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Oxidation kinetics and non-Marcusian charge transfer in dimensionally confined semiconductors

Author

Listed:
  • Ning Xu

    (Nanjing University)

  • Li Shi

    (Southeast University
    Nanjing University of Posts and Telecommunications)

  • Xudong Pei

    (Nanjing University)

  • Weiyang Zhang

    (Nanjing University)

  • Jian Chen

    (Nanjing University)

  • Zheng Han

    (Shanxi University)

  • Paolo Samorì

    (University of Strasbourg, CNRS, ISIS UMR 7006)

  • Jinlan Wang

    (Southeast University
    Suzhou Laboratory)

  • Peng Wang

    (University of Warwick)

  • Yi Shi

    (Nanjing University)

  • Songlin Li

    (Nanjing University)

Abstract

Electrochemical reactions represent essential processes in fundamental chemistry that foster a wide range of applications. Although most electrochemical reactions in bulk substances can be well described by the classical Marcus-Gerischer charge transfer theory, the realistic reaction character and mechanism in dimensionally confined systems remain unknown. Here, we report the multiparametric survey on the kinetics of lateral photooxidation in structurally identical WS2 and MoS2 monolayers, where electrochemical oxidation occurs at the atomically thin monolayer edges. The oxidation rate is correlated quantitatively with various crystallographic and environmental parameters, including the density of reactive sites, humidity, temperature, and illumination fluence. In particular, we observe distinctive reaction barriers of 1.4 and 0.9 eV for the two structurally identical semiconductors and uncover an unusual non-Marcusian charge transfer mechanism in these dimensionally confined monolayers due to the limit in reactant supplies. A scenario of band bending is proposed to explain the discrepancy in reaction barriers. These results add important knowledge into the fundamental electrochemical reaction theory in low-dimensional systems.

Suggested Citation

  • Ning Xu & Li Shi & Xudong Pei & Weiyang Zhang & Jian Chen & Zheng Han & Paolo Samorì & Jinlan Wang & Peng Wang & Yi Shi & Songlin Li, 2023. "Oxidation kinetics and non-Marcusian charge transfer in dimensionally confined semiconductors," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-39781-y
    DOI: 10.1038/s41467-023-39781-y
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    References listed on IDEAS

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    1. Yuan Liu & Xidong Duan & Hyeon-Jin Shin & Seongjun Park & Yu Huang & Xiangfeng Duan, 2021. "Promises and prospects of two-dimensional transistors," Nature, Nature, vol. 591(7848), pages 43-53, March.
    2. Mao-Lin Chen & Xingdan Sun & Hang Liu & Hanwen Wang & Qianbing Zhu & Shasha Wang & Haifeng Du & Baojuan Dong & Jing Zhang & Yun Sun & Song Qiu & Thomas Alava & Song Liu & Dong-Ming Sun & Zheng Han, 2020. "A FinFET with one atomic layer channel," Nature Communications, Nature, vol. 11(1), pages 1-7, December.
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