Abstract
Perovskite solar cells represent a promising class of photovoltaics that have achieved exceptional levels of performance within a short time. Such high efficiencies often depend on the use of molecule-based selective contacts that form highly ordered molecular assemblies. Although this high degree of ordering usually benefits charge-carrier transport, it is disrupted by structure deformation and phase transformation when subjected to external stresses, which limits the long-term operational stability of perovskite solar cells. Here we demonstrate a molecular contact with an orthogonal π-skeleton that shows better resilience to external stimuli than commonly used conjugated cores. This molecular design yields a disordered, amorphous structure that is not only highly stable but also demonstrates exceptional charge selectivity and transport capability. The perovskite solar cells fabricated with this orthogonal π-skeleton molecule exhibited enhanced long-term durability in accelerated-ageing tests. This orthogonal π-skeleton functionality opens new opportunities in molecular design for applications in organic electronics.
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Acknowledgements
We thank L. Liu, Y. Nie, C. Mu, X. Miao, T. Zhou, X. Lu, Y. Chen, Z. Chen, Y. Cheng, D. Gu, C. Wang and M. Zhou for assistance with the characterizations. J. Xue acknowledges a grant from the National Natural Science Foundation of China (grant number 62274146). J. Xue and R.W. acknowledge grants (grant numbers LR24F040001, LD22E020002 and LD24E020001) from the Natural Science Foundation of Zhejiang Province of China. J. Xue acknowledges a grant of financial support from the Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering (2021SZ-FR006), and support from the Foundation for Innovative Research Groups of the National Natural Science Foundation of China (grant number 61721005). R.W. acknowledges a grant from the National Natural Science Foundation of China (grant number 62474143) and support from the Key R&D Program of Zhejiang (2024SSYS0061) This work was also supported by the National Natural Science Foundation of China (grant number 62204209), the Fundamental Research Funds for the Central Universities (226-2022-00200), the Zhejiang Key Laboratory of Low-Carbon Intelligent Synthetic Biology (2024ZY01025) and Muyuan Laboratory (programme ID 14136022401). H.-F.W. acknowledges a National Key Instrumentation Development grant from the National Natural Science Foundation of China (grant number 21727802).
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Contributions
J. Xue, R.W., J.Z. and Y.L. conceived the idea. J.Z. synthesized all the molecules. J.Z., R.L. and L.T. fabricated the perovskite films and devices. J.Z. and Y.L. performed the data analysis under the supervision of R.W. and J. Xue. K.Z., J. Shen, D.J., Z.P., L.Y., Q.L., S.Z., L.J., S.C., S.W., Y.T., J. Xu, X.Z., P.S., X.W., W.F., P.S., X.S. and J. Sun assisted with the characterizations and device fabrication. L.Z. and L.-Z.C. conducted the SFG-VS experiment with J.Z. under the supervision of H.-F.W. G.W., W.S. and T.D. performed the theoretical calculations. D.Y. provided insightful discussions. J. Xue wrote the manuscript. All the authors discussed the results and commented on the manuscript.
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Zhou, J., Luo, Y., Li, R. et al. Molecular contacts with an orthogonal π-skeleton induce amorphization to enhance perovskite solar cell performance. Nat. Chem. 17, 564–570 (2025). https://doi.org/10.1038/s41557-025-01732-z
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DOI: https://doi.org/10.1038/s41557-025-01732-z
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