Reduced-Dimensional α-CsPbX3 Perovskites for Efficient and Stable Photovoltaics

Inorganic CsPbX3 perovskites have gained great attention owing to their excellent thermal stability and carrier transport properties. However, the power conversion efficiency (PCE) of solution-processed CsPbX3 perovskite solar cells is still far inferior to that of their hybrid analogues. Insufficient film thickness and undesirable phase transition are the two major obstacles limiting their device performance. Here, we show that by adopting a new precursor pair, cesium acetate (CsAc) and hydrogen lead trihalide (HPbX3), we were able to overcome the notorious solubility limitation for Cs precursors to fabricate high-quality CsPbX3 perovskite films with large film thickness (similar to 500 nm). We further introduced a judicious amount of phenylethylammonium iodide (PEAI) into the system to induce reduced-dimensional perovskite formation. Unprecedentedly, the resulting quasi-2D perovskites significantly suppressed undesirable phase transition and thus reduced the film's trap density. Following this approach, we reported a state-of-the-art PCE to date, 12.4%, for reduced-dimensional alpha-CsPbI3 perovskite photovoltaics with greatly improved performance longevity.