Femtosecond phase-resolved microscopy of plasmon dynamics in individual gold nanospheres

TL;DR

This paper introduces a phase-sensitive four-wave mixing microscopy technique that enables ultrafast, background-free measurement of dielectric function changes in individual gold nanoparticles, advancing nanoscale optical analysis.

Contribution

The study presents a novel heterodyne FWM microscopy method for phase-resolved ultrafast spectroscopy of single metallic nanoparticles, providing new insights into their plasmon dynamics.

Findings

Resolved ultrafast dielectric changes in single gold NPs

Quantitative analysis via electron temperature and density

Applicable to various metal nanostructures

Abstract

The selective optical detection of individual metallic nanoparticles (NPs) with high spatial and temporal resolution is a challenging endeavour, yet is key to the understanding of their optical response and their exploitation in applications from miniaturised optoelectronics and sensors to medical diagnostics and therapeutics. However, only few reports on ultrafast pump-probe spectroscopy on single small metallic NPs are available to date. Here, we demonstrate a novel phase-sensitive four-wave mixing (FWM) microscopy in heterodyne detection to resolve for the first time the ultrafast changes of real and imaginary part of the dielectric function of single small (<40nm) spherical gold NPs. The results are quantitatively described via the transient electron temperature and density in gold considering both intraband and interband transitions at the surface plasmon resonance. This novel microscopy technique enables background-free detection of the complex susceptibility change even in highly scattering environments and can be readily applied to any metal nanostructure.