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A series of carbazole/benzimidazole-based molecules, namely, o -CbzBiz, m -CbzBiz, and p -CbzBiz, were readily synthesized in three steps by integrating carbazole with benzimidazole via the ortho -, meta -, and para -positions of phenyl linked to N -phenyl carbazole. These bipolar molecules exhibited a maximum UV absorption band ranging from 310 to 327 nm and a maximum emission band ranging from 380 to 400 nm. Density functional theory calculations showed that the twist angles between the donor and acceptor moieties of these molecules were from 54.9 to 67.1°. Such a twisted structure hampered the π-electron conjugation within the molecule and resulted in high-lying LUMO levels and triplet energies, which make them suitable to be applied as host materials in OLED devices. Our results showed that a maximum external quantum efficiency (EQE) of OLED reached 21.8% when p -CbzBiz was applied as the host of a green phosphorescent emitter, i.e., Ir(ppy) 2 (acac). In addition, a maximum EQE of OLED reached 16.7% when o- CbzBiz with the host of a green TADF emitter, i.e., 4CzIPN. Moreover, these devices exhibited lower efficiency roll-off than the CBP-hosted device using the same emitters, which demonstrated the bipolar charge carrier property of carbazole/benzimidazole-based molecules.

acs omega

Carbazole/Benzimidazole-Based Bipolar Molecules as the Hosts for Phosphorescent and Thermally Activated Delayed Fluorescence Emitters for Efficient OLEDs