The cooperativity between the σ-hole and π-hole interactions in the ClO···XONO2/XONO···NH3 (X?=?Cl, Br, I) complexes
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- 作者：Ting Lang ; Xiaoyan Li ; Lingpeng Meng ; Shijun Zheng ; Yanli Zeng
- 关键词：σ ; Hole interaction ; π ; Hole interaction ; Cooperativity ; Electrostatic potential
- 刊名：Structural Chemistry
- 出版年：2015
- 出版时间：February 2015
- 年：2015
- 卷：26
- 期：1
- 页码：213-221
- 全文大小：2,686 KB
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文摘
The second-order M?ller–lesset perturbation theory (MP2) calculations have been performed to investigate the cooperativity between the σ-hole and π-hole interactions in the ClO···XONO2/XONO···NH3 (X?=?Cl, Br, I) complexes. The σ-holes and π-holes have been found on the outer surfaces of XONO2/XONO: the σ-hole is outside the halogen atoms approximately along the extension of X–O bond, and the π-hole is above and below the nitrogen atom and the terminal oxygen atom. Both the σ-hole and π-hole interaction energies are consistent with the most positive electrostatic potentials (V S, max) of the σ-holes and π-holes, indicating that electrostatic interactions play an important role in the σ-hole and π-hole interactions. From a two- to a three-body interaction, the interaction energies, binding distances, and infrared vibrational frequencies prove that there is negative cooperativity between the σ-hole and π-hole interactions. In the formation of the σ-hole and π-hole interactions, the electric fields of the negative sites ClO and NH3 cause the decrease of the electronic density of the σ-hole and π-hole regions of XONO2. Due to the negative effect between the σ-hole and π-hole interactions, the decreased regions of electronic density of the σ-hole and π-hole are somewhat contracted.