The controlled growth of two-dimensional (2D) perovskite atop three-dimensional (3D) perovskite films reduces interfacial recombination and impedes ion migration, thus improving the performance and stability of perovskite solar cells (PSCs). Unfortunately, the random orientation of the spontaneously formed 2D phase atop the pre-deposited 3D perovskite film can deteriorate charge extraction owing to energetic disorder, limiting the maximum attainable efficiency and long-term stability of the PSCs. Here, we introduce a meta-amidinopyridine ligand and the solvent post-dripping step to generate a highly ordered 2D perovskite phase on the surface of a 3D perovskite film. The reconstructed 2D/3D perovskite interface exhibits reduced energetic disorder and yields cells with improved performance compared with control 2D/3D samples. PSCs fabricated with the meta-amidinopyridine-induced phase-pure 2D perovskite passivation show a maximum power conversion efficiency of 26.05% (a certified value of 25.44%). Under damp heat and outdoor tests, the encapsulated PSCs maintain 82% and 75% of their initial PCE after 1000 h and 840 h, respectively, demonstrating improved practical durability.
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