期刊
NATURE MATERIALS
卷 18, 期 9, 页码 977-+出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41563-019-0433-1
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资金
- National Natural Science Foundation of China [91833304, 51673080, 11804156]
- National Key R&D Programme of China [2016YFB0401001]
- National Key Basic Research and Development Programme of China (973 programme) [2015CB655003]
- Nanjing Tech Start-up Grant [38274017104]
- Georgia Institute of Technology, Georgia Research Alliance
- Vasser-Woolley Foundation
- EPSRC [EP/M01083X/1, EP/M005143/1]
- China Scholarship Council
- Cambridge Trust
- Royal Society [UF130278]
- Talents Cultivation Programme (Jilin University, China)
- programme 'JLUSTIRT' [2019TD-33]
- Kyulux
- EPSRC [EP/M01083X/1, EP/M005143/1] Funding Source: UKRI
With their unusual electronic structures, organic radical molecules display luminescence properties potentially relevant to lighting applications; yet, their luminescence quantum yield and stability lag behind those of other organic emitters. Here, we designed donor-acceptor neutral radicals based on an electron-poor perchlorotriphenylmethyl or tris(2,4,6-trichlorophenyl) methyl radical moiety combined with different electron-rich groups. Experimental and quantum-chemical studies demonstrate that the molecules do not follow the Aufbau principle: the singly occupied molecular orbital is found to lie below the highest (doubly) occupied molecular orbital. These donor-acceptor radicals have a strong emission yield (up to 54%) and high photostability, with estimated half-lives reaching up to several months under pulsed ultraviolet laser irradiation. Organic light-emitting diodes based on such a radical emitter show deep-red/near-infrared emission with a maximal external quantum efficiency of 5.3%. Our results provide a simple molecular-design strategy for stable, highly luminescent radicals with non-Aufbau electronic structures.
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