Abstract
Two-dimensional surface passivation has been shown to be useful for achieving state-of-the-art perovskite optoelectronics, and the microstructural and phase heterogeneities of two-dimensional perovskite passivators can influence their roles. However, the synthesis of co-homogenized, stable microstructure and phase in such passivators remains challenging. Herein we leverage a [6,6]-phenyl-C61-butyric acid methyl ester molecular interlayer to mediate the reaction of the two-dimensional passivator and perovskite, leading to a uniform purer-phase two-dimensional perovskite capping layer. This interlayer mitigates the grain-boundary etching encountered in conventional approaches, creating molecular passivation directly onto the perovskite surface. The inverted perovskite solar cells made with the interlayer feature a laminate-structured perovskite heterointerface at the electron-extracting side, which contributes to improved charge energetics and film stability, owing to the regulated band alignment and laminate-layer protection, respectively. Power conversion efficiencies up to 25.97% are achieved, together with enhanced device stabilities under protocols standardized by the International Summit on Organic Photovoltaic Stability, showing T90 lifetimes (the time at which they maintain 90% of their efficiency) of over 1,000 h in both the damp-heat test (85 °C, 85% relative humidity) and maximum power point tracking under one-sun illumination. Lattice-resolved insights are provided to link the microstructure to device performance, shedding light on the significance of passivator-microstructure uniformity and reliability on the performance of perovskite optoelectronics.

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The authors declare that data supporting the findings of this study are available within the paper and its Supplementary Information files. Source data are provided with this paper.
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Acknowledgements
Y. Zhou acknowledges the Excellent Young Scientists Fund (no. 52222318) from the National Natural Science Foundation of China (NSFC); the General Research Fund (nos 12302822 and 12300923) and the Collaborative Research Fund (no. C2001-23Y) from the Hong Kong Research Grants Council (RGC); the NSFC/RGC Collaborative Research Scheme (no. CRS_HKUST203/23); and the startup grant from the HKUST. Y. Zhou also acknowledges the support from the China Merchants Group, particularly China Merchants Testing Certification International Co., Ltd. and China Merchants Research Institute of Advanced Technology Co., Ltd., for translating fundamental research to future technology innovation. S.C. acknowledges the startup grants from the Department of Applied Physics, Hong Kong Polytechnic University (1-BDCM), the General Research Fund (no. 15306122) and the Early Career Scheme (no. 25305023) from the Hong Kong RGC.
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Y. Zhou and S.C. supervised the project. Z.L., S.C. and Y. Zhou conceived the idea and designed the experiments. Z.L. performed the film synthesis and electron-microscopy characterizations. W.W. conducted the data analysis of 4D-STEM. P.G. performed the device fabrication and performance testing, some materials characterizations (PL, XRD and so on) and device and film stability tests. Y. Zhang contributed to the illustrations and assisted in materials characterization. Y. Zhou, S.C., Z.L. and P.G. prepared the manuscript. All co-authors contributed to reviewing and revising the manuscript.
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Nature Synthesis thanks Guangfu Luo and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Primary Handling Editor: Alexandra Groves, in collaboration with the Nature Synthesis team.
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Li, Z., Guo, P., Zhang, Y. et al. Synthesis of a lattice-resolved laminate-structured perovskite heterointerface. Nat. Synth 4, 1078–1087 (2025). https://doi.org/10.1038/s44160-025-00787-7
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DOI: https://doi.org/10.1038/s44160-025-00787-7
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