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Marcus inverted region of charge transfer from low-dimensional semiconductor materials

Author

Listed:
  • Junhui Wang

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences)

  • Tao Ding

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences)

  • Kaimin Gao

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences
    University of the Chinese Academy of Sciences)

  • Lifeng Wang

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences
    University of the Chinese Academy of Sciences)

  • Panwang Zhou

    (Shandong University)

  • Kaifeng Wu

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences
    University of the Chinese Academy of Sciences)

Abstract

A key process underlying the application of low-dimensional, quantum-confined semiconductors in energy conversion is charge transfer from these materials, which, however, has not been fully understood yet. Extensive studies of charge transfer from colloidal quantum dots reported rates increasing monotonically with driving forces, never displaying an inverted region predicted by the Marcus theory. The inverted region is likely bypassed by an Auger-like process whereby the excessive driving force is used to excite another Coulomb-coupled charge. Herein, instead of measuring charge transfer from excitonic states (coupled electron-hole pairs), we build a unique model system using zero-dimensional quantum dots or two-dimensional nanoplatelets and surface-adsorbed molecules that allows for measuring charge transfer from transiently-populated, single-charge states. The Marcus inverted region is clearly revealed in these systems. Thus, charge transfer from excitonic and single-charge states follows the Auger-assisted and conventional Marcus charge transfer models, respectively. This knowledge should enable rational design of energetics for efficient charge extraction from low-dimensional semiconductor materials as well as suppression of the associated energy-wasting charge recombination.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-26705-x
    DOI: 10.1038/s41467-021-26705-x
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    References listed on IDEAS

    as
    1. 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.
    2. Lifeng Wang & Zongwei Chen & Guijie Liang & Yulu Li & Runchen Lai & Tao Ding & Kaifeng Wu, 2019. "Observation of a phonon bottleneck in copper-doped colloidal quantum dots," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    3. Runchen Lai & Yangyi Liu & Xiao Luo & Lan Chen & Yaoyao Han & Meng Lv & Guijie Liang & Jinquan Chen & Chunfeng Zhang & Dawei Di & Gregory D. Scholes & Felix N. Castellano & Kaifeng Wu, 2021. "Shallow distance-dependent triplet energy migration mediated by endothermic charge-transfer," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    4. Xiao Luo & Yaoyao Han & Zongwei Chen & Yulu Li & Guijie Liang & Xue Liu & Tao Ding & Chengming Nie & Mei Wang & Felix N. Castellano & Kaifeng Wu, 2020. "Mechanisms of triplet energy transfer across the inorganic nanocrystal/organic molecule interface," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
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