Free Electron-Plasmon Coupling Strength and Near-Field Retrieval through Electron Energy-Dependent Cathodoluminescence Spectroscopy.

Tightly confined optical near fields in plasmonic nanostructures play a pivotal role in important applications ranging from optical sensing to light harvesting. Energetic electrons are ideally suited to probing optical near fields by collecting the resulting cathodoluminescence (CL) light emission. Intriguingly, the CL intensity is determined by the near-field profile along the electron propagation direction, but the retrieval of such field from measurements has remained elusive. Furthermore, the conditions for optimum electron near-field coupling in plasmonic systems are critically dependent on such field and remain experimentally unexplored. In this work, we use electron energy-dependent CL spectroscopy to study the tightly confined dipolar mode in plasmonic gold nanoparticles. By systematically studying gold nanoparticles with diameters in the range of 20-100 nm and electron energies from 4 to 30 keV, we determine how the coupling between swift electrons and the optical near fields depends on the energy of the incoming electron. The strongest coupling is achieved when the electron speed equals the mode phase velocity, meeting the so-called phase-matching condition. In aloof experiments, the measured data are well reproduced by electromagnetic simulations, which explain that larger particles and faster electrons favor a stronger electron near-field coupling. For penetrating electron trajectories, scattering at the particle produces severe corrections of the trajectory that defy existing theories based on the assumption of nonrecoil condition. Therefore, we develop a first-order recoil correction model that allows us to account for inelastic electron scattering, rendering better agreement with measured data. Finally, we consider the albedo of the particles and find that, to approach unity coupling, a highly confined electric field and very slow electrons are needed, both representing experimental challenges. Our findings explain how to reach unity-order coupling between free electrons and confined excitations, helping us understand fundamental aspects of light-matter interaction at the nanoscale.

Phase-retrieval Fourier microscopy of partially temporally coherent nanoantenna radiation patterns.

We report an experimental technique for determining phase-resolved radiation patterns of single nanoantennas by phase-retrieval defocused imaging. A key property of nanoantennas is their ability to imprint spatial coherence, for instance, on fluorescent sources. Yet, measuring emitted wavefronts in absence of a reference field is difficult. We realize a defocused back focal plane microscope to measure phase even for partially temporally coherent light and benchmark the method using plasmonic bullseye antenna scattering. We outline the limitations of defocused imaging which are set by spectral bandwidth and antenna mode structure. This work is a first step to resolve wavefronts from fluorescence controlled by nanoantennas.

Super-Resolution without Imaging: Library-Based Approaches Using Near-to-Far-Field Transduction by a Nanophotonic Structure.

Super-resolution imaging is often viewed in terms of engineering narrow point spread functions, but nanoscale optical metrology can be performed without real-space imaging altogether. In this paper, we investigate how partial knowledge of scattering nanostructures enables extraction of nanoscale spatial information from far-field radiation patterns. We use principal component analysis to find patterns in calibration data and use these patterns to retrieve the position of a point source of light. In an experimental realization using angle-resolved cathodoluminescence, we retrieve the light source position with an average error below λ/100. The patterns found by principal component analysis reflect the underlying scattering physics and reveal the role the scattering nanostructure plays in localization success. The technique described here is highly general and can be applied to gain insight into and perform subdiffractive parameter retrieval in various applications.

Electrons Generate Self-Complementary Broadband Vortex Light Beams Using Chiral Photon Sieves.

Planar electron-driven photon sources have been recently proposed as miniaturized light sources, with prospects for ultrafast conjugate electron-photon microscopy and spectral interferometry. Such sources usually follow the symmetry of the electron-induced polarization: transition-radiation-based sources, for example, only generate p-polarized light. Here we demonstrate that the polarization, the bandwidth, and the directionality of photons can be tailored by utilizing photon-sieve-based structures. We design, fabricate, and characterize self-complementary chiral structures made of holes in an Au film and generate light vortex beams with specified angular momentum orders. The incoming electron interacting with the structure generates chiral surface plasmon polaritons on the structured Au surface that scatter into the far field. The outcoupled radiation interferes with transition radiation creating TE- and TM-polarized Laguerre-Gauss light beams with a chiral intensity distribution. The generated vortex light and its unique spatiotemporal features can form the basis for the generation of structured-light electron-driven photon sources.

Phase-Resolved Surface Plasmon Scattering Probed by Cathodoluminescence Holography.

High-energy (1-100 keV) electrons can coherently couple to plasmonic and dielectric nanostructures, creating cathodoluminescence (CL) of which the spectral features reveal details of the material's resonant modes at a deep-subwavelength spatial resolution. While CL provides fundamental insight in optical modes, detecting its phase has remained elusive. Here, we use Fourier-transform CL holography to determine the far-field phase distribution of fields scattered from plasmonic nanoholes, nanocubes, and helical nanoapertures and reconstruct the angle-resolved phase distributions. From the derived fields, we derive the relative strength and phase of induced scattering dipoles. Fourier-transform CL holography opens up a new world of coherent light scattering and surface wave studies with nanoscale spatial resolution.

Tunable plasmonic HfN nanoparticles and arrays.

We present the fabrication of tunable plasmonic hafnium nitride (HfN) nanoparticles. HfN is a metallic refractory material with the potential of supporting plasmon resonances in the visible range, similar to silver and gold, but with the additional benefits of high melting point, chemical stability, and mechanical hardness. However, the preparation of HfN nanoparticles and the experimental demonstration of their plasmonic potential are still in their infancy. Here, high quality HfN thin films were fabricated, for which ellipsometry shows their plasmonic potential. From these thin films, nanorods and nanotriangles were milled using a focused ion beam and the plasmon resonances were identified using cathodoluminescence mapping. As an alternative fabrication strategy, an optimized electron-beam lithography procedure was used to prepare arrays of HfN nanoparticles, which also exhibited clear surface plasmon resonances. These results pave the way to further explore HfN nanoparticles in plasmonically-powered applications where materials robustness is essential.

Probing the Band Structure of Topological Silicon Photonic Lattices in the Visible Spectrum.

We study two-dimensional hexagonal photonic lattices of silicon Mie resonators with a topological optical band structure in the visible spectral range. We use 30 keV electrons focused to nanoscale spots to map the local optical density of states in topological photonic lattices with deeply subwavelength resolution. By slightly shrinking or expanding the unit cell, we form hexagonal superstructures and observe the opening of a band gap and a splitting of the double-degenerate Dirac cones, which correspond to topologically trivial and nontrivial phases. Optical transmission spectroscopy shows evidence of topological edge states at the domain walls between topological and trivial lattices.

Spatial Resolution of Coherent Cathodoluminescence Super-Resolution Microscopy.

We investigate the nanoscale excitation of Ag nanocubes with coherent cathodoluminescence imaging spectroscopy (CL) to resolve the factors that determine the spatial resolution of CL as a deep-subwavelength imaging technique. The 10-30 keV electron beam coherently excites localized plasmons in 70 nm Ag cubes at 2.4 and 3.1 eV. The radiation from these plasmon modes is collected in the far-field together with the secondary electron intensity. CL line scans across the nanocubes show exponentially decaying tails away from the cube that reveal the evanescent coupling of the electron field to the resonant plasmon modes. The measured CL decay lengths range from 8 nm (10 keV) to 12 nm (30 keV) and differ from the calculated ones by only 1-3 nm. A statistical model of electron scattering inside the Ag nanocubes is developed to analyze the secondary electron images and compare them with the CL data. The Ag nanocube edges are derived from the CL line scans with a systematic error less than 3 nm. The data demonstrate that CL probes the electron-induced plasmon fields with nanometer accuracy.