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Molecular-templated pre-assembly of self-assembled monolayer for perovskite solar cells and modules with improved reverse-bias stability

Abstract

Perovskite solar modules, particularly those using ultrathin self-assembled monolayer (SAM)-based hole transport layers, suffer from reverse-bias instability. Here we identified that discontinuous SAM distribution causes shunting and a lower breakdown voltage, while indium tin oxide-triggered electrochemical deprotonation of formamidinium ions leads to reduced long-term stability under reverse-bias conditions. To address these issues, we developed a molecular-templated pre-assembly strategy driven by hydrogen-bonding interactions between the SAM and a polycarbazole template. This approach ensures homogeneous clusters in solution and strong substrate interactions, yielding dense and uniform layers. Subsequently, we prepared minimodules with 24.0% efficiency (certified steady-state efficiency of 23.2%) and improved reverse-bias stability. Small-area devices retained 95% efficiency after 300 h at −4.8 V, while minimodules exhibited a T98 lifetime of 312 h under negative open-circuit voltage stress. We showed that a single bypass diode can protect at least 16 subcells, setting a new reliability benchmark for scalable perovskite photovoltaics.

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Fig. 1: Degradation mechanism at the buried interface under reverse bias.
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Fig. 2: Molecular-templated pre-assembly reinforces the buried interface.
The alternative text for this image may have been generated using AI.
Fig. 3: Efficiency and long-term stability of PSCs.
The alternative text for this image may have been generated using AI.
Fig. 4: Efficiency and long-term stability of PSMs.
The alternative text for this image may have been generated using AI.

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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.

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Acknowledgements

Y.H. acknowledges the support from the Agency for Science, Technology and Research (A*STAR) through an MTC IRG Grant (M23M6c0108). The authors of this paper are affiliated to the Solar Energy Research Institute of Singapore (SERIS), a research institute at the National University of Singapore (NUS). SERIS is supported by the National University of Singapore (NUS), the National Research Foundation Singapore (NRF), the Energy Market Authority of Singapore (EMA) and the Singapore Economic Development Board (EDB). We acknowledge that the computational work involved in this research was fully supported by NUS IT’ s Research Computing group (grant no. NUSREC-HPC-00001). We acknowledge J. Zheng and V. Kumar for their help with the lock-in thermography measurements. We acknowledge support of the MD simulations by Huasuan Technology. J.A.S. acknowledges the financial support of the Australian Research Council (DE230100173). We thank the staff of the BL11 NCD-SWEET beamline of ALBA Synchrotron for their assistance in recording the synchrotron X-ray scattering data.

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Contributions

Y.H., X.W., R.L. and N.L. conceived the idea and designed the experiments. Y.H. supervised the project. X.W. and J.L. fabricated the solar cells and modules. R.L. performed the DFT calculations and theoretical analysis. S.U. and A.N. conducted the lock-in thermography and analysed the data. X.Y. synthesized PolyCz-C4H9. X.W., T.W., Z.Z., Y.W., J.H., J.C., Z.J., Z.S., X.D., X.N., J.A.S., E.S. and Z.D. assisted with the device and materials characterizations. X.W., R.L., N.L., T.W. and Y.H. analysed the data and wrote the paper. Y.H., X.W., R.L., N.L., T.W. and J.L. reviewed and edited the paper. All authors read and commented on the paper.

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Correspondence to Yi Hou.

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Y.H. is the founder of Singfilm Solar, a company commercializing perovskite photovoltaics. The remaining authors declare no competing interests.

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Wang, X., Luo, R., Li, N. et al. Molecular-templated pre-assembly of self-assembled monolayer for perovskite solar cells and modules with improved reverse-bias stability. Nat Energy (2026). https://doi.org/10.1038/s41560-026-02014-9

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