Ultrafast Plasmonic Control of Second Harmonic Generation

Efficient frequency conversion techniques are crucial to the development of plasmonic metasurfaces for information processing and signal modulation. In principle, nanoscale electric-field confinement in nonlinear materials enables higher harmonic conversion efficiencies per unit volume than those attainable in bulk materials. Here we demonstrate efficient second-harmonic generation (SHG) in a serrated nanogap plasmonic geometry that generates steep electric field gradients on a dielectric metasurface. An ultrafast pump is used to control plasmon-induced electric fields in a thin-film material with inversion symmetry that, without plasmonic enhancement, does not exhibit an an even-order nonlinear optical response. The temporal evolution of the plasmonic near-field is characterized with ~100as resolution using a novel nonlinear interferometric technique. The ability to manipulate nonlinear signals in a metamaterial geometry as demonstrated here is indispensable both to understanding the ultrafast nonlinear response of nanoscale materials, and to producing active, optically reconfigurable plasmonic devices