Toward Complete Optical Coupling to Confined Surface Polaritons.

Optical coupling between propagating light and confined surface polaritons plays a pivotal role in the practical design of nanophotonic devices. However, the coupling efficiency decreases dramatically with the degree of mode confinement due to the mismatch that exists between the light and polariton wavelengths, and despite the intense efforts made to explore different mechanisms proposed to circumvent this problem, the realization of a flexible scheme to efficiently couple light to polaritons remains a challenge. Here, we experimentally demonstrate an efficient coupling of light to surface-plasmon polaritons assisted by engineered dipolar scatterers placed at an optimum distance from the surface. Specifically, we fabricate gold disks separated by a silica spacer from a planar gold surface and seek to achieve perfect coupling conditions by tuning the spacer thickness for a given scatterer geometry that resonates at a designated optical frequency. We measure a maximum light-to-plasmon coupling cross section of the order of the square of the light wavelength at an optimum distance that results from the interplay between a large particle-surface interaction and a small degree of surface-driven particle-dipole quenching, both of which are favored at small separations. Our experiments, in agreement with both analytical theory and electromagnetic simulations, support the use of optimally placed engineered scatterers as a disruptive approach to solving the long-standing problem of in/out-coupling in nanophotonics.

Singular and Nonsingular Transitions in the Infrared Plasmons of Nearly Touching Nanocube Dimers.

Narrow gaps between plasmon-supporting materials can confine infrared electromagnetic energy at the nanoscale, thus enabling applications in areas such as optical sensing. However, in nanoparticle dimers, the nature of the transition between touching (zero gap) and nearly nontouching (nonzero gap ≲15 nm) regimes is still a subject of debate. Here, we observe both singular and nonsingular transitions in infrared plasmons confined to dimers of fluorine-doped indium oxide nanocubes when moving from touching to nontouching configurations depending on the dimensionality of the contact region. Through spatially resolved electron energy-loss spectroscopy, we find a continuous spectral evolution of the lowest-order plasmon mode across the transition for finite touching areas, in excellent agreement with the simulations. This behavior challenges the widely accepted idea that a singular transition always emerges in the near-touching regime of plasmonic particle dimers. The apparent contradiction is resolved by theoretically examining different types of gap morphologies, revealing that the presence of a finite touching area renders the transition nonsingular, while one-dimensional and point-like contacts produce a singular behavior in which the lowest-order dipolar mode in the touching configuration, characterized by a net induced charge in each of the particles, becomes unphysical as soon as they are separated. Our results provide valuable insights into the nature of dimer plasmons in highly doped semiconductors.

Toward Optimum Coupling between Free Electrons and Confined Optical Modes.

Free electrons are excellent tools to probe and manipulate nanoscale optical fields with emerging applications in ultrafast spectromicroscopy and quantum metrology. However, advances in this field are hindered by the small probability associated with the excitation of single optical modes by individual free electrons. Here, we theoretically investigate the scaling properties of the electron-driven excitation probability for a wide variety of optical modes including plasmons in metallic nanostructures and Mie resonances in dielectric cavities, spanning a broad spectral range that extends from the ultraviolet to the infrared region. The highest probabilities for the direct generation of three-dimensionally confined modes are observed at low electron and mode energies in small structures, with order-unity (∼100%) coupling demanding the use of <100 eV electrons interacting with eV polaritons confined down to tens of nanometers in space. Electronic transitions in artificial atoms also emerge as practical systems to realize strong coupling to few-eV free electrons. In contrast, conventional dielectric cavities reach a maximum probability in the few-percent range. In addition, we show that waveguide modes can be generated with higher-than-unity efficiency by phase-matched interaction with grazing electrons, suggesting a practical method to create multiple excitations of a localized optical mode by an individual electron through funneling the so-generated propagating photons into a confining cavity─an alternative approach to direct electron-cavity interaction. Our work provides a roadmap to optimize electron-photon coupling with potential applications in electron spectromicroscopy as well as nonlinear and quantum optics at the nanoscale.

Steering and cloaking of hyperbolic polaritons at deep-subwavelength scales.

Polaritons are well-established carriers of light, electrical signals, and even heat at the nanoscale in the setting of on-chip devices. However, the goal of achieving practical polaritonic manipulation over small distances deeply below the light diffraction limit remains elusive. Here, we implement nanoscale polaritonic in-plane steering and cloaking in a low-loss atomically layered van der Waals (vdW) insulator, α-MoO3, comprising building blocks of customizable stacked and assembled structures. Each block contributes specific characteristics that allow us to steer polaritons along the desired trajectories. Our results introduce a natural materials-based approach for the comprehensive manipulation of nanoscale optical fields, advancing research in the vdW polaritonics domain and on-chip nanophotonic circuits.

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.

Quantum-mechanical effects in photoluminescence from thin crystalline gold films.

Luminescence constitutes a unique source of insight into hot carrier processes in metals, including those in plasmonic nanostructures used for sensing and energy applications. However, being weak in nature, metal luminescence remains poorly understood, its microscopic origin strongly debated, and its potential for unraveling nanoscale carrier dynamics largely unexploited. Here, we reveal quantum-mechanical effects in the luminescence emanating from thin monocrystalline gold flakes. Specifically, we present experimental evidence, supported by first-principles simulations, to demonstrate its photoluminescence origin (i.e., radiative emission from electron/hole recombination) when exciting in the interband regime. Our model allows us to identify changes to the measured gold luminescence due to quantum-mechanical effects as the gold film thickness is reduced. Excitingly, such effects are observable in the luminescence signal from flakes up to 40 nm in thickness, associated with the out-of-plane discreteness of the electronic band structure near the Fermi level. We qualitatively reproduce the observations with first-principles modeling, thus establishing a unified description of luminescence in gold monocrystalline flakes and enabling its widespread application as a probe of carrier dynamics and light-matter interactions in this material. Our study paves the way for future explorations of hot carriers and charge-transfer dynamics in a multitude of material systems.

Engineering 2D Material Exciton Line Shape with Graphene/h-BN Encapsulation.

Control over the optical properties of atomically thin two-dimensional (2D) layers, including those of transition metal dichalcogenides (TMDs), is needed for future optoelectronic applications. Here, the near-field coupling between TMDs and graphene/graphite is used to engineer the exciton line shape and charge state. Fano-like asymmetric spectral features are produced in WS2, MoSe2, and WSe2 van der Waals heterostructures combined with graphene, graphite, or jointly with hexagonal boron nitride (h-BN) as supporting or encapsulating layers. Furthermore, trion emission is suppressed in h-BN encapsulated WSe2/graphene with a neutral exciton red shift (44 meV) and binding energy reduction (30 meV). The response of these systems to electron beam and light probes is well-described in terms of 2D optical conductivities of the involved materials. Beyond fundamental insights into the interaction of TMD excitons with structured environments, this study opens an unexplored avenue toward shaping the spectral profile of narrow optical modes for application in nanophotonic devices.

Electrons catch light pulses on the fly.

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

Radiative loss of coherence in free electrons: a long-range quantum phenomenon.

Quantum physics rules the dynamics of small objects as they interact over microscopic length scales. Nevertheless, quantum correlations involving macroscopic distances can be observed between entangled photons as well as in atomic gases and matter waves at low temperatures. The long-range nature of the electromagnetic coupling between charged particles and extended objects could also trigger quantum phenomena over large distances. Here, we reveal a manifestation of quantum mechanics that involves macroscopic distances and results in a nearly complete depletion of coherence associated with which-way free-electron interference produced by electron-radiation coupling in the presence of distant extended objects. This is a ubiquitous effect that we illustrate through a rigorous theoretical analysis of a two-path electron beam interacting with a semi-infinite metallic plate and find the inter-path coherence to vanish proportionally to the path separation at zero temperature and exponentially at finite temperature. The investigated regime of large distances originates in the coupling of the electron to radiative modes assisted by diffraction at material structures but without any involvement of material excitations. Besides the fundamental interest of this macroscopic quantum phenomenon, our results suggest an approach to measuring the vacuum temperature and nondestructively sensing the presence of distant objects.

Ultraconfined Plasmons in Atomically Thin Crystalline Silver Nanostructures.

The ability to confine light down to atomic scales is critical for the development of applications in optoelectronics and optical sensing as well as for the exploration of nanoscale quantum phenomena. Plasmons in metallic nanostructures with just a few atomic layers in thickness can achieve this type of confinement, although fabrication imperfections down to the subnanometer scale hinder actual developments. Here, narrow plasmons are demonstrated in atomically thin crystalline silver nanostructures fabricated by prepatterning silicon substrates and epitaxially depositing silver films of just a few atomic layers in thickness. Specifically, a silicon wafer is lithographically patterned to introduce on-demand lateral shapes, chemically process the sample to obtain an atomically flat silicon surface, and epitaxially deposit silver to obtain ultrathin crystalline metal films with the designated morphologies. Structures fabricated by following this procedure allow for an unprecedented control over optical field confinement in the near-infrared spectral region, which is here illustrated by the observation of fundamental and higher-order plasmons featuring extreme spatial confinement and high-quality factors that reflect the crystallinity of the metal. The present study constitutes a substantial improvement in the degree of spatial confinement and quality factor that should facilitate the design and exploitation of atomic-scale nanoplasmonic devices for optoelectronics, sensing, and quantum-physics applications.

Nanophotonics for pair production.

The transformation of electromagnetic energy into matter represents a fascinating prediction of relativistic quantum electrodynamics that is paradigmatically exemplified by the creation of electron-positron pairs out of light. However, this phenomenon has a very low probability, so positron sources rely instead on beta decay, which demands elaborate monochromatization and trapping schemes to achieve high-quality beams. Here, we propose to use intense, strongly confined optical near fields supported by a nanostructured material in combination with high-energy photons to create electron-positron pairs. Specifically, we show that the interaction between near-threshold γ-rays and polaritons yields higher pair-production cross sections, largely exceeding those associated with free-space photons. Our work opens an unexplored avenue toward generating tunable pulsed positrons from nanoscale regions at the intersection between particle physics and nanophotonics.

Lorentz microscopy of optical fields.

In electron microscopy, detailed insights into nanoscale optical properties of materials are gained by spontaneous inelastic scattering leading to electron-energy loss and cathodoluminescence. Stimulated scattering in the presence of external sample excitation allows for mode- and polarization-selective photon-induced near-field electron microscopy (PINEM). This process imprints a spatial phase profile inherited from the optical fields onto the wave function of the probing electrons. Here, we introduce Lorentz-PINEM for the full-field, non-invasive imaging of complex optical near fields at high spatial resolution. We use energy-filtered defocus phase-contrast imaging and iterative phase retrieval to reconstruct the phase distribution of interfering surface-bound modes on a plasmonic nanotip. Our approach is universally applicable to retrieve the spatially varying phase of nanoscale fields and topological modes.

Multi-plasmon effects and plasmon satellites in photoemission from nanostructures.

Plasmons can be excited during photoemission and produce spectral photoelectron features that yield information on the nanoscale optical response of the probed materials. However, these so-called plasmon satellites have so far been observed only for planar surfaces, while their potential for the characterization of nanostructures remains unexplored. Here, we theoretically demonstrate that core-level photoemission from nanostructures can display spectrally narrow plasmonic features, reaching relatively high probabilities similar to the direct peak. Using a nonperturbative quantum-mechanical framework, we find a dramatic effect of nanostructure morphology and dimensionality as well as universal scaling laws for the plasmon-satellite probabilities. In addition, we introduce a pump-probe scheme in which plasmons are optically excited prior to photoemission, leading to plasmon losses and gains in the photoemission spectra and granting us access to the ultrafast dynamics of the sampled nanostructure. These results emphasize the potential of plasmon satellites to explore multi-plasmon effects and ultrafast electron-plasmon dynamics in metal-based nanoparticles and two-dimensional nanoislands.

Generation and control of localized terahertz fields in photoemitted electron plasmas.

Dense micron-sized electron plasmas, such as those generated upon irradiation of nanostructured metallic surfaces by intense femtosecond laser pulses, constitute a rich playground to study light-matter interactions, many-body phenomena, and out-of-equilibrium charge dynamics. Besides their fundamental interest, laser-induced plasmas hold great potential for the generation of localized terahertz radiation pulses. However, the underlying mechanisms ruling the formation and evolution of such plasmas are not yet well understood. Here, we develop a comprehensive microscopic theory to predictably describe the spatiotemporal dynamics of laser-pulse-induced plasmas. Through detailed analysis of electron emission, metal screening, and plasma cloud interactions, we investigate the spatial, temporal, and spectral characteristics of the so-generated terahertz fields, which can be extensively controlled through the metal morphology and the illumination conditions. We further describe the interaction with femtosecond electron beams to explain recent ultrafast electron microscopy experiments, whereby the position and temporal dependence of the observed electron acceleration permits assessing the associated terahertz field. Besides its potential application to the design of low-frequency light sources, our work contributes fundamental insight into the generation and dynamics of micron-scale electron plasmas and their interaction with ultrafast electron pulses.

µeV electron spectromicroscopy using free-space light.

The synergy between free electrons and light has recently been leveraged to reach an impressive degree of simultaneous spatial and spectral resolution, enabling applications in microscopy and quantum optics. However, the required combination of electron optics and light injection into the spectrally narrow modes of arbitrary specimens remains a challenge. Here, we demonstrate microelectronvolt spectral resolution with a sub-nanometer probe of photonic modes with quality factors as high as 104. We rely on mode matching of a tightly focused laser beam to whispering gallery modes to achieve a 108-fold increase in light-electron coupling efficiency. By adapting the shape and size of free-space optical beams to address specific physical questions, our approach allows us to interrogate any type of photonic structure with unprecedented spectral and spatial detail.

Spatiotemporal Electron Beam Focusing through Parallel Interactions with Shaped Optical Fields.

The ability to modulate free electrons with light has emerged as a powerful tool to produce attosecond electron wave packets. However, research has so far aimed at the manipulation of the longitudinal wave function component, while the transverse degrees of freedom have primarily been utilized for spatial rather than temporal shaping. Here, we show that the coherent superposition of parallel light-electron interactions in transversally separate zones allows for a simultaneous spatial and temporal compression of a convergent electron wave function, enabling the formation of sub-Ångström focal spots of attosecond duration. Specifically, spots spanning just ∼3% of the light optical cycle are shown to be formed, accompanied by an increase by only a factor of 2 in spatial extension relative to an unperturbed beam. The proposed approach will facilitate the exploration of previously inaccessible ultrafast atomic-scale phenomena, in particular enabling attosecond scanning transmission electron microscopy.

Free-electron interactions with van der Waals heterostructures: a source of focused X-ray radiation.

The science and technology of X-ray optics have come far, enabling the focusing of X-rays for applications in high-resolution X-ray spectroscopy, imaging, and irradiation. In spite of this, many forms of tailoring waves that had substantial impact on applications in the optical regime have remained out of reach in the X-ray regime. This disparity fundamentally arises from the tendency of refractive indices of all materials to approach unity at high frequencies, making X-ray-optical components such as lenses and mirrors much harder to create and often less efficient. Here, we propose a new concept for X-ray focusing based on inducing a curved wavefront into the X-ray generation process, resulting in the intrinsic focusing of X-ray waves. This concept can be seen as effectively integrating the optics to be part of the emission mechanism, thus bypassing the efficiency limits imposed by X-ray optical components, enabling the creation of nanobeams with nanoscale focal spot sizes and micrometer-scale focal lengths. Specifically, we implement this concept by designing aperiodic vdW heterostructures that shape X-rays when driven by free electrons. The parameters of the focused hotspot, such as lateral size and focal depth, are tunable as a function of an interlayer spacing chirp and electron energy. Looking forward, ongoing advances in the creation of many-layer vdW heterostructures open unprecedented horizons of focusing and arbitrary shaping of X-ray nanobeams.

Exciton-assisted electron tunnelling in van der Waals heterostructures.

The control of elastic and inelastic electron tunnelling relies on materials with well-defined interfaces. Two-dimensional van der Waals materials are an excellent platform for such studies. Signatures of acoustic phonons and defect states have been observed in current-to-voltage measurements. These features can be explained by direct electron-phonon or electron-defect interactions. Here we use a tunnelling process that involves excitons in transition metal dichalcogenides (TMDs). We study tunnel junctions consisting of graphene and gold electrodes separated by hexagonal boron nitride with an adjacent TMD monolayer and observe prominent resonant features in current-to-voltage measurements appearing at bias voltages that correspond to TMD exciton energies. By placing the TMD outside of the tunnelling pathway, we demonstrate that this tunnelling process does not require any charge injection into the TMD. The appearance of such optical modes in electrical transport introduces additional functionality towards van der Waals material-based optoelectronic devices.

Interrogating Quantum Nonlocal Effects in Nanoplasmonics through Electron-Beam Spectroscopy.

A rigorous account of quantum nonlocal effects is paramount for understanding the optical response of metal nanostructures and for designing plasmonic devices at the nanoscale. Here, we present a scheme for retrieving the quantum surface response of metals, encapsulated in the Feibelman d-parameters, from electron energy-loss spectroscopy (EELS) and cathodoluminescence (CL) measurements. We theoretically demonstrate that quantum nonlocal effects have a dramatic impact on EELS and CL spectra, in the guise of spectral shifts and nonlocal damping, when either the system size or the inverse wave vector in extended structures approaches the nanometer scale. Our concept capitalizes on the unparalleled ability of free electrons to supply deeply subwavelength near-fields and, thus, probe the optical response of metals at length scales in which quantum-mechanical effects are apparent. These results pave the way for a widespread use of the d-parameter formalism, thereby facilitating a rigorous yet practical inclusion of nonclassical effects in nanoplasmonics.

Visualizing the Nanoscopic Field Distribution of Whispering-Gallery Modes in a Dielectric Sphere by Cathodoluminescence.

A spherical dielectric particle can sustain the so-called whispering-gallery modes (WGMs), which can be regarded as circulating electromagnetic waves, resulting in the spatial confinement of light inside the particle. Despite the wide adoption of optical WGMs as a major light confinement mechanism in salient practical applications, direct imaging of the mode fields is still lacking and only partially addressed by simple photography and simulation work. The present study comprehensively covers this research gap by demonstrating the nanoscale optical-field visualization of self-interference of light extracted from excited modes through experimentally obtained photon maps that directly portray the field distributions of the excited eigenmodes. To selectively choose the specific modes at a given light emission detection angle and resonance wavelength, we use cathodoluminescence-based scanning transmission electron microscopy supplemented with angle-, polarization-, and wavelength-resolved capabilities. Equipped with semi-analytical simulation tools, the internal field distributions of the whispering-gallery modes reveal that radiation emitted by a spherical resonator at a given resonance frequency is composed of the interference between multiple modes, with one or more of them being comparatively dominant, leading to a resulting distribution featuring complex patterns that explicitly depend on the detection angle and polarization. Direct visualization of the internal fields inside resonators enables a comprehensive understanding of WGMs that can shed light on the design of nanophotonic applications.