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Ligand-engineered bandgap stability in mixed-halide perovskite LEDs

Author

Listed:
  • Yasser Hassan

    (University of Oxford)

  • Jong Hyun Park

    (Ulsan National Institute of Science and Technology (UNIST))

  • Michael L. Crawford

    (University of Oregon)

  • Aditya Sadhanala

    (University of Oxford
    Centre for Nano Science and Engineering, Indian Institute of Science
    University of Cambridge)

  • Jeongjae Lee

    (Seoul National University)

  • James C. Sadighian

    (University of Oregon)

  • Edoardo Mosconi

    (Istituto CNR di Scienze e Tecnologie Chimiche ‘Giulio Natta’ (CNR-SCITEC))

  • Ravichandran Shivanna

    (University of Cambridge)

  • Eros Radicchi

    (Istituto CNR di Scienze e Tecnologie Chimiche ‘Giulio Natta’ (CNR-SCITEC)
    University of Perugia)

  • Mingyu Jeong

    (School of Energy and Chemical Engineering, Perovtronics Research Center, Low Dimensional Carbon Materials Center, Ulsan National Institute of Science and Technology (UNIST))

  • Changduk Yang

    (School of Energy and Chemical Engineering, Perovtronics Research Center, Low Dimensional Carbon Materials Center, Ulsan National Institute of Science and Technology (UNIST))

  • Hyosung Choi

    (Hanyang University)

  • Sung Heum Park

    (Pukyong National University)

  • Myoung Hoon Song

    (Ulsan National Institute of Science and Technology (UNIST))

  • Filippo Angelis

    (Istituto CNR di Scienze e Tecnologie Chimiche ‘Giulio Natta’ (CNR-SCITEC)
    University of Perugia
    CompuNet, Istituto Italiano di Tecnologia)

  • Cathy Y. Wong

    (University of Oregon
    University of Oregon
    University of Oregon)

  • Richard H. Friend

    (University of Cambridge)

  • Bo Ram Lee

    (Pukyong National University)

  • Henry J. Snaith

    (University of Oxford)

Abstract

Lead halide perovskites are promising semiconductors for light-emitting applications because they exhibit bright, bandgap-tunable luminescence with high colour purity1,2. Photoluminescence quantum yields close to unity have been achieved for perovskite nanocrystals across a broad range of emission colours, and light-emitting diodes with external quantum efficiencies exceeding 20 per cent—approaching those of commercial organic light-emitting diodes—have been demonstrated in both the infrared and the green emission channels1,3,4. However, owing to the formation of lower-bandgap iodide-rich domains, efficient and colour-stable red electroluminescence from mixed-halide perovskites has not yet been realized5,6. Here we report the treatment of mixed-halide perovskite nanocrystals with multidentate ligands to suppress halide segregation under electroluminescent operation. We demonstrate colour-stable, red emission centred at 620 nanometres, with an electroluminescence external quantum efficiency of 20.3 per cent. We show that a key function of the ligand treatment is to ‘clean’ the nanocrystal surface through the removal of lead atoms. Density functional theory calculations reveal that the binding between the ligands and the nanocrystal surface suppresses the formation of iodine Frenkel defects, which in turn inhibits halide segregation. Our work exemplifies how the functionality of metal halide perovskites is extremely sensitive to the nature of the (nano)crystalline surface and presents a route through which to control the formation and migration of surface defects. This is critical to achieve bandgap stability for light emission and could also have a broader impact on other optoelectronic applications—such as photovoltaics—for which bandgap stability is required.

Suggested Citation

  • Yasser Hassan & Jong Hyun Park & Michael L. Crawford & Aditya Sadhanala & Jeongjae Lee & James C. Sadighian & Edoardo Mosconi & Ravichandran Shivanna & Eros Radicchi & Mingyu Jeong & Changduk Yang & H, 2021. "Ligand-engineered bandgap stability in mixed-halide perovskite LEDs," Nature, Nature, vol. 591(7848), pages 72-77, March.
  • Handle: RePEc:nat:nature:v:591:y:2021:i:7848:d:10.1038_s41586-021-03217-8
    DOI: 10.1038/s41586-021-03217-8
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    Citations

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    Cited by:

    1. Rohit Abraham John & Yiğit Demirağ & Yevhen Shynkarenko & Yuliia Berezovska & Natacha Ohannessian & Melika Payvand & Peng Zeng & Maryna I. Bodnarchuk & Frank Krumeich & Gökhan Kara & Ivan Shorubalko &, 2022. "Reconfigurable halide perovskite nanocrystal memristors for neuromorphic computing," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    2. Yang Bryan Cao & Daquan Zhang & Qianpeng Zhang & Xiao Qiu & Yu Zhou & Swapnadeep Poddar & Yu Fu & Yudong Zhu & Jin-Feng Liao & Lei Shu & Beitao Ren & Yucheng Ding & Bing Han & Zhubing He & Dai-Bin Kua, 2023. "High-efficiency, flexible and large-area red/green/blue all-inorganic metal halide perovskite quantum wires-based light-emitting diodes," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    3. Kyeong-Yoon Baek & Woocheol Lee & Jonghoon Lee & Jaeyoung Kim & Heebeom Ahn & Jae Il Kim & Junwoo Kim & Hyungbin Lim & Jiwon Shin & Yoon-Joo Ko & Hyeon-Dong Lee & Richard H. Friend & Tae-Woo Lee & Jeo, 2022. "Mechanochemistry-driven engineering of 0D/3D heterostructure for designing highly luminescent Cs–Pb–Br perovskites," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    4. Weilun Li & Mengmeng Hao & Ardeshir Baktash & Lianzhou Wang & Joanne Etheridge, 2023. "The role of ion migration, octahedral tilt, and the A-site cation on the instability of Cs1-xFAxPbI3," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    5. Sudhir Kumar & Tommaso Marcato & Frank Krumeich & Yen-Ting Li & Yu-Cheng Chiu & Chih-Jen Shih, 2022. "Anisotropic nanocrystal superlattices overcoming intrinsic light outcoupling efficiency limit in perovskite quantum dot light-emitting diodes," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    6. Hongjin Li & Xiaofang Zhu & Dingshuo Zhang & Yun Gao & Yifeng Feng & Zichao Ma & Jingyun Huang & Haiping He & Zhizhen Ye & Xingliang Dai, 2024. "Thermal management towards ultra-bright and stable perovskite nanocrystal-based pure red light-emitting diodes," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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