Numerical Modeling of Transient Absorption in Hybrid Dual-Plasmonic Au/CuS Nanostructures

TL;DR

This paper uses numerical modeling to analyze transient absorption in hybrid Au/CuS nanostructures, clarifying the dual-plasmonic behavior and Landau damping mechanisms observed experimentally.

Contribution

It introduces a numerical approach to simulate transient absorption in hybrid plasmonic nanostructures, supporting experimental findings and elucidating underlying physical mechanisms.

Findings

Numerical simulations confirm the UFO-shaped geometry of nanostructures.

Size ratio between Au and CuS influences plasmonic response.

Simulation results qualitatively match experimental transient absorption data.

Abstract

Transient absorption in plasmonic materials has recently attracted attention of the chemistry and optics communities as a technique to understand dynamic processes and hot carriers generation on ultrafast timescales. In this context, hybrid Au/CuS nanostructures were recently investigated via ultrafast pump-probe transient absorption spectroscopy revealing an exotic dual-plasmonic behavior. Namely, the excitation of a localized surface plasmon resonance (LSPR) in Au (pump at 551 nm) or CuS (pump at 1051 nm), leads to a transient response in the counterpart. This phenomenon was attributed to Landau damping, which stems from hot carrier generation and injection mechanisms at the interface between the two materials. Here, we employ numerical modeling to further clarify the origin of such response in hybrid Au/CuS nanostructures. The geometry of the hybrid nanostructures is first investigated via steady-state simulations (only probe), confirming an UFO-shaped configuration. We provide clarification on the role of the size ratio between Au and CuS. Finally, we present the simulation of transient absorption in the pump-probe regime, which qualitatively replicates our experimental observations, thus identifying the plasmonic response modified via Landau damping as the main governing mechanism. Our numerical approach provides an important tool for the modeling of transient absorption spectroscopy and can support experimental research on dual-plasmonic materials for applications in spectroscopy, photocatalysis, thermoplasmonics, sensing, and energy harvesting.