Interfacial dipole engineering by self-assembled molecules in n-i-p and p-i-n perovskite solar cells

作者：Mengde Zhai, Tianhao Wu, Kaihuai Du, Cheng Chen, Naoyuki Shibayama, Khongorzul Narmandakh, Abdul Haseeb Hassan Khan, Ying‐Chiao Wang, Juan Shang, Aleksandar Staykov, Jun Tae Song, Shintaro Ida, Pangpang Wang, Sunao Yamada, Kaoru Tamada, Shuai Zhao, Aili Wang, Zhanglin Guo, Toshinori Matsushima, Tsutomu Miyasaka, Ming Cheng · 发表于：Nature Communications · 年份：2026 · DOI：10.1038/s41467-026-69198-2 · 被引用次数：10 · 研究领域：Perovskite Materials and Applications、Organic Electronics and Photovoltaics、TiO2 Photocatalysis and Solar Cells

Self-assembled molecules are widely used as bottom interfacial layers in inverted perovskite solar cells, yet their application to perovskite top surfaces remains poorly understood. Here, we develop two self-assembled molecules for perovskite surface modification and interfacial optimization with the hole transport layer. Through solvent engineering, ordered and uniform molecular packing is achieved on the perovskite surface. These molecules optimize surface energetics and promote efficient hole transfer when coupled with a homologous hole transport layer. Their large molecular dipoles tune interfacial energy alignment and reduce energetic offsets, thereby accelerating charge extraction from the perovskite layer. This dipole-driven interfacial modulation is effective in both normal and inverted device architectures. As a result, a power conversion efficiency of 26.18% (certified 26.23%) is achieved in normal-structure devices, together with improved operational stability under maximum power point tracking. This work establishes a viable strategy for perovskite surface engineering using self-assembled molecules. Zhai et al. report newly designed self-assembled molecules exhibiting strong and ordered anchoring on the perovskite surface to reduce defects and modulate the dipole-induced energy-level, enabling certified efficiencies of 26.23% in a normal device structure, which are also applicable to inverted perovskite solar cells.