A unified electrostatic and cavitation model for first-principles molecular dynamics in solution.
A unified electrostatic and cavitation model for first-principles molecular dynamics in solution.
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DOI：
10.1063/1.2168456
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发表时间：
2005-10
期刊：
影响因子：
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通讯作者：
D. Scherlis;J. Fattebert;F. Gygi;M. Cococcioni;N. Marzari
中科院分区：
文献类型：
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作者：
D. Scherlis;J. Fattebert;F. Gygi;M. Cococcioni;N. Marzari
静电连续溶剂模型由[Fattebert和Gygi J. 23，662（2002）; Int. J. Quantum Chem.93，139（2003）]与基于溶质表面的自然量子力学定义的空化能的第一原理公式相结合。尽管它的简单性，通过这种方法计算出的空化贡献被发现是在显着的协议，通过更复杂的算法依赖于一个大的参数集。我们的模型允许非常有效的汽车Parrinello模拟有限或扩展系统的解决方案，并证明了一个水平的准确性一样好，建立量子化学连续溶剂方法。我们应用这种方法来研究四氰基乙烯二聚体在二氯甲烷中，提供有价值的结构和动力学的见解的二聚现象。
The electrostatic continuum solvent model developed by [Fattebert and Gygi J. Comput. Chem. 23, 662 (2002); Int. J. Quantum Chem. 93, 139 (2003)] is combined with a first-principles formulation of the cavitation energy based on a natural quantum-mechanical definition for the surface of a solute. Despite its simplicity, the cavitation contribution calculated by this approach is found to be in remarkable agreement with that obtained by more complex algorithms relying on a large set of parameters. Our model allows for very efficient Car-Parrinello simulations of finite or extended systems in solution and demonstrates a level of accuracy as good as that of established quantum-chemistry continuum solvent methods. We apply this approach to the study of tetracyanoethylene dimers in dichloromethane, providing valuable structural and dynamical insights on the dimerization phenomenon.