First-Principles Parametrization of Polarizable Coarse-Grained Force Fields for Ionic Liquids.
First-Principles Parametrization of Polarizable Coarse-Grained Force Fields for Ionic Liquids.
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DOI：
10.1021/acs.jctc.7b00903
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发表时间：
2018-01
影响因子：
5.5
通讯作者：
F. Uhlig;Johannes Zeman;Jens Smiatek;Christian Holm-
中科院分区：
文献类型：
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作者：
F. Uhlig;Johannes Zeman;Jens Smiatek;Christian Holm-
我们提出了一种用于分子液体模拟的显式偶极极化力场的从头算参数化方案。该方案原则上允许任意粗粒度表示。力场中的所有参数都是根据第一原理，基于简单的物理论证得出的。只有一个拟合参数进入参数化，即粒子大小的全局比例因子，该参数会进行调整以重现实验质量密度。作为重要的例子，首次导出了具有不同烷基链长的1-烷基-3-甲基咪唑阳离子(烷基=乙基、丁基、己基)以及六氟磷酸根阴离子和四氟硼酸根阴离子的可极化粗粒力场。我们的发现与实验结果和进一步的原子模拟结果是一致的。因此，在极化率发挥重要作用的地方，例如对储能设备的模拟，可以忠实地使用力场。
We present an ab initio parametrization scheme for explicitly dipole-polarizable force fields for the simulation of molecular liquids. The scheme allows for, in principle, arbitrarily coarse-grained representations. All parameters in the force field are derived from first-principles, based on simple physical arguments. Only one fit parameter enters the parametrization, a global scaling factor for the size of the particles, which is adjusted to reproduce the experimental mass density. As important examples and for the first time, polarizable coarse-grained force fields are derived for 1-alkyl-3-methylimidazolium cations with varying alkyl-chain lengths (alkyl = ethyl, butyl, hexyl) and hexafluorophosphate and tetrafluoroborate anions. Our findings are in good agreement with experimental results and results of further atomistic simulations. Hence, the force fields can be faithfully used where polarizability is expected to play a significant role, such as simulations of energy storage devices.