  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
