We report a measurement on the temporal response of a plasmonic antenna at the femtosecond time scale. The antenna consists of a square array of nanometer-size gold rods. We find that the far-field dispersion of light reflected from the plasmonic antenna is less than that of a 1.2 mm thick glass slide. Assuming a simple oscillating dipole model this implies that the near-field of the antenna may be used as an electron switch that responds faster than 20 fs. Alternatively, ultrafast electron diffraction may be used to investigate the near-field dynamics of the plasmonic antenna.
We investigate the chiroptical response of a single plasmonic nanohelix interacting with a weakly-focused circularly-polarized Gaussian beam. The optical scattering at the fundamental resonance is characterized experimentally, and the chiral behavior of the nanohelix is explained based on a multipole analysis. The angularly resolved emission of the excited nanohelix is verified experimentally and it validates the theoretical results. Further, we study the first higher-order resonance and explain the formation of chiral dipoles in both cases.
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
Starting from first principles, we theoretically model the nonlinear temporal dynamics of gold-based plasmonic devices resulting from the heating of their metallic components. At optical frequencies, the gold susceptibility is determined by the interband transitions around the X,L points in the first Brillouin zone and thermo-modulational effects ensue from Fermi smearing of the electronic energy distribution in the conduction band. As a consequence of light-induced heating of the conduction electrons, the optical susceptibility becomes nonlinear. In this paper we describe, for the first time to our knowledge, the effects of the thermo-modulational nonlinearity of gold on the propagation of surface plasmon polaritons guided on gold nanowires. We introduce a novel nonlinear Schroedinger-like equation to describe pulse propagation in such nanowires, and we predict the appearance an intense spectral red-shift caused by the delayed thermal response.
The nonlinear optical response of materials to exciting light is enhanced by resonances between the incident laser frequencies and the energy levels of the excited material. Traditionally, in molecular nonlinear spectroscopy one tunes the input laser frequencies to the molecular energy levels for highly enhanced doubly or triply resonant interactions. With metasurfaces the situation is different, and by proper design of the nanostructures, one may tune the material energy levels to match the incoming laser frequencies. Here we use multi-parameter genetic algorithm methodologies to optimize the nonlinear Four Wave Mixing response, and show that the intuitive conventional approach of trying to match the transmission spectrum to the relevant laser frequencies indeed leads to strong enhancement, but not necessarily to the optimal design. We demonstrate, experimentally and by direct nonlinear field calculations, that the near field mode distribution and spatial modes overlap are the dominant factor for optimized design.
Femtosecond-scale polarization state conversion is experimentally found in optical response of a plasmonic nanograting by means of time-resolved polarimetry. Simultaneous measurements of the Stokes parameters as a function of time with an averaging time-gate of 130 fs reveal a remarkable alteration of polarization state inside a single fs-pulse reflected from a plasmonic crystal. Time-dependent depolarization is experimentally found and described within an analytical model which predicts the four-fold enhancement of the polarization conversion effect with the use of the narrower gate. The effect is attributed to excitation of time-delayed polarization-sensitive surface plasmons with a highly birefringent Fano-type spectral profile.
Maria Becker
,Wayne Cheng-Wei Huang
,Herman Batelaan
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(2012)
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"Measurement of the Ultrafast Temporal Response of a Plasmonic Antenna"
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Hermanus Batelaan
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