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The selective optical detection of individual metallic nanoparticles (NPs)with high spatial and temporal resolution is a challenging endeavour, yet iskey to the understanding of their optical response and their exploitation inapplications from miniaturised optoelectronics and sensors to medicaldiagnostics and therapeutics. However, only few reports on ultrafast pump-probespectroscopy on single small metallic NPs are available to date. Here, wedemonstrate a novel phase-sensitive four-wave mixing (FWM) microscopy inheterodyne detection to resolve for the first time the ultrafast changes ofreal and imaginary part of the dielectric function of single small (<40nm)spherical gold NPs. The results are quantitatively described via the transientelectron temperature and density in gold considering both intraband andinterband transitions at the surface plasmon resonance. This novel microscopytechnique enables background-free detection of the complex susceptibilitychange even in highly scattering environments and can be readily applied to anymetal nanostructure.

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