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Deciphering exciton-generation processes in quantum-dot electroluminescence

Author

Listed:
  • Yunzhou Deng

    (Zhejiang University)

  • Xing Lin

    (Zhejiang University)

  • Wei Fang

    (Zhejiang University)

  • Dawei Di

    (International Research Center for Advanced Photonics, Zhejiang University)

  • Linjun Wang

    (Zhejiang University)

  • Richard H. Friend

    (University of Cambridge)

  • Xiaogang Peng

    (Zhejiang University)

  • Yizheng Jin

    (Zhejiang University)

Abstract

Electroluminescence of colloidal nanocrystals promises a new generation of high-performance and solution-processable light-emitting diodes. The operation of nanocrystal-based light-emitting diodes relies on the radiative recombination of electrically generated excitons. However, a fundamental question—how excitons are electrically generated in individual nanocrystals—remains unanswered. Here, we reveal a nanoscopic mechanism of sequential electron-hole injection for exciton generation in nanocrystal-based electroluminescent devices. To decipher the corresponding elementary processes, we develop electrically-pumped single-nanocrystal spectroscopy. While hole injection into neutral quantum dots is generally considered to be inefficient, we find that the intermediate negatively charged state of quantum dots triggers confinement-enhanced Coulomb interactions, which simultaneously accelerate hole injection and hinder excessive electron injection. In-situ/operando spectroscopy on state-of-the-art quantum-dot light-emitting diodes demonstrates that exciton generation at the ensemble level is consistent with the charge-confinement-enhanced sequential electron-hole injection mechanism probed at the single-nanocrystal level. Our findings provide a universal mechanism for enhancing charge balance in nanocrystal-based electroluminescent devices.

Suggested Citation

  • Yunzhou Deng & Xing Lin & Wei Fang & Dawei Di & Linjun Wang & Richard H. Friend & Xiaogang Peng & Yizheng Jin, 2020. "Deciphering exciton-generation processes in quantum-dot electroluminescence," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
  • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-15944-z
    DOI: 10.1038/s41467-020-15944-z
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    Cited by:

    1. Siyu He & Xiaoqi Tang & Yunzhou Deng & Ni Yin & Wangxiao Jin & Xiuyuan Lu & Desui Chen & Chenyang Wang & Tulai Sun & Qi Chen & Yizheng Jin, 2023. "Anomalous efficiency elevation of quantum-dot light-emitting diodes induced by operational degradation," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Yaxiao Lian & Dongchen Lan & Shiyu Xing & Bingbing Guo & Zhixiang Ren & Runchen Lai & Chen Zou & Baodan Zhao & Richard H. Friend & Dawei Di, 2022. "Ultralow-voltage operation of light-emitting diodes," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    3. Xingtong Chen & Xiongfeng Lin & Likuan Zhou & Xiaojuan Sun & Rui Li & Mengyu Chen & Yixing Yang & Wenjun Hou & Longjia Wu & Weiran Cao & Xin Zhang & Xiaolin Yan & Song Chen, 2023. "Blue light-emitting diodes based on colloidal quantum dots with reduced surface-bulk coupling," Nature Communications, Nature, vol. 14(1), pages 1-9, December.

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