| Summary: | Abstract To achieve highly‐efficient organic light‐emitting diodes (OLEDs), great efforts have been devoted into constructing thermally activated delayed fluorescence (TADF) with high horizontal dipole ratios (Θ//). Here, we proposed a design strategy by integrating a rigid electron‐accepting oxygen‐bridged boron core with triple electron‐donating groups, which exhibited a “shamrock‐shape”, namely BO‐3DMAC and BO‐3DPAC. Benefiting from the rigid and large‐planar skeletons brought by shamrock‐shaped design, BO‐3DMAC and BO‐3DPAC exhibit high Θ// of 84%/70% and 93%/94% in neat/doped films, respectively, and finally furnish excellent external quantum efficiencies (EQEs) of up to 28.3% and 38.7% in 20 wt% doped OLEDs with sky‐blue emission, as well as adequate EQEs of up to 21.0% and 16.7% in nondoped OLEDs. This work unveils a promising strategy to establish high‐Θ// TADF emitters by constructing large‐planar molecular structures using shamrock‐shaped design.
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