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Many-Body Interaction Governs the Ultrafast Relaxation Dynamics of Hot Holes in CuS Nanoflakes and Photocatalytic Efficiency-Enhanced CuS/Ag2S Nanocomposites
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    Many-Body Interaction Governs the Ultrafast Relaxation Dynamics of Hot Holes in CuS Nanoflakes and Photocatalytic Efficiency-Enhanced CuS/Ag2S Nanocomposites
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    • Soumya Mukherjee
      Soumya Mukherjee
      Department of Physical Sciences, Indian Institute of Science Education and Research Kolkata, Nadia, Mohanpur 741246, West Bengal, India
    • Anjan Kumar NM
      Anjan Kumar NM
      Department of Physical Sciences, Indian Institute of Science Education and Research Kolkata, Nadia, Mohanpur 741246, West Bengal, India
    • Saranya Ramesh
      Saranya Ramesh
      Department of Physical Sciences, Indian Institute of Science Education and Research Kolkata, Nadia, Mohanpur 741246, West Bengal, India
    • B. Karthikeyan*
      B. Karthikeyan
      Department of Physics, National Institute of Technology Tiruchirappalli, Tiruchirappalli 620015, Tamil Nadu, India
      *Email: [email protected]
    • N. Kamaraju*
      N. Kamaraju
      Department of Physical Sciences, Indian Institute of Science Education and Research Kolkata, Nadia, Mohanpur 741246, West Bengal, India
      *Email: [email protected]
      More by N. Kamaraju
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    ACS Applied Optical Materials

    Cite this: ACS Appl. Opt. Mater. 2023, 1, 7, 1332–1342
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    https://doi.org/10.1021/acsaom.3c00153
    Published July 4, 2023
    Copyright © 2023 American Chemical Society

    Abstract

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    A detailed nondegenerate ultrafast pump-probe transmission study of CuS nanoflakes and CuS/Ag2S nanocomposites with varying pump fluences is conducted in this work. The measured transient transmission data for CuS are found to originate from a strong photoinduced bleaching of intrinsic holes and a weaker photoinduced absorption of excited electrons. First-order decay-based multiexponential modeling of transient transmission data for CuS reveals three hole decay channels (∼240–410 fs, ∼24–144 ps, ≳10 μs) along with the electron decay channel of ∼1.0–2.6 ps, whereas for CuS/Ag2S, the weaker electron decay channel disappears due to the localization of hot electrons in the conduction band of Ag2S and an additional hole decay channel appears, making a total of four decay channels for the holes (∼230–470 fs, ∼10–49 ps, ≳10 μs, ∼132–326 ps). When the pump fluence is varied, these decay time constants are found to change considerably, indicating the presence of higher-order decay processes, which must be considered in the theoretical modeling of the decay of excited carriers. Therefore, we have modeled the time evolution of hot hole density using the empirical kinetic rate equation and extracted the higher-order rate constants. Both the second- and third-order rate constants are found to be almost one order lesser for CuS/Ag2S, compared to those of CuS, indicating that the overall decay process is getting slower for CuS/Ag2S, causing enhanced photocatalytic activity.

    Copyright © 2023 American Chemical Society

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    Supporting Information

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    This article is cited by 3 publications.

    1. Yuhao Jin, Zhenyi Zhang, Huijuan Zheng, Xianghan Cheng, Longlong Geng, Zheng Zhou, Haixiang Han. Unveiling the Formation Mechanism for Binary Semiconductor Nanoclusters: a Two-Step Pathway to a Double-Shell Structured Copper Sulfide Nanocluster. ACS Nano 2024, 18 (49) , 33681-33695. https://doi.org/10.1021/acsnano.4c13264
    2. Pradeep Kumar, Bhaskar De, Rishabh Tripathi, Rohan Singh. Exciton-exciton interaction: A quantitative comparison between complimentary phenomenological models. Physical Review B 2024, 109 (15) https://doi.org/10.1103/PhysRevB.109.155423
    3. Soumya Mukherjee, Anjan Kumar NM, Ayan Mondal, Venkataramanan Mahalingam, N. Kamaraju. Trapping and exciton-exciton annihilation assisted ultrafast carrier dynamics in nanosheets of 2H–MoSe2 and Cr doped 1T/2H–MoSe2. The Journal of Chemical Physics 2023, 159 (16) https://doi.org/10.1063/5.0173311

    ACS Applied Optical Materials

    Cite this: ACS Appl. Opt. Mater. 2023, 1, 7, 1332–1342
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsaom.3c00153
    Published July 4, 2023
    Copyright © 2023 American Chemical Society

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