Charge Polarization Tunable Interfaces for Perovskite Solar Cells and Modules

Interfacial localized charges and interfacial losses from incompatible underlayers are critical factors limiting the efficiency improvement and market-integration of perovskite solar cells (PSCs). Herein, a novel interfacial chemical tuning strategy is proposed involving proton transfer between the amine head of pyridoxamine (PM) and the phosphonic acid anchoring group of [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz), with simultaneous enhancement of charge delocalization through electrostatic attraction between opposite charged molecules. The Me-4PACz-PM charge polarization interface modulates the nickel oxide (NiO_x) charge states and the coordination environment at buried interfaces, consequently enhancing p-type conductivity and obtaining a more compatible band arrangement. The high-coverage and wettability of the NiO_x/Me-4PACz-PM underlayer also facilitate the deposition of high-quality perovskite films, releasing lattice strain and mitigating trap-assisted non-radiative recombination. Attributing to the implementation of charge polarization tunable interfaces, small-area devices and modules with an aperture area of 69 cm² achieved impressive power conversion efficiencies (PCEs) of 26.34% (certified 25.48%) and 21.94% (certified 20.50%), respectively, and unencapsulated devices maintained their initial PCEs ≈90% after aging for 2000 h (ISOS-L-1) and 1500 h (ISOS-D-1). The broad applicability of charge polarization tunable interfaces and the successful scaling of large-area modules provide a reference for expanding PSCs applications.