| Summary: | Abstract In doped organic light‐emitting diodes (OLEDs), the host materials play an important role in emitting layers. Most studies about host materials mainly focus on their energy levels and carrier transport behaviors, while less attention is paid to their influence on the dipole orientation of dopants, which closely associate with the light out‐coupling efficiency (ηout) of the device. Herein, a linear polar host material (l‐CzTRZ) consisting of carbazole donor, triazine acceptor, and the conjugated para‐terphenyl skeleton is developed and its crystal and electronic structures, thermal and electrochemical stabilities, optical property, and carrier transport ability are investigated. l‐CzTRZ prefers ordered horizontal orientation and favors electron transport in neat film. More importantly, it can promote horizontal dipole orientation for the dopants via dipole‐dipole interaction, furnishing an excellent horizontal dipole ratio of 91.5% and thus a high ηout of 43% for the phosphorescent dopant (PO‐01‐TB). Consequently, the OLED with l‐CzTRZ host and PO‐01‐TB dopant attains state‐of‐the‐art electroluminescence efficiencies of 135.5 cd A−1, 135.7 lm W−1 and 41.3%, with a small roll‐off of 9.7% at 5000 cd m−2 luminance. The presented significant impact of the host on the dipole orientation of the dopant shall enlighten the design of host materials to improve OLED performance.
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