Hole-Transport Management Enables 23%-Efficient and Stable Inverted Perovskite Solar Cells with 84% Fill Factor

NiO(x)-based inverted perovskite solar cells (PSCs) have presented great potential toward low-cost, highly efficient and stable next-generation photovoltaics. However, the presence of energy-level mismatch and contact-interface defects between hole-selective contacts (HSCs) and perovskite-active layer (PAL) still limits device efficiency improvement. Here, we report a graded configuration based on both interface-cascaded structures and p-type molecule-doped composites with two-/three-dimensional formamidinium-based triple-halide perovskites. We find that the interface defects-induced non-radiative recombination presented at HSCs/PAL interfaces is remarkably suppressed because of efficient hole extraction and transport. Moreover, a strong chemical interaction, halogen bonding and coordination bonding are found in the molecule-doped perovskite composites, which significantly suppress the formation of halide vacancy and parasitic metallic lead. As a result, NiO(x)-based inverted PSCs present a power-conversion-efficiency over 23% with a high fill factor of 0.84 and open-circuit voltage of 1.162 V, which are comparable to the best reported around 1.56-electron volt bandgap perovskites. Furthermore, devices with encapsulation present high operational stability over 1,200 h during T(90) lifetime measurement (the time as a function of PCE decreases to 90% of its initial value) under 1-sun illumination in ambient-air conditions. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-023-01088-4.