J-Aggregation Enhances the Electroluminescence Performance of a Sky-Blue Thermally Activated Delayed-Fluorescence Emitter in Nondoped Organic Light-Emitting Diodes.

A pivotal thermally activated delayed-fluorescence (TADF) emitter, DspiroAc-TRZ, was developed, and it exhibits greatly enhanced electroluminescence performance in nondoped organic light-emitting diodes (OLEDs) owing to the concurrent manipulation of aggregation behavior and monomolecular structure. The delicate non-planar packing pattern in the DspiroAc-TRZ crystal can not only lead to highly efficient solid-state luminescence but also form a loose intermolecular packing pattern, greatly decreasing the HOMO or LUMO overlaps in dimers and shortening the triplet exciton diffusion length. In addition, the rigid donor and acceptor moieties in DspiroAc-TRZ can rigidify the molecular backbone, resulting in a tiny geometric vibrational relaxation in the excited state. Impressively, high photoluminescent quantum yields of 78.5 and 83.7% were achieved for the DspiroAc-TRZ single crystal and nondoped film. A high external quantum efficiency (EQE) of 25.7% was achieved in a nondoped sky-blue TADF OLED, which is higher than any reported EQE value of nondoped sky-blue TADF OLEDs so far.