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:

Expanding the low-dimensional interface engineering toolbox for efficient perovskite solar cells

Abstract

Three-dimensional/low-dimensional perovskite solar cells afford improved efficiency and stability. The design of low-dimensional capping materials is constrained to tuning the A-site organic cation, as Pb2+ and Sn2+ are the only options for the metal cation. Here we unlock access to a library of low-dimensional capping materials with metal cations beyond Pb2+/Sn2+ by processing a full precursor solution containing both metal and ammonium halides. This enables easier synthetic control of the low-dimensional capping layer and greater versatility for low-dimensional interface engineering. We demonstrate that a zero-dimensional zinc-based halogenometallate (PEA2ZnX4; PEA = phenethylammonium, X = Cl/I) induces more robust surface passivation and stronger n–N isotype three-dimensional/low-dimensional heterojunctions than its lead-based counterpart. We exhibit p–i–n solar cells with 24.1% efficiency (certified 23.25%). Our cells maintain 94.5% initial efficiency after >1,000 h of operation at the maximum power point. Our findings expand the material library for low-dimensional interface engineering and stabilization of highly efficient three-dimensional/low-dimensional perovskite solar cells.

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

Access options

Buy this article

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

Fig. 1: Fabrication diagram of the 3D/LD stack films and structural characterization.
Fig. 2: Device architecture and photovoltaic parameter evolution with LD capping materials.
Fig. 3: Comparison of optoelectronic properties.
Fig. 4: Device performance and stability.

Similar content being viewed by others

Data availability

All of the data needed to evaluate the conclusions in this study are included in the article, its Supplementary Information and Source Data. The data that support the findings of this study are openly available in DR-NTU (Data) at https://doi.org/10.21979/N9/G6R8YGSource Data are provided with this paper.

References

  1. Zhang, T. et al. Stable and efficient 3D–2D perovskite-perovskite planar heterojunction solar cell without organic hole transport layer. Joule 2, 2706–2721 (2018).

    Article  Google Scholar 

  2. Jung, E. H. et al. Efficient, stable and scalable perovskite solar cells using poly(3-hexylthiophene). Nature 567, 511–515 (2019).

    Article  Google Scholar 

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

    Article  Google Scholar 

  4. Wang, Y. et al. Thermodynamically stabilized β-CsPbI3-based perovskite solar cells with efficiencies >18%. Science 365, 591–595 (2019).

    Article  Google Scholar 

  5. Jang, Y.-W. et al. Intact 2D/3D halide junction perovskite solar cells via solid-phase in-plane growth. Nat. Energy 6, 63–71 (2021).

    Article  Google Scholar 

  6. Xue, J. et al. Reconfiguring the band-edge states of photovoltaic perovskites by conjugated organic cations. Science 371, 636–640 (2021).

    Article  Google Scholar 

  7. Zhang, F. et al. Metastable Dion–Jacobson 2D structure enables efficient and stable perovskite solar cells. Science 375, 71–76 (2022).

    Article  Google Scholar 

  8. Yang, G. et al. Stable and low-photovoltage-loss perovskite solar cells by multifunctional passivation. Nat. Photon. 15, 681–689 (2021).

    Article  MathSciNet  Google Scholar 

  9. Tan, S. et al. Stability-limiting heterointerfaces of perovskite photovoltaics. Nature https://doi.org/10.1038/s41586-022-04604-5 (2022).

  10. Azmi, R. et al. Damp heat-stable perovskite solar cells with tailored-dimensionality 2D/3D heterojunctions. Science 376, 73–77 (2022).

    Article  Google Scholar 

  11. Grancini, G. & Nazeeruddin, M. K. Dimensional tailoring of hybrid perovskites for photovoltaics. Nat. Rev. Mater. 4, 4–22 (2018).

    Article  Google Scholar 

  12. Li, X., Hoffman, J. M. & Kanatzidis, M. G. The 2D halide perovskite rulebook: how the spacer influences everything from the structure to optoelectronic device efficiency. Chem. Rev. 121, 2230–2291 (2021).

    Article  Google Scholar 

  13. Zhang, F. et al. Advances in two-dimensional organic–inorganic hybrid perovskites. Energy Environ. Sci. 13, 1154–1186 (2020).

    Article  Google Scholar 

  14. Choi, H. S. & Kim, H. S. 3D/2D bilayered perovskite solar cells with an enhanced stability and performance. Materials 13, 3868 (2020).

    Article  Google Scholar 

  15. Mahmud, M. A. et al. Origin of efficiency and stability enhancement in high‐performing mixed dimensional 2D–3D perovskite solar cells: a review. Adv. Funct. Mater. 32, 2009164 (2021).

    Article  Google Scholar 

  16. Wu, G. et al. Surface passivation using two dimensional perovskites towards efficient and stable perovskite solar cells. Adv. Mater. 34, 2105635 (2021).

    Article  Google Scholar 

  17. Bai, Y. et al. Dimensional engineering of a graded 3D–2D halide perovskite interface enables ultrahigh VOC enhanced stability in the p–i–n photovoltaics. Adv. Energy Mater. 7, 1701038 (2017).

    Article  Google Scholar 

  18. Ye, T. et al. Efficient and ambient-air-stable solar cell with highly oriented 2D@3D perovskites. Adv. Funct. Mater. 28, 1801654 (2018).

    Article  Google Scholar 

  19. Alharbi, E. A. et al. Atomic-level passivation mechanism of ammonium salts enabling highly efficient perovskite solar cells. Nat. Commun. 10, 3008 (2019).

    Article  Google Scholar 

  20. Liu, Y. et al. Ultrahydrophobic 3D/2D fluoroarene bilayer-based water-resistant perovskite solar cells with efficiencies exceeding 22%. Sci. Adv. 5, eaaw2543 (2019).

    Article  Google Scholar 

  21. Zhu, H. et al. Tailored amphiphilic molecular mitigators for stable perovskite solar cells with 23.5% efficiency. Adv. Mater. 32, 1907757 (2020).

    Article  Google Scholar 

  22. Yang, B. et al. Interfacial passivation engineering of perovskite solar cells with fill factor over 82% and outstanding operational stability on n–i–p architecture. ACS Energy Lett. 6, 3916–3923 (2021).

    Article  Google Scholar 

  23. Li, F. et al. Regulating surface termination for efficient inverted perovskite solar cells with greater than 23% efficiency. J. Am. Chem. Soc. 142, 20134–20142 (2020).

    Article  Google Scholar 

  24. Rademeyer, M., Tsouris, C., Billing, D. G., Lemmerer, A. & Charmant, J. Robust motifs in 2-phenylethylammonium and related tetrahalometallates. CrystEngComm 13, 3485–3497 (2011).

    Article  Google Scholar 

  25. Qin, C. et al. Stable room-temperature continuous-wave lasing in quasi-2D perovskite films. Nature 585, 53–57 (2020).

    Article  Google Scholar 

  26. Liang, L., Luo, H., Hu, J., Li, H. & Gao, P. Efficient perovskite solar cells by reducing interface‐mediated recombination: a bulky amine approach. Adv. Energy Mater. 10, 2000197 (2020).

    Article  Google Scholar 

  27. Itoh, K., Hinasada, A., Matsunaga, H. & Nakamura, E. Disordered structure of Rb2ZnCl4 in the normal phase. J. Phys. Soc. Jpn. 52, 664–670 (1983).

    Article  Google Scholar 

  28. Lopez, A. & Anderson, R. L. Photocurrent spectra of Ge–GaAs heterojunctions. Solid-State Electron. 7, 695–700 (1964).

    Article  Google Scholar 

  29. Sharma, B. L. & Purohit, R. K. Semiconductor Heterojunctions (Pergamon, 1974).

  30. Bachmann, J. Atomic Layer Deposition in Energy Conversion Applications (John Wiley & Sons, 2017).

  31. Wang, F. et al. Interface dipole induced field‐effect passivation for achieving 21.7% efficiency and stable perovskite solar cells. Adv. Funct. Mater. 31, 2008052 (2020).

    Article  Google Scholar 

  32. Liu, J. et al. Efficient and stable perovskite-silicon tandem solar cells through contact displacement by MgFx. Science 377, 302–306 (2022).

    Article  Google Scholar 

  33. Zhang, P. et al. Triethyl phosphate in an antisolvent: a novel approach to fabricate high-efficiency and stable perovskite solar cells under ambient air conditions. Mater. Chem. Front. 5, 7628–7637 (2021).

    Article  Google Scholar 

  34. Chen, P. et al. In situ growth of 2D perovskite capping layer for stable and efficient perovskite solar cells. Adv. Funct. Mater. 28, 1706923 (2018).

    Article  Google Scholar 

  35. Ye, S. et al. Resolving spectral mismatch errors for perovskite solar cells in commercial class AAA solar simulators. J. Phys. Chem. Lett. 11, 3782–3788 (2020).

    Article  Google Scholar 

  36. Kiermasch, D., Gil-Escrig, L., Bolink, H. J. & Tvingstedt, K. Effects of masking on open-circuit voltage and fill factor in solar cells. Joule 3, 16–26 (2019).

    Article  Google Scholar 

  37. 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  Google Scholar 

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

    Article  Google Scholar 

  39. Lee, K., Murray, É. D., Kong, L., Lundqvist, B. I. & Langreth, D. C. Higher-accuracy van der Waals density functional. Phys. Rev. B 82, 081101 (2010).

    Article  Google Scholar 

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

    Article  Google Scholar 

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

    Article  MathSciNet  Google Scholar 

Download references

Acknowledgements

This work is supported by the Ministry of Singapore under its AcRF Tier 1 (Project RG6/21 (2021-T1-001-072) to Y.M.L.) and Tier 2 grants (MOE2019-T2-1-006 to T.C.S., MOE2019-T2-1-085 to Y.M.L. and MOE-T2EP50120-0004 to T.C.S.), and the National Research Foundation (NRF) Singapore under its NRF Investigatorship (NRF-NRFI2018-04 to T.C.S.). We thank the Facility for Analysis, Characterisation, Testing and Simulation (FACTS) (Nanyang Technological University, Singapore) for allowing us to use their electron microscopy, UPS instrument and X-ray facilities. We also thank the Solar Energy Research Institute of Singapore (SERIS) for PV authentication tests. We would like to thank Professor J. Bisquert (Universitat Jaume I) for the discussion on Mott–Schottky analysis. The computational work for this article was fully performed on resources of the National Supercomputing Centre, Singapore (https://www.nscc.sg).

Author information

Authors and Affiliations

Authors

Contributions

T.C.S., Y.M.L., S.Y. and H.R. conceived the idea for the manuscript and designed the experiments. S.Y. and H.R. performed sample preparation, device fabrication, optimization and characterization. M.F. and Y.G. conducted the TRPL measurements. Z.Y. and S.T. performed the UPS measurements. L.X. prepared the sample lamella by FIB. L.X. and C.B. conducted the TEM measurements. B.C. performed the SEM measurements. S.Y. and Q.Z. performed the KPFM measurements. H.R. conducted the XRD and GIWAXS measurements. D.H.L.S. conducted the TOF-SIMS measurements. Q.X. performed DFT calculations. B.W. performed the photoluminescence imaging analysis. H.H., Y.W. and X.X assisted device fabrication. All of the authors were involved in discussions of data analysis and commented on the manuscript. T.C.S., Y.M.L., S.Y. and H.R. wrote and revised the manuscript. T.C.S. and Y.M.L. led the project.

Corresponding authors

Correspondence to Yeng Ming Lam or Tze Chien Sum.

Ethics declarations

Competing interests

The authors declare no competing interests.

Peer review

Peer review information

Nature Energy thanks Wanyi Nie and the other, anonymous, reviewer(s) 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

Supplementary Notes 1–4, Figs. 1–41, Tables 1–18 and references.

Reporting Summary

Supplementary Video 1

The proposed FP capping process.

Supplementary Data 1

Source Data for Supplementary Fig. 36.

Supplementary Data 2

Source Data for Supplementary Tables 5–8 and 11–17.

Source data

Source Data Fig. 4

Source Data for Fig. 4b,d.

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

Ye, S., Rao, H., Feng, M. et al. Expanding the low-dimensional interface engineering toolbox for efficient perovskite solar cells. Nat Energy 8, 284–293 (2023). https://doi.org/10.1038/s41560-023-01204-z

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41560-023-01204-z

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