Abstract
Inorganic perovskite solar cells could benefit from surface passivation using 2D/3D perovskite heterostructures. However, conventional spacer cations fail to exchange with the tightly bonded Cs cation in the inorganic perovskite to form 2D layers atop; or, when they do enable formation of a 2D layer, they migrate under heat, degrading device performance. Here we investigate the mechanisms behind 2D/3D heterostructure formation and stabilization. We find that 2D/3D heterostructure formation is driven by interactions between ammonium groups and [PbI6]4− octahedra. We thus incorporate electron-withdrawing fluorine to enhance inorganic–organic cation interdiffusion and promote heterostructure formation. We note that stability relies on interactions between the entire spacer cations and [PbI6]4− octahedra. We therefore introduce anchoring groups that double cation desorption energies, preventing cation migration at elevated temperatures. CsPbI3/(perfluoro-1,4-phenylene)dimethanammonium lead iodide heterostructures enable an efficiency of 21.6% and a maximum power point operating stability at 85 °C of 950 h. We demonstrate 16-cm2 modules with an efficiency of 19.8%.
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The data that support the findings of this study are provided in Supplementary Information. Source data are provided with this paper.
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Acknowledgements
M.K.N. acknowledges support from the European Union’s Horizon 2020 research and innovation programme (number 763977). E.H.S. acknowledges support from the award 70NANB19H005 from the US Department of Commerce, National Institute of Standards and Technology, as part of the Center for Hierarchical Materials Design (CHiMaD). J.D.F. and M.G.K. acknowledge support from the National Science Foundation under grant number DMR-2019444 (National Science Foundation Center for Integration of Modern Optoelectronic Materials on Demand, IMOD, X-ray crystallographic and optical studies of 2D perovskites). I.W.G. was supported by US Department of Energy, Office of Science, Basic Energy Sciences, under award number DE-SC-0012541 (single-crystal X-ray crystal structure determination). K.R. thanks the Research Council of Lithuania via grant number S-MIP-20-20 and the funding received from the World Federation of Scientists (WFS) fellowship. This work made use of the EPIC facility of Northwestern University’s NUANCE Center, which has received support from the SHyNE Resource (National Science Foundation ECCS-2025633), the IIN and Northwestern’s MRSEC programme (National Science Foundation DMR-1720139). We thank C. Ballif and C. Wolf for assisting with module measurements. We also acknowledge O.A. Syzgantseva and M.A. Syzgantseva for suggestions on theoretical calculations and C. Igci and S. Dai for support with material synthesis and characterization. A.S.R.B. acknowledges support from King Abdullah University of Science and Technology through the Ibn Rushd Postdoctoral Fellowship Award.
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C.L. conceived of the idea and proposed the experimental design. C.L. and Y.Y. performed the device fabrication and characterizations. A.L., Z.W., H.Z. and B.C. gave suggestions on the paper writing. J.D.F. and I.W.G. performed synthesis, physico-chemical analysis and crystallographic single-crystal analysis. C.B.M. performed DFT calculation. R.P.R., K.R., R.S. and V.G. synthesized organic halides. B.D., Y.D., L.Z., Z.W. and X.Z. helped with the device fabrication. H.C., H.W. and A.S.R.B. helped with photoluminescence (PL) measurement. N.S. performed the GIWAXS measurement. K.R., P.J.D., M.G.K., M.K.N. and E.H.S. supervised the project. C.L. wrote the first draft of the paper. All the authors contributed to the revision and comments to the paper.
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Liu, C., Yang, Y., Fletcher, J.D. et al. Cation interdiffusion control for 2D/3D heterostructure formation and stabilization in inorganic perovskite solar modules. Nat Energy 10, 981–990 (2025). https://doi.org/10.1038/s41560-025-01817-6
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DOI: https://doi.org/10.1038/s41560-025-01817-6
