Far-field Petahertz Sampling of Plasmonic Fields

The collective response of metal nanostructures to optical excitation leads to localized plasmon generation with nanoscale field confinement driving applications in e.g. quantum optics, optoelectronics, and nanophotonics, where a bottleneck is the ultrafast loss of coherence by different damping channels. The present understanding is built-up on indirect measurements dictated by the extreme timescales involved. Here, we introduce a straightforward field sampling method that allows to measure the plasmonic field of arbitrary nanostructures in the most relevant petahertz regime. We compare experimental data for colloidal nanoparticles to finite-difference-time-domain calculations, which show that the dephasing of the plasmonic excitation can be resolved with sub-cycle resolution. Furthermore, we observe a substantial reshaping of the spectral phase of the few-cycle pulse induced by this collective excitation and we demonstrate ad-hoc pulse shaping by tailoring the plasmonic sample. The results pave the way towards both a fundamental understanding of ultrafast energy transformation in nanosystems and practical applications of nanostructures in extreme scale spatio-temporal control of light.
Comment: 31 pages, 19 figures