Approximating quantum many-body intermolecular interactions in molecular clusters using classical polarizable force fields
Approximating quantum many-body intermolecular interactions in molecular clusters using classical polarizable force fields
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DOI：
10.1063/1.3121323
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发表时间：
2009-04-28
影响因子：
4.4
通讯作者：
Beran, Gregory J. O.
中科院分区：
文献类型：
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作者：
Beran, Gregory J. O.
多体分子间相互作用展开为分子团簇和凝聚相系统的有效量子力学处理提供了一条有前途的途径，但计算昂贵的三体和更高的条款往往是不平凡的。当涉及极性分子时，这些多体项通常由静电感应效应主导，这可以相对容易地近似。我们证明了一个准确的和廉价的混合量子/经典模型，其中一个和两个身体的相互作用计算量子力学，而多体感应效应近似与一个简单的经典极化力场。虽然典型的混合量子/经典模型将系统在空间上划分为不同的量子和经典区域，但这里展示的模型基于多体相互作用序列中的顺序进行划分。这使得整个系统的空间均匀的治疗，这可以证明有利于研究范围广泛的凝聚相分子系统。(C)2009年美国物理学会。[DOI：10.1063/1.3121323]
Many-body intermolecular interaction expansions provide a promising avenue for the efficient quantum mechanical treatment of molecular clusters and condensed-phase systems, but the computationally expensive three-body and higher terms are often nontrivial. When polar molecules are involved, these many-body terms are typically dominated by electrostatic induction effects, which can be approximated relatively easily. We demonstrate an accurate and inexpensive hybrid quantum/classical model in which one-and two-body interactions are computed quantum mechanically, while the many-body induction effects are approximated with a simple classical polarizable force field. Whereas typical hybrid quantum/classical models partition a system spatially into distinct quantum and classical regions, the model demonstrated here partitions based on the order in the many-body interaction series. This enables a spatially homogeneous treatment of the entire system, which could prove advantageous in studying a wide range of condensed-phase molecular systems. (C) 2009 American Institute of Physics. [DOI: 10.1063/1.3121323]