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Low-loss contacts on textured substrates for inverted perovskite solar cells

Nature volume 624, pages 289–294 (2023)Cite this article

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Abstract

Inverted perovskite solar cells (PSCs) promise enhanced operating stability compared to their normal-structure counterparts1,2,3. To improve efficiency further, it is crucial to combine effective light management with low interfacial losses4,5. Here we develop a conformal self-assembled monolayer (SAM) as the hole-selective contact on light-managing textured substrates. Molecular dynamics simulations indicate that cluster formation during phosphonic acid adsorption leads to incomplete SAM coverage. We devise a co-adsorbent strategy that disassembles high-order clusters, thus homogenizing the distribution of phosphonic acid molecules, and thereby minimizing interfacial recombination and improving electronic structures. We report a laboratory-measured power conversion efficiency (PCE) of 25.3% and a certified quasi-steady-state PCE of 24.8% for inverted PSCs, with a photocurrent approaching 95% of the Shockley–Queisser maximum. An encapsulated device having a PCE of 24.6% at room temperature retains 95% of its peak performance when stressed at 65 °C and 50% relative humidity following more than 1,000 h of maximum power point tracking under 1 sun illumination. This represents one of the most stable PSCs subjected to accelerated ageing: achieved with a PCE surpassing 24%. The engineering of phosphonic acid adsorption on textured substrates offers a promising avenue for efficient and stable PSCs. It is also anticipated to benefit other optoelectronic devices that require light management.

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Fig. 1: Molecular dynamics simulations of phosphonic acid adsorption with and without molecular additives.
Fig. 2: Homogeneity of self-assembled monolayers formed on FTO substrates.
Fig. 3: Materials properties of perovskite films on different FTO/SAM substrates.
Fig. 4: Photovoltaic performance of perovskite solar cells.

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Data availability

All data are available in the main text or the supplementary materials. Further data are available from the corresponding author on reasonable request.

Code availability

The codes and postanalysis tools for molecular dynamics simulations are available in the following repository: https://doi.org/10.5281/zenodo.8393081.

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Acknowledgements

This research was made possible by the US Department of the Navy, Office of Naval Research Grant (N00014-20-1-2572). This work was supported in part by Ontario Research Fund-Research Excellence programme (ORF7-Ministry of Research and Innovation, Ontario Research Fund-Research Excellence Round 7). This work was also supported under award number OSR-CRG2020-4350.2. M.W. acknowledges funding from the European Union’s Horizon 2020 Research and Innovation programme under the Marie Skłodowska-Curie grant agreement no. 101026353. T.H., H.R.A. and K.R.G. gratefully acknowledge funding from the National Science Foundation under award no. DMR-2102257. L.X. acknowledges support by National Natural Science Foundation of China (no. 61935016, 52173153) and the Electron Microscopy Laboratory of Peking University for the use of electron microscopes. M.G.K. acknowledges support by the Office of Naval Research under award number N00014-20-1-2725. A.A. acknowledges support by the Office of Naval Research under award number N00014-20-1-2573. P.S. acknowledges the support of the Vanier Canada Graduate Scholarship. This work made use of the NUFAB and Keck-II facilities of 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). We thank D. Kopilovic for providing the LED spectrum and J. Gao for assisting with the SEM measurements.

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Author notes

  1. These authors contributed equally: So Min Park, Mingyang Wei, Nikolaos Lempesis

Authors and Affiliations

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

    So Min Park, Heejong Shin, Deokjae Choi, Yi Yang, Bin Chen, Mercouri G. Kanatzidis & Edward H. Sargent

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

    So Min Park, Maral Vafaie, Eui Dae Jung, Da Bin Kim & Edward H. Sargent

  3. Laboratory of Photonics and Interfaces, Ecole Polytechnique Fédérale de Lausanne, Lausanne, Switzerland

    Mingyang Wei, Felix T. Eickemeyer, Shaik M. Zakeeruddin & Michael Grätzel

  4. Laboratory of Computational Chemistry and Biochemistry, Ecole Polytechnique Fédérale de Lausanne, Lausanne, Switzerland

    Nikolaos Lempesis, Lorenzo Agosta, Virginia Carnevali & Ursula Rothlisberger

  5. State Key Laboratory for Artificial Microstructure and Mesoscopic Physics, Department of Physics, Peking University, Beijing, P. R. China

    Wenjin Yu & Lixin Xiao

  6. Department of Chemistry, University of Kentucky, Lexington, KY, USA

    Tareq Hossain, Harindi R. Atapattu & Kenneth R. Graham

  7. Department of Mechanical and Industrial Engineering, University of Toronto, Toronto, Ontario, Canada

    Peter Serles & Tobin Filleter

  8. Department of Materials Science and Engineering, and Organic and Carbon Electronics Laboratories (ORaCEL), North Carolina State University, Raleigh, NC, USA

    Kasra Darabi & Aram Amassian

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

    Edward H. Sargent

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  1. So Min Park
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Contributions

S.M.P., M.W., M.G. and E.H.S. conceived the idea and proposed the experimental and modelling design. N.L., L.A., V.C. and U.R. carried out the molecular dynamics simulation. S.M.P. fabricated all the devices and conducted the characterization. T.H., H.R.A. and K.R.G. performed XPS, UPS and IPES characterization and data analysis. W.Y. and L.X. carried out the HAADF-STEM measurements. F.T.E., M.W., S.M.Z. and M.G. conducted the photoluminescence and EQE characterization and data analysis. M.W. measured DLS. H.S. conducted cyclic voltammetry measurements and data analysis. D.C. performed UV–visible spectroscopy characterization. Y.Y. and M.G.K. measured TOF-SIMS. K.D. and A.A. performed the GIWAXS measurements. M.V., E.D.J. and D.B.K. helped with the device fabrication and material characterization. P.S. and T.F. performed the KPFM measurements. M.W., S.M.P., N.L., M.G. and E.H.S. co-wrote the manuscript. All authors contributed to data analysis, and read and commented on the manuscript.

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Correspondence to Michael Grätzel or Edward H. Sargent.

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Supplementary information

Supplementary Information

Supplementary Notes 1–5, Figs. 1–28, Tables 1–3 and refs.

Reporting Summary

Supplementary Video 1

Classical molecular dynamics simulations of 2PACz adsorption.

Supplementary Video 2

Classical molecular dynamics simulations of 2PACz:3-MPA adsorption.

Supplementary Video 3

AIMD simulations of 2PACz-3-MPA adsorption.

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Park, S.M., Wei, M., Lempesis, N. et al. Low-loss contacts on textured substrates for inverted perovskite solar cells. Nature 624, 289–294 (2023). https://doi.org/10.1038/s41586-023-06745-7

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