Many-Body Interaction Governs the Ultrafast Relaxation Dynamics of Hot Holes in CuS Nanoflakes and Photocatalytic Efficiency-Enhanced CuS/Ag2S NanocompositesClick to copy article linkArticle link copied!
- Soumya MukherjeeSoumya MukherjeeDepartment of Physical Sciences, Indian Institute of Science Education and Research Kolkata, Nadia, Mohanpur 741246, West Bengal, IndiaMore by Soumya Mukherjee
- Anjan Kumar NMAnjan Kumar NMDepartment of Physical Sciences, Indian Institute of Science Education and Research Kolkata, Nadia, Mohanpur 741246, West Bengal, IndiaMore by Anjan Kumar NM
- Saranya RameshSaranya RameshDepartment of Physical Sciences, Indian Institute of Science Education and Research Kolkata, Nadia, Mohanpur 741246, West Bengal, IndiaMore by Saranya Ramesh
- B. Karthikeyan*B. Karthikeyan*Email: [email protected]Department of Physics, National Institute of Technology Tiruchirappalli, Tiruchirappalli 620015, Tamil Nadu, IndiaMore by B. Karthikeyan
- N. Kamaraju*N. Kamaraju*Email: [email protected]Department of Physical Sciences, Indian Institute of Science Education and Research Kolkata, Nadia, Mohanpur 741246, West Bengal, IndiaMore by N. Kamaraju
Abstract

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.
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