Ultra-fast triplet-triplet-annihilation-mediated high-lying reverse intersystem crossing triggered by participation of nπ*-featured excited states

Yanju Luo, Kai Zhang, Zhenming Ding, Ping Chen (), Xiaomei Peng, Yihuan Zhao, Kuan Chen, Chuan Li, Xujun Zheng, Yan Huang, Xuemei Pu, Yu Liu (), Shi-Jian Su (), Xiandeng Hou and Zhiyun Lu ()
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Yanju Luo: Sichuan University
Kai Zhang: Changzhou University
Zhenming Ding: Changzhou University
Ping Chen: Southwest University
Xiaomei Peng: South China University of Technology
Yihuan Zhao: Sichuan University
Kuan Chen: Sichuan University
Chuan Li: Sichuan University
Xujun Zheng: Sichuan University
Yan Huang: Sichuan University
Xuemei Pu: Sichuan University
Yu Liu: Changzhou University
Shi-Jian Su: South China University of Technology
Xiandeng Hou: Sichuan University
Zhiyun Lu: Sichuan University

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract The harvesting of ‘hot’ triplet excitons through high-lying reverse intersystem crossing mechanism has emerged as a hot research issue in the field of organic light-emitting diodes. However, if high-lying reverse intersystem crossing materials lack the capability to convert ‘cold’ T1 excitons into singlet ones, the actual maximum exciton utilization efficiency would generally deviate from 100%. Herein, through comparative studies on two naphthalimide-based compounds CzNI and TPANI, we revealed that the ‘cold’ T1 excitons in high-lying reverse intersystem crossing materials can be utilized effectively through the triplet-triplet annihilation-mediated high-lying reverse intersystem crossing process if they possess certain triplet-triplet upconversion capability. Especially, quite effective triplet-triplet annihilation-mediated high-lying reverse intersystem crossing can be triggered by endowing the high-lying reverse intersystem crossing process with a 3ππ*→1nπ* character. By taking advantage of the permanent orthogonal orbital transition effect of 3ππ*→1nπ*, spin–orbit coupling matrix elements of ca. 10 cm−1 can be acquired, and hence ultra-fast mediated high-lying reverse intersystem crossing process with rate constant over 109 s−1 can be realized.

Date: 2022
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DOI: 10.1038/s41467-022-34573-2

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