arXiv subjects

F. Javier García de Abajo

Publications and source records attributed to F. Javier García de Abajo.

At least 37 records · Page 2Linked to original sources

arXiv2025

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↗

arXiv2024

Free-Space Optical Modulation of Free Electrons in the Continuous-Wave Regime

The coherent interaction between free electrons and optical fields can produce free-electron compression and push the temporal resolution of ultrafast electron microscopy to the attosecond regime. However, a large electron-light interaction is required to attain a strong compression, generally necessitating short light and electron pulses combined with optical scattering at nanostructures. Here, we theoretically investigate an alternative configuration based on stimulated Compton scattering, whereby two counterpropagating Gaussian light beams induce energy jumps in a colinear electron beam by multiples of their photon-energy difference. Strong recoil effects are produced by extending the electron-light interaction over millimetric distances, enabling a dramatic increase in temporal compression and substantially reshaping the electron spectra for affordable laser powers. Beyond its fundamental interest, our work introduces a practical scheme to achieve a large temporal compression of continuous electron beams without involving optical scattering by material structures.

quant-ph↗

arXiv2024

Rydberg-atom manipulation through strong interaction with free electrons

Optically trapped Rydberg atoms are a suitable platform to explore quantum many-body physics mediated by long-range atom--atom interactions that can be engineered through externally applied light fields. However, this approach is limited to dipole-allowed transitions and a spatial resolution of the order of the optical wavelength. Here, we theoretically investigate the interaction between free electrons and individual Rydberg atoms as an approach to induce nondipolar transitions with subnanometer spatial precision and a substantial degree of control over the final atomic states. We observe unity-order excitation probabilities produced by a single electron for suitably chosen combinations of electron energies and electron-beam distance to the atom. We further discuss electron--atom entanglement in combination with lateral shaping of the electron followed by postselection. Our results support free electrons as powerful tools to manipulate Rydberg atoms in previously inaccessible ways.

physics.atom-ph↗

arXiv2024

Free-electron coupling to surface polaritons mediated by small scatterers

The ability of surface polaritons (SPs) to enhance and manipulate light fields down to deep-subwavelength length scales enables applications in optical sensing and nonlinear optics at the nanoscale. However, the wavelength mismatch between light and SPs prevents direct optical excitation of surface-bound modes, thereby limiting the widespread development of SP-based photonics. Free electrons are a natural choice to directly excite strongly confined SPs because they can supply field components of high momentum at designated positions with subnanometer precision. Here, we theoretically explore free-electron--SP coupling mediated by small scatterers and show that low-energy electrons can efficiently excite surface modes with a maximum probability reached at an optimum surface--scatterer distance. By aligning the electron beam with a periodic array of scatterers placed near a polariton-supporting interface, in-plane Smith--Purcell emission results in the excitation of surface modes along well-defined directions. Our results support using scattering elements to excite SPs with low-energy electrons.

cond-mat.mes-hall↗

arXiv2024

Probing Plexciton Emission from 2D Materials on Gold Nanotrenches

Probing strongly coupled quasiparticle excitations at their intrinsic length scales offers unique insights into their properties and facilitates the design of devices with novel functionalities. In this work, we investigate the formation and emission characteristics of plexcitons, arising from the interaction between surface plasmons in narrow gold nanotrenches and excitons in monolayer WSe2. We study this strong plasmon-exciton coupling in both the far-field and the near-field. Specifically, we observe a Rabi splitting in the far-field reflection spectra of about 80 meV under ambient conditions, consistent with our theoretical modeling. Using a custom-designed near-field probe, we find that plexciton emission originates predominantly from the lower-frequency branch, which we can directly probe and map the local field distribution. We precisely determine the plexciton extension, similar to the trench width, with nanometric precision via collecting spectra at controlled probe locations. Our work opens exciting prospects for nanoscale mapping and engineering of plexcitons in complex nanostructures with potential applications in nanophotonic devices, optoelectronics, and quantum electrodynamics in nanoscale cavities.

cond-mat.mes-hall↗

arXiv2024

Toward Optimum Coupling between Free Electrons and Confined Optical Modes

Free electrons are unique 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. 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 ($\sim100$\%) coupling demanding the use of $<100$~eV electrons interacting with $<1$~eV polaritons confined down to tens of nm. 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 an efficient 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.

physics.optics↗

arXiv2024

Thermal radiation forces on planar structures with asymmetric optical response

Light carries momentum and, upon interaction with material structures, can exert forces on them. Here, we show that a planar structure with asymmetric optical response is spontaneously accelerated when placed in an environment at a different temperature. This phenomenon originates from the imbalance in the exchange rates of photons between both sides of the structure and the environment. Using a simple theoretical model, we calculate the force acting on the planar structure and its terminal velocity in vacuum, and analyze their dependence on the initial temperature and the geometrical properties of the system for different realistic materials. Our results unravel an alternative approach to manipulating objects in the nano and microscale that does not require an external source of radiation.

physics.optics↗

arXiv2024

Quantum effects in the interaction of low-energy electrons with light

The interaction between free electrons and nanoscale optical fields has emerged as a unique platform to investigate ultrafast processes in matter and explore fundamental quantum phenomena. In particular, optically modulated electrons are employed in ultrafast electron microscopy as noninvasive probes that push the limits of spatiotemporal and spectral resolution down to the picometer--attosecond--microelectronvolt range. Electron kinetic energies well above the involved photon energies are commonly employed, rendering the electron--light coupling efficiency low and, thus, only providing limited access to the wealth of quantum nonlinear phenomena underlying the dynamical response of nanostructures. Here, we theoretically investigate electron--light interactions when photons and electrons have comparable energies, revealing strong quantum and recoil effects that include a nonvanishing coupling of surface-scattered electrons to plane waves of light, inelastic electron backscattering from localized optical fields, and strong electron--light coupling under grazing electron diffraction by an illuminated crystal surface. Our results open new vistas in electron--light--matter interactions with promising applications in ultrafast electron microscopy.

cond-mat.mes-hall↗

arXiv2024

Guiding light with surface exciton-polaritons in atomically thin superlattices

Two-dimensional materials give access to the ultimate physical limits of Photonics with appealing properties for ultracompact optical components such as waveguides and modulators. Specifically, in monolayer semiconductors, a strong excitonic resonance leads to a sharp oscillation in permittivity; at energies close to an exciton, the real part of the permittivity can reach high positive values or even become negative. This extreme optical response enables surface exciton-polaritons to guide visible light bound to an atomically thin layer. However, such ultrathin waveguides support a transverse electric (TE) mode with low confinement and a transverse magnetic (TM) mode with short propagation. Here, we propose that realistic semiconductor-insulator-semiconductor superlattices consisting of monolayer WS$_2$ and hexagonal boron nitride (hBN) can improve the properties of both TE and TM modes. Compared to a single monolayer, a heterostructure with a 1-nm hBN spacer improves the confinement of the TE mode from 1.2 to around 0.5 $μ$m, whereas the out-of-plane extension of the TM mode increases from 25 to 50 nm. We propose two simple additivity rules for mode confinement valid in the ultrathin film approximation for heterostructures with increasing spacer thickness. Stacking additional WS2 monolayers into superlattices further enhances the waveguiding properties. Our results underscore the potential of monolayer superlattices as a platform for visible nanophotonics with promising optical, electrical, and magnetic tunability

physics.optics↗

arXiv2023

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↗

arXiv2023

Engineering 2D material exciton lineshape 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. Remarkable advances have been achieved through alloying, chemical and electrical doping, and applied strain. However, the integration of TMDs with other 2D materials in van der Waals heterostructures (vdWHs) to tailor novel functionalities remains largely unexplored. Here, the near-field coupling between TMDs and graphene/graphite is used to engineer the exciton lineshape and charge state. Fano-like asymmetric spectral features are produced in WS$_{2}$, MoSe$_{2}$ and WSe$_{2}$ vdWHs 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 WSe$_{2}$/graphene with a neutral exciton redshift (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.

cond-mat.mes-hall↗

arXiv2023

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↗

arXiv2023

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 gamma-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 at the intersection between particle physics and nanophotonics.

physics.optics↗

arXiv2023

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.

cond-mat.mes-hall↗

arXiv2023

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 approach 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.

cond-mat.mes-hall↗

arXiv2023

Attosecond electron microscopy by free-electron homodyne detection

Time-resolved electron microscopy aims at tracking nanoscale excitations and dynamic states of matter with a temporal resolution ultimately reaching the attosecond regime. Periodically time-varying fields in an illuminated specimen cause free-electron inelastic scattering, which enables the spectroscopic imaging of near-field intensities. However, access to the evolution of nanoscale fields and structures within the light cycle requires a sensitivity to the optical phase. Here, we introduce Free-Electron Homodyne Detection (FREHD) as a universally applicable approach to electron microscopy of phase-resolved optical responses at high spatiotemporal resolution. In this scheme, a phase-controlled reference interaction serves as the local oscillator to extract arbitrary sample-induced modulations of a free-electron wave function. We demonstrate this principle through the phase-resolved imaging of plasmonic fields with few-nanometer spatial and sub-cycle temporal resolutions. Due to its sensitivity to both phase- and amplitude-modulated electron beams, FREHD measurements will be able to detect and amplify weak signals stemming from a wide variety of microscopic origins, including linear and nonlinear optical polarizations, atomic and molecular resonances and attosecond-modulated structure factors.

physics.optics↗

arXiv2023

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 can achieve this type of confinement, although fabrication imperfections down to the subnanometer scale hinder actual developments. Here, we demonstrate narrow plasmons in atomically thin crystalline silver nanostructures fabricated by prepatterning silicon substrates and epitaxially depositing silver films of just a few atomic layers in thickness. Combined with on-demand lateral shaping, this procedure allows for an unprecedented control over optical field confinement in the near-infrared spectral region. Specifically, we observe fundamental and higher-order plasmons featuring extreme spatial confinement and high-quality factors that reflect the crystallinity of the metal. Our approach holds potential for the design and exploitation of atomic-scale nanoplasmonic devices in optoelectronics, sensing, and quantum-physics applications.

cond-mat.mes-hall↗

arXiv2023

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 potential for the generation of localized terahertz radiation pulses. However, the underlying mechanisms ruling the formation and evolution of these plasmas is 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 with fundamental insight on the generation and dynamics of micron-scale electron plasmas and their interaction with ultrafast electron pulses.

cond-mat.mes-hall↗