Kim Dongwook, Lee Eun Cheol, Kim Kwang S, Tarakeshwar P
Center for Superfunctional Materials, Department of Chemistry, Pohang University of Science and Technology, San 31, Hyojadong, Pohang 790-784, Korea.
J Phys Chem A. 2007 Aug 16;111(32):7980-6. doi: 10.1021/jp073337x. Epub 2007 Jul 26.
Cation-pi and the corresponding anion-pi interactions have in general been investigated as binary complexes despite their association with counterions. However, a recent study of the ammonia channel highlights the important but overlooked role of anions in cation-pi interactions. In an effort to examine the structural and energetic consequences of the presence of counterions, we have carried out detailed ab initio calculations on some model cation-pi-anion ternary complexes and evaluated the nonpair potential terms, three-body contributions, and attractive and repulsive energy components of the interaction energy. The presence of the anion in the vicinity of the pi system leads to a large redistribution of electron density and hence leads to an inductive stabilization. The resulting electronic and geometrical changes have important consequences in both chemical and biological systems. Compared to cation-pi-anion ternary complexes, the magnitude of the cation-pi interaction in pi-cation-anion ternary complexes is markedly lower because of charge transfer from the anion to the cation.
尽管阳离子-π相互作用及相应的阴离子-π相互作用与抗衡离子有关联,但通常都是作为二元复合物来研究的。然而,最近一项关于氨通道的研究突出了阴离子在阳离子-π相互作用中重要却被忽视的作用。为了研究抗衡离子存在时的结构和能量后果,我们对一些模型阳离子-π-阴离子三元复合物进行了详细的从头计算,并评估了非成对势项、三体贡献以及相互作用能的吸引和排斥能量成分。π体系附近存在阴离子会导致电子密度的大量重新分布,从而导致诱导稳定化。由此产生的电子和几何变化在化学和生物系统中都有重要影响。与阳离子-π-阴离子三元复合物相比,由于电荷从阴离子转移到阳离子,π-阳离子-阴离子三元复合物中阳离子-π相互作用的强度明显更低。