Capturing Many-Body Interactions with Classical Dipole Induction Models.
Capturing Many-Body Interactions with Classical Dipole Induction Models.
复制标题
使用经典偶极感应模型捕获多体相互作用
DOI：
10.1021/acs.jctc.7b00225
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发表时间：
2017-06-13
影响因子：
5.5
通讯作者：
Ren P
中科院分区：
文献类型：
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作者：
Liu C;Qi R;Wang Q;Piquemal JP;Ren P
非加性多体相互作用对凝聚相体系的结构和热力学性质具有重要意义。在这项工作中，我们使用Møller - plesset二阶微扰理论（MP2）研究了大量常见有机/生化分子簇的多体相互作用能，这些分子簇由18种化学物质组成，涵盖9种常见有机元素。理论物理。[j].中华科学杂志，1994,6(6):618。我们评估了基于电穴的偶极感应模型捕捉多体相互作用能的能力。比较了AMOEBA力场使用的原始模型和参数、将阻尼参数重新优化为MP2数据的变型模型和修改了适用于永久电场的阻尼函数形式的变型模型。总的来说，我们发现简单的经典原子偶极子模型能够在各种分子间构型的各种有机分子中捕获3体和4体相互作用能。通过改进Thole模型，可以进一步提高与MP2结果的一致性。这些模型还在含有金属/卤素离子的系统上进行了测试，以检验其准确性和可转移性。这一工作表明，施加于永久静电场的阻尼函数的形式强烈地影响了短分子间分离时极化能的距离依赖。
The nonadditive many-body interactions are significant for structural and thermodynamic properties of condensed phase systems. In this work we examined the many-body interaction energy of a large number of common organic/biochemical molecular clusters, which consist of 18 chemical species and cover nine common organic elements, using the Møller–Plesset perturbation theory to the second order (MP2) [Møller et al. Phys. Rev.1934, 46, 618.]. We evaluated the capability of Thole-based dipole induction models to capture the many-body interaction energy. Three models were compared: the original model and parameters used by the AMOEBA force field, a variation of this original model where the damping parameters have been reoptimized to MP2 data, and a third model where the damping function form applied to the permanent electric field is modified. Overall, we find the simple classical atomic dipole models are able to capture the 3- and 4-body interaction energy across a wide variety of organic molecules in various intermolecular configurations. With modified Thole models, it is possible to further improve the agreement with MP2 results. These models were also tested on systems containing metal/halogen ions to examine the accuracy and transferability. This work suggests that the form of damping function applied to the permanent electrostatic field strongly affects the distance dependence of polarization energy at short intermolecular separations.