Efficient and stable Ruddlesden–Popper perovskite solar cell with tailored interlayer molecular interaction

Two-dimensional Ruddlesden–Popper phase (2DRP) perovskites are known to exhibit improved photostability and environmental stability compared with their three-dimensional (3D) counterparts. However, fundamental questions remain over the interaction between the bulky alkylammoniums and the 2DRP perovskite framework. Here, we unambiguously demonstrate that a sulfur–sulfur interaction is present for a new bulky alkylammonium, 2-(methylthio)ethylamine hydrochloride (MTEACl). In addition to a weaker van der Waals interaction, the interaction between sulfur atoms in two MTEA molecules enables a (MTEA)₂(MA)₄Pb₅I₁₆ (n = 5) perovskite framework with enhanced charge transport and stabilization. The result is 2DRP perovskite solar cells with significantly improved efficiency and stability. Cells with a power conversion efficiency as high as 18.06% (17.8% certified) are achieved, along with moisture tolerance for up to 1,512 h (under 70% humidity conditions), thermal stability for 375 h (at 85 °C) and stability under continuous light stress (85% of the initial efficiency retained over 1,000 h of operation at the maximum power point).