Publication date: 17th February 2025
Metal halide perovskites have emerged as outstanding semiconductors for solar cells due to their excellent optoelectronic properties. Among these materials, formamidinium lead iodide (FAPbI3) is particularly notable as a competitive candidate for single-junction solar cells because of its optimal bandgap. However, a significant challenge is that the photoactive α-phase FAPbI3 can easily undergo phase transition to an undesired δ-phase FAPbI3 under ambient conditions. Additionally, most highly efficient perovskite solar cells are achieved through solvent-quenching technique, but researchers face difficulties applying this method to large-scale production. In contrast, gas quenching is a potential fabrication method for large-scale device fabrication, yet the perovskite thin films fabricated from traditional DMF/DMSO solvent system using this method suffer from poor electronic properties and stability. In this context, achieving high-quality α-FAPbI3 via the gas-quenching is challenging, but it holds great promise for ensuring long-term stability in industrialised single-junction perovskite solar cells. Here, we utilised a DMF/NMP solvent system for FAPbI3 through the gas-quenching method. The power conversion efficiency (PCE) of neat-FAPbI3 from DMF/NMP is 21.0%, significantly higher than that of solar cells made with the DMF/DMSO system. We also introduce a bulk additive to modulate crystallisation kinetics and demonstrate that this additive effectively suppresses the formation of δ-phase. This treatment enhances the crystal quality of α-FAPbI3, leading to improved crystallinity, absolute photoluminescence (PL), time-resolved photoluminescence (TRPL) lifetime, device efficiency, and long-term stability. We fabricated inverted-structured FAPbI3 perovskite solar cells using the gas-assisted technique and FAPbI3 with the additive shows better device performance, achieving a PCE of 21.8%, an open-circuit voltage (VOC) of 1.09 V, a short-circuit current density (JSC) of 24.60 mA/cm2, and a (FF) fill factor of 0.81. We also investigate how these different crystallisation kinetics are influenced by the chemical environments of perovskite precursor inks. The research approach can also be applied to understand and manipulate crystallisation from other precursor inks, unlocking a promising pathway for producing high-quality perovskite thin films.
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