Abstract
Buried defects at the interface between the wide-bandgap perovskite and the self-assembled monolayer (SAM) limit the performance of p–i–n solar cells, particularly in textured monolithic perovskite–silicon tandem solar cells. Here we reveal that uncontrolled perovskite crystallization dynamics on conventional SAMs drives the co-evolution of electronic defects and morphological degradation at the buried interface. This stems from structural and energetic incompatibility between the perovskite precursor solution and the SAM. To precisely control the perovskite crystallization, we develop a tailored SAM that mitigates defect formation and enhances interfacial electronic coupling. Integrated into a perovskite–silicon tandem solar cell, this approach enables a power conversion efficiency of 33.86% (certified as 33.59%) for a device with a 1-cm2 area and a power conversion efficiency of 29.25% (certified as 28.53%) for an area of 16 cm2. The tandem device demonstrates remarkable operational stability, retaining more than 90% of the initial power conversion efficiency after 2,000 h of operational under 1-sun illumination.
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The main data supporting the findings of this study are available in the article and the Supplementary Information. All other data related to this work are available from the corresponding authors on request. Source data are provided with this paper.
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Acknowledgements
X.Y. acknowledges grants by the National Natural Science Foundation of China (U23A20354 and 62025403), National Key Research and Development Program of China (2023YFB4202504), the Baima Lake Laboratory Joint Funds of the Zhejiang Provincial Natural Science Foundation of China (LBMHD24E020002) and ‘Pioneer’ and ‘Leading Goose’ R&D Program of Zhejiang (2024C01092). M.L. acknowledges funding support from the National Natural Science Foundation of China (21975219). P.H. acknowledges funding support from the National Natural Science Foundation of China (62304201) and ‘Pioneer’ and ‘Leading Goose’ R&D Program of Zhejiang (2025C01154).
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D.Z., B.Y. and P.H. conceived the idea, designed the experiments and wrote the original draft. B.Y. contributed to DMPP’s synthesis and structural characterization. D.Z. fabricated the devices and conducted the J–V, EQE, SEM, PL, XPS, XRD and stability measurements. D.Z. and R.X. contributed to the device fabrication and certification. R.X. and Y.C. contributed to the extra tandem certification in ESTI. D.Z. and H.Z. contributed to the PL mapping measurements. H.X. and Z.N. contributed to the DLCP measurements and related analysis. R.L. and B.L. contributed to the TAS and TID tests. J.W. assisted in the in situ characterizations and data processing. R.X. and J.G. designed and prepared the silicon bottom cells. X.Y., M.L. and P.H. provided funding support. X.Y., M.L. and P.H. revised the paper. P.H., X.Y., M.L., J.G. and D.Y. supervised the experimental development, led the project and reviewed the paper. All authors discussed the results and commented on the paper.
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Nature Photonics thanks Zhaoning Song and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Supplementary Text 1, Figs. 1–40, Tables 1–3 and References.
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Characterization of SAM properties for Fig. 1, mechanism of SAM-regulated perovskite growth for Fig. 2, performance and optoelectronic characterization of PSCs for Fig. 3 and photovoltaic and stability performance of perovskite–silicon tandem solar cells for Fig. 4.
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Zhang, D., Yan, B., Xia, R. et al. Perovskite crystallization control via an engineered self-assembled monolayer in perovskite–silicon tandem solar cells. Nat. Photon. 20, 40–48 (2026). https://doi.org/10.1038/s41566-025-01778-y
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DOI: https://doi.org/10.1038/s41566-025-01778-y
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