论文标题
使用分布点电荷的可极化多极分子动力学
Polarizable Multipolar Molecular Dynamics Using Distributed Point Charges
论文作者
论文摘要
分布式点电荷模型（DCM）及其最小变体（MDCM）已与广泛用于冷凝相模拟的工具集成在一起，包括基于病毒的Barostat和用于热力学整合的慢增长算法。最小的DCM通过系统的方法进一步开发，以减少静电相互作用能量中的拟合错误，而新的基于碎片的方法为大型分子提供了相当大的MDCM拟合过程的加速，而较不偏置的电荷站点数量增加。最后，在本工作中还引入了极化（M）DCM。这些发展用于具有常用模拟条件的普通力场的凝聚相模拟。 （M）开发并应用了一系列广泛使用的水力场和氟苯（PHF）的DCM当量以及原始模型，以评估对静电期重新构成的影响。 Comparisons of the molecular electrostatic potential (MEP), electrostatic interaction energies, and bulk properties from molecular dynamics simulations for a range of models from simple TIP$n$P ($n = 3-5$) to the polarizable, multipolar iAMOEBA models for water and an existing quadrupolar model for PhF confirm that DCMs retain the accuracy of the original models, providing a homogeneous, efficient, and generic point charge用于力场开发和多层次模拟的多极静电模型的替代方案。
Distributed point charge models (DCM) and their minimal variants (MDCM) have been integrated with tools widely used for condensed-phase simulations, including a virial-based barostat and a slow-growth algorithm for thermodynamic integration. Minimal DCM is further developed with a systematic approach to reduce fitting errors in the electrostatic interaction energy and a new fragment-based approach offers considerable speedup of the MDCM fitting process for larger molecules with increased numbers of off-centered charged sites. Finally, polarizable (M)DCM is also introduced in the present work. The developments are used in condensed-phase simulations of popular force fields with commonly applied simulation conditions. (M)DCM equivalents for a range of widely used water force fields and for fluorobenzene (PhF) are developed and applied along with the original models to evaluate the impact of reformulating the electrostatic term. Comparisons of the molecular electrostatic potential (MEP), electrostatic interaction energies, and bulk properties from molecular dynamics simulations for a range of models from simple TIP$n$P ($n = 3-5$) to the polarizable, multipolar iAMOEBA models for water and an existing quadrupolar model for PhF confirm that DCMs retain the accuracy of the original models, providing a homogeneous, efficient, and generic point charge alternative to a multipolar electrostatic model for force field development and multilevel simulations.
