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Álvaro Rodríguez Echarri

Publications and source records attributed to Álvaro Rodríguez Echarri.

13 recordsLinked to original sources

Synthesizing free-electron wave functions by stimulated near-field interactions

Stimulated electron-optical-near-field interactions imprint a coherent, phase-coherent modulation on the wave function of a free electron, of which the free-space dispersion subsequently converts into a train of attosecond density peaks. Light thereby becomes a tool for synthesizing the electron wave function itself, setting when, where, and how narrowly the electron density concentrates. Here we study photon-induced near-field electron microscopy (PINEM) to gain control over that synthesis in two stages: first for a single PINEM interaction, whose design parameters we obtain in closed form, and then for multiple PINEM interactions acting in parallel, which extends the control across space and time. The design rules follow from decomposing the propagated density into temporal harmonics, which we classify into three: (i) the arrival time of the attosecond train, fixed by the optical phase of the coupling; (ii) the distance at which the train forms, set by diffraction at the point where all classical trajectories converge; and (iii) the pulse duration, fixed by the imprinted energy spread. We evaluate these parameters for a scanning-electron-microscope (SEM) configuration at 10~keV, where the compression completes within tens of micrometers from the interaction region, with results 20% better than previous approaches. Letting the electron then interact with several spatially separated near fields in parallel, normal to the trajectory, each pathway carrying its own coupling strength and optical phase, we show that retaining or erasing which-path information changes both the propagated density and the measurable energy spectrum, the latter providing in turn a measure of the mutual coherence of the driving fields. These results establish PINEM as a quantitative synthesis tool for free-electron wave functions in compact, low-voltage electron microscopes.

physics.optics↗

Near-field effects on cathodoluminescence outcoupling in perovskite thin films

Halide perovskite semiconductors are a promising material for high-efficiency solar cells. Their optical properties can vary within and between crystallographic grains. We present spatially-resolved cathodoluminescence (CL) spectroscopy at 2 keV and 5 keV on polycrystalline CsPbBr3 perovskite films to study these variations at the nanoscale. The CL maps show a strongly reduced intensity near the polycrystalline grain boundaries. We perform numerical simulations of the far-field emission of the electron beam-generated optical near fields using the surface profiles from AFM as input. We find that near grain boundaries the light outcoupling is strongly reduced due to enhanced internal reflection and light trapping at the curved surfaces. Lateral variations in CL intensity inside grains are due to Fabry-Perot-like resonances in the film, with the substrate acting as a back reflector. Our results show that near-field coupling and interference effects can dominate nanoscale luminescence maps of halide perovskite films. The results are broadly relevant for the analysis of cathodoluminescence and photoluminescence of corrugated thin films.

cond-mat.mtrl-sci↗

Active steering of cathodoluminescence through a generalized Smith-Purcell effect

Optical metasurfaces can shape the near fields of energetic electrons, enabling Smith-Purcell (SP) emission. We introduce a generalized SP effect relying on finite periodic arrays whose elements possess individually tunable polarizabilities, allowing us to explore higher-order SP radiation. By controlling the amplitude and phase of each of the elements, we show through rigorous theory the ability to create an SP steering device. In particular, we explore the active tuning capabilities of doped graphene, and thermally driven phase-change materials, which we compare with standard passive plasmonic structures made of gold and silver. Our results establish programmable electron-driven light sources and spectroscopic probes spanning the terahertz-to-visible range, advancing tunable metasurfaces for next-generation electron-photon technologies.

physics.optics↗

Nonreciprocal plasmons in one-dimensional carbon nanostructures

The directional control of light in miniaturized plasmonic waveguides holds appealing possibilities for emerging nanophotonic technologies, but is hindered by the intrinsic reciprocal optical response of conventional plasmonic materials. While the ability of graphene to sustain large electrical currents shows promise for nonreciprocal plasmonics, studies have been limited to extended samples characterized by linear electrical dispersion. Here, we theoretically explore quantum finite-size and nonlocal effects in the nonreciprocal response of mesoscale plasmonic waveguides comprised of drift-biased graphene nanoribbons (GNRs) and carbon nanotubes (CNTs). Using atomistic simulation methods based on tight-binding electronic states and self-consistent mean-field optical response, we reveal that a moderate electrical bias can significantly break reciprocity for propagation of guided plasmon modes in GNRs and CNTs exhibiting electronic band gaps. The excitation by a nearby point dipole emitter and subsequent propagation of guided plasmon modes can thus be actively controlled by the applied current, which can further be leveraged to mediate nonlocal interactions of multiple emitters. Our results establish graphene nanostructures as a promising atomically thin platform for nonreciprocal nanophotonics.

cond-mat.mes-hall↗

Atomically thin silver films for enhanced nanoscale nonlinear optics

The inherently weak nonlinear optical response of bulk materials remains a fundamental limitation in advancing photonic technologies. Nanophotonics addresses this challenge by tailoring the size and morphology of nanostructures to manipulate the optical near field, thus modulating the nonlinear response. Here, we explore a complementary strategy based on engineering the electronic band structure in the mesoscopic regime to enhance optical nonlinearities. Specifically, we demonstrate an increase in second-harmonic generation (SHG) from crystalline silver films as their thickness is reduced down to just a few atomic monolayers. Operating at the boundary between bulk and two-dimensional systems, these ultra-thin films exhibit a pronounced enhancement of SHG with decreasing thickness. This enhancement stems from quantum confinement effects that modify the interaction between electronic states and incident light, which we explain based on quantum-mechanical calculation. Our atomically-thin crystalline silver films provide a new means to overcome the small interaction volumes inherent to nanophotonic platforms, enabling efficient nanoscale nonlinear optics with potential applications in photonics, sensing, and quantum technologies.

physics.optics↗

Roadmap for Photonics with 2D Materials

Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combination with layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary collection of those directions, where 2D materials contribute with polaritons of unique characteristics such as strong spatial confinement, large optical-field enhancement, long lifetimes, high sensitivity to external stimuli (e.g., electric and magnetic fields, heating, and strain), a broad spectral range from the far infrared to the ultraviolet, and hybridization with spin and momentum textures of electronic band structures. The explosion of photonics with 2D materials as a vibrant research area is producing breakthroughs, including the discovery and design of new materials and metasurfaces with unprecedented properties as well as applications in integrated photonics, light emission, optical sensing, and exciting prospects for applications in quantum information, and nanoscale thermal transport. This Roadmap summarizes the state of the art in the field, identifies challenges and opportunities, and discusses future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

cond-mat.mtrl-sci↗

Relativistic electron energy-loss spectroscopy in cylindrical waveguides and holes

Swift electrons passing near or through metallic structures have proven to be an excellent tool for studying plasmons and other types of confined optical modes involving collective charge oscillations in the materials hybridized with electromagnetic fields. In this work, we provide a general analytical framework for the simulation of electron energy-loss spectroscopy (EELS) in infinite systems with cylindrical symmetry, such as wires, holes, and optical fibers. While EELS theory is well developed for electrons moving parallel to the direction of translational symmetry, we introduce closed-form analytical solutions for perpendicular electron trajectories. These analytical results are corroborated by comparison to numerical simulations based on a frequency-domain boundary-element method and a discontinuous-Galerkin time-domain finite-element method. Numerical methods further allow us to study termination effects in finite-sized cylindrical objects such as nanorods. The present study of the interaction between free electrons and cylindrically symmetric photonics systems can find application in the analysis of EELS spectra and the design of free-electron--photonic hybrid systems.

physics.optics↗

Real-time surface plasmon polariton propagation in silver nanowires

Electron microscopy techniques such as electron energy-loss spectroscopy (EELS) facilitate the spatio-spectral characterization of plasmonic nanostructures. In this work, a time-dependent perspective is presented, which significantly enhances the utility of EELS. Specifically, silver nanowires offer the material and geometric features for various high-quality plasmonic excitations. This provides an ideal illustrative system for combined experimental-theoretical analyses of the different plasmonic excitations and their real-time dynamics. It is demonstrated how the plasmonic excitations propagating inside the wire repeatedly interact with the swift electrons in an EELS configuration. In addition, the role of azimuthal modes, often overlooked for very thin wires, is observed and analyzed in both the energy-loss spectrum and the dynamical perspective. Such a complete understanding of the interaction of electrons and plasmonic excitation is key for the design of efficient plasmonic sensors, the study of hot electron dynamics in metals, and applications in the context of electron quantum optics, where full control of the spatial and temporal characteristics of the fields at the nanometer and femtosecond scales is highly desirable.

physics.optics↗

Electron beams traversing spherical nanoparticles: analytic and numerical treatment

We present an analytic, Mie theory-based solution for the energy-loss and the photon-emission probabilities in the interaction of spherical nanoparticles with electrons passing nearby and through them, in both cathodoluminescence and electron energy-loss spectroscopies. In particular, we focus on the case of penetrating electron trajectories, for which the complete fully electrodynamic and relativistic formalism has not been reported as yet. We exhibit the efficiency of this method in describing collective excitations in matter through calculations for a dispersive and lossy system, namely a sphere described by a Drude permittivity. Subsequently, we use the analytic solution to corroborate the implementation of electron-beam sources in a state-of-the-art numerical method for problems in electrodynamics, the discontinuous Galerkin time-domain (DGTD) method. We show that the two approaches produce spectra in good mutual agreement, and demonstrate the versatility of DGTD via simulations of spherical nanoparticles characterized by surface roughness. The possibility of simultaneously employing both kinds of calculations (analytic and numerical) facilitates a better understanding of the rich optical response of nanophotonic architectures excited by fast electron beams.

cond-mat.mes-hall↗

Generation of entangled waveguided photon pairs by free electrons

Entangled photon pairs are a key resource in future quantum-optical communication and information technologies. While high-power laser light propagating in bulk nonlinear optical crystals is conventionally used to generate entangled photons that are routed into optical configurations, such schemes suffer from low efficiency due to the weak intrinsic nonlinear optical response of known materials and losses associated with photon in- and out-coupling. Here, we propose a scheme to generate entangled polariton pairs directly within optical waveguides using free electrons, whereby the measured energy loss of undeflected electrons heralds the production of counter-propagating polaritons pairs that are entangled in energy and direction of emission. As a paradigmatic example, we study the excitation of plasmon polaritons in metal strip waveguides that, within specific frequency regimes, strongly enhance light-matter interactions that lead to two-plasmon generation in comparison to the probability of single-plasmon excitation. We demonstrate that, under appropriate conditions, an electron energy loss detected in an optimal frequency range can reliably signal the generation of a plasmon pair entangled in energy and momentum. Our proposed scheme can be directly applied to other types of optical waveguides for in situ generation of entangled photon pairs in quantum-optics applications.

physics.optics↗

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 unravelling nanoscale carrier dynamics largely unexploited. Here, we reveal quantum-mechanical effects emanating in the luminescence from thin monocrystalline gold flakes. Specifically, we present experimental evidence, supported by first-principles simulations, to demonstrate its photoluminescence origin 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 modelling, thus establishing a unified description of luminescence in gold 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.

cond-mat.mtrl-sci↗

Direct generation of entangled photon pairs in nonlinear optical waveguides

Entangled photons are pivotal elements in emerging quantum information technologies. While several schemes are available for the production of entangled photons, they typically require the assistance of cumbersome optical elements to couple them to other components involved in logic operations. Here, we introduce a scheme by which entangled photon pairs are directly generated as guided mode states in optical waveguides. The scheme relies on the intrinsic nonlinearity of the waveguide material, circumventing the use of bulky optical components. Specifically, we consider an optical fiber under normal illumination, so that photon down-conversion can take place to waveguide states emitted with opposite momentum into a spectral region populated by only two accessible modes. By additionally configuring the external illumination to interfere different incident directions, we can produce maximally entangled photon-pair states, directly generated as waveguide modes with conversion efficiencies that are competitive with respect to existing macroscopic schemes. These results should find application in the design of more efficient and compact quantum optics devices.

quant-ph↗

Anisotropic Second Harmonic Generation From Monocrystalline Gold Flakes

Noble metals with well-defined crystallographic orientation constitute an appealing class of materials for controlling light-matter interactions on the nanoscale. Nonlinear optical processes, being particularly sensitive to anisotropy, are a natural and versatile probe of crystallinity in nano-optical devices. Here we study the nonlinear optical response of monocrystalline gold flakes, revealing a polarization dependence in second-harmonic generation from the {111} surface that is markedly absent in polycrystalline films. Apart from suggesting an approach for directional enhancement of nonlinear response in plasmonic systems, we anticipate that our findings can be used as a rapid and non-destructive method for characterization of crystal quality and orientation that may be of significant importance in future applications.

physics.optics↗