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Inhibiting defect passivation failure in perovskite for perovskite/Cu(In,Ga)Se2 monolithic tandem solar cells with certified efficiency 27.35%

Abstract

Thin-film tandem solar cells with wide-bandgap perovskites and Cu(In,Ga)Se2 hold promise for cost-effective lightweight photovoltaics. However, the power conversion efficiency and stability of perovskite/Cu(In,Ga)Se2 tandem solar cells are not yet comparable to single-junction counterparts due to recombination losses and photothermal-induced degradation in wide-bandgap perovskites. In this study, we show that common strategies for perovskite passivation often fail under combined thermal and illumination stresses due to the passivator desorption. We demonstrate a robust passivator with deliberately designed functional groups that inhibits passivator desorption regardless of perovskite surface termination, enhances resistance to photothermal stresses and substantially suppresses phase segregation. The wide-bandgap perovskite solar cells achieved a champion power conversion efficiency of 23.5% with negligible degradation after 1,000 hours of continuous operation under 1-sun illumination at approximately 50 °C. When integrated into perovskite/Cu(In,Ga)Se2 tandem cells, they achieved the steady state power conversion efficiency of 27.93% (certified 27.35%), with stable operation for over 420 hours at ~38 °C in ambient air.

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Fig. 1: Passivation failure behaviour under photothermal stress and its suppression.
Fig. 2: DFT and ab initio molecular dynamic studies of interaction between aromatic ammonium cations and perovskite.
Fig. 3: Optoelectronic characterization of WBG perovskite films and devices.
Fig. 4: PV performance and stability of perovskite/CIGS TSCs.

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Acknowledgements

We acknowledge funding support from the National Key Research and Development Program of China (grant number 2020YFB0408002), the Beijing Natural Science Foundation (Z240024), the National Natural Science Foundation of China (grant numbers 22279083, 22461160281, 52202241, W2412076, 22479015). G.L. is grateful to the Qing Lan Project for financial support.

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Contributions

Q.C., Y.J. and F.P. conceived the idea. F.P. designed the device structures for single-junction WBG PSCs and top cells of the TSCs. Shuping Lin, X.H., M.Z., B.L. and D.Z. fabricated and optimized CIGS bottom cells. F.P. designed the experiments. Z.Z. and Shiju Lin assisted in device preparation. Z.Z. performed the DFT calculations and ab initio molecular dynamics simulation. J.X. helped with the analysis of the theoretical computation. X.Z. helped with the device performance test and analysis of film ageing data. Y.Z. fabricated the normal bandgap perovskite solar cells. Yanrun Chen helped with the in situ PL test. K.L. helped with the NMR measurements. L.W. and G.L. performed the TPV/TPC measurements. D.Q. and J.W. helped with the PLQY measurements. H.L. helped with the TRPL test. J.T. performed the dark JV test. W.Z. and Yihua Chen helped with the MPP test. Q.C., Y.J., F.P. and Z.Z wrote and revised the manuscript. All authors were involved in discussions of data analysis and commented on the manuscript.

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Correspondence to Yan Jiang or Qi Chen.

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Supplementary Figs. 1–53, Tables 1–6, Notes 1–2, Videos 1–3 and Refs. 1–14.

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Ab initio molecular dynamics of control perovskite surface.

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Ab initio molecular dynamics of PEA+ perovskite surface.

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Ab initio molecular dynamics of TAR 3 perovskite surface.

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Pei, F., Lin, S., Zhang, Z. et al. Inhibiting defect passivation failure in perovskite for perovskite/Cu(In,Ga)Se2 monolithic tandem solar cells with certified efficiency 27.35%. Nat Energy 10, 824–835 (2025). https://doi.org/10.1038/s41560-025-01761-5

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