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Minimizing heat generation in quantum dot light-emitting diodes by increasing quasi-Fermi-level splitting

Abstract

Minimizing heat accumulation is essential to prolonging the operational lifetime of quantum dot light-emitting diodes (QD-LEDs). Reducing heat generation at the source is the ideal solution, which requires high brightness and quantum efficiency at low driving voltages. Here we propose to enhance the brightness of QD-LEDs at low driving voltages by using a monolayer of large QDs to reduce the packing number in the emitting layer. This strategy allows us to achieve a higher charge population per QD for a given number of charges without charge leakage, enabling enhanced quasi-Fermi-level splitting and brightness at low driving voltage. Due to the minimized heat generation, these LEDs show a high power conversion efficiency of 23% and a T95 operation lifetime (the time for the luminance to decrease to 95% of the initial value) of more than 48,000 h at 1,000 cd m−2.

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Fig. 1: Mitigating heat generation in QD-LEDs by achieving high brightness at low driving voltages.
Fig. 2: Characterizations of QD-LEDs.
Fig. 3: Electron quasi-Fermi-level splitting measurements.
Fig. 4: Device temperature at different brightnesses.
Fig. 5: Device stability tests.

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Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request. They are also available at figshare: https://doi.org/10.6084/m9.figshare.22817639, or from the attached Source Data files. Source data are provided with this paper.

References

  1. Sadi, T., Radevici, I. & Oksanen, J. Thermophotonic cooling with light-emitting diodes. Nat. Photon. 14, 205–214 (2020).

    Article  CAS  Google Scholar 

  2. Ong, W.-L., Rupich, S. M., Talapin, D. V., McGaughey, A. J. H. & Malen, J. A. Surface chemistry mediates thermal transport in three-dimensional nanocrystal arrays. Nat. Mater. 12, 410–415 (2013).

    Article  CAS  Google Scholar 

  3. Dai, X. et al. Solution-processed, high-performance light-emitting diodes based on quantum dots. Nature 515, 96–99 (2014).

    Article  CAS  Google Scholar 

  4. Li, X. et al. Bright colloidal quantum dot light-emitting diodes enabled by efficient chlorination. Nat. Photon. 12, 159–164 (2018).

    Article  CAS  Google Scholar 

  5. Shen, H. et al. Visible quantum dot light-emitting diodes with simultaneous high brightness and efficiency. Nat. Photon. 13, 192–197 (2019).

    Article  CAS  Google Scholar 

  6. Deng, Y. et al. Solution-processed green and blue quantum-dot light-emitting diodes with eliminated charge leakage. Nat. Photon. 16, 505–511 (2022).

    Article  CAS  Google Scholar 

  7. Tauc, J. The share of thermal energy taken from the surroundings in the electro-luminescent energy radiated from a p–n junction. Cech. Fiz. Z. 7, 275–276 (1957).

    Google Scholar 

  8. Wurfel, P. The chemical-potential of radiation. J. Phys. C 15, 3967–3985 (1982).

    Article  Google Scholar 

  9. Su, Q. & Chen, S. M. Thermal assisted up-conversion electroluminescence in quantum dot light emitting diodes. Nat. Commun. 13, 369 (2022).

    Article  CAS  Google Scholar 

  10. Lin, X. et al. Highly-efficient thermoelectric-driven light-emitting diodes based on colloidal quantum dots. Nano Res. 15, 9402–9409 (2022).

    Article  CAS  Google Scholar 

  11. Li, N. et al. Ultra-low-power sub-photon-voltage high-efficiency light-emitting diodes. Nat. Photon. 13, 588–592 (2019).

    Article  CAS  Google Scholar 

  12. Pal, B. N. et al. ‘Giant’ CdSe/CdS core/shell nanocrystal quantum dots as efficient electroluminescent materials: strong influence of shell thickness on light-emitting diode performance. Nano Lett. 12, 331–336 (2012).

    Article  CAS  Google Scholar 

  13. Park, Y. S., Lim, J. & Klimov, V. I. Asymmetrically strained quantum dots with non-fluctuating single-dot emission spectra and subthermal room-temperature linewidths. Nat. Mater. 18, 249–255 (2019).

    Article  CAS  Google Scholar 

  14. Qin, H. Y. et al. Single-dot spectroscopy of zinc-blende CdSe/CdS core/shell nanocrystals: nonblinking and correlation with ensemble measurements. J. Am. Chem. Soc. 136, 179–187 (2014).

    Article  CAS  Google Scholar 

  15. Lim, J., Park, Y.-S. & Klimov, V. I. Optical gain in colloidal quantum dots achieved with direct-current electrical pumping. Nat. Mater. 17, 42–49 (2018).

    Article  CAS  Google Scholar 

  16. Lim, J., Park, Y. S., Wu, K. F., Yun, H. J. & Klimov, V. I. Droop-free colloidal quantum dot light-emitting diodes. Nano Lett. 18, 6645–6653 (2018).

    Article  CAS  Google Scholar 

  17. Lee, T. et al. Bright and stable quantum dot light-emitting diodes. Adv. Mater. 34, 202106276 (2021).

    Google Scholar 

  18. Qian, L., Zheng, Y., Xue, J. & Holloway, P. H. Stable and efficient quantum-dot light-emitting diodes based on solution-processed multilayer structures. Nat. Photon. 5, 543–548 (2011).

    Article  CAS  Google Scholar 

  19. Neyts, K. A. Simulation of light emission from thin-film microcavities. J. Opt. Soc. Am. A 15, 962–971 (1998).

    Article  Google Scholar 

  20. Yang, Y. et al. High-efficiency light-emitting devices based on quantum dots with tailored nanostructures. Nat. Photon. 9, 259–266 (2015).

    Article  CAS  Google Scholar 

  21. Mashford, B. S. et al. High-efficiency quantum-dot light-emitting devices with enhanced charge injection. Nat. Photon. 7, 407–412 (2013).

    Article  CAS  Google Scholar 

  22. Cao, W. et al. Highly stable QLEDs with improved hole injection via quantum dot structure tailoring. Nat. Commun. 9, 2608 (2018).

    Article  Google Scholar 

  23. Lin, J. et al. High-performance quantum-dot light-emitting diodes using NiOX hole-injection layers with a high and stable work function. Adv. Funct. Mater. 30, 201907265 (2020).

    Article  Google Scholar 

  24. Liu, D. et al. Highly stable red quantum dot light-emitting diodes with long T95 operation lifetimes. J. Phys. Chem. Lett. 11, 3111–3115 (2020).

    Article  CAS  Google Scholar 

  25. Efros, A. L. et al. Band-edge exciton in quantum dots of semiconductors with a degenerate valence band: dark and bright exciton states. Phys. Rev. B 54, 4843–4856 (1996).

    Article  CAS  Google Scholar 

  26. Pu, C. et al. Electrochemically-stable ligands bridge the photoluminescence–electroluminescence gap of quantum dots. Nat. Commun. 11, 937 (2020).

    Article  CAS  Google Scholar 

  27. Chen, S. et al. On the degradation mechanisms of quantum-dot light-emitting diodes. Nat. Commun. 10, 765 (2019).

    Article  CAS  Google Scholar 

  28. Sun, Y. et al. Investigation on thermally induced efficiency roll-off: towards efficient and ultra-bright quantum-dot light-emitting diodes. ACS Nano 13, 11433–11442 (2019).

    Article  CAS  Google Scholar 

  29. Scholz, S., Kondakov, D., Lüssem, B. & Leo, K. Degradation mechanisms and reactions in organic light-emitting devices. Chem. Rev. 115, 8449–8503 (2015).

    Article  CAS  Google Scholar 

  30. Benisty, H., Stanley, R. & Mayer, M. Method of source terms for dipole emission modification in modes of arbitrary planar structures. J. Opt. Soc. Am. A 15, 1192–1201 (1998).

    Article  Google Scholar 

  31. Cho, C. & Greenham, N. C. Computational study of dipole radiation in re‐absorbing perovskite semiconductors for optoelectronics. Adv. Sci. 8, 2003559 (2020).

    Article  Google Scholar 

Download references

Acknowledgements

We gratefully acknowledge financial support from the National Natural Science Foundation of China (grant numbers U22A2072, 52272167, 62234006, 81788101, 11761131011, 51872275), the National Key R&D Program of China (grant number 2018YFA0306600), and the Postgraduate Cultivating Innovation and Quality Improvement Action Plan of Henan University (grant number SYLYC2022127).

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Contributions

H.S. and F.F. conceived the concept and designed the experiments. H.S., F.F. and Z.D. supervised the project. Y.G., X.L. and J.S. synthesized the materials, fabricated the devices and collected the performance data of the QD-LEDs. B.L. and Y.S. developed the thermal simulation model and the electrical pump optical probe spectroscopy. F.F., H.S. and B.L. wrote the manuscript. All authors contributed to the scientific discussion and editing the manuscript.

Corresponding authors

Correspondence to Huaibin Shen, Fengjia Fan or Zuliang Du.

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Nature Nanotechnology thanks Yanping Wang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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

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Source Data Fig. 1

Fig. 1 source data in spreadsheet.

Source Data Fig. 2

Fig. 2 source data in spreadsheet.

Source Data Fig. 3

Fig. 3 source data in spreadsheet.

Source Data Fig. 4

Fig. 4 source data in spreadsheet.

Source Data Fig. 5

Fig. 5 source data in spreadsheet.

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Gao, Y., Li, B., Liu, X. et al. Minimizing heat generation in quantum dot light-emitting diodes by increasing quasi-Fermi-level splitting. Nat. Nanotechnol. 18, 1168–1174 (2023). https://doi.org/10.1038/s41565-023-01441-z

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