Impact of Substrate Heating and Cooling Rates on Crystallization and Inverted Solar Cells Performance of Co-evaporated CsPbI₂Br Perovskite Thin Films
Shijun Shi a b, Masato Sotome b, Kazuteru Nonomura b c, Hiroshi Segawa b c, Takashi Kondo a b
a Department of Advanced Interdisciplinary Studies, Graduate School of Engineering, University of Tokyo
b Research Center for Advanced Science and Technology, University of Tokyo
c Department of General Systems Studies, Graduate School of Arts and Sciences, University of Tokyo
Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV25)
Roma, Italy, 2025 May 12th - 14th
Organizers: Filippo De Angelis, Francesca Brunetti and Claudia Barolo
Oral, Shijun Shi, presentation 135
Publication date: 17th February 2025

All-inorganic perovskite solar cells (PSCs) utilizing CsPbI₂Br have emerged as promising candidates for next-generation photovoltaic technologies, owing to their superior stability against humidity, thermal fluctuations, and ultraviolet radiation [1], as well as their ideal bandgap of 1.9 eV [2]. These properties make CsPbI₂Br particularly suitable for tandem solar cells with silicon counterparts. Nevertheless, challenges such as rapid crystallization inherent to the spin-coating process often result in non-uniform morphologies and defect-rich films, thereby compromising device performance and reliability.

To address these limitations, we employed physical vapor co-deposition (PVD) to fabricate CsPbI₂Br thin films under controlled conditions, which allows precise control over deposition parameters and substrate temperature to fabricate high-quality films. Initially, thin films were deposited via co-evaporation of CsBr and PbI₂ onto glass substrates at substrate temperatures (Tsub) of 23°C and 100°C. Films deposited at 100°C exhibited superior optical and structural qualities, including enhanced absorption coefficients, compared to those produced via spin-coating [3] or PVD methods without substrate heating [4]. Building on these results, CsPbI₂Br thin films were subsequently deposited on FTO/PTAA (hole transport layer) substrates under identical conditions to construct inverted solar cells with the architecture FTO/PTAA/CsPbI₂Br/C₆₀/BCP/Ag. Following deposition, the films were annealed at 300°C for 10 seconds in nitrogen and cooled either rapidly or slowly (~0.051°C/s). Rapid cooling produced irregular surfaces and high defect densities, resulting in a maximum PCE of 4.21%. In contrast, slow cooling enhanced surface smoothness and crystallinity, as corroborated via SEM analysis, leading to an improved PCE of 5.82%. Additionally, slow cooling caused a color shift from pale brown to rich dark brown, indicating enhanced crystallinity. This study underscores the importance of substrate heating and controlled post-annealing cooling to achieve high-quality CsPbI₂Br films with improved photovoltaic performance and stability, providing valuable insights for further improvements in CsPbI₂Br-based inverted PSCs.

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