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Dipole–dipole-interaction-assisted self-assembly of quantum dots for highly efficient light-emitting diodes

Abstract

The external quantum efficiency of state-of-the-art quantum dot light-emitting diodes is limited by the low photon out-coupling efficiency. Light-emitting diodes using oriented nanostructures such as nanorods, nanoplatelets and dot-in-disc nanocrystals favour photon out-coupling; however, their internal quantum efficiency is often compromised and thus achieving a net gain has proved challenging. Here we report isotropic-shaped quantum dots featuring a mixed-crystallographic structure composed of wurtzite and zinc blende phases. The wurtzite phase promotes dipole–dipole interactions that orient quantum dots in solution-processed films, whereas the zinc blende phase helps lift the electronic state degeneracy to enable directional light emission. These combined features improve photon out-coupling without compromising internal quantum efficiency. Fabricated light-emitting diodes exhibit an external quantum efficiency of 35.6% and can be continuously operated with an initial brightness of 1,000 cd m2 for 4.5 years with a minimal performance loss of about 5%.

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Fig. 1: Synthesis of polytypic QDs with large permanent dipole moments.
Fig. 2: Characterization of polytypic QDs and their orientation.
Fig. 3: Simulations and experimental studies of QD-LED devices.
Fig. 4: PCE and lifetime tests of QD-LED devices.

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Data availability

The data that support the findings of this study are available from the corresponding authors on reasonable request. They are also available at figshare: https://doi.org/10.6084/m9.figshare.24236629. Source Data are provided with this paper.

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Acknowledgements

We gratefully acknowledge the financial support from the National Natural Science Foundation of China (grant nos. U22A2072, 52272167 and BE3250011 to H.B.S., F.J.F. and J.L., respectively), Innovation Program for Quantum Science and Technology (grant no. 2021ZD0301603 to F.J.F), the National Key Research and Development Program of China (grant no. 2022YFA1505100 to J.L), the Fundamental Research Funds for the Central Universities (grant no. 23X010301599 to J.L), and Shanghai Pilot Program for Basic Research—Shanghai Jiao Tong University. We thank the Hefei Advanced Computing Center and thank the Shanghai Synchrotron Radiation Facility for the provision of GIWAXS tests at the beamline BL16B1.

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Contributions

F.J.F. and H.B.S. conceptualized the work and designed the experiments. H.B.S., F.J.F., J.F.D. and E.H.S. supervised the project. H.Y.X. and Y.S. performed the BFP and dielectric spectroscopy experiments and fitting, as well as the transfer matrix computations. P.H.Z., J.J.S and Y.G. synthesized the materials, fabricated the devices and collected the performance data of the QD-LEDs. J.X., S.C.F. and O.V. performed DFT calculations. Z.J.Z. contributed to dielectric spectroscopy experiments. C.M.Y., Y.F.H. and J.L. performed GIWAXS measurements and analyses. H.Y.X., F.J.F., H.B.S., J.M.P. and E.H.S. wrote the paper. All authors contributed to the scientific discussion about this work.

Corresponding authors

Correspondence to Huaibin Shen, Jiangfeng Du, Edward H. Sargent or Fengjia Fan.

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Nature Photonics thanks Chih-Jen Shih, Jiwoong Yang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Xu, H., Song, J., Zhou, P. et al. Dipole–dipole-interaction-assisted self-assembly of quantum dots for highly efficient light-emitting diodes. Nat. Photon. 18, 186–191 (2024). https://doi.org/10.1038/s41566-023-01344-4

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