Publication date: 17th February 2025
Inorganic metal halide (IMH) perovskites have garnered significant attention in the field of perovskite photovoltaics due to their exceptional thermal stability compared to organic-inorganic hybrid counterparts. Since their initial report in 2015, IMH perovskites have achieved power-conversion efficiencies (PCEs) exceeding 20% [1]. However, the limited solubility of inorganic compounds in conventional solvents poses challenges for uniform film deposition and crystallization using lab-scale solution-processing techniques. To address these issues, researchers have explored alternative solvent systems and processing techniques, including crystallization regulation, composition engineering, interface engineering, and novel charge transport layers [2]. Thermal evaporation (TE), a well-established method in the semiconductor industry, presents a promising approach for fabricating IMH perovskite films, particularly cesium-based compositions, by circumventing the solubility limitations of wet-chemistry approaches. TE is also suitable for the fabrication of oxygen-sensitive or metastable perovskites such as cesium lead mixed halide (CsPbI2Br). In this study, we investigated the effect of substrate temperature on characteristics of stoichiometrically balanced CsPbI2Br thin films fabricated by co-evaporation of CsBr and PbI2 precursors under high vacuum conditions. While previous reports on thermally evaporated CsPbI2Br emphasized the need for high post-annealing temperatures (>260 °C) [2, 3] or utilizing multiple deposition sources [4] to obtain good film morphology, we demonstrated the importance of applying substrate temperature during film fabrication, coupled with a mild post-annealing temperature at 150 °C. The substrate heating during deposition resulted in films with improved crystallinity and phase stability. Additionally, passivation of the perovskite layer with phenethylammonium chloride (PEACl) and the integration of NiOx/MeO-2PACz as a hybrid hole transport layer (HTL), resulted in a PCEs of 13.21% in p-i-n PSCs based on vacuum-deposited CsPbI2Br films with a bandgap of 1.9 eV. Notably, encapsulated devices maintained 80% of their initial efficiency under 1-sun illumination for 450 hours. This study underscores the most promising approaches for optimizing CsPbI2Br perovskite vacuum deposition and enhancing the performance of p-i-n solar cell architectures.