Controlling Interfacial Amidation Reaction Rate to Regulate Crystal Growth toward High-Performance FAPbBr3-Based Inverted Light-Emitting Diodes

Controlling interfacial reactions is critical for zinc oxide (ZnO)-based inverted perovskite light-emitting diodes (PeLEDs), boosting the external quantum efficiency (EQE) of the near-infrared device to above 20%. However, violent interfacial reactions between the bromine-based perovskites and ZnO-based films severely limit the performance of inverted green PeLEDs, whose efficiency and stability lag far behind those of their near-infrared counterparts. Here, a controllable interfacial amidation between the bromine-based perovskites and magnesium-doped ZnO (ZnMgO) film utilizing caprylyl sulfobetaine (SFB) is realized. The SFB molecules strongly interact with formamidinium bromide, decelerating the amidation reaction between formamidinium and carboxylate groups on the ZnMgO film, thus regulating the crystallization of FAPbBr₃. Combined with the passivation of benzylamine, a FAPbBr₃ bulk film directly deposited on a ZnMgO substrate with single-crystal characteristics is obtained, exhibiting a high photoluminescence quantum yield of above 80%. The resultant PeLEDs demonstrate a peak EQE of exceeding 20% at a high luminance of 120,000 cd m^-2 and a half lifetime of 26 min at 11,000 cd m^-2, representing the state-of-the-art inverted green electroluminescence. This work resolves the crucial issues of violent interfacial reactions and provides a strategy toward inverted green PeLEDs with outstanding performance.