Few-femtosecond plasmon dephasing of a single metallic nanostructure from optical response function reconstruction by...

The precise characterization of the ultrafast optical response of metals and metallic nanostructures has remained an experimental challenge. We probe the few-femtosecond electronic dephasing of a local surface plasmon polariton excitation using symmetry-selective second-harmonic (SH) Rayleigh scattering of a nanoscopic conical gold tip as an individual plasmonic nanostructure. The full reconstruction of the optical response function of the plasmon excitation with phase and amplitude without any model assumptions is demonstrated from the analysis of the two-dimensional spectrogram obtained by simultaneous time- and frequency-domain SH measurements, using interferometric frequency resolved optical gating. The measured dephasing time of T(2) = 18 +/- 5 fs indicates the plasmon damping is dominated by nonradiative decay, consistent with a Drude-Sommerfeld dielectric response for gold. Even for the nominally homogeneous localized plasmon response, deviations are observed from the ideal harmonic oscillator phase behavior, which may reflect the underlying inhomogeneous electronic response with its different scattering channels. The presented technique is generally applicable for the reconstruction of the plasmon dynamics of complex nanostructures: information that cannot be obtained by conventional dark-field scattering.