Host-guest chemistry of rotaxanes and catenanes:: application of a polarizable all-atom force field to cyclobis(paraquat-p-phenylene) complexes with disubstituted benzenes and biphenyls
Host-guest chemistry of rotaxanes and catenanes:: application of a polarizable all-atom force field to cyclobis(paraquat-p-phenylene) complexes with disubstituted benzenes and biphenyls
复制标题
DOI：
10.1039/a905160k
复制
发表时间：
1999-11-01
期刊：
影响因子：
--
通讯作者：
Jorgensen, WL
中科院分区：
文献类型：
--
作者：
Kaminski, GA;Jorgensen, WL
利用分子力学和蒙特卡罗统计力学对环双（百草枯对亚苯基）与联苯胺、联苯酚、1,4-二氨基苯和苯对苯二酚在气相和液态 CH,CN 溶液中的主客体配合物进行了建模。这些配合物是各种自组装轮烷和索烷的重要结构元素，有望在纳米级器件中得到应用。然而，它们的高度电荷性质给精确建模带来了潜在的挑战。特别是，通过使用具有或不具有非加性静电极化项的全原子力场计算缔合能，已经考虑了显式极化的需要。包含 PF6- 抗衡离子的影响也已得到解决。极化通常会增强气相相互作用，但对配合物的结构和溶液中结合的相对自由能影响不大，这与实验数据相当一致。
Modeling of host-guest complexes of cyclobis(paraquat-p-phenylene) with benezidine, biphenol, 1,4-diaminobenzene, and benzohydroquinone in the gas-phase and in liquid CH,CN solution with molecular mechanics and Monte Carlo statistical mechanics has been performed. The complexes are important structural elements for a wide variety of self-assembling rotaxanes and catenanes with prospective use in nanoscale devices. However, their highly charged nature presents potential challenges for accurate modeling. In particular, the need for explicit polarization has been considered through computation of association energies using an all-atom force field with and without non-additive electrostatic polarization terms. The effect of including PF6- counterions has also been addressed. Polarization generally strengthens the gas-phase interactions, but has modest effects on the structures of the complexes and on the relative free energies of binding in solution, which are in reasonable agreement with experimental data.