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Highly Efficient Quasi-2D Perovskite Light-Emitting Diodes Incorporating a TADF Dendrimer as an Exciton-Retrieving Additive.

Although small organics or polymer additives have been introduced to enhance film formation and radiative recombination of perovskite light-emitting diodes (PeLEDs), the exciton utilization and quantum efficiency need further optimization. Here, we introduce a thermal-activated delayed fluorescence (TADF) dendrimer as an additive to enhance the surface coverage and reduce the trap state of the grain boundary. More importantly, the TADF nature of such an additive can retrieve the exciton dissociated from perovskite or trapped by the grain boundary and then transfer the energy back to emissive perovskite through the Förster energy transfer process. Since the triplets can be reused by reverse intersystem crossing in such a TADF additive, the theoretical exciton utilization is 100%. As a result, the optimized PeLEDs cooperating with a TADF additive achieved a high current efficiency of 39.0 cd A-1 and an ultrabright luminescence of 18,000 cd m-2, which are almost 5 times higher than those of the control device without an additive. Moreover, the device stability monitored by half-lifetime at 1000 cd m-2 enhanced 2 times after introducing the TADF dendrimer as an additive. The parent dendrimer without a TADF feature was also synthesized as an additive to explore the mechanism action, which found that 54% enhancement of device efficiency can be attributed to defect passivating, while 46% was assigned to retrieved energy. This research first demonstrates that the TADF dendrimer is a promising exciton-retrieving additive for enhancing the performance of PeLEDs by passivating defect, filling up grain boundary, and retrieving leakage exciton.