Accelerating Photogenerated Hole Tunneling through Passivation Layers via Reducing Interplanar Spacing for Efficient and Stable Perovskite Solar Cells

Interfacial passivation engineering plays a crucial role in the explosive development of perovskite solar cells (PSCs). However, previous studies on passivation layers mainly focused on the defect-passivation mechanism rather than the interfacial charge transport efficiency. Here, by precisely tuning the interplanar spacing of the ammonium iodide passivation layer, we elucidate the promoting effect of the reduced interplanar spacing of the passivation layer on the photogenerated hole tunneling efficiency at the interface of the hole transport layer and perovskite. Compared with the commonly used phenethylammonium iodide passivation layer with a wider interplanar spacing, 2-chlorobenzylammonium iodide with a narrower interplanar spacing can help break through the thickness limitation of the passivation layer, thus showing a better comprehensive passivation effect. Therefore, we demonstrate photovoltaic devices with an enhanced fill factor (FF) and open-circuit voltage (VOC), which yield a high power conversion efficiency (PCE) of up to 23.1%. We thus identify an efficient scheme to achieve optimal passivation conditions for high-performance PSCs.