Highly Orientational Order Perovskite Induced by In situ‐generated 1D Perovskitoid for Efficient and Stable Printable Photovoltaics

Abstract Employing low‐dimensional perovskite has been proven to be a promising approach to enhance the efficiency and stability of perovskite solar cells. Here, thiopheniformamidine hydrochloride is introduced into CH₃NH₃PbI₃‐based printable mesoscopic perovskite solar cells, to form 1D iodide lead thiophenamidine (TFPbI₃) in situ. This judiciously designed low‐dimensional perovskite can effectively passivate the defect of perovskite and induce the perovskite crystals to grow in a direction perpendicular to the substrate. Thus, the obtained 1D@3D perovskite could suppress the charge recombination and promote the charge transfer significantly. Benefiting from its dual effect and robustness, a significantly improved power conversion efficiency of 17.42% is yielded. The authors also develop high‐performance printable mesoscopic perovskite solar cells with a champion efficiency approaching 13% for aperture area about 11.8 cm², as well as outstanding operational stability, retaining 90% of the original power conversion efficiency after 1000 hours of continuous illumination at the maximum power point in air.