Development and Implementation of Atomically Anisotropic First-Principles Force Fields: A Benzene Case Study
Development and Implementation of Atomically Anisotropic First-Principles Force Fields: A Benzene Case Study
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原子各向异性第一原理力场的开发和实施：苯案例研究
DOI：
10.1021/acs.jpca.2c07244
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发表时间：
2023
期刊：
影响因子：
--
通讯作者：
Schmidt, J. R.
中科院分区：
文献类型：
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作者：
Janicki, Tesia D.;Van Vleet, Mary J.;Schmidt, J. R.
π相互作用是化学和生物化学系统中的重要基序。然而，由于其各向异性的电子密度和分子间相互作用的复杂平衡，芳香族分子代表了精确和可转移力场开发的持续挑战。从历史上看，从头算芳族化合物力场没有表现出良好的准确性，相对于散装性能或仅用于研究气相二聚体。使用苯作为一个概念的证明，在这里，我们展示了我们自己的nab initioMASTIFF力场结合了原子各向异性的分子间相互作用的描述，产生一个准确和强大的模型芳族相互作用，无论相。与现有的模型相比，MASTIFF苯力场不仅对液相性质具有准确性，而且还提供了对气相和固相的可传递性。此外，我们引入了一个计算效率高的OpenMM插件，使可定制的各向异性分子间的功能形式，并可以通用于任何MD模拟中的非球形原子功能的模型是必需的。总的来说，我们的研究结果表明，原子级各向异性的重要性，使下一代从头力场的发展。
π-interactions are an important motif in chemical and biochemical systems. However, due to their anisotropic electron densities and complex balance of intermolecular interactions, aromatic molecules represent an ongoing challenge for accurate and transferable force field development. Historically,ab initioforce fields for aromatics have not exhibited good accuracy with respect to bulk properties or have only been used to study gas-phase dimers. Using benzene as a proof of concept, herein we show how our ownab initioMASTIFF force field incorporates an atomically anisotropic description of intermolecular interactions to yield an accurate and robust model for aromatic interactions irrespective of phase. Compared to existing models, the MASTIFF benzene force field not only is accurate for liquid phase properties but also offers transferability to the gas and solid phases. Additionally, we introduce a computationally efficient OpenMM plugin which enables customizable anisotropic intermolecular functional forms and which can be generically used in any MD simulation where a model for nonspherical atomic features is required. Overall, our results demonstrate the importance of atomic-level anisotropy in enabling next-generationab initioforce field development.