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Comprehensive defect suppression in perovskite nanocrystals for high-efficiency light-emitting diodes

Nature Photonics volume 15, pages 148–155 (2021)Cite this article

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Abstract

Electroluminescence efficiencies of metal halide perovskite nanocrystals (PNCs) are limited by a lack of material strategies that can both suppress the formation of defects and enhance the charge carrier confinement. Here we report a one-dopant alloying strategy that generates smaller, monodisperse colloidal particles (confining electrons and holes, and boosting radiative recombination) with fewer surface defects (reducing non-radiative recombination). Doping of guanidinium into formamidinium lead bromide PNCs yields limited bulk solubility while creating an entropy-stabilized phase in the PNCs and leading to smaller PNCs with more carrier confinement. The extra guanidinium segregates to the surface and stabilizes the undercoordinated sites. Furthermore, a surface-stabilizing 1,3,5-tris(bromomethyl)-2,4,6-triethylbenzene was applied as a bromide vacancy healing agent. The result is highly efficient PNC-based light-emitting diodes that have current efficiency of 108 cd A−1 (external quantum efficiency of 23.4%), which rises to 205 cd A−1 (external quantum efficiency of 45.5%) with a hemispherical lens.

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Fig. 1: Structure of FA1–xGAxPbBr3 PNCs.
Fig. 2: Structural and photophysical effects of GA on FA1–xGAxPbBr3 PNCs.
Fig. 3: Defect analysis of FA1–xGAxPbBr3 PNCs.
Fig. 4: Characteristics of PeLEDs based on FA1–xGAxPbBr3 PNCs.
Fig. 5: Characteristics of PeLEDs with a TBTB interlayer.
Fig. 6: Device lifetime of PeLEDs.

Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding author on reasonable request.

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Acknowledgements

This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (NRF-2016R1A3B1908431). A.K., R.B.W., and A.M.R. acknowledge the support of the US Department of Energy, Office of Basic Energy Sciences, under grant no. DE-SC0019281 and also the computational support from NERSC of the DOE. P.T. acknowledges the scholarship from Chinese Scholarship Council (CSC). H.J.B. acknowledges funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 834431) and the Spanish Ministry of Economy and Competitiveness (MINECO) via the Unidad de Excelencia María de Maeztu CEX2019-000919-M and MAT2017-88821-R. A.S., S.N. and R.H.F. acknowledge support from the UKRI Global Challenge Research Fund project, SUNRISE (EP/P032591/1) and UKIERI projects. S.N. acknowledges funding and support from Royal Society-SERB Newton International Fellowship.

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  1. These authors contributed equally: Young-Hoon Kim, Sungjin Kim, Arvin Kakekhani.

Authors and Affiliations

  1. Department of Materials Science and Engineering, Seoul National University, Seoul, Republic of Korea

    Young-Hoon Kim, Sungjin Kim, Jinwoo Park, Yong-Hee Lee, Dong-Hyeok Kim, Seung Hyeon Jo, Gyeong-Su Park, Young-Woon Kim & Tae-Woo Lee

  2. School of Chemical and Biological Engineering, Institute of Engineering Research, Research Institute of Advanced Materials, Nano Systems Institute, Seoul National University, Seoul, Republic of Korea

    Young-Hoon Kim, Sungjin Kim, Jinwoo Park, Dong-Hyeok Kim, Seung Hyeon Jo & Tae-Woo Lee

  3. Department of Chemistry, University of Pennsylvania, Philadelphia, PA, USA

    Arvin Kakekhani, Robert B. Wexler, Peng Tan & Andrew M. Rappe

  4. School of Electrical Engineering, Korea Advanced Institute of Science and Technology, Daejeon, Republic of Korea

    Jaehyeok Park & Seunghyup Yoo

  5. Department of Materials Science and Engineering, University of Tennessee, Knoxville, TN, USA

    Hengxing Xu & Bin Hu

  6. Cavendish Laboratory, University of Cambridge, Cambridge, UK

    Satyawan Nagane, Aditya Sadhanala & Richard H. Friend

  7. Instituto de Ciencia Molecular, Universidad de Valencia, Paterna, Spain

    Laura Martínez-Sarti & Henk J. Bolink

  8. Department of Physics, Harbin Institute of Technology, Harbin, China

    Peng Tan

  9. Clarendon Laboratory, Department of Physics, University of Oxford, Oxford, UK

    Aditya Sadhanala

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Contributions

Y.-H.K., S.K. and A.K. equally contributed to this work. Y.-H.K., S.K. and T.-W. L. initiated and designed the study. Y.-H.K. and S.K. performed experiments and analysed data. A.K., R.B.W. and P.T. performed the simulations, analysed data, helped understand the structures and mechanisms behind the great efficiency. J.P., D.-H.K. and S.H.J. helped to analyse the data. H.X. and B.H. performed and analysed magnetic field-dependent characteristics. Y.-H.L. and Y.-W.K. measured and analysed TEM. L.M.-S. and H.J.B. commented on the synthesis of nanocrystals. J.P. (KAIST) and S.Y. performed optical simulation of the devices. A.S., S.N. and R.H.F. performed the PLQE measurements and analysis. A.M.R. and T.-W.L. supervised the study. All authors discussed the results and commented on the manuscript.

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Correspondence to Andrew M. Rappe or Tae-Woo Lee.

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Supplementary Figs. 1–17, Discussion and Tables 1–6.

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Kim, YH., Kim, S., Kakekhani, A. et al. Comprehensive defect suppression in perovskite nanocrystals for high-efficiency light-emitting diodes. Nat. Photonics 15, 148–155 (2021). https://doi.org/10.1038/s41566-020-00732-4

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