Nahid Talebi

Toroidal Plasmonic Eigenmodes in Oligomer Nanocavities for the Visible

Plasmonics has become one of the most vibrant areas in research with technological innovations impacting fields from telecommunications to medicine. Many fascinating applications of plasmonic nanostructures employ electric dipole and higher-order multipole resonances. Also magnetic multipole resonances are recognized for their unique properties. Besides these multipolar modes that easily radiate into free space, other types of electromagnetic resonances exist, so-called toroidal eigenmodes, which have been largely overlooked historically. They are strongly bound to material structures and their peculiar spatial structure renders them practically invisible to conventional optical microscopy techniques. In this Letter, we demonstrate toroidal modes in a metal ring formed by an oligomer of holes. Combined energy-filtering transmission electron microscopy and three-dimensional finite difference time domain analysis reveal their distinct features. For the study of these modes that cannot be excited by optical far-field spectroscopy, energy-filtering transmission electron microscopy emerges as the method of choice. Toroidal moments bear great potential for novel applications, for example, in the engineering of Purcell factors of quantum-optical emitters inside toroidal cavities.

Hybridized metal slit eigenmodes as an illustration of Babinet's principle

By energy-filtering transmission electron microscopy (EFTEM), we observe Fabry-Pérot-like surface plasmon resonances (SPRs) along the length of rectangular single and double slits drilled into free-standing thin silver films. These eigenmodes hybridize in closely situated slits. The nature of their lateral coupling is uncovered from finite-element simulations, which show that the symmetry and energy sequence of hybrid modes is governed by Babinet complementarity principles. Interestingly, the modes of a double slit system, being proto-self-complementary, may alternatively be explained by magnetic interactions between slit fields or by electrostatic interactions across the metallic bridge separating the slits.

Numerical simulations of interference effects in photon-assisted electron energy-loss spectroscopy

Although the electromagnetic resonances of individual nanostructures can be studied by electron or photon interactions alone, exciting new possibilities open up through the simultaneous use of both. In photon-induced near-field electron microscopy (PINEM), for example, single nanostructures are optically excited by short, intense pulses and concurrently imaged with high spatial resolution by fast electrons, which act as negligible probes of electric fields. Controlling their relative arrival time provides access to the dynamics of the electromagnetic response in the near field by recording images of the electron energy loss (or gain) spectra. In this paper, we investigate the transition from optically dominated PINEM to conventional, electron-dominated electron energy-loss spectroscopy (EELS). During the systematic reduction of optical excitation intensity to zero, a novel electro-optical interference effect emerges. It reveals itself at those optical field strengths that lead to prominently visible constructive and destructive interference patterns of the optical and electron radiation fields which are scattered by a nanostructure. The interference patterns reported here allow one to achieve higher temporal, energy and spatial resolutions of the modal dynamics in electron microscopy.

Breaking the mode degeneracy of surface plasmon resonances in a triangular system

In this paper, we present a systematic investigation of symmetry-breaking in the plasmonic modes of triangular gold nanoprisms. Their geometrical C(3v) symmetry is one of the simplest possible that allows degeneracy in the particles mode spectrum. It is reduced to the nondegenerate symmetries C(v) or E by positioning additional, smaller gold nanoprisms in close proximity, either in a lateral or a vertical configuration. Corresponding to the lower symmetry of the system, its eigenmodes also feature lower symmetries (C(v)), or preserve only the identity (E) as symmetry. We discuss how breaking the symmetry of the plasmonic system not only breaks the degeneracy of some lower order modes, but also how it alters the damping and eigenenergies of the observed Fano-type resonances.

Wedge Dyakonov Waves and Dyakonov Plasmons in Topological Insulator Bi2Se3 Probed by Electron Beams.

Bi2Se3 has recently attracted a lot of attention because it has been reported to be a platform for the realization of three-dimensional topological insulators. Due to this exotic characteristic, it supports excitations of a two-dimensional electron gas at the surface and, hence, formation of Dirac-plasmons. In addition, at higher energies above its bandgap, Bi2Se3 is characterized by a naturally hyperbolic electromagnetic response, with an interesting interplay between type-I and type-II hyperbolic behaviors. However, still not all the optical modes of Bi2Se3 have been explored. Here, using mainly electron energy-loss spectroscopy and corresponding theoretical modeling we investigate the full photonic density of states that Bi2Se3 sustains, in the energy range of 0.8 eV-5 eV. We show that at energies below 1 eV, this material can also support wedge Dyakonov waves. Furthermore, at higher energies a huge photonic density of states is excited in structures such as waveguides and resonators made of Bi2Se3 due to the hyperbolic dispersion.

Excitation of Mesoscopic Plasmonic Tapers by Relativistic Electrons: Phase Matching versus Eigenmode Resonances

We investigate the optical modes in three-dimensional single-crystalline gold tapers by means of electron energy-loss spectroscopy. At the very proximity to the apex, a broad-band excitation at all photon energies from 0.75 to 2 eV, which is the onset for interband transitions, is detected. At large distances from the apex, though, we observe distinct resonances with energy dispersions roughly proportional to the inverse local radius. The nature of these phenomena is unraveled by finite difference time-domain simulations of the taper and an analytical treatment of the energy loss in fibers. Our calculations and the perfect agreement with our experimental results demonstrate the importance of phase-matching between electron field and radiative taper modes in mesoscopic structures. The local taper radius at the electron impact location determines the selective excitation of radiative modes with discrete angular momenta.

A directional, ultrafast and integrated few-photon source utilizing the interaction of electron beams and plasmonic nanoantennas

The possibility of using plasmonic nanoantennas in interaction with electron beams to form a wideband few-photon source is demonstrated here using numerical investigations. The generated photons are guided inside a waveguide, which is coupled to the nanoantennas. Using two replicas of a nanoantenna at an optimized distance, and providing a guided path for the emitted photon from the first nanoantenna to the second one by positioning a resonator feedback element, it is possible to form an interference between the photons generated by the two nanoantennas. The interference phenomenon is used to produce a unidirectional flow of power in the waveguide, as well as a high collection efficiency. The investigations are carried out in a self-consistent way, utilizing a conjugate Maxwell and Lorentz system of equations, in order to be able to simulate the modulation of the electron velocity due to the interaction with an optical system which is initially at rest.

Plasmonic nanofocusing – grey holes for light

Abstract Improving the resolution and sensitivity in all-optical microscopy and spectroscopy is inevitably one of the most important challenges in contemporary optical and nanoscience. Here, we discuss a novel approach, plasmonic nanofocusing, towards broadband, coherent all-optical microscopy with ultrahigh temporal and spatial resolution. The conceptual idea is to launch radially symmetric surface plasmon polariton modes onto the shaft of a sharp, conical metal taper. While propagating towards the apex of the pointed taper, the spatial extent of the plasmonic mode gradually shrinks, from several microns in diameter to a spot size of less than 10 nm at the pointed apex of the conical taper. Concomitantly, the local field amplitude of the plasmon mode gradually increases, resulting in a pronounced field enhancement at the apex and – thus – a bright and spatially isolated coherent light source with dimensions far below the diffraction limit. In this review, we characterize the optical properties of such three-dimensional conical metal tapers and demonstrate nanofocusing of radially symmetric plasmon modes. We use this nanolight source for coherent light scattering spectroscopy and demonstrate the sensitivity enhancement resulting from the pronounced spatial field confinement. It is shown that such off-resonant plasmonic nanoantennas facilitate the creation of nanofocused light spots with few-cycle time resolution. As a first application of this ability to nanolocalize ultrashort plasmon wavepackets, we demonstrate remotely-triggered multiphoton-induced photoemission from the very apex of the taper and implement this novel ultrafast electron gun in a point-projection electron microscope. Our results not only indicate the favourable optical properties of this plasmonic nanolens but also suggest that it may find interesting applications in ultrafast scanning optical spectroscopy and might enable new types of ultrafast electron holography and scanning tunnelling microscopy.

Real-space Imaging of Plasmonic Modes of Gold Tapers by EFTEM and EELS

Plasmonic nanoparticles have been extensively studied in the literature due to their ability of supporting localized surface plasmon (LSP) modes. Such structures can localize optical energy on the nanometer scale which opens up the field of optical nanoantennas. Application of nanoantennas in ultrafast optics requires large bandwidth. Unfortunately, the bandwidths of presently realized nanoantennas are small, despite their large radiative and Ohmic losses. Moreover, the coupling efficiency of far-field optical radiation to single nanoantennas is quite low, which is because of the extremely small volume of interaction.

Schrödinger electrons interacting with optical gratings: quantum mechanical study of the inverse Smith–Purcell effect

Slow swift electrons with low self-inertia interact differently with matter and light in comparison with their relativistic counterparts: they are easily recoiled, reflected, and also diffracted form optical gratings and nanostructures. As a consequence, they can be also better manipulated into the desired shape. For example, they get bunched quite fast in interaction with acceleration gratings in presence of an external electromagnetic radiation, a phenomenon which can be desirable in development of superradiant coherent light sources. Here, I examine the spatiotemporal behavior of pulsed electron wave packets at low energies interacting with pulsed light and optical gratings, using a quantum-mechanical self-consistent numerical toolbox which is introduced here. It will be shown that electron pulses are accelerated very fast in interaction with the near-field of the grating, demanding that a synchronicity condition is met. To prevent the electrons to be transversely deflected from the grating a symmetric double-grating configuration is necessary. It is found that even in this configuration, diffraction due to the interaction of the electron with the standing-wave light inside the gap between the gratings, is a source of defocusing. Moreover, the longitudinal broadening of the electron pulse directly affects the final shape of the electron wave packet due to the occurrence of multiple electron-photon scatterings. These investigations pave the way towards the design of more efficient electron-driven photon sources and accelerators.