Angle-resolved cathodoluminescence imaging polarimetry

Cathodoluminescence spectroscopy (CL) allows characterizing light emission in bulk and nanostructured materials and is a key tool in fields ranging from materials science to nanophotonics. Previously, CL measurements focused on the spectral content and angular distribution of emission, while the polarization was not fully determined. Here we demonstrate a technique to access the full polarization state of the cathodoluminescence emission, that is the Stokes parameters as a function of the emission angle. Using this technique, we measure the emission of metallic bullseye nanostructures and show that the handedness of the structure as well as nanoscale changes in excitation position induce large changes in polarization ellipticity and helicity. Furthermore, by exploiting the ability of polarimetry to distinguish polarized from unpolarized light, we quantify the contributions of different types of coherent and incoherent radiation to the emission of a gold surface, silicon and gallium arsenide bulk semiconductors. This technique paves the way for in-depth analysis of the emission mechanisms of nanostructured devices as well as macroscopic media.Comment: 8 figures. Includes supplementary informatio

Directional emission from leaky and guided modes in GaAs nanowires measured by cathodoluminescence

8 págs.; 4 figs.We measure the polarization-resolved angular emission distribution from thin and thick GaAs nanowires (diameters ∼110 and ∼180 nm) with cathodoluminescence polarimetry. The nanowires, which horizontally rest on a thin carbon film, are excited by a 5 keV electron beam and emit band gap luminescence at a central wavelength of 870 nm. The emission can couple to different waveguide modes that propagate along the wire, are dependent on the wire diameter, and determine the directionality and polarization of the emission. Although each measured nanowire can support different modes, the polarized emission is dominated by the TM01 waveguide mode in all cases, independently of wire diameter. When exciting the nanowires close to the end facets, the thin and thick wires exhibit opposite directional emission. The emission from thin nanowires is dominated by a leaky TM01 mode that leads to emission toward the opposite end facet (emission to the right when exciting the left-side edge). For the thick wires, however, the TM01 mode is guided but also lossy due to absorption in the substrate. In such a case, the wires emit toward the excited end facet (to the left when exciting the left-side edge). The emission directionality switches for nanowire diameters in the range of 145-170 nm. We show that the measurements agree well with both a simple 1D current model and numerical simulations. The high spatial resolution of angle- and polarization-resolved cathodoluminescence spectroscopy provides detailed insight into the nanoscale emission and propagation of light in semiconductor nanowires. Copyright © 2016 American Chemical SocietyThis work is part of the Stichting voor Fundamenteel Onderzoek der Materie (FOM) as well as the Dutch Technology Foundation STW, which are financially supported by the Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO) and the Dutch Ministry of Economic Affairs. It is also part of NanoNextNL, a nanotechnology program funded by the Dutch Ministry of Economic Affairs, part of an industrial partnership program between Philips and FOM, and is supported by the European Research Council (ERC). The Spanish Ministerio de Economıía y Competitividad is also acknowledged for financial support through the grants NANOPLAS+ (FIS2012-31070) and LENSBEAM (FIS2015- 69295-C3-2-P).Peer Reviewe

Near-infrared spectroscopic cathodoluminescence imaging polarimetry on silicon photonic crystal waveguides

We measure polarization- and wavelength-resolved spectra and spatial emission intensity distributions from silicon photonic crystal waveguides in the near-infrared spectral range using spectroscopic cathodoluminescence imaging polarimetry. A 30 keV electron beam, incident along the surface normal of the sample, acts as an ultrabroadband and deeply subwavelength excitation source. For photonic crystal waveguides with a broad range of design parameters, we observe a dominant emission intensity distribution that is strongly confined to the waveguide. For a period of 420 nm and a hole radius of 120 nm, this occurs at a wavelength of 1425 nm. The polarization-resolved measurements demonstrate that this feature is fully linearly polarized along the waveguide axis. Comparing the modal pattern and polarization to calculations of the electric field profiles confirms that we measure the odd TE waveguide mode of the system. This result demonstrates that the electron beam can couple to modes dominated by in-plane field components in addition to the more commonly observed modes dominated by out-of-plane field components. From the emission directionality, we conclude that we sample a leaky portion of the odd waveguide mode

Angle-Resolved Cathodoluminescence Imaging Polarimetry

Cathodoluminescence spectroscopy (CL) allows characterizing light emission in bulk and nanostructured materials and is a key tool in fields ranging from materials science to nanophotonics. Previously, CL measurements focused on the spectral content and angular distribution of emission, while the polarization was not fully determined. Here we demonstrate a technique to access the full polarization state of the cathodoluminescence emission, that is the Stokes parameters as a function of the emission angle. Using this technique, we measure the emission of metallic bullseye nanostructures and show that the handedness of the structure as well as nanoscale changes in excitation position induce large changes in polarization ellipticity and helicity. Furthermore, by exploiting the ability of polarimetry to distinguish polarized from unpolarized light, we quantify the contributions of different types of coherent and incoherent radiation to the emission of a gold surface, silicon and gallium arsenide bulk semiconductors. This technique paves the way for in-depth analysis of the emission mechanisms of nanostructured devices as well as macroscopic media

Gallium Plasmonics: Deep Subwavelength Spectroscopic Imaging of Single and Interacting Gallium Nanoparticles

Gallium has recently been demonstrated as a phase-change plasmonic material offering UV tunability, facile synthesis, and a remarkable stability due to its thin, self-terminating native oxide. However, the dense irregular nanoparticle (NP) ensembles fabricated by molecular-beam epitaxy make optical measurements of individual particles challenging. Here we employ hyperspectral cathodoluminescence (CL) microscopy to characterize the response of single Ga NPs of various sizes within an irregular ensemble by spatially and spectrally resolving both in-plane and out-of-plane plasmonic modes. These modes, which include hybridized dipolar and higher-order terms due to phase retardation and substrate interactions, are correlated with finite difference time domain (FDTD) electrodynamics calculations that consider the Ga NP contact angle, substrate, and native Ga/Si surface oxidation. This study experimentally confirms previous theoretical predictions of plasmonic size-tunability in single Ga NPs and demonstrates that the plasmonic modes of interacting Ga nanoparticles can hybridize to produce strong hot spots in the ultraviolet. The controlled, robust UV plasmonic resonances of gallium nanoparticles are applicable to energy- and phase-specific applications such as optical memory, environmental remediation, and simultaneous fluorescence and surface-enhanced Raman spectroscopies

Nanoscale Spatial Coherent Control over the Modal Excitation of a Coupled Plasmonic Resonator System

We demonstrate coherent control over the optical response of a coupled plasmonic resonator by high-energy electron beam excitation. We spatially control the position of an electron beam on a gold dolmen and record the cathodoluminescence and electron energy loss spectra. By selective coherent excitation of the dolmen elements in the near field, we are able to manipulate modal amplitudes of bonding and antibonding eigenmodes. We employ a combination of CL and EELS to gain detailed insight in the power dissipation of these modes at the nanoscale as CL selectively probes the radiative response and EELS probes the combined effect of Ohmic dissipation and radiation

Fano-Resonances in High Index Dielectric Nanowires for Directional Scattering

International audienceHigh refractive index dielectric nanostructures provide original optical properties thanks to the occurrence of size- and shape-dependent optical resonance modes. These modes commonly present a spectral overlap of broad, low-order modes (\textit{e.g}. dipolar modes) and much narrower, higher-order modes. The latter are usually characterized by a rapidly varying frequency-dependent phase, which - in superposition with the lower order mode of approximately constant phase - leads to typical spectral features known as Fano resonances. Interestingly, such Fano resonances occur in dielectric nanostructures of the simplest shapes. In spheroidal nanoparticles, interference between broad magnetic dipole and narrower electric dipole modes can be observed. In high aspect-ratio structures like nanowires, either the electric or the magnetic dipolar mode (depending on the illumination conditions) interferes with higher order multipole contributions of the same nature (electric or magnetic). Using the analytical Mie theory, we analyze the occurrence of Fano resonances in high-index dielectric nanowires and discuss their consequences like unidirectional scattering. By means of numerical simulations, we furthermore study the impact on those Fano resonances of the shape of the nanowire cross-sections as well as the coupling of two parallel nanowires. The presented results show that all-dielectric nanostructures, even of simple shapes, provide a reliable low-loss alternative to plasmonic nanoantennas