Electron beam imaging and spectroscopy of plasmonic nanoantenna resonances

Abstract

Nanoantennas are metal structures that provide strong optical coupling between a nanoscale volume and the far field. This coupling is mediated by surface plasmons, oscillations of the free electrons in the metal. Increasing the control over the resonant plasmonic field distribution opens up a wide range of applications of nanoantennas operating both in receiving and transmitting mode. This thesis presents how the dispersion and confinement of surface plasmons in nanoantennas are resolved and further engineered. Fabrication of nanostructures is done using focused ion beam milling (FIB) in metallic surfaces. We demonstrate that patterning in single-crystal substrates allows us to precisely control the geometry in which plasmons are confined. The nanoscale properties of the resonant plasmonic fields are resolved using a new technique developed in this thesis: angle- and polarization controlled cathodoluminescence (CL) imaging spectroscopy. The use of a tightly focused e lectron beam allows us to probe the optical antenna properties with deep subwavelength resolution. We show using this technique that nanoantennas consisting of 500-1200 nm long polycrystalline Au nanowires support standing plasmon waves. We directly observe the plasmon wavelengths which we use to derive the dispersion relation of guided nanowire plasmons. A 590-nm-long ridge-shaped nanoantenna was fabricated using FIB milling on a single-crystal Au substrate, demonstrating a level of control over the fabrication impossible with polycrystalline metals. CL experiments show that the ridge supports multiple-order resonances. The confinement of surface plasmons to the ridge is confirmed by boundary-element-method (BEM) calculations. The resonant modes in plasmonic whispering gallery cavities consisting of a FIB-fabricated circular groove are resolved. We find an excellent agreement between boundary element method calculations and the measured CL emission from the ring-shaped cavities. The c alculations show that the ring supports resonances with increasing azimuthal or radial order. The smallest cavity fits only one wavelength in its circumference. We theoretically show that in these cavities, spontaneous emission can be enhanced over a broad spectral band due to the small modal volume of the plasmon resonances. A Purcell factor >2000 was found. We further study the mode symmetries and coupling of the ring resonances using far-field excitation, fluorescence, angle-resolved cathodoluminescence and photoelectron emission microscopy. We demonstrate spectral reshaping of emitters, mode-specific angular emission patterns, and a mode-selective excitation by incoming light, and we directly resolve the modal fields at high resolution. In the next chapter, we present metal-insulator-metal plasmon waveguides in which we engineer the dispersion to reach a refractive index of zero. Using spatially- and angle-resolved CL we directly observe the spatial mode profiles and determine t he dispersion relation of plasmon modes. At the cutoff frequency, the emission pattern corresponds to that of a line dipole antenna demonstrating the entire waveguide is in phase (n=0). A strongly enhanced density of optical states is directly observed at cutoff from the enhanced CL intensity. Finally, we present 5 possible applications: a localized surface plasmon sensor, a plasmon ring laser, template stripping technique, an in-situ monitor of ionoluminescence and cathodoluminescence in a FIB system and a single-photon source