Dual Strategy Based on Quantum Dot Doping and Phenylethylamine Iodide Surface Modification for High-Performance and Stable Perovskite Solar Cells

High-quality perovskite films (PFs) are crucial for achieving high-performance perovskite solar cells (PSCs). Herein, we report a dual-modification strategy via incorporating CsPbBr₃ QDs into MAPbI₃ perovskite bulk and capping the interface of the perovskite/hole transport layer (HTL) with phenylethylamine iodide (PEAI) to improve perovskite crystallinity and interface contact properties to acquire high-quality PFs with fewer defects. CsPbBr₃ QDs promoted perovskite grain growth and reduced bulk defects, while PEAI surface modification passivated interfaces, improved hydrophobic properties, and prevented carrier recombination at the perovskite/HTL interface. Benefiting from growth control and the effective suppression of both bulk and interface carrier recombination, the resulting devices show a greatly improved photoelectric conversion efficiency (PCE) from 17.21% of the reference cells to 21.04% with a champion Voc of 1.15 V, Jsc of 23.30 mA/cm², and fill factor (FF) of 78.6%. Furthermore, the dual-modification strategy endows PFs with promoted moisture tolerance, and the nonencapsulated PSCs retain 75% of their initial efficiency after aging for 30 days at 40% relative humidity and room temperature, which is significantly higher than the 59% value of the original PSCs. Good operational stability and the maintained efficiency of the target device over time suggest the potential for future commercialization.