Unveiling the Role of Langevin and Trap-Assisted Recombination in Long Lifespan OLEDs Employing Thermally Activated Delayed Fluorophores

Recent research studies on noble-metal-free thermally activated delayed fluorescent (TADF) materials have boosted the efficiencies of organic light-emitting diodes (OLEDs) to unity. However, the short lifespan still hinders their further practical application. Carrier recombination pathways have been reported to have a significant influence on the efficiencies of TADF devices, though their effects on device lifetimes remain rarely studied. Here, we have designed and synthesized five pyrimidine or pyrazine/carbazole isomers as hosts for TADF OLEDs to explore the inherent role of Langevin recombination (LR) and trap-assisted recombination (TAR) in device lifetimes. It is revealed that for LR dominant devices, lifetimes would increase by reducing the host triplet energy levels, whereas for TAR dominant devices, lifetimes are insensitive to the host triplet excitons as recombination mainly takes place on dopants. Still, LR dominant devices are favored as they offer more room for optimization. We further apply this concept in designing a stable LR dominant blue TADF device, achieving a long LT50 (lifespan up to 50% of the initial luminance) of 269 h and high external quantum efficiency of 17.9% at 1000 cd m^-2 simultaneously.