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Halide homogenization for low energy loss in 2-eV-bandgap perovskites and increased efficiency in all-perovskite triple-junction solar cells

Nature Energy volume 9, pages 70–80 (2024)Cite this article

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Abstract

Monolithic all-perovskite triple-junction solar cells have the potential to deliver power conversion efficiencies beyond those of state-of-art double-junction tandems and well beyond the detailed-balance limit for single junctions. Today, however, their performance is limited by large deficits in open-circuit voltage and unfulfilled potential in both short-circuit current density and fill factor in the wide-bandgap perovskite sub cell. Here we find that halide heterogeneity—present even immediately following materials synthesis—plays a key role in interfacial non-radiative recombination and collection efficiency losses under prolonged illumination for Br-rich perovskites. We find that a diammonium halide salt, propane-1,3-diammonium iodide, introduced during film fabrication, improves halide homogenization in Br-rich perovskites, leading to enhanced operating stability and a record open-circuit voltage of 1.44 V in an inverted (p–i–n) device; ~86% of the detailed-balance limit for a bandgap of 1.97 eV. The efficient wide-bandgap sub cell enables the fabrication of monolithic all-perovskite triple-junction solar cells with an open-circuit voltage of 3.33 V and a champion PCE of 25.1% (23.87% certified quasi-steady-state efficiency).

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Fig. 1: Photovoltaic performance of 1.97 eV wide-bandgap PSCs.
Fig. 2: Photostability and cell performance of 1.97 eV wide-bandgap PSCs during in situ PL and J–V measurements.
Fig. 3: Structure, composition and formation kinetics of Br-rich wide-bandgap perovskite films.
Fig. 4: Photovoltaic performance and simulations of monolithic all-perovskite triple-junction solar cells.

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All data generated or analysed during this study are included in the published article and its Supplementary Information and Source Data files. Further data that support the findings of this study are available from the corresponding authors on reasonable request. Source data are provided with this paper.

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Acknowledgements

We thank D. Ginger and F. Jiang of the University of Washington for facilitating the PiFM and discussions on PL mapping experiments. This work was partly supported by the Ontario Research Fund Research Excellence programme (ORF7: Ministry of Research and Innovation, Ontario Research Fund Research Excellence Round 7). This work was also supported by the King Abdullah University of Science and Technology under award number OSR-2020-CRG9-4350.2. The authors from the Eindhoven University of Technology acknowledge funding by The Netherlands Organization for Scientific Research (NWO) through the Joint Solar Programme III (project 680.91.011) and the Spinoza prize awarded to R.A.J.J. and by the Ministry of Education, Culture and Science (Gravity programme 024.001.035). We also acknowledge Solliance, a partnership of R&D organizations from The Netherlands, Belgium and Germany working in thin-film photovoltaic solar energy. J.W. and R.A.J.J. acknowledge funding from the EU’s Horizon Europe research and innovation under grant agreement number 101075605 (SuPerTandem). K.H. acknowledges the Department of Energy, Basic Energy Sciences DE-SC0013957 for supporting his PiFM microscopy work in support of the project. A.D. would like to thank the Penrose Scholarship for funding his studentship. R.A.O. and G.K. acknowledge financial support from the Engineering and Physical Sciences Research Council (EPSRC) (under EP/R025193/1). S.H. and H.J.S. acknowledge funding from the EU’s Horizon Europe research and innovation programme under grant agreement number 101075330 (NEXUS). H.J.S. also acknowledges funding from the EPSRC UK under EP/S004947/1. We thank the Canadian Light Source (CLS) for support through a travel grant. GIWAXS patterns were collected at the BXDS Beamline at the CLS with the assistance of A. Leontowich and C.-Y. Kim. The CLS is funded by NSERC, the Canadian Institutes of Health Research, Canada Foundation for Innovation, the Government of Saskatchewan, Western Economic Diversification Canada and the University of Saskatchewan. We thank T. Song for efficiency certification in NREL.

Author information

Author notes

  1. These authors contributed equally: Junke Wang, Lewei Zeng, Dong Zhang, Aidan Maxwell, Hao Chen.

Authors and Affiliations

  1. The Edward S. Rogers Sr. Department of Electrical and Computer Engineering, University of Toronto, Toronto, Ontario, Canada

    Junke Wang, Lewei Zeng, Aidan Maxwell, Hao Chen, Zaiwei Wang, Chongwen Li, Sam Teale, Luke Grater, Bin Chen & Edward H. Sargent

  2. Molecular Materials and Nanosystems, Institute for Complex Molecular Systems, Eindhoven University of Technology, partner of Solliance, Eindhoven, The Netherlands

    Junke Wang, Dong Zhang, Kunal Datta, Alessandro Caiazzo, Willemijn H. M. Remmerswaal, Nick R. M. Schipper, Riccardo Ollearo, Laura Bellini, Martijn M. Wienk & René A. J. Janssen

  3. TNO, partner of Solliance, Eindhoven, The Netherlands

    Dong Zhang

  4. Materials Simulation and Modelling, Department of Applied Physics, Eindhoven University of Technology, Eindhoven, The Netherlands

    Zehua Chen

  5. Department of Chemistry, University of Washington, Seattle, WA, USA

    Kevin Ho

  6. Department of Physics, University of Oxford, Oxford, United Kingdom

    Akash Dasgupta, Shuaifeng Hu & Henry J. Snaith

  7. Department of Materials Science and Metallurgy, University of Cambridge, Cambridge, United Kingdom

    Gunnar Kusch & Rachel A. Oliver

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

    Bin Chen & Edward H. Sargent

  9. Dutch Institute for Fundamental Energy Research, Eindhoven, The Netherlands

    René A. J. Janssen

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

    Edward H. Sargent

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  1. Junke Wang
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Contributions

J.W., L.Z., D.Z., M.M.W., R.A.J.J. and E.H.S. planned the research and analysed the results. J.W. and L.Z. fabricated the triple-junction cells. J.W., L.Z., H.C., A.M. and C.L. prepared the triple cells for certifications. J.W. optimized the wide-bandgap sub cells and coordinated all the characterization of materials and devices. H.C. optimized the mid-bandgap sub cell. A.M. and C.L. optimized the narrow-bandgap sub cell. W.H.M.R. performed the absolute PL and QFLS analysis. K.D. developed and helped measure the in situ PL/J − V characteristics and wrote the LabVIEW code. A.C. performed the XPS and in situ absorption measurements. L.Z., N.R.M.S. and L.B. fabricated and characterized perovskite thin films for stability. Z.C. performed DFT calculations. K.H. performed PiFM and analysed the data. A.D. performed luminescence mapping and analysis. S.H. helped analyse the XRD data and crystallization dynamics. H.J.S. facilitated and supervised the luminescence imaging experiments. G.K. and R.A.O. carried out the SEM cathodoluminescence measurements and analysis. R.O. performed the transient photocurrent measurements. S.T. and L.G. performed the GIWAX measurements. D.Z. performed optical simulations and provided the IOH substrates for triple-junction cells. Z.W. and B.C. provided valuable suggestions for optimizing the wide-bandgap sub cell and 3 J device configurations. J.W. wrote the first manuscript, and all authors commented on it. E.H.S. and R.A.J.J. supervised the project.

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Correspondence to René A. J. Janssen or Edward H. Sargent.

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H.J.S. is cofounder and CSO of Oxford PV Ltd. All other authors declare no competing interests.

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Wang, J., Zeng, L., Zhang, D. et al. Halide homogenization for low energy loss in 2-eV-bandgap perovskites and increased efficiency in all-perovskite triple-junction solar cells. Nat Energy 9, 70–80 (2024). https://doi.org/10.1038/s41560-023-01406-5

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