Publication date: 5th November 2025
Functional organic molecules capable of defect passivation in halide perovskite crystals work for suppressing charge recombination loss, leading to enhancement of photovoltage.1 Amino group-bearing molecules, such as phenylethylamine (PEA) halide and amino acids, are widely applied for passivation of organic/inorganic perovskites. We modified the perovskite-hole transport layer (HTL) interface with an oriented PEABr monolayer and improved VOC close to 1.2V for a 1.51 eV bandgap perovskite, minimizing the VOC loss (0.3V) from the SQ limit, similar to the best performance of GaAs device. While interfacial modification using oriented functional monolayers enhance the photovoltaic performance, recombination caused by iodine defects in the bulk polycrystalline structure is a key target for improving performance. Regarding all-inorganic perovskites (CsPbX3, X=I, Br, bandgap of 1.9 to 2.1eV), iodine defects are passivated with 2,5-thiophenedicarboxylic acid (TDCA) and the CsPbX3 devices achieve high VOC of 1.4 to 1.5V.2 As visible-light absorbers, CsPbX3 devices achieve power conversion efficiency (PCE) over 34% under indoor lighting.3 Recent cell designs are evolving to use self-assembled monolayers (SAMs) at the interface, and inverted devices architecture typically use SAMs at the perovskite-TCO electrode interface. Although many bifunctional molecules have been used as p-type SAMs capable of selective hole transport, relatively few devices utilize n-type SAMs. A challenge of our device design opened the door to the possibility of creating lattice-matched SAM-modified interfaces in perovskite solar cells.4 We started research to design a new device architecture in which interfaces of perovskite layer are fully functionalized with SAMs. Junction interfaces were modified with p-type SAM and n-type SAM that replace HTL and electron transport layer (ETL), respectively. SAM-based devices were fabricated for different perovskite compositions, and all photovoltaic devices free of charge transport layers exhibited good photovoltaic performance with perfect bifacial power generation. They demonstrated high stability against long term light soaking as an advantage of not using bulk HTL and ETL layers.5 This method of interface modifications will be effective for fabrication of lead-free perovskite solar cells.6,7 It will also be applied to fabrication of plastic film type flexible modules, which is a goal of our module development project. Recent advances in the architecture of perovskite solar cells based on interfacial molecular engineering will be presented.
References
1. T. Miyasaka, editor, Perovskite Photovoltaics and Optoelectronics ―From Fundamentals to Advanced Applications―, Wiley-VCH, Weinheim, 2021, ISBN: 978-3-527-34748-3.
2. Z. Guo, S. Zhao, N. Shibayama, A. K. Jena, I. Takei, T. Miyasaka, Adv. Funct. Mater. 2022, 32, 2207554.
3. Z. Guo, A. K. Jena, and T. Miyasaka, ACS Energy Lett. 2023, 8, 90.
4. T. Wu, T. B. Raju, J. Shang, L. Wu, J. T. Song, C. A. M. Senevirathne, A. Staykov, S. Wang, S. Ida, N. Shibayama, T. Miyasaka, T. Matsushima, and Z. Guo, Adv. Mater. 2025, 37, 2414576.
5. Z. Hu, N. Saito, M. Ikegami, N. Shibayama, and T. Miyasaka, submitted.
6. N. B. C. Guerrero, M. D. Perez, N. Shibayama, and T. Miyasaka, Chem. Sci. 2025,16, 5807.
7. L. Cojocaru, A. J. Jena, M. Yamamiya, Y. Numata, M. Ikegami, and T. Miyasaka, Adv. Sci. 2024, 11, 2406998
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