Abstract
Concurrently achieving high efficiency, narrowband emission, and low efficiency roll-off remains a challenging task for realizing stable blue organic light-emitting diodes (OLEDs) with high color purity. To tackle this issue, herein, two isomeric pairs of B,N-doped multi-resonance thermally activated delayed fluorescence (MR-TADF) emitters, namely, 2,3-Tp-BuDABNA-R and 3,4-Tp-BuDABNA-R (R=H, 3,5-Xyl), featuring triptycene (Tp) moieties fused into the 2,3- and 3,4-positions of the B,N core, respectively, are presented. Both isomeric forms exhibit blue emissions with near-unity photoluminescence (PL) quantum yields in their doped host films. Notably, the 3,4-Tp-fused emitter shows 6-fold faster reverse intersystem crossing (RISC) compared to the 2,3-Tp-fused emitter, albeit with PL spectral broadening. Along with a smaller activation energy of RISC, the stronger spin–orbit coupling between the singlet (S1) and triplet (T2) excited states of the 3,4-Tp-fused emitter is suggested to facilitate the RISC process. Furthermore, a high-frequency vibration in the Tp-fused benzene ring, accompanied by a large reorganization energy, is found to mainly contribute to the spectral broadening of the 3,4-Tp-fused emitter. Blue TADF-OLEDs based on each isomeric emitter similarly achieve a high maximum external quantum efficiency of ∼ 26%. Remarkably, the devices with the 3,4-isomer exhibit significantly reduced efficiency roll-offs compared to the 2,3-isomer, demonstrating that isomer engineering of MR emitters can have a distinct impact on controlling device performance.
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