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Local nanoscale phase impurities are degradation sites in halide perovskites

Author

Listed:
  • Stuart Macpherson

    (University of Cambridge)

  • Tiarnan A. S. Doherty

    (University of Cambridge
    University of Cambridge)

  • Andrew J. Winchester

    (Femtosecond Spectroscopy Unit, Okinawa Institute of Science and Technology Graduate University)

  • Sofiia Kosar

    (Femtosecond Spectroscopy Unit, Okinawa Institute of Science and Technology Graduate University)

  • Duncan N. Johnstone

    (University of Cambridge)

  • Yu-Hsien Chiang

    (University of Cambridge)

  • Krzysztof Galkowski

    (University of Cambridge
    Nicolaus Copernicus University)

  • Miguel Anaya

    (University of Cambridge
    University of Cambridge)

  • Kyle Frohna

    (University of Cambridge)

  • Affan N. Iqbal

    (University of Cambridge
    University of Cambridge)

  • Satyawan Nagane

    (University of Cambridge)

  • Bart Roose

    (University of Cambridge)

  • Zahra Andaji-Garmaroudi

    (University of Cambridge)

  • Kieran W. P. Orr

    (University of Cambridge
    University of Cambridge)

  • Julia E. Parker

    (Diamond Light Source, Harwell Science and Innovation Campus)

  • Paul A. Midgley

    (University of Cambridge)

  • Keshav M. Dani

    (Femtosecond Spectroscopy Unit, Okinawa Institute of Science and Technology Graduate University)

  • Samuel D. Stranks

    (University of Cambridge
    University of Cambridge)

Abstract

Understanding the nanoscopic chemical and structural changes that drive instabilities in emerging energy materials is essential for mitigating device degradation. The power conversion efficiency of halide perovskite photovoltaic devices has reached 25.7 per cent in single-junction and 29.8 per cent in tandem perovskite/silicon cells1,2, yet retaining such performance under continuous operation has remained elusive3. Here we develop a multimodal microscopy toolkit to reveal that in leading formamidinium-rich perovskite absorbers, nanoscale phase impurities, including hexagonal polytype and lead iodide inclusions, are not only traps for photoexcited carriers, which themselves reduce performance4,5, but also, through the same trapping process, are sites at which photochemical degradation of the absorber layer is seeded. We visualize illumination-induced structural changes at phase impurities associated with trap clusters, revealing that even trace amounts of these phases, otherwise undetected with bulk measurements, compromise device longevity. The type and distribution of these unwanted phase inclusions depends on the film composition and processing, with the presence of polytypes being most detrimental for film photo-stability. Importantly, we reveal that both performance losses and intrinsic degradation processes can be mitigated by modulating these defective phase impurities, and demonstrate that this requires careful tuning of local structural and chemical properties. This multimodal workflow to correlate the nanoscopic landscape of beam-sensitive energy materials will be applicable to a wide range of semiconductors for which a local picture of performance and operational stability has yet to be established.

Suggested Citation

  • Stuart Macpherson & Tiarnan A. S. Doherty & Andrew J. Winchester & Sofiia Kosar & Duncan N. Johnstone & Yu-Hsien Chiang & Krzysztof Galkowski & Miguel Anaya & Kyle Frohna & Affan N. Iqbal & Satyawan N, 2022. "Local nanoscale phase impurities are degradation sites in halide perovskites," Nature, Nature, vol. 607(7918), pages 294-300, July.
  • Handle: RePEc:nat:nature:v:607:y:2022:i:7918:d:10.1038_s41586-022-04872-1
    DOI: 10.1038/s41586-022-04872-1
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    Citations

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    Cited by:

    1. Chenxu Zhao & Zhiwen Zhou & Masaud Almalki & Michael A. Hope & Jiashang Zhao & Thibaut Gallet & Anurag Krishna & Aditya Mishra & Felix T. Eickemeyer & Jia Xu & Yingguo Yang & Shaik M. Zakeeruddin & Al, 2024. "Stabilization of highly efficient perovskite solar cells with a tailored supramolecular interface," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Dejian Yu & Fei Cao & Jinfeng Liao & Bingzhe Wang & Chenliang Su & Guichuan Xing, 2022. "Direct observation of photoinduced carrier blocking in mixed-dimensional 2D/3D perovskites and the origin," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    3. Songhua Cai & Zhipeng Li & Yalan Zhang & Tanghao Liu & Peng Wang & Ming-Gang Ju & Shuping Pang & Shu Ping Lau & Xiao Cheng Zeng & Yuanyuan Zhou, 2024. "Intragrain impurity annihilation for highly efficient and stable perovskite solar cells," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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