Core/Shell ZnO/ZnS Nanoparticle Electron Transport Layers Enable Efficient All‐Solution‐Processed Perovskite Light‐Emitting Diodes

Abstract Solution‐processed perovskite‐based light‐emitting diodes (PeLEDs) are promising candidates for low‐cost, large‐area displays, while severe deterioration of the perovskite light‐emitting layer occurs during deposition of electron transport layers from solution in an issue. Herein, core/shell ZnO/ZnS nanoparticles as a solution‐processed electron transport layer in PeLED based on quasi‐2D PEA₂Cs_n−1Pb_nBr_3n+1 (PEA = phenylethylammonium) perovskite are employed. The deposition of ZnS shell mitigates trap states on ZnO core by anchoring sulfur to oxygen vacancies, and at the same time removes residual hydroxyl groups, which helps to suppress the interfacial trap‐assisted non‐radiative recombination and the deprotonation reaction between the perovskite layer and ZnO. The core/shell ZnO/ZnS nanoparticles show comparably high electron mobility to pristine ZnO nanoparticles, combined with the reduced energy barrier between the electron transport layer and the perovskite layer, improving the charge injection balance in PeLEDs. As a result, the optimized PeLEDs employing core/shell ZnO/ZnS nanoparticles as a solution‐processed electron transport layer exhibit high peak luminance reaching 32 400 cd m⁻², external quantum efficiency of 10.3%, and 20‐fold extended longevity as compared to the devices utilizing ZnO nanoparticles, which represents one of the highest overall performances for solution‐processed PeLEDs.