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The critical role of composition-dependent intragrain planar defects in the performance of MA1–xFAxPbI3 perovskite solar cells

Nature Energy volume 6, pages 624–632 (2021)Cite this article

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Abstract

Perovskite solar cells show excellent power conversion efficiencies, long carrier diffusion lengths and low recombination rates. This encourages a view that intragrain defects are electronically benign with little impact on device performance. In this study we varied the methylammonium (MA)/formamidinium (FA) composition in MA1–xFAxPbI3 (x = 0–1), and compared the structure and density of the intragrain planar defects with device performance, otherwise keeping the device nominally the same. We found that charge carrier lifetime, open-circuit voltage deficit and current density–voltage hysteresis correlate empirically with the density and structure of {111}c planar defects (x = 0.5–1) and {112}t twin boundaries (x = 0–0.1). The best performance parameters were found when essentially no intragrain planar defects were evident (x = 0.2). Similarly, reducing the density of {111}c planar defects through MASCN vapour treatment of FAPbI3 (x ≈ 1) also improved performance. These observations suggest that intragrain defect control can provide an important route for improving perovskite solar cell performance, in addition to well-established parameters such as grain boundaries and interfaces.

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Fig. 1: Microstructural characteristics of MA1–xFAxPbI3.
Fig. 2: Material characterizations and device properties.
Fig. 3: Schematics of the proposed {111}c twinning structure in MA1–xFAxPbI3.
Fig. 4: Ion migration activation energy in MA1–xFAxPbI3 films.

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Source data are provided with this paper. All other data generated or analysed during this study are included in the published article and its Supplementary Information files.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (NSFC 91963209) and the Australian Government through the Australian Renewable Energy Agency and the ARC Discovery Grants DP150104483 and DP200103070. W.L., M.U.R., U.B. and Y.-B.C. acknowledge the support from the Australian Centre for Advanced Photovoltaics. The authors acknowledge use of facilities within the Monash Centre for Electron Microscopy, a node of Microscopy Australia, and the Monash X-Ray Platform. M.U.R. and W.L. are grateful to L. Bourgeois for expert advice on the operation of the JEOL 2100F transmission electron microscope. W.L. acknowledges support from the National Natural Science Foundation of China (NSFC 51802241) and the Fundamental Research Funds for the Central Universities (WUT: 2019IVB055 and 2019IVA066). Y.Z. was supported by the Hong Kong Research Grants Council (Project no. 15305020) and a Hong Kong Polytechnic University grant (Project no. ZVRP).

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Author notes

  1. These authors contributed equally: Wei Li, Mathias Uller Rothmann, Ye Zhu.

Authors and Affiliations

  1. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, People’s Republic of China

    Wei Li, Chenquan Yang & Yi-Bing Cheng

  2. Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory, Xianhu Hydrogen Valley, Foshan, People’s Republic of China

    Wei Li & Yi-Bing Cheng

  3. Department of Materials Science and Engineering, Monash University, Melbourne, Victoria, Australia

    Mathias Uller Rothmann, Yen Yee Choo & Joanne Etheridge

  4. Department of Applied Physics, Research Institute for Smart Energy, The Hong Kong Polytechnic University, Hong Kong, People’s Republic of China

    Ye Zhu

  5. Centre for Micro-Photonics, Swinburne University of Technology, Melbourne, Victoria, Australia

    Weijian Chen & Xiaoming Wen

  6. Hunan Key Laboratory of Super Microstructure and Ultrafast Process, School of Physics and Electronics, Central South University, Changsha, People’s Republic of China

    Yongbo Yuan

  7. Department of Chemical Engineering, Monash University, Melbourne, Victoria, Australia

    Udo Bach

  8. ARC Centre of Excellence in Exciton Science, Monash University, Melbourne, Victoria, Australia

    Udo Bach

  9. Manufacturing Flagship, Commonwealth Scientific and Industrial Research Organization, Clayton, Victoria, Australia

    Udo Bach

  10. Melbourne Centre for Nanofabrication, Clayton, Victoria, Australia

    Udo Bach

  11. Monash Centre for Electron Microscopy, Monash University, Melbourne, Victoria, Australia

    Joanne Etheridge

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Contributions

W.L., M.U.R. and Y.Z. contributed equally to this work. W.L., M.U.R., U.B., Y.-B.C. and J.E. conceived and designed the experiments. W.L. and M.U.R. carried out sample preparation. W.L. and M.U.R. performed the electron microscopy, and W.L., M.U.R., Y.Z. and J.E. analysed the data. W.L., Y.Y. and C.Y. carried out the temperature-dependent conductivity tests and data analysis. W.L. is grateful to R. Zhu from Oxford Instruments for operation of the conductive atomic force microscope. W.L., M.U.R., Y.Z. and J.E. wrote the manuscript. All authors contributed to the discussion of the results and revision of the manuscript.

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Correspondence to Yi-Bing Cheng, Udo Bach or Joanne Etheridge.

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Li, W., Rothmann, M.U., Zhu, Y. et al. The critical role of composition-dependent intragrain planar defects in the performance of MA1–xFAxPbI3 perovskite solar cells. Nat Energy 6, 624–632 (2021). https://doi.org/10.1038/s41560-021-00830-9

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