The degradation mechanism of multi-resonance thermally activated delayed fluorescence materials

被引：1
作者：
Jhun, Byung Hak [1 ]
Park, Yerin [2 ,3 ]
Kim, Hwang Suk [4 ]
Baek, Ji Hye [1 ]
Kim, Joonghyuk [4 ]
Lee, Eunji [2 ,3 ]
Moon, Hyejin [2 ,3 ]
Oh, Changjin [2 ,3 ]
Jung, Yongsik [4 ]
Choi, Seunghee [5 ]
Baik, Mu-Hyun [2 ,3 ]
You, Youngmin [1 ]
机构：
[1] Yonsei Univ, Dept Chem & Biomol Engn, Seoul 03722, South Korea
[2] Korea Adv Inst Sci & Technol KAIST, Dept Chem, Daejeon 34141, South Korea
[3] Inst Basic Sci IBS, Ctr Catalyt Hydrocarbon Functionalizat, Daejeon 34141, South Korea
[4] Samsung Elect Co Ltd, Samsung Adv Inst Technol, Suwon 16678, Gyeonggi Do, South Korea
[5] Ewha Womans Univ, Div Chem Engn & Mat Sci, Seoul 03760, South Korea
来源：
NATURE COMMUNICATIONS | 2025年 / 16卷 / 01期
基金：
新加坡国家研究基金会;
关键词：
LIGHT-EMITTING-DIODES; SMALL-MOLECULE; ORGANIC ELECTROPHOSPHORESCENCE; BASIS-SETS; EFFICIENT; EMITTERS; CARBAZOLE; COMPLEXES; EMISSION; LIFETIME;
D O I：
10.1038/s41467-024-55620-0
中图分类号：
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号：
07 ; 0710 ; 09 ;
摘要：
1,4-Azaborine-based arenes are promising electroluminescent emitters with thermally activated delayed fluorescence (TADF), offering narrow emission spectra and high quantum yields due to a multi-resonance (MR) effect. However, their practical application is constrained by their limited operational stability. This study investigates the degradation mechanism of MR-TADF molecules. Electroluminescent devices incorporating these compounds display varied operational lifetimes, uncorrelated with excitonic stability or external quantum efficiency roll-off. Bulk electrolysis reveals significant instability in the radical cationic forms of MR-TADF compounds, with device lifetime linked to the Faradaic yield of oxidation. Comprehensive chemical analyses corroborate that the degradation byproducts originated from intramolecular cyclization of radical cation, followed by hydrogen atom transfer. The mechanism is further supported by enhanced stability observed in a deuterated MR-TADF emitter, attributed to a secondary kinetic isotope effect. These findings provide insights into the stabilizing effects of deuteration and mechanism-driven strategies for designing MR-TADF compounds with improved operational longevity.
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页数：14
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