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Spin blockade and phonon bottleneck for hot electron relaxation observed in n-doped colloidal quantum dots

Author

Listed:
  • Junhui Wang

    (Chinese Academy of Sciences)

  • Lifeng Wang

    (Chinese Academy of Sciences
    University of the Chinese Academy of Sciences)

  • Shuwen Yu

    (Chinese Academy of Sciences)

  • Tao Ding

    (Chinese Academy of Sciences
    University of Science and Technology of China)

  • Dongmei Xiang

    (Chinese Academy of Sciences)

  • Kaifeng Wu

    (Chinese Academy of Sciences)

Abstract

Understanding and manipulating hot electron dynamics in semiconductors may enable disruptive energy conversion schemes. Hot electrons in bulk semiconductors usually relax via electron-phonon scattering on a sub-picosecond timescale. Quantum-confined semiconductors such as quantum dots offer a unique platform to prolong hot electron lifetime through their size-tunable electronic structures. Here, we study hot electron relaxation in electron-doped (n-doped) colloidal CdSe quantum dots. For lightly-doped dots we observe a slow 1Pe hot electron relaxation (~10 picosecond) resulting from a Pauli spin blockade of the preoccupying 1Se electron. For heavily-doped dots, a large number of electrons residing in the surface states introduce picosecond Auger recombination which annihilates the valance band hole, allowing us to observe 300-picosecond-long hot electrons as a manifestation of a phonon bottleneck effect. This brings the hot electron energy loss rate to a level of sub-meV per picosecond from a usual level of 1 eV per picosecond. These results offer exciting opportunities of hot electron harvesting by exploiting carrier-carrier, carrier-phonon and spin-spin interactions in doped quantum dots.

Suggested Citation

  • Junhui Wang & Lifeng Wang & Shuwen Yu & Tao Ding & Dongmei Xiang & Kaifeng Wu, 2021. "Spin blockade and phonon bottleneck for hot electron relaxation observed in n-doped colloidal quantum dots," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-020-20835-4
    DOI: 10.1038/s41467-020-20835-4
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    Cited by:

    1. Junhui Wang & Tao Ding & Kaimin Gao & Lifeng Wang & Panwang Zhou & Kaifeng Wu, 2021. "Marcus inverted region of charge transfer from low-dimensional semiconductor materials," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    2. Xingzhi Wang & Yan Gao & Xiaonan Liu & Huaiyu Xu & Ruixiang Liu & Jiaojiao Song & Bo Li & Huaibin Shen & Fengjia Fan, 2024. "Strong high-energy exciton electroluminescence from the light holes of polytypic quantum dots," Nature Communications, Nature, vol. 15(1), pages 1-8, December.

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