Efficient and stable green organic light-emitting diode utilizing an asymmetric butterfly-shaped chromophore with enhanced reverse intersystem crossing and suppressed exciton annihilation

Chemical Engineering Journal(2023)

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摘要
Intermolecular electron-exchange interactions involving long-lived triplet state excitons dominate the quenching process of the films. In this work, a butterfly-shaped thermally activated delayed fluorescence (TADF) emitter 10,10,-(5-((3,5-di(9H-carbazol-9-yl)phenyl)sulfonyl)-1,3-phenylene)bis(9,9-dimethyl-9,10-dihydroacridine) (BCZ-DPS-BAD) with diphenylsulfone skeleton is constructed by modulating the rigid steric hindrance on the electron donor fragment to weaken intermolecular electron-exchange interactions. Analysis of the ground and excited state properties, crystal structure, steady-state and transient photophysical characteristics reveals that BCZ-DPS-BAD exhibits loose intermolecular arrangements with no direct facing close packing and weak 7c-7c interactions of 4.18 angstrom and 4.67 angstrom. The triplet state excitons can swiftly return to the single exciton state in accordance with a short delayed fluorescence lifetime (2.3 mu s) and a quick reverse intersystem crossing rate (1.85 x 106 s(-1)), obstructing the way for the triplet state to lose energy. A remarkable maximum external quantum efficiency of 21.8 %, maximum current efficiency of 56.8 cd/A and exciton utilization rate of 82 % is achieved for BCZ-DPS-BAD-based green non-doped OLED, concomitant with Commission Internationale d'Eclairage (CIE) coordinates of (0.30, 0.50). Notably, BCZ-DPS-BAD behaves stable non-doped OLED performance with efficiency roll-off of 4 % at 1000 cd m(-2).
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关键词
Thermally activated delayed fluorescence,Steric hindrance,Weak intermolecular electron-exchange interactions,Fast reverse intersystem crossing process
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