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Suppressed phase segregation for triple-junction perovskite solar cells

Nature volume 618, pages 74–79 (2023)Cite this article

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Abstract

The tunable bandgaps and facile fabrication of perovskites make them attractive for multi-junction photovoltaics1,2. However, light-induced phase segregation limits their efficiency and stability3,4,5: this occurs in wide-bandgap (>1.65 electron volts) iodide/bromide mixed perovskite absorbers, and becomes even more acute in the top cells of triple-junction solar photovoltaics that require a fully 2.0-electron-volt bandgap absorber2,6. Here we report that lattice distortion in iodide/bromide mixed perovskites is correlated with the suppression of phase segregation, generating an increased ion-migration energy barrier arising from the decreased average interatomic distance between the A-site cation and iodide. Using an approximately 2.0-electron-volt rubidium/caesium mixed-cation inorganic perovskite with large lattice distortion in the top subcell, we fabricated all-perovskite triple-junction solar cells and achieved an efficiency of 24.3 per cent (23.3 per cent certified quasi-steady-state efficiency) with an open-circuit voltage of 3.21 volts. This is, to our knowledge, the first reported certified efficiency for perovskite-based triple-junction solar cells. The triple-junction devices retain 80 per cent of their initial efficiency following 420 hours of operation at the maximum power point.

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Fig. 1: Properties of Rb/Cs mixed-cation inorganic perovskites.
Fig. 2: The phenomena and mechanism of suppressed LIPS.
Fig. 3: PV performance of 2.0-eV single-junction PSCs.
Fig. 4: PV performance and stability of all-perovskite TJSCs.

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Data availability

All data are available in the paper or its Supplementary Information. The crystallographic files (CIF) for the compounds reported in this work can be found as depositions in the Cambridge Crystallographic Data Centre (CCDC) based on the following deposition numbers: 2211086 (CsPbI1.46Br1.54), 2211087 (CsPbI1.73Br1.27) and 2211088 (Rb0.22Cs0.78PbI1.65Br1.35).

Code availability

The codes and post-analysis tools for calculations are available from the FHI-aims website: https://fhi-aims.org.

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Acknowledgements

This research was made possible by a US Department of the Navy, Office of Naval Research grant (N00014-20-1-2572), and the US Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE) under the Solar Energy Technologies Office Award Number DE-EE0008753. This work was supported in part by the Ontario Research Fund-Research Excellence programme (ORF7-Ministry of Research and Innovation, Ontario Research Fund-Research Excellence Round 7). M.G.K. was supported by the Office of Naval Research (ONR) under grant N00014-20-1-2725. At King Abdullah University of Science and Technology (KAUST), this work was supported by the under award no. OSR-2020-CRG9-4350.2. This work was also supported by the Natural Sciences and Engineering Council of Canada and the Vanier Canada Graduate Scholarship. Z.W. acknowledges the Banting Postdoctoral Fellowships Program of Canada. D.J.K. acknowledges the support of the University of Warwick. The UK High-Field Solid-State NMR Facility used in this research was funded by EPSRC and BBSRC (EP/T015063/1), as well as the University of Warwick, including via part funding through Birmingham Science City Advanced Materials Projects 1 and 2 supported by Advantage West Midlands (AWM) and the European Regional Development Fund (ERDF). The crystallographic experiments made use of the IMSERC Crystallography and Physical Characterization facilities at Northwestern University, which received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-2025633), and Northwestern University. The purchase of the Ag-microsource used to collect both single and powder diffraction data was supported by the Major Research Instrumentation Program for the National Science Foundation under the award CHE-1920248. This work also made use of the EPIC facility at Northwestern University’s NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-2025633), the IIN and Northwestern’s MRSEC programme (NSF DMR-1720139). Computations were performed on the Niagara supercomputer at the SciNet HPC Consortium. SciNet is funded by the Canada Foundation for Innovation; the Government of Ontario; Ontario Research Fund Research Excellence; and the University of Toronto. A.B. was supported, in part, by a fellowship through the National Defense Science and Engineering Graduate (NDSEG) Fellowship Program, sponsored by the Air Force Research Laboratory (AFRL), the Office of Naval Research (ONR) and Army Research Office (ARO). We thank Tao Song for efficiency certification in NREL. Z.W. thanks Yicheng Zhao, Zhenyi Ni and Emre Yengel for discussion about LIPS. A.B. acknowledges Christos D. Malliakas for assistance with the single-crystal measurements and discussions and thanks Abishek K. Iyler, Craig Laing and Michael Quintero for discussions.

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Author notes

  1. These authors contributed equally: Zaiwei Wang, Lewei Zeng, Tong Zhu, Hao Chen

Authors and Affiliations

  1. Department of Electrical and Computer Engineering, University of Toronto, Toronto, Ontario, Canada

    Zaiwei Wang, Lewei Zeng, Tong Zhu, Hao Chen, Bin Chen, Chongwen Li, Aidan Maxwell, Junke Wang, Sam Teale, Suhas Mahesh, Sasa Wang, Shuangyan Hu, Eui Dae Jung, Mingyang Wei, So Min Park, Luke Grater & Edward H. Sargent

  2. Department of Chemistry, Northwestern University, Evanston, IL, USA

    Bin Chen, Adam Balvanz, Merx G. Kanatzidis & Edward H. Sargent

  3. Department of Physics, University of Warwick, Coventry, UK

    Dominik J. Kubicki

  4. Department of Physics and Astronomy and Wright Center for Photovoltaics Innovation and Commercialization, The University of Toledo, Toledo, OH, USA

    Chongwen Li, Biwas Subedi, Zhaoning Song, Nikolas J. Podraza & Yanfa Yan

  5. KAUST Solar Center (KSC), Physical Sciences and Engineering Division (PSE), King Abdullah University of Science and Technology (KAUST), Thuwal, Kingdom of Saudi Arabia

    Esma Ugur, Erkan Aydin & Stefaan De Wolf

  6. Department of Materials Science and Engineering, Northwestern University, Evanston, IL, USA

    Roberto dos Reis, Matthew Cheng & Vinayak P. Dravid

  7. Department of Applied Physical Sciences, University of North Carolina at Chapel Hill, Chapel Hill, NC, USA

    Guang Yang & Jinsong Huang

  8. Department of Materials Science and Engineering, University of Toronto, Toronto, Ontario, Canada

    Deying Luo & Zheng-Hong Lu

  9. Department of Physics, Center for Optoelectronics Engineering Research, Yunnan University, Kunming, China

    Juntao Hu & Zheng-Hong Lu

  10. Laboratory of Photonics and Interfaces, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fedérale de Lausanne (EPFL), Lausanne, Switzerland

    Mingyang Wei & Michael Grätzel

  11. Department of Electrical and Computer Engineering, Northwestern University, Evanston, IL, USA

    Edward H. Sargent

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Contributions

Z.W. conceived the idea of this project. L.Z. and Z.W. fabricated the 2.0-eV bandgap devices and triple-junction solar cells for performance and fabricated the perovskite films for characterizations. H.C., L.Z. and Z.W. fabricated the 1.6-eV bandgap cells. L.Z., Z.W., A.M. and C.L. fabricated the 1.22-eV bandgap cells. T.Z. carried out the DFT calculations and analysed the data. H.C. prepared NiOx nanoparticles and developed the surface passivation of the inorganic perovskite layers and 1.6-eV perovskite layers. B.C. helped with experimental design and data analysis. D.J.K. carried out the solid-state NMR characterization, prepared the corresponding powders and analysed the data. A.B. prepared the crystals and carried out the crystal XRD and data analysis. C.L. carried out EQE measurements. E.U. carried out the PL mapping and QFLS analysis. R.d.R. and M.C. carried out the TEM-EDS and data analysis. G.Y. measured transient ion-migration currents and carried out data analysis. B.S. performed PDS characterizations and data analysis. D.L. and J. Hu carried out the depth-profile X-ray photoelectron spectroscopy characterization and data analysis. S.D.W. carried out the atomic force microscopy characterization. L.Z. and Z.W. carried out the UV–vis measurements, XRD measurements, PL measurements, J–V measurements and stability measurements. Z.W. wrote the original draft. E.H.S., L.W., T.Z., D.J.K. and A.M., helped to review and edit the manuscript. E.H.S. secured funding. All the authors contributed to the discussion of the results and the final manuscript preparation.

Corresponding author

Correspondence to Edward H. Sargent.

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Supplementary information

Supplementary Information

Supplementary Methods, Figs. 1–25, Tables 1–13, Notes 1–12 and References.

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Supplementary Data

CIFs 1–3: CIF 1, CsPbI1.46Br1.54; CIF 2, CsPbI1.73Br1.27; CIF 3, Rb0.22Cs0.78PbI1.65Br1.35.

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Wang, Z., Zeng, L., Zhu, T. et al. Suppressed phase segregation for triple-junction perovskite solar cells. Nature 618, 74–79 (2023). https://doi.org/10.1038/s41586-023-06006-7

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