Cylindrical Metalens for Generation and Focusing of Free-Electron Radiation.

Metasurfaces constitute a powerful approach to generate and control light by engineering optical material properties at the subwavelength scale. Recently, this concept was applied to manipulate free-electron radiation phenomena, rendering versatile light sources with unique functionalities. In this Letter, we experimentally demonstrate spectral and angular control over coherent light emission by metasurfaces that interact with free-electrons under grazing incidence. Specifically, we study metalenses based on chirped metagratings that simultaneously emit and shape Smith-Purcell radiation in the visible and near-infrared spectral regime. In good agreement with theory, we observe the far-field signatures of strongly convergent and divergent cylindrical radiation wavefronts using in situ hyperspectral angle-resolved light detection in a scanning electron microscope. Furthermore, we theoretically explore simultaneous control over the polarization and wavefront of Smith-Purcell radiation via a split-ring-resonator metasurface, enabling tunable operation by spatially selective mode excitation at nanometer resolution. Our work highlights the potential of merging metasurfaces with free-electron excitations for versatile and highly tunable radiation sources in wide-ranging spectral regimes.

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.

Electron-beam spectroscopy for nanophotonics.

Progress in electron-beam spectroscopies has recently enabled the study of optical excitations with combined space, energy and time resolution in the nanometre, millielectronvolt and femtosecond domain, thus providing unique access into nanophotonic structures and their detailed optical responses. These techniques rely on ~1-300 keV electron beams focused at the sample down to sub-nanometre spots, temporally compressed in wavepackets a few femtoseconds long, and in some cases controlled by ultrafast light pulses. The electrons undergo energy losses and gains (also giving rise to cathodoluminescence light emission), which are recorded to reveal the optical landscape along the beam path. This Review portraits these advances, with a focus on coherent excitations, emphasizing the increasing level of control over the electron wavefunctions and ensuing applications in the study and technological use of optically resonant modes and polaritons in nanoparticles, 2D materials and engineered nanostructures.

High-Index Dielectric Metasurfaces Performing Mathematical Operations.

Image processing and edge detection are at the core of several newly emerging technologies, such as augmented reality, autonomous driving, and more generally object recognition. Image processing is typically performed digitally using integrated electronic circuits and algorithms, implying fundamental size and speed limitations, as well as significant power needs. On the other hand, it can also be performed in a low-power analog fashion using Fourier optics, requiring, however, bulky optical components. Here, we introduce dielectric metasurfaces that perform optical image edge detection in the analog domain using a subwavelength geometry that can be readily integrated with detectors. The metasurface is composed of a suitably engineered array of nanobeams designed to perform either first- or second-order spatial differentiation. We experimentally demonstrate the second-derivative operation on an input image, showing the potential of all-optical edge detection using a silicon metasurface geometry working at a numerical aperture as large as 0.35.

Application and validity of the effective medium approximation to the optical properties of nano-textured silicon coated with a dielectric layer.

The emergence of nanotextures in photovoltaics has resulted in challenges associated with optical modelling. Whilst rigorous methods exist to accurately solve these textures, the computational effort required limits the scope of modeling applications. The effective medium approximation (EMA) is a potential alternative to provide rapid modeling results which can be easily integrated with ray tracing of large complex structures. However, the validity of this technique is strongly dependent on the size of features relative to the wavelength of interest, making the application of EMA ambiguous for many situations. This paper aims to address this issue by comparing the simulated results between EMA and finite element methods for three randomly distributed silicon textures with and without a dielectric layer. Criteria for which the EMA approach is valid are proposed and generalized using ratios between root-mean-square roughness, correlation length and incident wavelength, making these limits broadly applicable, beyond that of just the nanotexture under specific solar spectrum regimes. The results in this work apply to random, isotropic textures under normally incident light. Based on the proposed criteria, the validity of different optical simulation techniques for a set of industrial photovoltaic textures is discussed. This analysis reveals a region within which neither geometric optics nor EMA are adequate for calculating the reflectivity of a textured surface, and hence FDTD or other new approaches are required.

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.

Nanoscale Relative Emission Efficiency Mapping Using Cathodoluminescence g(2) Imaging.

Cathodoluminescence (CL) imaging spectroscopy provides two-dimensional optical excitation images of photonic nanostructures with a deep-subwavelength spatial resolution. So far, CL imaging was unable to provide a direct measurement of the excitation and emission probabilities of photonic nanostructures in a spatially resolved manner. Here, we demonstrate that by mapping the cathodoluminescence autocorrelation function g(2) together with the CL spectral distribution the excitation and emission rates can be disentangled at every excitation position. We use InGaN/GaN quantum wells in GaN nanowires with diameters in the range 200-500 nm as a model system to test our new g(2) mapping methodology and find characteristic differences in excitation and emission rates both between wires and within wires. Strong differences in the average CL intensity between the wires are the result of differences in the emission efficiencies. At the highest spatial resolution, intensity variations observed within wires are the result of excitation rates that vary with the nanoscale geometry of the structures. The fact that strong spatial variations observed in the CL intensity are not only uniquely linked to variations in emission efficiency but also linked to excitation efficiency has profound implications for the interpretation of the CL data for nanostructured geometries in general.

Nonlocal Metasurfaces for Optical Signal Processing.

Optical analog signal processing has been gaining significant attention as a way to overcome the speed and energy limitations of digital techniques. Metasurfaces offer a promising avenue towards this goal due to their efficient manipulation of optical signals over deeply subwavelength volumes. To date, metasurfaces have been proposed to transform signals in the spatial domain, e.g., for beam steering, focusing, or holography, for which angular-dependent responses, or nonlocality, are unwanted features that must be avoided or mitigated. Here, we show that the metasurface nonlocality can be engineered to enable signal manipulation in the momentum domain over an ultrathin platform. We explore nonlocal metasurfaces performing basic mathematical operations, paving the way towards fast and power-efficient ultrathin devices for edge detection and optical image processing.

Metal-Insulator-Semiconductor Nanowire Network Solar Cells.

Metal-insulator-semiconductor (MIS) junctions provide the charge separating properties of Schottky junctions while circumventing the direct and detrimental contact of the metal with the semiconductor. A passivating and tunnel dielectric is used as a separation layer to reduce carrier recombination and remove Fermi level pinning. When applied to solar cells, these junctions result in two main advantages over traditional p-n-junction solar cells: a highly simplified fabrication process and excellent passivation properties and hence high open-circuit voltages. However, one major drawback of metal-insulator-semiconductor solar cells is that a continuous metal layer is needed to form a junction at the surface of the silicon, which decreases the optical transmittance and hence short-circuit current density. The decrease of transmittance with increasing metal coverage, however, can be overcome by nanoscale structures. Nanowire networks exhibit precisely the properties that are required for MIS solar cells: closely spaced and conductive metal wires to induce an inversion layer for homogeneous charge carrier extraction and simultaneously a high optical transparency. We experimentally demonstrate the nanowire MIS concept by using it to make silicon solar cells with a measured energy conversion efficiency of 7% (∼11% after correction), an effective open-circuit voltage (Voc) of 560 mV and estimated short-circuit current density (Jsc) of 33 mA/cm(2). Furthermore, we show that the metal nanowire network can serve additionally as an etch mask to pattern inverted nanopyramids, decreasing the reflectivity substantially from 36% to ∼4%. Our extensive analysis points out a path toward nanowire based MIS solar cells that exhibit both high Voc and Jsc values.

Controlling magnetic and electric dipole modes in hollow silicon nanocylinders.

We propose a dielectric nanoresonator geometry consisting of hollow dielectric nanocylinders which support geometrical resonances. We fabricate such hollow Si particles with an outer diameter of 108-251 nm on a Si substrate, and determine their resonant modes with cathodo-luminescence (CL) spectroscopy and optical dark-field (DF) scattering measurements. The scattering behavior is numerically investigated in a systematic fashion as a function of wavelength and particle geometry. We find that the additional design parameter as a result of the introduction of a center gap can be used to control the relative spectral spacing of the resonant modes, which will enable additional control over the angular radiation pattern of the scatterers. Furthermore, the gap offers direct access to the enhanced magnetic dipole modal field in the center of the particle.

Plasmomechanical Resonators Based on Dimer Nanoantennas.

Nanomechanical resonators are highly suitable as sensors of minute forces, displacements, or masses. We realize a single plasmonic dimer antenna of subwavelength size, integrated with silicon nitride nanobeams. The sensitive dependence of the antenna response on the beam displacement creates a plasmomechanical system of deeply subwavelength size in all dimensions. We use it to demonstrate transduction of thermal vibrations to scattered light fields and discuss the noise properties and achievable coupling strengths in these systems.

Dielectric Scattering Patterns for Efficient Light Trapping in Thin-Film Solar Cells.

We demonstrate an effective light trapping geometry for thin-film solar cells that is composed of dielectric light scattering nanocavities at the interface between the metal back contact and the semiconductor absorber layer. The geometry is based on resonant Mie scattering. It avoids the Ohmic losses found in metallic (plasmonic) nanopatterns, and the dielectric scatterers are well compatible with nearly all types of thin-film solar cells, including cells produced using high temperature processes. The external quantum efficiency of thin-film a-Si:H solar cells grown on top of a nanopatterned Al-doped ZnO, made using soft imprint lithography, is strongly enhanced in the 550-800 nm spectral band by the dielectric nanoscatterers. Numerical simulations are in good agreement with experimental data and show that resonant light scattering from both the AZO nanostructures and the embedded Si nanostructures are important. The results are generic and can be applied on nearly all thin-film solar cells.

Single-Step Soft-Imprinted Large-Area Nanopatterned Antireflection Coating.

We demonstrate an effective nanopatterned antireflection coating on glass that is based on sol-gel chemistry and large-area substrate-conformal soft-imprint technology. The printed 120 nm tall silica nanocylinders with a diameter of 245 nm in a square array with 325 nm pitch form an effective-index (n = 1.20) antireflection coating that reduces the double-sided reflection from a borosilicate glass slide from 7.35% to 0.57% (averaged over the visible spectral range) with a minimum reflectance <0.05% at 590 nm. The nanoglass coating is made using a simple process involving only spin-coating and an imprint step, without vacuum technology or annealing required. The refractive index of the nanoglass layers can be tailored over a broad range by controlling the geometry (1.002 < n < 1.44 in theory), covering a wide range that is not achievable with natural materials. We demonstrate that the nanoglass coating effectively eliminates glare from smart-phone display windows and significantly improves the efficiency of glass-encapsulated solar cells. These features, that are achieved over an angular range as wide as ±50°, together with strong hydrophobicity and mechanical durability, make nanoglass coatings a promising technology to improve the functionality of optoelectronic devices based on glass encapsulation.

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.

Photoelectron imaging of modal interference in plasmonic whispering gallery cavities.

We use three-photon photoemission electron microscopy (PEEM) to investigate the interference of coherently excited dipolar and quadrupolar resonant modes of plasmonic whispering gallery resonators formed by circular grooves patterned into a flat Au surface. Optical scattering and cathodoluminescence spectroscopy are used to characterize the cavity resonance spectra for a wide range of cavity radii and groove depths. Using PEEM, we directly resolve the interference between the modal field distribution of dipolar and quadrupolar modes that are coherently excited at λ = 795 nm under oblique incidence. Characteristic asymmetries in the photoelectron images for both TM and TE excitation are a direct consequence of the coherent excitation of the resonant modes.

Plasmon nanomechanical coupling for nanoscale transduction.

We demonstrate plasmon-mechanical coupling in a metalized nanomechanical oscillator. A coupled surface plasmon is excited in the 25 nm wide gap between two metalized silicon nitride beams. The strong plasmonic dispersion allows the nanomechanical beams' thermal motion at a frequency of 4.4 MHz to be efficiently transduced to the optical transmission, with a measured displacement spectral density of 1.11 × 10(-13) m/Hz(1/2). When exciting the second-order plasmonic mode at λ = 780 nm we observe optical-power-induced frequency shifts of the mechanical oscillator. Our results show that novel functionality of plasmonic nanostructures can be achieved through coupling to engineered nanoscale mechanical oscillators.

The planar parabolic optical antenna.

One of the simplest and most common structures used for directing light in macroscale applications is the parabolic reflector. Parabolic reflectors are ubiquitous in many technologies, from satellite dishes to hand-held flashlights. Today, there is a growing interest in the use of ultracompact metallic structures for manipulating light on the wavelength scale. Significant progress has been made in scaling radiowave antennas to the nanoscale for operation in the visible range, but similar scaling of parabolic reflectors employing ray-optics concepts has not yet been accomplished because of the difficulty in fabricating nanoscale three-dimensional surfaces. Here, we demonstrate that plasmon physics can be employed to realize a resonant elliptical cavity functioning as an essentially planar nanometallic structure that serves as a broadband unidirectional parabolic antenna at optical frequencies.

Evolution of light-induced vapor generation at a liquid-immersed metallic nanoparticle.

When an Au nanoparticle in a liquid medium is illuminated with resonant light of sufficient intensity, a nanometer scale envelope of vapor-a "nanobubble"-surrounding the particle, is formed. This is the nanoscale onset of the well-known process of liquid boiling, occurring at a single nanoparticle nucleation site, resulting from the photothermal response of the nanoparticle. Here we examine bubble formation at an individual metallic nanoparticle in detail. Incipient nanobubble formation is observed by monitoring the plasmon resonance shift of an individual, illuminated Au nanoparticle, when its local environment changes from liquid to vapor. The temperature on the nanoparticle surface is monitored during this process, where a dramatic temperature jump is observed as the nanoscale vapor layer thermally decouples the nanoparticle from the surrounding liquid. By increasing the intensity of the incident light or decreasing the interparticle separation, we observe the formation of micrometer-sized bubbles resulting from the coalescence of nanoparticle-"bound" vapor envelopes. These studies provide the first direct and quantitative analysis of the evolution of light-induced steam generation by nanoparticles from the nanoscale to the macroscale, a process that is of fundamental interest for a growing number of applications.

Angular Dispersion of Free-Electron-Light Coupling in an Optical Fiber-Integrated Metagrating.

Free electrons can couple to optical material excitations on nanometer-length and attosecond-time scales, opening-up unique opportunities for both the generation of radiation and the manipulation of the electron wave function. Here, we exploit the Smith-Purcell effect to experimentally study the coherent coupling of free electrons and light in a circular metallo-dielectric metagrating that is fabricated onto the input facet of a multimode optical fiber. Using hyperspectral angle-resolved (HSAR) far-field imaging inside a scanning electron microscope, we probe the angular dispersion of Smith-Purcell radiation (SPR) that is simultaneously generated in free space and inside the fiber by an electron beam that grazes the metagrating at a nanoscale distance. Furthermore, we analyze the spectral distribution of SPR that is emitted into guided optical modes and correlate it with the numerical aperture of the fiber. By varying the electron energy between 5 and 30 keV, we observe the emission of SPR from the ultraviolet to the near-infrared spectral range, and up to the third emission order. In addition, we detect incoherent cathodoluminescence that is generated by electrons penetrating the input facet of the fiber and scattering inelastically. As a result, our HSAR measurements reveal a Fano resonance that is coupled to a Rayleigh anomaly of the metagrating, and that overlaps with the angular dispersion of second-order SPR at 20 keV. Our findings demonstrate the potential of optical fiber-integrated metasurfaces as a versatile platform to implement novel ultrafast light sources and to synthesize complex free-electron quantum states with light.

Electrons catch light pulses on the fly.

Energy exchange between electrons and photons enables ultrafast probing of materials.