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Understanding and manipulating the crystallization of Sn–Pb perovskites for efficient all-perovskite tandem solar cells

Abstract

All-perovskite tandem solar cells are promising as next-generation high-efficiency photovoltaic devices. However, further progress in tin-lead (Sn–Pb) mixed perovskites, which are essential as the narrow-bandgap bottom sub-cell, is hampered by unbalanced crystallization processes, leading to inhomogeneous films and reduced power conversion efficiency (PCE). Here we provide a complete understanding of the formation of Sn–Pb films, from the precursor solution to the final film. We find that the total crystallization barrier for Sn-based perovskites is limited by the desorption of dimethyl sulfoxide (DMSO), while Pb-based perovskites experience a smaller DMSO desorption barrier. By engineering the reaction barrier in mixed films via tailoring the DMSO content, we obtain synchronous Sn–Pb perovskite crystallization and high-quality homogeneous films. On the basis of this understanding, we demonstrate single-junction Sn–Pb perovskite solar cells with a PCE of 22.88% and all-perovskite tandem devices with a certified PCE of 28.87%, fabricated by antisolvent-free methods. The unencapsulated tandem devices retain 87% of their initial PCE after about 450 h with maximum power point tracking under 1 sun illumination.

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Fig. 1: The evolution routes of Sn- and Pb-based perovskites from the intermediate to perovskite phase.
Fig. 2: Balancing the crystallization barrier of Sn- and Pb-based perovskites via precisely tuning the DMSO/[Pb + Sn] ratio.
Fig. 3: Device performance of optimized Sn–Pb NBG PSCs.
Fig. 4: Device performance of all-perovskite TSCs.

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All data are available in the main text or Supplementary Information. The data are available from the corresponding authors upon reasonable request.

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Acknowledgements

All work was supported by the National Natural Science Foundation of China (62134003 to J.T. and 62174064 to C.C.), the Major State Basic Research Development Program of China (2023YFB3608900 to J.T.), Guangdong Provincial Key Laboratory of Manufacturing Equipment Digitization (2023B1212060012 to C.C.), the Innovation Project of Optics Valley Laboratory (OVL2024ZD002 to C.C. and OVL2021BG008 to J.T.), Fundamental Research Funds for the Central Universities (2021XXJS028 to C.C.), the Innovation Fund of WNLO and the National Natural Science Foundation of China/Research Grants Council of Hong Kong Joint Research Scheme (22361162608 to A.L.). We also appreciate measurement support from Die & Mould Technology, the Analytical and Testing Center of Huazhong University of Science and Technology, the open and Shared Service Platform for Large Instruments and Equipment of School of Optical and Electronic Information of Huazhong University of Science and Technology and the Center for Nanoscale Characterization & Devices (CNCD), WNLO-HUST for facility access.

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Contributions

J.T., C.C. and H.S. conceived the idea and directed the overall project. X.Y. and T.M. fabricated all the devices and conducted the characterizations. A.Z., C.G. and M.L. helped to set up laboratory equipment and optimize the vacuum-assisted devices. H.H. and X.L. participated in the discussion and performed thermogravimetric analysis measurement. S.Y. performed maximum power point tracking measurements. W.Y., Y.Z. and J.Y. helped to fabricate and optimize Sn–Pb perovskite film. Z.L. and X.S developed the synthesis of 4PADCB. Y.Z. helped to discuss and analyse data. X.Y., C.C. and J.T. wrote the manuscript with the help of T.M. All authors discussed the results and commented on the paper.

Corresponding authors

Correspondence to Chao Chen, Haisheng Song or Jiang Tang.

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Nature Photonics thanks Yinghuan Kuang, Michael Saliba and Hairen Tan for their contribution to the peer review of this work.

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Supplementary Note 1, Figs. 1–37, Tables 1–4 and References.

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Yang, X., Ma, T., Hu, H. et al. Understanding and manipulating the crystallization of Sn–Pb perovskites for efficient all-perovskite tandem solar cells. Nat. Photon. 19, 426–433 (2025). https://doi.org/10.1038/s41566-025-01616-1

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