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Quantum-size-tuned heterostructures enable efficient and stable inverted perovskite solar cells

Nature Photonics volume 16, pages 352–358 (2022)Cite this article

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Abstract

The energy landscape of reduced-dimensional perovskites (RDPs) can be tailored by adjusting their layer width (n). Recently, two/three-dimensional (2D/3D) heterostructures containing n = 1 and 2 RDPs have produced perovskite solar cells (PSCs) with >25% power conversion efficiency (PCE). Unfortunately, this method does not translate to inverted PSCs due to electron blocking at the 2D/3D interface. Here we report a method to increase the layer width of RDPs in 2D/3D heterostructures to address this problem. We discover that bulkier organics form 2D heterostructures more slowly, resulting in wider RDPs; and that small modifications to ligand design induce preferential growth of n ≥ 3 RDPs. Leveraging these insights, we developed efficient inverted PSCs (with a certified quasi-steady-state PCE of 23.91%). Unencapsulated devices operate at room temperature and around 50% relative humidity for over 1,000 h without loss of PCE; and, when subjected to ISOS-L3 accelerated ageing, encapsulated devices retain 92% of initial PCE after 500 h.

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Fig. 1: Quasi-2D treatment and its effect on RDP distribution.
Fig. 2: Comparison of 2D and quasi-2D treatments using different 2D ligands.
Fig. 3: Formation of quasi-2D perovskite capping layers from density functional theory.
Fig. 4: Quantifying the conduction band offset of 2D and quasi-2D surface treatments.
Fig. 5: Carrier extraction and performance of quasi-2D-treated PSCs.

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Source data are provided with this paper. All the data supporting the findings of this study are available within this article and its Supplementary Information. Any additional information can be obtained from corresponding authors upon request.

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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 the Ontario Research Fund-Research Excellence program (ORF7-Ministry of Research and Innovation, Ontario Research Fund-Research Excellence Round 7). We appreciate the Shanghai Synchrotron Radiation Facility (beamline 14B and 16B) and X. Gao and Z. Su for their help with GIWAXS characterization. Z.N. is grateful for support by the National Key Research Program (2021YFA0715502, 2016YFA0204000) and the National Science Fund of China (61935016). S.M.P., H.R.A. and K.R.G. acknowledge the US Department of Energy under Grant DE-SC0018208 for supporting the UPS and IPES measurements. T.F. and T.C. acknowledge the Canadian Foundation for Innovation and the Natural Science and Engineering Council of Canada (NSERC) for KPFM measurements. F.L and Y.G. were funded by the King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR) under Award No: OSR-CARF/CCF-3079 and OSR-2018-CRG7-3737.

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Author notes

  1. Yi Hou

    Present address: Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore, Singapore

  2. These authors contributed equally: Hao Chen, Sam Teale, Bin Chen, Yi Hou.

Authors and Affiliations

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

    Hao Chen, Sam Teale, Bin Chen, Yi Hou, Luke Grater, Tong Zhu, Koen Bertens, So Min Park, Mingyang Wei, Andrew K. Johnston, Eui Hyuk Jung, Chun Zhou, Andrew H. Proppe, Sjoerd Hoogland & Edward H. Sargent

  2. School of Physical Science and Technology, ShanghaiTech University, Shanghai, China

    Hao Chen, Qilin Zhou, Kaimin Xu, Danni Yu, Congcong Han, Wenjia Zhou & Zhijun Ning

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

    So Min Park, Harindi R. Atapattu & Kenneth R. Graham

  4. KAUST Solar Center, Physical Sciences and Engineering Division (PSE), Materials Science and Engineering Program (MSE), King Abdullah University of Science and Technology (KAUST), Thuwal, Kingdom of Saudi Arabia

    Yajun Gao & Frédéric Laquai

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

    Teng Cui & Tobin Filleter

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Contributions

H.C., S.T., B.C. and Y.H. conceived the idea. H.C., K.B., L.G. and S.T. prepared samples for characterization. S.M.P. and H.R.A. performed UPS and IPES measurements, and S.M.P., H.R.A., S.T. and K.R.G. analysed the data. S.T. performed the TA experiments and analysed the data with Y.G. and F.L. The in situ TA system for use in this paper was developed by S.T., A.K.J. and A.H.P. The in situ measurements were performed by S.T. who also analysed the data. T.Z. performed the DFT calculations and analysed the data. B.C. performed PLQY measurements and H.C. measured the PL lifetimes. M.W. carried out the transient photocurrent and photovoltage measurements and S.T. analysed the data. S.T. performed SCAPS simulations. S.T. collected the thin-film X-ray diffraction patterns. C.H. and D.Y. performed the GIWAXS experiments and obtained the SEM images. S.T. and B.C. analysed the data. The KPFM measurements were performed by T.C., and T.F. analysed the data. H.C. and W.Z. carried out the SCLC measurements and S.T. analysed the data. S.T. conducted the c-AFM measurements. H.C. fabricated all the devices for performance and certification, B.C. and S.H. helped with device certification. B.C. built the heated MPP-tracking station. Q.Z., K.X. and C.Z. carried out the UPS on bulk 2D films. Z.N. and E.H.S. supervised and funded the work. S.T. wrote the draft manuscript with input from B.C. and E.H.S. All authors contributed to the revision of the final paper.

Corresponding authors

Correspondence to Zhijun Ning or Edward H. Sargent.

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Nature Photonics thanks Mohammad Khaja Nazeeruddin, Ling Xu the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Text 1–6 and Figs. 1–46.

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Source data

Source Data Fig. 1

Unprocessed UPS data for bulk 2D perovskite films.

Source Data Fig. 2

Unprocessed TA and in situ TA data.

Source Data Fig. 3

Coordinates from DFT calculations.

Source Data Fig. 4

Unprocessed IPES data from 2D/3D heterostructures.

Source Data Fig. 5

Normalized PL lifetimes and transient photocurrent data. Device J–V and stability data.

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Chen, H., Teale, S., Chen, B. et al. Quantum-size-tuned heterostructures enable efficient and stable inverted perovskite solar cells. Nat. Photon. 16, 352–358 (2022). https://doi.org/10.1038/s41566-022-00985-1

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