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.
This is a preview of subscription content, access via your institution
Access options
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$32.99 / 30 days
cancel any time
Subscribe to this journal
Receive 12 digital issues and online access to articles
$119.00 per year
only $9.92 per issue
Buy this article
- Purchase on SpringerLink
- Instant access to the full article PDF.
USD 39.95
Prices may be subject to local taxes which are calculated during checkout




Similar content being viewed by others
Data availability
All data are available in the main text or the Supplementary Information. Source data are provided with this paper.
References
Saliba, M., Correa-Baena, J.-P., Grätzel, M., Hagfeldt, A. & Abate, A. Perovskite solar cells: from the atomic level to film quality and device performance. Angew. Chem. Int. Ed. 57, 2554–2569 (2018).
Leijtens, T., Bush, K. A., Prasanna, R. & McGehee, M. D. Opportunities and challenges for tandem solar cells using metal halide perovskite semiconductors. Nat. Energy 3, 828–838 (2018).
Zheng, J. et al. Efficient flexible monolithic perovskite–CIGS tandem solar cell on conductive steel substrate. ACS Energy Lett. 9, 1545–1547 (2024).
Wang, L. et al. Cost analysis of perovskite/Cu(In,Ga)Se2 tandem photovoltaic with module replacement. ACS Energy Lett. 7, 1920–1925 (2022).
Tang, J. et al. Power generation density boost of bifacial tandem solar cells revealed by high throughput optoelectrical modelling. Energy Environ. Sci. 17, 6068–6078 (2024).
Jiang, Y. et al. High-mobility In2O3:H electrodes for four-terminal perovskite/CuInSe2 tandem solar cells. ACS Nano 14, 7502–7512 (2020).
Kothandaraman, R. K., Jiang, Y., Feurer, T., Tiwari, A. N. & Fu, F. Near-infrared-transparent perovskite solar cells and perovskite-based tandem photovoltaics. Small Methods 4, 2000395 (2020).
Zhang, Y. et al. Non-destructive buffer enabling near-infrared-transparent inverted inorganic perovskite solar cells toward 1,400 h light-soaking stable perovskite/Cu(In,Ga)Se2 tandem solar cells. J. Energy Chem. 97, 622–629 (2024).
Liang, B. et al. Quasi-flat narrow bandgap CIGS bottom cell application in perovskite/CIGS tandem solar cells. Energy Mater. Adv. 5, 0127 (2024).
Green, M. A. et al. Solar cell efficiency tables (version 64). Prog. Photovoltaics Res. Appl. 32, 425–441 (2024).
Huang, T. et al. Performance-limiting formation dynamics in mixed-halide perovskites. Sci. Adv. 7, eabj1799 (2021).
Niu, X. et al. Anion confinement for homogeneous mixed halide perovskite film growth by electrospray. Adv. Mater. 35, 2305822 (2023).
Slotcavage, D. J., Karunadasa, H. I. & McGehee, M. D. Light-induced phase segregation in halide-perovskite absorbers. ACS Energy Lett. 1, 1199–1205 (2016).
Susic, I., Gil-Escrig, L., Palazon, F., Sessolo, M. & Bolink, H. J. Quadruple-cation wide-bandgap perovskite solar cells with enhanced thermal stability enabled by vacuum deposition. ACS Energy Lett. 7, 1355–1363 (2022).
Jiang, Q. et al. Compositional texture engineering for highly stable wide-bandgap perovskite solar cells. Science 378, 1295–1300 (2022).
Lin, R. et al. All-perovskite tandem solar cells with improved grain surface passivation. Nature 603, 73–78 (2022).
Kim, D. H. et al. Bimolecular additives improve wide-band-gap perovskites for efficient tandem solar cells with CIGS. Joule 3, 1734–1745 (2019).
Pei, F. et al. A binary 2D perovskite passivation for efficient and stable perovskite/silicon tandem solar cells. Nat. Commun. 15, 7024 (2024).
Wang, G. et al. Molecular engineering of hole-selective layer for high band gap perovskites for highly efficient and stable perovskite-silicon tandem solar cells. Joule 7, 2583–2594 (2023).
Jošt, M. et al. Perovskite/CIGS tandem solar cells: from certified 24.2% toward 30% and beyond. ACS Energy Lett. 7, 1298–1307 (2022).
Al-Ashouri, A. et al. Monolithic perovskite/silicon tandem solar cell with >29% efficiency by enhanced hole extraction. Science 370, 1300–1309 (2020).
Chen, H. et al. Improved charge extraction in inverted perovskite solar cells with dual-site-binding ligands. Science 384, 189–193 (2024).
Park, S. M., Abtahi, A., Boehm, A. M. & Graham, K. R. Surface ligands for methylammonium lead iodide films: surface coverage, energetics, and photovoltaic performance. ACS Energy Lett. 5, 799–806 (2020).
La-Placa, M.-G. et al. Vacuum-deposited 2D/3D perovskite heterojunctions. ACS Energy Lett. 4, 2893–2901 (2019).
Chen, C. et al. Arylammonium-assisted reduction of the open-circuit voltage deficit in wide-bandgap perovskite solar cells: the role of suppressed ion migration. ACS Energy Lett. 5, 2560–2568 (2020).
Kim, D. et al. Efficient, stable silicon tandem cells enabled by anion-engineered wide-bandgap perovskites. Science 368, 155–160 (2020).
Wang, M. et al. Ammonium cations with high pKa in perovskite solar cells for improved high-temperature photostability. Nat. Energy 8, 1229–1239 (2023).
Szabó, G. & Kamat, P. V. How cation migration across a 2D/3D interface dictates perovskite solar cell efficiency. ACS Energy Lett. 9, 193–200 (2024).
Luo, L. et al. Stabilization of 3D/2D perovskite heterostructures via inhibition of ion diffusion by cross-linked polymers for solar cells with improved performance. Nat. Energy 8, 294–303 (2023).
Zheng, Y. et al. Downward homogenized crystallization for inverted wide-bandgap mixed-halide perovskite solar cells with 21% efficiency and suppressed photo-induced halide segregation. Adv. Funct. Mater. 32, 2200431 (2022).
Tan, S. et al. Surface reconstruction of halide perovskites during post-treatment. J. Am. Chem. Soc. 143, 6781–6786 (2021).
Hu, J. et al. Anchoring of halogen-cleaved organic ligands on perovskite surfaces. Energy Environ. Sci. 15, 5340–5349 (2022).
Jiang, Q. et al. Surface passivation of perovskite film for efficient solar cells. Nat. Photonics 13, 460–466 (2019).
Wu, T. et al. Elimination of light-induced degradation at the nickel oxide-perovskite heterojunction by aprotic sulfonium layers towards long-term operationally stable inverted perovskite solar cells. Energy Environ. Sci. 15, 4612–4624 (2022).
Shi, L. et al. Gas chromatography–mass spectrometry analyses of encapsulated stable perovskite solar cells. Science 368, eaba2412 (2020).
Yoon, S. J., Kuno, M. & Kamat, P. V. Shift happens. How halide ion defects influence photoinduced segregation in mixed halide perovskites. ACS Energy Lett. 2, 1507–1514 (2017).
Zhang, H. et al. Phase segregation due to ion migration in all-inorganic mixed-halide perovskite nanocrystals. Nat. Commun. 10, 1088 (2019).
Yang, S. et al. Stabilizing halide perovskite surfaces for solar cell operation with wide-bandgap lead oxysalts. Science 365, 473–478 (2019).
McMeekin, D. P. et al. Intermediate-phase engineering via dimethylammonium cation additive for stable perovskite solar cells. Nat. Mater. 22, 73–83 (2023).
Park, J. et al. Controlled growth of perovskite layers with volatile alkylammonium chlorides. Nature 616, 724–730 (2023).
Shi, P. et al. Oriented nucleation in formamidinium perovskite for photovoltaics. Nature 620, 323–327 (2023).
Wen, J. et al. Steric engineering enables efficient and photostable wide-bandgap perovskites for all-perovskite tandem solar cells. Adv. Mater. 34, 2110356 (2022).
Xu, J. et al. Triple-halide wide–band gap perovskites with suppressed phase segregation for efficient tandems. Science 367, 1097–1104 (2020).
Liu, J. et al. Efficient and stable perovskite-silicon tandem solar cells through contact displacement by MgFx. Science 377, 302–306 (2022).
Artuk, K. et al. A universal perovskite/C60 interface modification via atomic layer deposited aluminum oxide for perovskite solar cells and perovskite–silicon tandems. Adv. Mater. 36, 2311745 (2024).
Liu, C. et al. Bimolecularly passivated interface enables efficient and stable inverted perovskite solar cells. Science 382, 810–815 (2023).
Peña-Camargo, F. et al. Halide segregation versus interfacial recombination in bromide-rich wide-gap perovskite solar cells. ACS Energy Lett. 5, 2728–2736 (2020).
Wang, D. et al. Interfacial engineering of wide-bandgap perovskites for efficient perovskite/CZTSSe tandem solar cells. Adv. Funct. Mater. 32, 2107359 (2022).
Yang, G. et al. Defect engineering in wide-bandgap perovskites for efficient perovskite–silicon tandem solar cells. Nat. Photonics 16, 588–594 (2022).
Guan, H. et al. Low-dimensional 2-thiopheneethylammonium lead halide capping layer enables efficient single-junction methylamine-free wide-bandgap and tandem perovskite solar cells. Adv. Funct. Mater. 33, 2300860 (2023).
Hang, P. et al. Highly efficient and stable wide-bandgap perovskite solar cells via strain management. Adv. Funct. Mater. 33, 2214381 (2023).
Guan, H. et al. Regulating crystal orientation via ligand anchoring enables efficient wide-bandgap perovskite solar cells and tandems. Adv. Mater. 36, 2307987 (2024).
Yan, N. et al. Wide-bandgap perovskite solar cell using a fluoride-assisted surface gradient passivation strategy. Angew. Chem. Int. Ed. 62, e202216668 (2023).
Li, Z. et al. Stabilized hole-selective layer for high-performance inverted p–i–n perovskite solar cells. Science 382, 284–289 (2023).
Mariotti, S. et al. Interface engineering for high-performance, triple-halide perovskite–silicon tandem solar cells. Science 381, 63–69 (2023).
Han, Q. et al. High-performance perovskite/Cu(In,Ga)Se2 monolithic tandem solar cells. Science 361, 904–908 (2018).
Jošt, M. et al. 21.6%-efficient monolithic perovskite/Cu(In,Ga)Se2 tandem solar cells with thin conformal hole transport layers for integration on rough bottom cell surfaces. ACS Energy Lett. 4, 583–590 (2019).
Kafedjiska, I. et al. Advanced characterization and optimization of NiOx:Cu-SAM hole-transporting bi-layer for 23.4% efficient monolithic Cu(In,Ga)Se2-perovskite tandem solar cells. Adv. Funct. Mater. 33, 2302924 (2023).
Lin, S. et al. Adjustment of alkali element incorporations in Cu(In,Ga)Se2 thin films with wet chemistry Mo oxide as a hosting reservoir. Sol. Energy Mater. Sol. Cells 174, 16–24 (2018).
de Mello, J. C., Wittmann, H. F. & Friend, R. H. An improved experimental determination of external photoluminescence quantum efficiency. Adv. Mater. 9, 230–232 (1997).
Kresse, G. & Furthmüller, J. Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set. Comput. Mater. Sci. 6, 15–50 (1996).
Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54, 11169–11186 (1996).
Blöchl, P. E. Projector augmented-wave method. Phys. Rev. B 50, 17953–17979 (1994).
Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865–3868 (1996).
Weller, M. T., Weber, O. J., Frost, J. M. & Walsh, A. Cubic perovskite structure of black formamidinium lead iodide, α-[HC(NH2)2]PbI3, at 298 K. J. Phys. Chem. Lett. 6, 3209–3212 (2015).
Egger, D. A. & Kronik, L. Role of dispersive interactions in determining structural properties of organic–inorganic halide perovskites: insights from first-principles calculations. J. Phys. Chem. Lett. 5, 2728–2733 (2014).
Lee, J.-H., Bristowe, N. C., Bristowe, P. D. & Cheetham, A. K. Role of hydrogen-bonding and its interplay with octahedral tilting in CH3NH3PbI3. Chem. Commun. 51, 6434–6437 (2015).
Wang, Y. et al. Density functional theory analysis of structural and electronic properties of orthorhombic perovskite CH3NH3PbI3. Phys. Chem. Chem. Phys. 16, 1424–1429 (2014).
Grimme, S., Ehrlich, S. & Goerigk, L. Effect of the damping function in dispersion corrected density functional theory. J. Comput. Chem. 32, 1456–1465 (2011).
Wang, V., Xu, N., Liu, J.-C., Tang, G. & Geng, W.-T. VASPKIT: a user-friendly interface facilitating high-throughput computing and analysis using VASP code. Comput. Phys. Commun. 267, 108033 (2021).
Kühne, T. D. et al. CP2K: an electronic structure and molecular dynamics software package - quickstep: efficient and accurate electronic structure calculations. J. Chem. Phys. 152, 194103 (2020).
Nosé, S. A unified formulation of the constant temperature molecular dynamics methods. J. Chem. Phys. 81, 511–519 (1984).
VandeVondele, J. & Hutter, J. Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases. J. Chem. Phys. 127, 114105 (2007).
Grimme, S., Antony, J., Ehrlich, S. & Krieg, H. A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H–Pu. J. Chem. Phys. 132, 154104 (2010).
Lu, T. & Chen, F. Multiwfn: a multifunctional wavefunction analyzer. J. Comput. Chem. 33, 580–592 (2012).
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.
Author information
Authors and Affiliations
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 J–V 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.
Corresponding authors
Ethics declarations
Competing interests
The authors declare no competing interests.
Peer review
Peer review information
Nature Energy thanks the anonymous reviewers for their contribution to the peer review of this work.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Supplementary Information (download PDF )
Supplementary Figs. 1–53, Tables 1–6, Notes 1–2, Videos 1–3 and Refs. 1–14.
Supplementary Video 1 (download MP4 )
Ab initio molecular dynamics of control perovskite surface.
Supplementary Video 2 (download MP4 )
Ab initio molecular dynamics of PEA+ perovskite surface.
Supplementary Video 3 (download MP4 )
Ab initio molecular dynamics of TAR 3 perovskite surface.
Source data
Source Data Figs. 3b,g,h and 4c–e,g (download XLSX )
Statistical source data.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
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
Received:
Accepted:
Published:
Version of record:
Issue date:
DOI: https://doi.org/10.1038/s41560-025-01761-5
This article is cited by
-
Flexible perovskite/silicon tandem solar cells with 33.6% efficiency
Nature (2026)
-
Crystallization suppression of mixed-halide intermediates for perovskite/Cu(In,Ga)Se2 tandem solar cells with improved efficiency
Nature Energy (2026)
-
In situ dynamic regulation of strain at the buried interface of stable perovskite solar cells
Nature Photonics (2026)
-
Dimensionality engineering of perovskites for stable heterojunction-based photovoltaics
Nature Reviews Materials (2025)
-
Organic A-cations in metal halide perovskite photovoltaics
Nature Reviews Chemistry (2025)


