High‐Performance Narrowband Pure‐Red OLEDs with External Quantum Efficiencies up to 36.1% and Ultralow Efficiency Roll‐Off

High-color-purity blue and green organic light-emitting diodes (OLEDs) have been resolved thanks to the development of B/N-based polycyclic multiple resonance (MR) emitters. However, due to the derivatization limit of B/N polycyclic structures, the design of red MR emitters remains challenging. Herein, a series of novel red MR emitters is reported by para-positioning N-π-N, O-π-O, B-π-B pairs onto a benzene ring to construct an MR central core. These emitters can be facilely and modularly synthesized, allowing for easy fine-tuning of emission spectra by peripheral groups. Moreover, these red MR emitters display excellent photophysical properties such as near-unity photoluminescence quantum yield (PLQY), fast radiative decay rate (k_r ) up to 7.4 × 10⁷ s^-1 , and most importantly, narrowband emission with full-width at half-maximum (FWHM) of 32 nm. Incorporating these MR emitters, pure red OLEDs sensitized by phosphor realize state-of-the-art device performances with external quantum efficiency (EQE) exceeding 36%, ultralow efficiency roll-off (EQE remains as high as 25.1% at the brightness of 50 000 cd m^-2 ), ultrahigh brightness over 130 000 cd m^-2 , together with good device lifetime.