Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

A matrix-confined molecular layer for perovskite photovoltaic modules

Subjects

Abstract

Metal halide perovskites with remarkable optoelectronic properties have become a competitive candidate for supporting the efficiency progression of photovoltaics. As the latest reported power conversion efficiency of research cells is comparable to that of commercialized silicon cells1,2,3, the industrialization of perovskite solar cells is on the horizon4,5. However, most high-efficiency inverted perovskite solar cells based on self-assembled molecules (SAMs) face challenges owing to the aggregation and hydrophobicity of the SAMs. Here we report a ‘SAM-in-matrix’ strategy to distribute partial SAMs into a stable matrix of tris(pentafluorophenyl)borane, which breaks the original molecular-stacking-induced aggregation. Two-dimensional lattice Monte Carlo simulations and experimental results reveal that this strategy forms efficient charge transport channels. SAM-in-matrix hole-transport-layer-based devices show universally higher efficiencies for various SAMs, with compact surface coverage, good conductivity and substantially fewer buried nanovoids. Moreover, this strategy shows prominent application potential for scalable production. A SAM-in-matrix hole transport layer on fluorine-doped tin oxide/NiOx substrate facilitates the formation of large-area perovskite films with good crystalline quality and enhanced conductivity of NiOx. A 1 m × 2 m large-area perovskite solar module is thus achieved with a certified efficiency of 20.05%.

This is a preview of subscription content, access via your institution

Access options

Buy this article

USD 39.95

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Construction of Me4PA@BCF HTL.
Fig. 2: Structural and optoelectronic properties of perovskite films.
Fig. 3: Me4PA@BCF HTL for large-area perovskite films.
Fig. 4: Uniformly high film quality and good photovoltaic performance of large-area modules.

Similar content being viewed by others

Data availability

The data that support the findings of this study are available in the paper and its Supplementary Information. Source data are available from the corresponding authors upon request.

References

  1. Chen, H. et al. Improved charge extraction in inverted perovskite solar cells with dual-site-binding ligands. Science 384, 189–193 (2024).

    Article  ADS  CAS  PubMed  Google Scholar 

  2. Liu, S. et al. Buried interface molecular hybrid for inverted perovskite solar cells. Nature 632, 536–542 (2024).

    Article  ADS  Google Scholar 

  3. Zhao, K. et al. peri-Fused polyaromatic molecular contacts for perovskite solar cells. Nature 632, 301–306 (2024).

    Article  ADS  CAS  Google Scholar 

  4. Zhu, P. et al. Toward the commercialization of perovskite solar modules. Adv. Mater. 36, 2307357 (2024).

    Article  CAS  Google Scholar 

  5. Aydin, E. et al. Pathways toward commercial perovskite/silicon tandem photovoltaics. Science 383, eadh3849 (2024).

    Article  CAS  PubMed  Google Scholar 

  6. Xiao, Y., Yang, X., Zhu, R. & Snaith, H. J. Unlocking interfaces in photovoltaics. Science 384, 846–848 (2024).

    Article  ADS  CAS  Google Scholar 

  7. Zhang, S. et al. Minimizing buried interfacial defects for efficient inverted perovskite solar cells. Science 380, 404–409 (2023).

    Article  ADS  CAS  PubMed  Google Scholar 

  8. Wang, H. et al. Impurity-healing interface engineering for efficient perovskite submodules. Nature 634, 1091–1095 (2024).

    Article  ADS  CAS  PubMed  Google Scholar 

  9. Jiang, Q. & Zhu, K. Rapid advances enabling high-performance inverted perovskite solar cells. Nat. Rev. Mater. 9, 399–419 (2024).

    Article  ADS  CAS  Google Scholar 

  10. Li, Z. et al. Stabilized hole-selective layer for high-performance inverted p–i–n perovskite solar cells. Science 382, 284–289 (2023).

    Article  ADS  CAS  PubMed  Google Scholar 

  11. Li, L. et al. Flexible all-perovskite tandem solar cells approaching 25% efficiency with molecule-bridged hole-selective contact. Nat. Energy 7, 708–717 (2022).

    Article  ADS  CAS  Google Scholar 

  12. Li, N. et al. Barrier reinforcement for enhanced perovskite solar cell stability under reverse bias. Nat. Energy 9, 1264–1274 (2024).

    Article  ADS  CAS  Google Scholar 

  13. Li, C. et al. Rational design of Lewis base molecules for stable and efficient inverted perovskite solar cells. Science 379, 690–694 (2023).

    Article  ADS  CAS  PubMed  Google Scholar 

  14. Jiang, Q. et al. Surface reaction for efficient and stable inverted perovskite solar cells. Nature 611, 278–283 (2022).

    Article  ADS  CAS  PubMed  Google Scholar 

  15. Li, M., Liu, M., Qi, F., Lin, F. R. & Jen, A. K. Y. Self-assembled monolayers for interfacial engineering in solution-processed thin-film electronic devices: design, fabrication, and applications. Chem. Rev. 124, 2138–2204 (2024).

    Article  CAS  PubMed  Google Scholar 

  16. Park, S. M. et al. Low-loss contacts on textured substrates for inverted perovskite solar cells. Nature 624, 289–294 (2023).

    Article  ADS  CAS  PubMed  Google Scholar 

  17. Ren, Z. et al. Poly(carbazole phosphonic acid) as a versatile hole-transporting material for p–i–n perovskite solar cells and modules. Joule 7, 2894–2904 (2023).

    Article  CAS  Google Scholar 

  18. Liu, T. et al. Efficient perovskite solar modules enabled by a UV-stable and high-conductivity hole transport material. Sci. Adv. 11, eadu3493 (2025).

    Article  ADS  CAS  PubMed Central  PubMed  Google Scholar 

  19. Jiang, Q. et al. Towards linking lab and field lifetimes of perovskite solar cells. Nature 623, 313–318 (2023).

    Article  ADS  CAS  PubMed  Google Scholar 

  20. Peng, W. et al. A versatile energy-level-tunable hole-transport layer for multi-composition inverted perovskite solar cells. Energy Environ. Sci. 18, 874–883 (2025).

    Article  CAS  Google Scholar 

  21. Piers, W. E. & Chivers, T. Pentafluorophenylboranes: from obscurity to applications. Chem. Soc. Rev. 26, 345–354 (1997).

    Article  CAS  Google Scholar 

  22. Welch, G. C., Juan, R. R. S., Masuda, J. D. & Stephan, D. W. Reversible, metal-free hydrogen activation. Science 314, 1124–1126 (2006).

    Article  ADS  CAS  PubMed  Google Scholar 

  23. Rombach, F. M., Haque, S. A. & Macdonald, T. J. Lessons learned from spiro-OMeTAD and PTAA in perovskite solar cells. Energy Environ. Sci. 14, 5161–5190 (2021).

    Article  CAS  Google Scholar 

  24. Zhao, Y. et al. A bilayer conducting polymer structure for planar perovskite solar cells with over 1,400 h operational stability at elevated temperatures. Nat. Energy 7, 144–152 (2022).

    Article  ADS  CAS  Google Scholar 

  25. Gu, H. et al. Design optimization of bifacial perovskite minimodules for improved efficiency and stability. Nat. Energy 8, 675–684 (2023).

    Article  ADS  CAS  Google Scholar 

  26. Wang, X. et al. Regulating phase homogeneity by self-assembled molecules for enhanced efficiency and stability of inverted perovskite solar cells. Nat. Photon. 18, 1269–1275 (2024).

    Article  ADS  CAS  Google Scholar 

  27. Zhou, J. et al. Molecular contacts with an orthogonal π-skeleton induce amorphization to enhance perovskite solar cell performance. Nat. Chem. 17, 564–570 (2025).

    Article  CAS  PubMed  Google Scholar 

  28. Wang, H. et al. Interfacial residual stress relaxation in perovskite solar cells with improved stability. Adv. Mater. 31, 1904408 (2019).

    Article  CAS  Google Scholar 

  29. Zheng, Z. et al. Pre-buried additive for cross-layer modification in flexible perovskite solar cells with efficiency exceeding 22%. Adv. Mater. 34, 2109879 (2022).

    Article  CAS  Google Scholar 

  30. Miao, Y. et al. Green solvent enabled scalable processing of perovskite solar cells with high efficiency. Nat. Sustain. 6, 1465–1473 (2023).

    Article  Google Scholar 

  31. Jiang, Q. et al. Surface passivation of perovskite film for efficient solar cells. Nat. Photon. 13, 460–466 (2019).

    Article  ADS  CAS  Google Scholar 

  32. Li, G. et al. Overcoming the limitations of sputtered nickel oxide for high-efficiency and large-area perovskite solar cells. Adv. Sci. 4, 1700463 (2017).

    Article  Google Scholar 

  33. Di Girolamo, D. et al. Progress, highlights and perspectives on NiO in perovskite photovoltaics. Chem. Sci. 11, 7746–7759 (2020).

    Article  PubMed  Google Scholar 

  34. Boyd, C. C. et al. Overcoming redox reactions at perovskite-nickel oxide interfaces to boost voltages in perovskite solar cells. Joule 4, 1759–1775 (2020).

    Article  CAS  Google Scholar 

  35. Li, J. et al. Enhancing the efficiency and longevity of inverted perovskite solar cells with antimony-doped tin oxides. Nat. Energy 9, 308–315 (2024).

    Article  ADS  CAS  Google Scholar 

  36. 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).

    Article  CAS  Google Scholar 

  37. Yang, Y. et al. Inverted perovskite solar cells with over 2,000 h operational stability at 85 °C using fixed charge passivation. Nat. Energy 9, 37–46 (2024).

    Article  ADS  CAS  Google Scholar 

  38. Yu, S. et al. Homogenized NiOx nanoparticles for improved hole transport in inverted perovskite solar cells. Science 382, 1399–1404 (2023).

    Article  ADS  CAS  PubMed  Google Scholar 

  39. Zhang, J. et al. Regulation of crystallization by Introducing a multistage growth template affords efficient and stable inverted perovskite solar cells. Energy Environ. Sci. 18, 3235–3247 (2025).

    Article  CAS  Google Scholar 

  40. Xu, P. et al. Retarding the growth kinetics of chemical bath deposited nickel oxide films for efficient inverted perovskite solar cells and minimodules. Adv. Mater. 37, 2505087 (2025).

    Article  CAS  Google Scholar 

  41. Kim, Y. et al. Ionic highways from covalent assembly in highly conducting and stable anion exchange membrane fuel cells. J. Am. Chem. Soc. 141, 18152–18159 (2019).

    Article  ADS  CAS  PubMed  Google Scholar 

  42. Becke, A. D. Density-functional thermochemistry. I. The effect of the exchange-only gradient correction. J. Chem. Phys. 96, 2155–2160 (1992).

    Article  ADS  CAS  Google Scholar 

  43. Wu, Q. & Yang, W. Empirical correction to density functional theory for van der Waals interactions. J. Chem. Phys. 116, 515–524 (2002).

    Article  ADS  CAS  Google Scholar 

  44. Giannozzi, P. et al. Advanced capabilities for materials modelling with Quantum ESPRESSO. J. Phys. Condens. Matter 29, 465901 (2017).

    Article  CAS  PubMed  Google Scholar 

  45. 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).

    Article  ADS  CAS  Google Scholar 

  46. 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).

    Article  CAS  Google Scholar 

  47. Blöchl, P. E. Projector augmented-wave method. Phys. Rev. B 50, 17953–17979 (1994).

    Article  ADS  Google Scholar 

  48. Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865–3868 (1996).

    Article  ADS  CAS  PubMed  Google Scholar 

  49. Monkhorst, H. J. & Pack, J. D. Special points for Brillouin-zone integrations. Phys. Rev. B 13, 5188–5192 (1976).

    Article  ADS  MathSciNet  Google Scholar 

Download references

Acknowledgements

This work was supported by the National Natural Science Foundation of China (NSFC, grant nos. 22025505, 22220102002, 22522903, 52203334, 22479098 and 52403330), the Natural Science Foundation of Shanghai (grant nos. 23ZR1432300 and 23ZR1428000), the China Postdoctoral Science Foundation (grant nos. 2024M761964 and GZB20250060) and the Oceanic Interdisciplinary Program of Shanghai Jiao Tong University (grant no. SL2022ZD105). We thank the Shanghai Synchrotron Radiation Facility for the assistance with the GIWAXS measurements. We thank the Instrumental Analysis Centers at Shanghai Jiao Tong University and School of Environmental Science and Engineering for assistance with the material characterizations. We thank B. Dai for the assistance with the ssNMR measurements.

Author information

Authors and Affiliations

Authors

Contributions

Y. Zhao, Y. Chen, Y.M. and Y.G. designed and directed the research. Y. Liang, Yao Wang and Y. Zou carried out the fabrication and characterization of the perovskite films and PSCs. G.C., K.M., C.Z. and C.O. assisted with the fabrication of large modules. M.F., T.Z., R.X. and Y. Lou assisted with the modification of the PSCs. Yanming Wang, Y. Cho, Y. Chang and T.L. performed the theoretical calculations. Y. Liang carried out the AFM and photoluminescence mapping measurements and data analysis. B.L. participated in the SEM, HRTEM and time-of-flight secondary-ion mass spectrometry characterizations and data analysis. L.L. and N.Z. performed the time-resolved photoluminescence and photoluminescence quantum yield measurements. Y. Zhao, Y. Chen, Y.M., Y.G., Y. Liang, Yao Wang and Y. Zou wrote the paper with input from all authors.

Corresponding authors

Correspondence to Yanfeng Miao, Yongsheng Guo, Yuetian Chen or Yixin Zhao.

Ethics declarations

Competing interests

The authors declare no competing interests.

Peer review

Peer review information

Nature 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 )

This Supplementary Information file contains Supplementary Figs. 1–49, Table 1, Notes 1 and 2, and References.

Reporting Summary (download PDF )

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.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Liang, Y., Chen, G., Wang, Y. et al. A matrix-confined molecular layer for perovskite photovoltaic modules. Nature 648, 91–96 (2025). https://doi.org/10.1038/s41586-025-09785-3

Download citation

  • Received:

  • Accepted:

  • Published:

  • Version of record:

  • Issue date:

  • DOI: https://doi.org/10.1038/s41586-025-09785-3

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing