Operando Electron Spin Resonance to Elucidate the Factors Governing Device Performance of Perovskite Solar Cells
Kazuhiro Marumoto a b c
a Department of Materials Science, Institute of Pure and Applied Sciences, University of Tsukuba, Tsukuba, lbaraki, 305-8573, Japan
b Research Center for Organic-Inorganic Quantum Spin Science and Technology (OIQSST), University of Tsukuba, Tsukuba, Ibaraki 305-8573, Japan
c Tsukuba Research Center for Energy Materials Science (TREMS), University of Tsukuba, Tsukuba, Ibaraki 305-8571, Japan
Proceedings of Asia-Pacific Conference on Perovskite, Organic Photovoltaics&Optoelectronics (IPEROP25)
Kyoto, Japan, 2025 January 19th - 21st
Organizers: Atsushi Wakamiya and Hideo Ohkita
Invited Speaker Session, Kazuhiro Marumoto, presentation 008
Publication date: 4th October 2024

Perovskite solar cells (PSCs) are expected to become one of the next-generation solar cells owing to their advantages such as low cost, flexibility, and high efficiency. Much research has been carried out to improve device performance and the dominant factors governing the device performance have been elucidated. However, not enough research has been conducted from a microscopic viewpoint at the molecular level [1,2]. In this study, solar-cell devices and thin-film samples were fabricated using perovskite with mixed cations and mixed halogens, and the charge states including charge diffusion and charge formation at the interfaces between hole- or electron-transport layers (HTL or ETL) and perovskite layers were investigated by a microscopic method with high sensitivity, electron spin resonance (ESR). We have utilized the ESR method to study the charge states and charge transfer in organic and perovskite solar cells and their materials under not only dark conditions but also under device operation [3-10]. The ESR investigation under device operation is called as an operando ESR method [4,7,8]. In the dark state, charge diffusion occurs in stacked films of HTL or ETL and perovskite. This causes a vacuum level shift at the interfaces between HTL or ETL and perovskite, forming band bending at the perovskite interface. This band bending has been shown to dominate device performance during device operation. The results of lead- and tin-based PSCs will be presented.

This work was supported by JSPS KAKENHI Grant no. 24K01325, Japan, by JST PRESTO, Japan, by the University of Tsukuba, Organization for the Promotion of Strategic Research Initiatives, Japan, by JST ALCA Grant no JPMJAL1603, Japan, by JST MIRAI Grant nos. JPMJMI20C5, JPMJMI22C1, and JPMJMI22E2, Japan, and by NEDO Green Innovation, Japan. The author would like to thank to A. Sato, Y. Chen, Dr. D. Xue, Dr. S. Yamaguchi, T. Watanabe, H. Kimata, M. Motohashi, Y. Wang of University of Tsukuba, Japan, Prof. A. Wakamiya, Dr. T. Nakamura, A. Shimazaki, Dr. M. Ozaki, Dr. R. Murdey, Dr. M. A. Truong, Dr. S. Hu of Kyoto University, Japan, and Prof. S. Hayase of The University of Electro-Communications, Japan for their collaboration works.

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