Nucleation Regulation and Mesoscopic Dielectric Screening in α-FAPbI

Tian, Ruijia; Liu, Chang; Meng, Yuanyuan; Wang, Yaohua; Cao, Ruikun; Tang, Bencan; Walsh, Darren; Do, Hainam; Wu, Haodong; Wang, Kai; Sun, Kexuan; Yang, Shuncheng; Zhu, Jintao; Li, Xin; Ge, Ziyi

Abstract

While significant advancements in power conversion efficiencies (PCEs) of α-FAPbI perovskite solar cells (PSCs) have been made, attaining controllable perovskite crystallization is still a considerable hurdle. This challenge stems from the initial formation of δ-FAPbI , a more energetically stable phase than the desired black α-phase, during film deposition. This disrupts the heterogeneous nucleation of α-FAPbI , causing the formation of mixed phases and defects. To this end, polarity engineering using molecular additives, specifically ((methyl-sulfonyl)phenyl)ethylamines (MSPEs) are introduced. The findings reveal that the interaction of PbI -MSPEs-FAI intermediates is enhanced with the increased polarity of MSPEs, which in turn expedites the nucleation of α-FAPbI . This leads to the development of high-quality α-FAPbI films, characterized by vertical crystal orientation and reduced residual stresses. Additionally, the increased dipole moment of MSPE at perovskite grain boundaries attenuates Coulomb attractions among charged defects and screens carrier capture process, thereby diminishing non-radiative recombination. Utilizing these mechanisms, PSCs treated with highly polar 2-(4-MSPE) achieve an impressive PCE of 25.2% in small-area devices and 20.5% in large-area perovskite solar modules (PSMs) with an active area of 70 cm . These results demonstrate the effectiveness of this strategy in achieving controllable crystallization of α-FAPbI , paving the way for scalable-production of high-efficiency PSMs. [Abstract copyright: © 2023 Wiley-VCH GmbH.]

Citation

Tian, R., Liu, C., Meng, Y., Wang, Y., Cao, R., Tang, B., Walsh, D., Do, H., Wu, H., Wang, K., Sun, K., Yang, S., Zhu, J., Li, X., & Ge, Z. (2024). Nucleation Regulation and Mesoscopic Dielectric Screening in α-FAPbI. Advanced Materials, 36(13), Article 2309998. https://doi.org/10.1002/adma.202309998

• Journal Article Type: Article
• Acceptance Date: Dec 11, 2023
• Online Publication Date: Dec 18, 2023
• Publication Date: Mar 28, 2024
• Deposit Date: Aug 13, 2024
• Publicly Available Date: Dec 19, 2024
• Journal: Advanced Materials
• Print ISSN: 0935-9648
• Electronic ISSN: 1521-4095
• Publisher: Wiley
• Peer Reviewed: Peer Reviewed
• Volume: 36
• Issue: 13
• Article Number: 2309998
• DOI: https://doi.org/10.1002/adma.202309998
• Keywords: Dielectric screening, Nonradiative decay, Polarity engineering, Perovskite solar modules, Nucleation regulation
• Public URL: https://nottingham-repository.worktribe.com/output/29257220
• Publisher URL: https://onlinelibrary.wiley.com/doi/10.1002/adma.202309998