We report a drastic increase of the damping time of plasmonic eigenmodes in resonant bull's eye (BE) nanoresonators to more than 35 fs. This is achieved by tailoring the groove depth of the resonator and by coupling the confined plasmonic field in the aperture to an extended resonator mode such that spatial coherence is preserved over distances of more than 10 μm. Experimentally, this is demonstrated by probing the plasmon dynamics at the field level using broadband spectral interferometry. The nanoresonator allows us to efficiently concentrate the incident field inside the central aperture of the BE and to tailor its local optical nonlinearity by varying the aperture geometry. By replacing the central circular hole with an annular ring structure, we obtain 50-times higher second harmonic generation efficiency, allowing us to demonstrate the efficient concentration of long-lived plasmonic modes inside nanoapertures by interferometric frequency-resolved autocorrelation. Such a light concentration in a nanoresonator with high quality factor has high potential for sensing and coherent control of light-matter interactions on the nanoscale.
A combination of helium- and gallium-ion beam milling together with a fast and reliable sketch-and-peel technique is used to fabricate gold nanorod dimer antennas with an excellent quality factor and with gap distances of less than 6 nm. The high fabrication quality of the sketch-and-peel technique compared to a conventional ion beam milling technique is proven by polarisation-resolved linear dark-field spectromicroscopy of isolated dimer antennas. We demonstrate a strong coupling of the two antenna arms for both fabrication techniques, with a quality factor of more than 14, close to the theoretical limit, for the sketch-and-peel–produced antennas compared to only 6 for the conventional fabrication process. The obtained results on the strong coupling of the plasmonic dimer antennas are supported by finite-difference time-domain simulations of the light-dimer antenna interaction. The presented fabrication technique enables the rapid fabrication of large-scale plasmonic or dielectric nanostructures arrays and metasurfaces with single-digit nanometer scale milling accuracy.
Surface plasmon polaritons (SPPs) are shortlived evanescent waves that can confine light at the surface of metallic nanostructures and transport energy over mesoscopic distances. They may be used to generate and process information encoded as optical signals to realize nanometerscale and ultrafast all-optical circuitry. The propagation properties of these SPPs are defined by the geometry and composition of the nanostructure. Due to their short, femtosecond lifetimes, it has so far proven difficult to track this propagation in the time domain and to directly study the effect of the propagation on the shape of a coherent SPP wavepacket. Here, we introduce an ultrabroadband far-field spectral interferometry method, allowing for the reconstruction of the plasmonic field in the time domain, to characterize coherent SPP propagation in metallic nanostructures. Group velocity and dispersion of SPPs are determined with high precision in a broad frequency range in the visible and near-infrared region, and the propagating SPP field is tracked with high time resolution over distances of tens of micrometers. Our results shed new light on the interplay between nanostructure geometry and coherent SPP propagation and hence are important for probing plasmon−matter interactions as well as for implementations of ultrafast plasmonic circuitry.
Sensing the scattered fields of single metallic nanostructures is a crucial step towards the applications of isolated plasmonic antennas, such as for the sensing of single molecules or nanoparticles. In the past, both near- and far-field spectroscopy methods have been applied to monitor single plasmonic resonances. So far, however, these spectral-domain techniques do not yet provide the femtosecond time resolution that is needed to probe the dynamics of plasmonic fields in the time domain. Here, we introduce a time-domain technique that combines broadband Fourier-transform spectroscopy and spatial modulation spectroscopy (FT-SMS) to quantitatively measure the extinction spectra of the isolated gold nanorods with a nominal footprint of 41×10 nm2. Using a phase-stable pulse pair for excitation, the technique is capable of rejecting off-resonant stray fields and providing absolute measurements of the extinction cross section. Our results indicate that the method is well suited for measuring the optical response of strongly coupled hybrid systems with high signal-to-noise ratio. It may form the basis for new approaches towards time-domain spectroscopy of single nanoantennas with few-cycle time resolution.
Metallic nanostructures
can transport electromagnetic fields in
the form of surface plasmon polariton (SPP) excitations, focus them
into nanometric spots, and transfer them to nearby nanostructures
by near-field coupling. This provides a basic functionality for designing
new plasmonic devices that can greatly enhance light–matter
coupling and facilitate ultrafast and efficient all-optical switching
on the nanoscale. Here, we study a prototypical device geometry, a
bow-tie antenna equipped with curved line gratings, for the efficient
coupling of light into and across the antenna nanogap. We experimentally
demonstrate the spectrally broadband launching and propagation of
SPP waves over more than 10 μm on one arm of the antenna, their
focusing into and transmission across the gap being studied by the
plasmon outcoupling on the other arm. A substantial increase in the
coupling efficiency for antennas with gap widths below 20 nm proves
that the optical near-field coupling between the two antenna arms
dominates the gap transmission. We find overall transmission efficiencies
for nanofocusing, gap transmission, and plasmon outcoupling of up
to 4%. A finite-difference time-domain simulation supports our experimental
findings. This makes such bow-tie couplers an interesting platform
for sensitively probing near-field coupling to single quantum emitters
and for the ultrafast switching of light by light on the nanoscale.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.