Abstract
While self-assembled monolayers (SAMs) have demonstrated remarkable success in iodide-based perovskite solar cells (PSCs), their application in bromide-based PSCs is fundamentally constrained by poor crystallization behavior and interfacial energy level misalignment. To overcome these limitations, the SAMs of (3-(3,7-bis(diphenylphosphoryl)-10H-phenoxazin- 10-yl)propyl) phosphonic acid (3,7-POPA) are designed and synthesized to address these challenges in FAPbBr_3-based PSCs. 3,7-POPA not only facilitates oriented crystallization of perovskite and defect minimization but also optimizes energy level alignment at the hole-selective interface, thereby significantly enhancing hole extraction efficiency. Consequently, optimized FAPbBr_3-based PSCs achieve a power conversion efficiency (PCE) of 10.79% with a record open circuit voltage (Voc) of 1.51 V. Remarkably, after operating at maximum power point for 1000 h, the encapsulated device maintains 90% of its initial PCE. The novel SAM-based hole transport strategy simultaneously resolves crystallization, defect, and energy-level challenges in Br-based PSCs, achieving record efficiency and stability for high-performance PSCs.