Ligand-engineered bandgap stability in mixed-halide perovskite LEDs

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, Hyosung Choi, Sung Heum Park, Myoung Hoon Song, Filippo Angelis, Cathy Y. Wong (), Richard H. Friend, Bo Ram Lee () and Henry J. Snaith ()
Additional contact information
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
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)
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)
Cathy Y. Wong: University of Oregon
Richard H. Friend: University of Cambridge
Bo Ram Lee: Pukyong National University
Henry J. Snaith: University of Oxford

Nature, 2021, vol. 591, issue 7848, 72-77

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41586-021-03217-8

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