Abstract
Hole-selective self-assembled monolayers (SAMs)1,2 have played a key role in driving the certified power conversion efficiency (PCE) of inverted perovskite solar cells3,4,5 to 26.7% (ref. 6). However, their instability often compromises the operational performance of devices, strongly hindering their practical applications7,8. Here we employ a cross-linkable co-SAM to enhance the conformational stability of hole-selective SAMs against external stresses, while suppressing the formation of defects and voids in SAM during self-assembly. The azide-containing SAM can be thermally activated to form a cross-linked and densely assembled co-SAM with a thermally stable conformation and preferred orientation. This effectively minimizes substrate surface exposure caused by wiggling of loose SAMs under thermal stress, preventing perovskite decomposition. This enables a certified PCE of 26.92% to be achieved for the best-performing cell, which also possesses excellent thermal stability with negligible decay under maximum-power-point tracking at 85 °C for 1,000 h. It also retains >98% of initial PCE after 700 repetitive thermal cycles between −40 °C and 85 °C, representing the state of the art of the field. This work offers an in-depth understanding of SAM degradation mechanisms to guide the design of a more robust buried interface for SAM-based devices adopting high-roughness substrates to realize highly efficient and durable perovskite solar cells.
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Acknowledgements
We thank M.Q.C. from City University of Hong Kong and Z.X.X. from the South University of Science and Technology for their support with long-term device stability tests. A.K.-Y.J. acknowledges sponsorship from the Lee Shau-Kee Chair Professor (Materials Science), and support from APRC grants of the City University of Hong Kong (grant nos. 9380086, 9610419, 9610440, 9610492 and 9610508), the TCFS (grant no. GHP/018/20SZ), MHKJFS (grant no. MHP/054/23) and MRP (grant no. MRP/040/21X) grants from the Innovation and Technology Commission of Hong Kong, the Green Tech Fund from the Environment and Ecology Bureau of Hong Kong (grant no. 202020164), and GRF (grant nos. 11304424, 11307621, 11316422 and 11308625) and CRS grants (CRS_CityU104/23, CRS_HKUST203/23) from the Research Grants Council of Hong Kong. This work was partially financially supported by the City University of Hong Kong (grant no. 9610739) via the ‘Fostering Innovation for Resilience and Sustainable Transformation’ project, which is officially endorsed by the United Nations Educational, Scientific and Cultural Organization under the International Decade of Sciences for Sustainable Development (2024–2033). J.Z. is grateful for sponsorship from the National Natural Science Foundation of China (grant no. 52002393). S.F.W. is grateful for the support from Start-up Fund (Lingnan University, Hong Kong). T.W. and Q.J. are grateful to the National Key R&D Program of China (grant no. 2023YFB3003001) and the National Natural Science Foundation of China (grant no. 52130101) for their support. We acknowledge Towngas Energy Chuangke (Shenzhen) for their assistance with device certification.
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Contributions
W.J., S.W. and A.J. conceived the original idea. W.J. refined the experimental protocol, and designed and synthesized JJ24 under the supervision of A.J. The perovskite films and devices were fabricated by G.Q., S.W. and J.Z. Data analysis was performed by W.J. and G.Q. under the guidance of S.W., J.Z. and A.J. Theoretical calculations were performed by L.C. and T.W. under the supervision of Q.J., X.H. and X.C., and C-T.W. assisted with characterization and device fabrication. F.R.L. and C.Y. provided helpful discussions. W.J. wrote the paper, which was revised by G.Q., S.W., J.Z. and A.J. All authors discussed the results and commented on the paper. A.J. supervised the project.
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Extended data figures and tables
Extended Data Fig. 1 J-V curves of other p-type SAMs toughened with JJ24.
J-V characteristics of the champion PSCs based on 4PACz, CbzPh and CbzBT with and without JJ24 cross-linking.
Extended Data Fig. 2 Long-term operational stability of devices based other p-type SAMs toughened with JJ24.
Long-term operational stability of the encapsulated PSCs based on different p-type SAM molecules at MPP tracking under continuous 1-sun equivalent illumination at 85 °C in ambient air with RH of 70–80%, complied with the ISOS-L-2 protocol.
Extended Data Fig. 3 Cross-sectional SEM images of perovskite films.
Cross-sectional SEM images of control and target perovskite films before and after ageing (under continuous illumination at 85 °C for 100 h).
Extended Data Fig. 4 XRD patterns of perovskite films.
XRD patterns of control and target perovskite films before and after ageing (under continuous illumination at 85 °C for 100 h).
Supplementary information
Supplementary Information
Supplementary Notes 1 and 2, Figs. 1–39, Tables 1–4 and references.
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Jiang, W., Qu, G., Huang, X. et al. Toughened self-assembled monolayers for durable perovskite solar cells. Nature 646, 95–101 (2025). https://doi.org/10.1038/s41586-025-09509-7
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DOI: https://doi.org/10.1038/s41586-025-09509-7
