Abstract
The trap states at both the upper and bottom interfaces of perovskite layers significantly impact non-radiative carrier recombination. The widely used solvent-based passivation methods result in the disordered distribution of surface components, posing challenges for the commercial application of large-area perovskite solar cells (PSCs). To address this issue, a novel NH(3) gas-assisted all-inorganic dual-interfaces passivation strategy is proposed. Through the gas treatment of the perovskite surface, NH(3) molecules significantly enhanced the iodine vacancy formation energy (1.54 eV) and bonded with uncoordinated Pb(2+) to achieve non-destructive passivation. Meanwhile, the reduction of the film defect states is accompanied by a decrease in the work function, which promotes carrier transport between the interface. Further, a stable passivation layer is constructed to manage the bottom interfacial defects using inorganic potassium tripolyphosphate (PT), whose ─P═O group effectively mitigated the charged defects and lowered the carrier transport barriers and nucleation barriers of PVK, while the gradient distribution of K(+) improved the crystalline quality of PVK film. Based on the dual-interface synergistic effect, the optimal MA-contained PSCs with an effective area of 0.1 cm(2) achieved an efficiency of 24.51% and can maintain 90% of the initial value after aging (10-20% RH and 20 °C) for 2000 h.