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Regulating surface potential maximizes voltage in all-perovskite tandems

A Publisher Correction to this article was published on 24 July 2023

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The open-circuit voltage (VOC) deficit in perovskite solar cells is greater in wide-bandgap (over 1.7 eV) cells than in perovskites of roughly 1.5 eV (refs. 1,2). Quasi-Fermi-level-splitting measurements show VOC-limiting recombination at the electron-transport-layer contact3,4,5. This, we find, stems from inhomogeneous surface potential and poor perovskite–electron transport layer energetic alignment. Common monoammonium surface treatments fail to address this; as an alternative, we introduce diammonium molecules to modify perovskite surface states and achieve a more uniform spatial distribution of surface potential. Using 1,3-propane diammonium, quasi-Fermi-level splitting increases by 90 meV, enabling 1.79 eV perovskite solar cells with a certified 1.33 V VOC and over 19% power conversion efficiency (PCE). Incorporating this layer into a monolithic all-perovskite tandem, we report a record VOC of 2.19 V (89% of the detailed balance VOC limit) and over 27% PCE (26.3% certified quasi-steady state). These tandems retained more than 86% of their initial PCE after 500 h of operation.

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Fig. 1: Analysis and strategies for the minimization of recombination between perovskite and ETL.
Fig. 2: Surface inhomogeneity and its remediation using surface-adsorbed molecular layers.
Fig. 3: Characterization of WBG perovskite solar cells.
Fig. 4: PV performance and stability of perovskite tandem solar cells.

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Data availability

All data are available in the main text or supplementary materials. The data that support the findings of this study are available from the corresponding authors on reasonable request.

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The code that supports the findings of this study is available from the corresponding authors on reasonable request.

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We thank J. Warby for a useful discussion that contributed to our understanding of perovskite–ETL interfaces, and T. Song and N. Kopidakis at NREL for device certification. Z.W. acknowledges the Banting Postdoctoral Fellowships Program of Canada. GIWAXS patterns were collected at the BXDS-WLE Beamline at CLS with the assistance of C.-Y. Kim and A. Leontowich. This research was made possible by the US Department of the Navy, Office of Naval Research (grant nos. N00014-20-1-2572 and N00014-20-1-2725) and the US Department of Energy’s Office of Energy Efficiency and Renewable Energy under Solar Energy Technologies Office Award no. 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). This work was also supported by the King Abdullah University of Science and Technology under award no. OSR-CRG2020-4350. This work was authored in part by the National Renewable Energy Laboratory, operated by Alliance for Sustainable Energy for the US Department of Energy under contract no. DE-AC36-08GO28308. NREL authors acknowledge support from the Operational Energy Capability Improvement Fund of the Department of Defense. The views expressed in the article do not necessarily represent the views of the Department of Energy or the US Government. CLS is funded by NSERC, the Canadian Institutes of Health Research, CFI, the Government of Saskatchewan, Western Economic Diversification Canada and the University of Saskatchewan. This work was also supported by the Natural Sciences and Engineering Council of Canada and the Vanier Canada Graduate Scholarship.

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Authors and Affiliations



H.C., A.M., S.T. and B.C. planned experiments and coordinated the work. H.C. fabricated WBG devices and tandems for performance and certification and fabricated perovskite films for characterization. H.C., A.M., C. Li and L.C. fabricated NBG devices and tandems. S.T. and A.M. wrote the original draft. S.T., B.C., E.U. and S.D.W. carried out optical spectroscopy of films and devices and performed data analysis. T.Z. carried out DFT calculations. G.H. and S.D.W. performed UPS measurements and data analysis. P.S. and T.F. carried out KPFM and data analysis. S.T. and L.G. performed GIWAXS measurements and analysed data. J.W., Z.W., L.Z., S.M.P. and L.G. helped optimize the single-junction and tandem device structure. R.A.A. conducted thermal admittance spectroscopy measurements. X.Z., J.M.L., C.X., B.S., C. Liu, Y. Yang, M.G.K. and N.J.P. assisted with device analysis and data interpretation. E.H.S., Y. Yan, S.D.W. and M.G.K. secured funding and helped to review and edit the manuscript.

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Correspondence to Yanfa Yan or Edward H. Sargent.

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Chen, H., Maxwell, A., Li, C. et al. Regulating surface potential maximizes voltage in all-perovskite tandems. Nature 613, 676–681 (2023).

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