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Perovskite solar cells (PSCs) with superior performance have been recognizedas a potential candidate in photovoltaic technologies. However, the defects inactive perovskite layer induce non-radiative recombination which restricts theperformance and stability of the PSCs. The construction of thiophene-based 2Dstructure is one of the significant approaches for surface passivation ofhybrid PSCs that may combine the benefits of the stability of 2D perovskitewith the high performance of 3D perovskite. Here, a sulfur-rich spacer cation2-thiopheneethylamine iodide (TEAI) is synthesized as a passivation agent forthe construction of three-dimensional/two-dimensional (3D/2D) perovskitebilayer structure. TEAI-treated PSCs possess a much higher efficiency (20.06%)compared to the 3D perovskite (MAFAPbI3) devices (17.42%). Time-resolvedphotoluminescence (TRPL) and femtosecond transient absorption (TA) spectroscopyare employed to investigate the effect of surface passivation on the chargecarrier dynamics of the 3D perovskite. Additionally, the stability test ofTEAI-treated perovskite devices reveals significant improvement in humid (RH ~56%) and thermal stability as the sulfur-based 2D (TEA)2PbI4 materialself-assembles on the 3D surface making the perovskite surface hydrophobic. Ourfindings provide a reliable approach to improve device stability andperformance successively, paving the way for industrialization of PSCs.

Improvement of both performance and stability of photovoltaic devices by in situ formation of a sulfur-based 2D perovskite