Dual Functionalization of Electron Transport Layer via Tailoring Molecular Structure for High-Performance Perovskite Light-Emitting Diodes

Great progress in modification and optimization of emission layer (EML) in perovskite light-emitting diodes (PeLEDs) results in a significant improvement in device efficiency. However, so far, less attention has been paid to the exploration of hole/electron injection and transporting layers to maximize the utilization of charge carriers for efficient and stable PeLEDs. At present, low electron mobility of electron transport layer (ETL) causes an unbalanced charge injection, and the defects at the ETL/perovskite interface limit the formation and utilization of generated excitons. Here, a series of compounds (BPBiTP, BPBiPN, and BPBiPA) flanked by diphenyl-1H-benzo[d]imidazole end groups have been developed as ETL materials, where the bridging units (benzene, naphthalene, anthracene) are manipulated to achieve dual functionality, namely, the high charge carrier mobility and effective passivation of perovskite surface. The coordinating end groups effectively reduce the trap state at the interface of ETL and EML due to their strong nucleophilic quality. H-aggregation of anthracene units and large transfer integral in BPBiPA lead to its superior electron mobility of 8.4 × 10–4 cm2 V–1 s–1 in the solid state, over 1 order of magnitude higher than that of the typical one (TPBi). Consequently, green PeLEDs with a maximum external quantum efficiency (EQE) of 19.7%, reduced efficiency roll-off, as well as extended operational lifetime have been achieved without any outcoupling technique. Our result demonstrated that optimization of ETL materials via improving both passivation capability and electron mobility is a powerful strategy for producing high-performance PeLEDs.