Thiophene-Based Two-Dimensional Dion–Jacobson Perovskite Solar Cells with over 15% Efficiency

Two-dimensional (2D) perovskites are emerging photovoltaic materials because of their highly tunable photophysical properties and improved environmental stability in comparison with 3D perovskites. Here, a thiophene-based bulky dication spacer, namely, 2,5-thiophenedimethylammonium (ThDMA), was developed and applicated in 2D Dion–Jacobson (DJ) perovskite. High-quality 2D DJ perovskite, (ThDMA)(MA)n–1PbnI3n+1 (nominal n = 5), with improved crystallinity, preferred vertical orientation, and enlarged spatially resolved carrier lifetime could be achieved by a one-step method using a mixed solvent of DMF/DMSO (v/v, 9:1). The optimized device exhibits a high efficiency of 15.75%, which is a record for aromatic spacer-based 2D DJ perovskite solar cells (PSCs). Moreover, the unencapsulated 2D DJ perovskite devices sustained over 95% of their original efficiency after storage in N2 for 1655 h. Importantly, both the light-soaking stability and thermal stability (T = 80 °C) of the 2D DJ perovksite devices are dramatically improved in comparison with their 3D counterparts. These results indicate that highly efficient and stable 2D DJ PSCs could be achieved by developing thiophene-based aromatic spacers as well as device engineering.