Abstract
Self-assembled monolayers (SAMs) represent an effective strategy for the development of perovskite solar cells (PSCs). High-performance PSCs are typically fabricated in an inert atmosphere because ambient moisture disrupts phosphonic-acid SAMs on transparent conductive oxides, leading to surface inhomogeneity and direct exposure of the transparent conductive oxide. However, this dependence on glovebox fabrication constrains scalability and cost-effective manufacturing. Here we present a ternary self-assembled molecular contact comprising glycerol dimethacrylate and 1-acetylguanidine that serves as a process-tolerant hole-selective contact. Glycerol dimethacrylate acts as a cosolvent during SAM deposition to improve film uniformity and is subsequently transformed into a hydrophilic binary network upon mild thermal curing, firmly anchoring the SAM to the substrate, whereas 1-acetylguanidine is incorporated to further suppress interfacial defects. Wide-bandgap PSCs fabricated in ambient conditions achieve a power conversion efficiency of 21.20% (1.00 cm2), with an open-circuit voltage of 1.28 V. When implemented in monolithic perovskite/silicon tandems, cells achieve a power conversion efficiency of 31.72% (certified 31.36%) and 32.60% for fabrication in ambient and inert conditions, respectively. These findings demonstrate that our tailored hole-selective contact provides a robust and process-tolerant interfacial engineering approach for high-efficiency perovskite and tandem photovoltaics manufactured under ambient conditions.
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Data availability
The data that support the findings of this study are available within the Article and its Supplementary Information. Source data are provided with this paper. All other data related to this study are available from the corresponding authors upon reasonable request.
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Acknowledgements
This work was supported by the HMG-UNIST Industry-Academia Joint Research Lab programme; the Basic Science Research Program (RS-2018-NR030954) funded by the Ministry of Science, ICT and Future Planning (MSIP) through the National Research Foundation of Korea (NRF); and the Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant (20213091010010, Super Solar Cells) funded by the Ministry of Trade, Industry and Energy (MOTIE), Republic of Korea. This publication is also based upon work supported by King Abdullah University of Science and Technology (KAUST) under Award Nos. ORFS-CRG12-2024-6475 and ORFS-CRG11-2022-5045. K.J.C. and S.I.S. acknowledge support from the InnoCORE programme of the Ministry of Science and ICT (1.260007.01).
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Contributions
G.K. and S.I.S. conceived the idea and designed the experiments. G.K., A.P., T.G.A. and R.A. further developed the concept for tandem application. G.K. fabricated the ambient-processed single-junction PSC. G.K. and Y.I.N. fabricated the ambient-processed TSCs. A.P. optimized and fabricated the inert-processed TSCs. Y.P. and S.H. characterized the surface properties of the SAM and the WBG perovskite films. A.P. also performed Kelvin probe force microscopy analysis. E.N. carried out large-area film deposition. J.K. and N.S. fabricated devices with different bandgap absorbers. G.K. and D.S.U. performed SEM measurements. D.S.U. conducted hyperspectral PL measurements and performed QFLS data analysis. A.P. and T.G.A. developed QFLS analysis methods for large-area films and devices. R.W. performed an operational stability test. I.F.I. characterized charge transport analyses. T.G.A. fabricated the silicon bottom cells for inert processing, while G.H., S.N. and K.D. assisted in the preparation of silicon bottom cells for ambient processing. G.K. and S.I.S. wrote the manuscript. All authors provided feedback and comments for the manuscript revision. K.J.C., S.D.W. and S.I.S. directed and supervised the project.
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S.I.S. and G.K. have filed a patent application related to this work (Monomer-Integrated Ultra-Compact Self-Assembled Monolayers Network Enabling High-Efficiency Perovskite/Silicon Tandem Solar Cells, Republic of Korea (KR), Application No. 10-2026-0044821). The other authors declare no competing interests.
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Supplementary Figs. 1–70, Notes 1–5 and Tables 1–9.
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Source data for Fig. 1. Includes numerical data underlying the FTIR spectra (Fig. 1d), XPS spectra (Fig. 1e) and XRD patterns (Fig. 1f).
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Source data for Fig. 2. Includes numerical data underlying the PL emission spectra (Fig. 2g), TRPL decay curves (Fig. 2h) and QFLS values (Fig. 2i).
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Source data for Fig. 3. Includes statistical distributions of photovoltaic parameters (Fig. 3b,e), J–V curves (Fig. 3c,d) and EQE spectra (Fig. 3f).
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Source data for Fig. 4. Includes J–V curves (Fig. 4c), statistical distributions of photovoltaic parameters (Fig. 4d), EQE spectra (Fig. 4e), thermal stability (Fig. 4f) and operational stability tracked by MPP tracking (Fig. 4g).
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Kim, G., Prasetio, A., Noh, Y.I. et al. Ternary self-assembled molecular contact for ambient-processed perovskite/silicon tandem solar cells. Nat. Photon. (2026). https://doi.org/10.1038/s41566-026-01925-z
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DOI: https://doi.org/10.1038/s41566-026-01925-z
