Multipolar Ewald methods, 2: applications using a quantum mechanical force field.
Multipolar Ewald methods, 2: applications using a quantum mechanical force field.
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DOI：
10.1021/ct500799g
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发表时间：
2015-02-10
影响因子：
5.5
通讯作者：
York, Darrin M.
中科院分区：
文献类型：
--
作者：
Giese, Timothy J.;Panteva, Maria T.;Chen, Haoyuan;York, Darrin M.
一个完全量子力学力场（QMFF）的基础上修改的“分而治之”（mDC）的框架适用于一系列的分子模拟应用程序，使用广义粒子网格埃瓦尔德方法扩展到多极电荷密度。模拟结果为三个示例应用：液态水，对硝基苯基磷酸盐在溶液中的反应，和结晶N，N-二甲基甘氨酸。使用参数化的mDC模型的液态水的模拟进行了比较TIP 3 P和TIP 4P/Ew水模型和实验。的mDC模型被证明是上级的集群结合能和一般可比的散装性能。对-硝基苯磷酸去磷酸化的解离途径的检查表明，与DFTB 3/3 OB和DFTB 3/OPHyd半经验模型的mDC方法评估括号的实验障碍，而DFTB 2和AM 1/d-PhoT QM/MM模拟表现出障碍的缺陷，后者是相关的，部分地，对-硝基苯酯离去基团pKa的异常低估。对结晶态N，N-二甲基甘氨酸进行了模拟，并将其整体结构和原子涨落与实验和一般AMBER力场（GAFF）进行了比较。QMFF，这是没有参数化的应用程序，被证明是在更好的协议与晶体学数据比GAFF。我们的模拟突出了一些可能受益于使用新的QMFF的应用领域，他们展示了使用最近开发的mDC框架开发准确的QMFF的进展。
A fully quantum mechanical force field (QMFF) based on a modified “divide-and-conquer” (mDC) framework is applied to a series of molecular simulation applications, using a generalized Particle Mesh Ewald method extended to multipolar charge densities. Simulation results are presented for three example applications: liquid water, p-nitrophenylphosphate reactivity in solution, and crystalline N,N-dimethylglycine. Simulations of liquid water using a parametrized mDC model are compared to TIP3P and TIP4P/Ew water models and experiment. The mDC model is shown to be superior for cluster binding energies and generally comparable for bulk properties. Examination of the dissociative pathway for dephosphorylation of p-nitrophenylphosphate shows that the mDC method evaluated with the DFTB3/3OB and DFTB3/OPhyd semiempirical models bracket the experimental barrier, whereas DFTB2 and AM1/d-PhoT QM/MM simulations exhibit deficiencies in the barriers, the latter for which is related, in part, to the anomalous underestimation of the p-nitrophenylate leaving group pKa. Simulations of crystalline N,N-dimethylglycine are performed and the overall structure and atomic fluctuations are compared with the experiment and the general AMBER force field (GAFF). The QMFF, which was not parametrized for this application, was shown to be in better agreement with crystallographic data than GAFF. Our simulations highlight some of the application areas that may benefit from using new QMFFs, and they demonstrate progress toward the development of accurate QMFFs using the recently developed mDC framework.
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显式极化：用于开发下一代力场的量子机械框架。
影响因子：
18.3
作者：
Gao, Jiali;Truhlar, Donald G.;Wang, Yingjie;Mazack, Michael J. M.;Loeffler, Patrick;Provorse, Makenzie R.;Rehak, Pavel
通讯作者：
Rehak, Pavel
影响因子：
3.3
作者：
Gao, JL
通讯作者：
Gao, JL
影响因子：
5.5
作者：
Cembran, Alessandro;Bao, Peng;Wang, Yingjie;Song, Lingchun;Truhlar, Donald G.;Gao, Jiali
通讯作者：
Gao, Jiali
影响因子：
4.4
作者：
DUNWEG, B;KREMER, K
通讯作者：
KREMER, K
影响因子：
5.5
作者：
Gaus, Michael;Cui, Qiang;Elstner, Marcus
通讯作者：
Elstner, Marcus