和各向同性极化率与实验相符，其精确度与理论上B3LYP / aug-cc-pVTZ的DFT计算相似。结果表明，相对于152个二聚体和聚类的预测偶极矩的DFT计算，将显式极化包含在模型中可将均方根偏差减少50％以上。最后，

更新日期：2018-10-03

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