文献类型： 外文期刊
作者： Liu, Guanghua 1 ; Gao, Lei 1 ; Han, Yi 2 ; Xiao, Yao 1 ; Du, Bochao 1 ; Gong, Jianye 1 ; Hu, Jinlian 4 ; Zhang, Fujin 5 ; Meng, He 1 ; Li, Xiang 6 ; Shi, Xueliang 8 ; Sun, Zhe 4 ; Wang, Jianguo 1 ; Dai, Gaole 3 ; Chi, Chunyan 2 ; Wang, Qing 1 ;
作者机构： 1.Inner Mongolia Univ, Sch Chem & Chem Engn, 235 West Univ St, Hohhot 010021, Peoples R China
2.Natl Univ Singapore, Dept Chem, 3 Sci Dr 3, Singapore 117543, Singapore
3.Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Minist Educ, Key Lab Organosilicon Chem & Mat Technol, 2318 Yuhangtang Rd, Hangzhou 311121, Zhejiang, Peoples R China
4.Tianjin Univ, Inst Mol Plus, Dept Chem, Tianjin Key Lab Mol Optoelect Sci, 92 Weijin Rd, Tianjin 300072, Peoples R China
5.Inner Mongolia Acad Agr & Anim Husb Sci, Inst Environm Resources & Analyt Tech, Zhao Jun Rd, Hohhot 010031, Peoples R China
6.Nanjing Agr Univ, Coll Sci, Lab Pesticide Sci, Nanjing 210095, Peoples R China
7.Nanjing Agr Univ, Coll Sci, Dept Chem, Nanjing 210095, Peoples R China
8.East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 200062, Peoples R China
关键词： Cationic Radical; Mixed Valence Complex; Nitrogen Doping; Quadrupole; Symmetry Broken Charge Separation
期刊名称：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION （ 影响因子：16.6； 五年影响因子：15.3 ）
ISSN： 1433-7851
年卷期： 2023 年
页码：
收录情况： SCI
摘要： A quadrupolar compound Pyr-BA with two pyrrole-type nitrogen atoms doped externally was prepared in this work. In high contrast with other pi ionic radicals, its cationic radical Pyr-BA center dot(+) undergoes unusual symmetry-broken charge separation (SB-CS), generating the mixed valence complex of Pyr-BA(+1-q)center dot center dot center dot Pyr-BA(+1+q), where q is the degree of charge transfer. Variable-temperature (VT) single-crystal analysis, absorption and EPR experiments all confirmed that aggregation and lower temperature would help to facilitate this SB-CS process. Gibbs energy calculations and gauge-including magnetically induced current simulation both validate that, for Pyr-BA center dot(+), SB-CS behavior is more favorable than the conventional dimerization mode. To the best of our knowledge, this is the first study that shows solid single-crystal evidence for spontaneous SB-CS between identical ionic radicals. Such a unique phenomenon is of great significance both in terms of fundamental aspects and uncharted material science.
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