Abstract

Perovskite-based optoelectronic devices are gaining much attention owing to their remarkable performance and low processing cost, particularly for solar cells. However, for perovskite light-emitting diodes, non-radiative charge recombination has limited the electroluminescence efficiency. Here we demonstrate perovskite–polymer bulk heterostructure light-emitting diodes exhibiting external quantum efficiencies of up to 20.1% (at current densities of 0.1–1 mA cm−2). The light-emitting diode emissive layer comprises quasi-two-dimensional and three-dimensional (2D/3D) perovskites and an insulating polymer. Photogenerated excitations migrate from quasi-2D to lower-energy sites within 1 ps, followed by radiative bimolecular recombination in the 3D regions. From near-unity external photoluminescence quantum efficiencies and transient kinetics of the emissive layer with and without charge-transport contacts, we find non-radiative recombination pathways to be effectively eliminated, consistent with optical models giving near 100% internal quantum efficiencies. Although the device brightness and stability (T50 = 46 h in air at peak external quantum efficiency) require further improvement, our results indicate the significant potential of perovskite-based photon sources.

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Data availability

The data that support the plots within this paper and other findings of this study are available in the University of Cambridge Repository (https://doi.org/10.17863/CAM.30616). Related research results are available from the corresponding authors upon reasonable request.

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Acknowledgements

B.Z. thanks the Cambridge Trust and China Scholarship Council for funding and support. S.B. is supported by a VINNMER Marie-Curie Fellowship. R.S. acknowledges support from the Royal Society Newton-Bhabha International Fellowship. M.A. acknowledges support from the President of the UAE’s Distinguished Student Scholarship Program (DSS), granted by the UAE’s Ministry of Presidential Affairs. XMaS is a mid-range facility supported by the Engineering and Physical Sciences Research Council (EPSRC). The authors thank all the XMaS beamline team staff for their support. P.G. thanks the ‘Thousand Talent Program’ for support. D.D. and R.H.F. thank the EPSRC for support. The research leading to these results has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 670405).

Author information

Affiliations

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

    • Baodan Zhao
    • , Vincent Kim
    • , Robin Lamboll
    • , Ravichandran Shivanna
    • , Florian Auras
    • , Johannes M. Richter
    • , Le Yang
    • , Linjie Dai
    • , Mejd Alsari
    • , Xiao-Jian She
    • , Jiangbin Zhang
    • , Neil C. Greenham
    • , Richard H. Friend
    •  & Dawei Di
  2. Department of Physics, University of Oxford, Clarendon Laboratory, Oxford, UK

    • Sai Bai
    •  & Henry J. Snaith
  3. Department of Physics, Chemistry and Biology (IFM), Linköping University, Linköping, Sweden

    • Sai Bai
  4. Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR) , Singapore, Singapore

    • Le Yang
  5. Laboratory of Advanced Functional Materials, Xiamen Institute of Rare Earth Materials, Haixi Institute, Chinese Academy of Sciences, Xiamen, China

    • Lusheng Liang
    •  & Peng Gao
  6. Department of Physics and Astronomy, University of Sheffield, Sheffield, UK

    • Samuele Lilliu
  7. The UAE Centre for Crystallography, Abu Dhabi, United Arab Emirates

    • Samuele Lilliu
  8. Institute of Advanced Materials (IAM), Nanjing Tech University, Nanjing, China

    • Jianpu Wang

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Contributions

B.Z. and D.D. developed and characterized the high-efficiency LEDs. D.D., B.Z. and L.Y. carried out the nano- to microsecond transient photoluminescence and electroluminescence studies. V.K. conducted the transient absorption experiments. J.M.R. performed the femto- to picosecond transient photoluminescence measurements. R.L. developed the optical model for the LED devices under the guidance of N.C.G. S.B. synthesised the MZO nanocrystals, tailored the MZO properties, and contributed to LED development. R.S. carried out the lateral photoluminescence experiments. F.A., L.L. and P.G. synthesized the perovskite precursors. L.D. performed the HR-TEM and atomic force microscopy measurements. X.-J.S. and B.Z. performed the SEM studies. F.A., M.A., P.G. and B.Z. carried out the XRD analysis. J.Z. helped with some transient measurements and PLQE calculations. D.D. and B.Z. analysed all the results and wrote the manuscript, which was revised by R.H.F. All authors contributed to the work and commented on the paper. D.D. planned the project and guided the work, with R.H.F.

Competing interests

R.H.F., H.J.S. and N.C.G. are co-founders of Heliochrome Ltd.

Corresponding authors

Correspondence to Richard H. Friend or Dawei Di.

Supplementary information

  1. Supplementary Information

    Additional data for chemical structure, morphology and device characterization

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DOI

https://doi.org/10.1038/s41566-018-0283-4