arXiv subjects

F. Javier García de Abajo

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

At least 73 records · Page 4Linked to original sources

arXiv2022

Unveiling the coupling of single metallic nanoparticles to whispering-gallery microcavities

Whispering-gallery mode resonators host multiple trapped narrowband circulating optical resonances that find applications in quantum electrodynamics, optomechanics, and sensing. However, the spherical symmetry and low field leakage of dielectric microspheres make it difficult to probe their high-quality optical modes using far-field radiation. Even so, local field enhancement from metallic nanoparticles (MNPs) coupled to the resonators can interface the optical far-field and the bounded cavity modes. In this work, we study the interaction between whispering-gallery modes and MNP surface plasmons with nanometric spatial resolution by using electron-beam spectroscopies in a scanning transmission electron microscope. We show that gallery modes are induced over a selective spectral range of the nanoparticle plasmons, and additionally, their polarization can be controlled by the induced dipole moment of the MNP. Our study demonstrates a viable mechanism to effectively excite high-quality-factor whispering-gallery modes and holds potential for applications in optical sensing and light manipulation.

physics.optics↗

arXiv2022

Quantum-phase two-dimensional materials

The modification of electronic band structures and the subsequent tuning of electrical, optical, and thermal material properties is a central theme in the engineering and fundamental understanding of solid-state systems. In this scenario, atomically thin materials offer an appealing platform because they are extremely susceptible to electric and magnetic gating, as well as to interlayer hybridization in stacked configurations, providing the means to customize and actively modulate their response functions. Here, we introduce a radically different approach to material engineering relying on the self-interaction that electrons in a two-dimensional material experience when an electrically neutral structure is placed in its vicinity. Employing rigorous theoretical methods, we show that electrons in a semiconductor atomic monolayer acquire a quantum phase resulting from the image potential induced by the presence of a neighboring periodic array of conducting ribbons, which in turn produces strong modifications in the optical, electrical, and thermal properties of the monolayer, specifically giving rise to the emergence of interband optical absorption, plasmon hybridization, and metal-insulator transitions. Beyond its fundamental interest, material engineering based on the quantum phase induced by noncontact neighboring structures represents a disruptive approach to tailor the properties of atomic layers for application in nanodevices.

cond-mat.mtrl-sci↗

arXiv2022

Doping-driven topological polaritons in graphene/α-MoO3 heterostructures

Controlling the charge carrier density provides an efficient way to trigger phase transitions and modulate the optoelectronic properties in natural materials. This approach could be used to induce topological transitions in the optical response of photonic systems. Here, we predict a topological transition in the isofrequency dispersion contours of hybrid polaritons supported by a two-dimensional heterostructure consisting of graphene and $α$-phase molybdenum trioxide ($α$-MoO3). By chemically changing the doping level of graphene, we experimentally demonstrate that the contour topology of polariton isofrequency surfaces transforms from open to closed shapes as a result of doping-dependent polariton hybridization. Moreover, by changing the substrate medium for the heterostructure, the dispersion contour can be further engineered into a rather flattened shape at the topological transition, thus supporting tunable polariton canalization and providing the means to locally control the topology. We demonstrate this idea to achieve extremely subwavelength focusing by using a 1.2-$μ$m-wide silica substrate as a negative refraction lens. Our findings open a disruptive approach toward promising on-chip applications in nanoimaging, optical sensing, and manipulation of nanoscale energy transfer.

physics.optics↗

arXiv2021

Approaching the Purcell factor limit with whispering-gallery hyperbolic phonon polaritons in hBN nanotubes

Enhanced light-matter interaction at the nanoscale is pivotal in the foundation of nonlinear optics, quantum optics, and nanophotonics, which are essential for a vast range of applications including single-photon sources, nanolasers, and nanosensors. In this context, the combination of strongly confined polaritons and low-loss nanocavities provides a promising way to enhance light-matter interaction, thus giving rise to a high density of optical states, as quantified by the so-called Purcell factor - the ratio of the decay rate of an optical quantum emitter to its value in free space. Here, we exploit whispering-gallery hyperbolic-phonon-polariton (WG-HPhP) modes in hBN nanotubes (BNNTs) to demonstrate record-high Purcell factors (~10^12) driven by the deep-subwavelength confinement of phonon polaritons and the low intrinsic losses in these atomically smooth nanocavities. Furthermore, the measured Purcell factor increases with decreasing BNNT radius down to 5 nm, a result that extrapolates to ~10^14 in a single-walled BNNT. Our study supports WG-HPhP modes in one-dimensional nanotubes as a powerful platform for investigating ultrastrong light-matter interactions, which open exciting perspectives for applications in single-molecular sensors and nanolasers.

physics.optics↗

arXiv2021

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↗

arXiv2021

Atomic Floquet physics revealed by free electrons

We theoretically investigate the ability of free electrons to yield information on the nonlinear Floquet dynamics of atomic systems subject to intense external illumination. By applying a quantum-mechanical formalism to describe the atom-electron interaction under the presence of a monochromatic classical light field, we observe multiple energy features that reveal a large departure from non-illumination conditions in two- and three-level illuminated atoms, including the emergence of energy features associated with direct electron-photon exchanges, as well as a varied set of Floquet resonances that strongly depend on the light intensity and frequency. Our results unveil a wealth of effects associated with the interaction between free electrons and optically driven electronic systems.

quant-ph↗

arXiv2021

Low-loss tunable infrared plasmons in the high-mobility perovskite (Ba,La)SnO$_3$

BaSnO$_3$ exhibits the highest carrier mobility among perovskite oxides, making it ideal for oxide electronics. Collective charge carrier oscillations, plasmons, are expected to arise in this material, thus providing a tool to control the nanoscale optical field for optoelectronics applications. Here, we demonstrate the existence of relatively long-lived plasmons supported by high-mobility charge carriers in La-doped BaSnO$_3$ (BLSO). By exploiting the high spatial and energy resolution of electron energy-loss spectroscopy with a focused beam in a scanning transmission electron microscope, we systematically investigate the dispersion, confinement ratio, and damping of infrared localized surface plasmons (LSP) in BLSO nanoparticles. We find that the LSPs in BLSO are highly spatially confined compared to those sustained by noble metals and have relatively low loss and high quality factor compared to other doped oxides. Further analysis clarifies the relation between plasmon damping and carrier mobility in BLSO. Our results support the use of nanostructured degenerate semiconductors for plasmonic applications in the infrared region and establish a relevant alternative to more traditional plasmonic materials.

physics.app-ph↗

arXiv2021

Inelastic Mach-Zehnder Interferometry with Free Electrons

We use a novel scanning electron Mach-Zehnder interferometer constructed in a conventional transmission electron microscope to perform inelastic interferometric imaging with free electrons. An electron wave function is prepared in two paths that pass on opposite sides of a gold nanoparticle, where plasmons are excited before the paths are recombined to produce electron interference. We show that the measured spectra are consistent with theoretical predictions, specifically that the interference signal formed by inelastically scattered electrons is pi out of phase with respect to that formed by elastically scattered electrons. This technique is sensitive to the phase of localized optical modes because the interference signal amounts to a substantial fraction of the transmitted electrons. We thus argue that inelastic interferometric imaging with our scanning electron Mach-Zehnder interferometer provides a new platform for controlling the transverse momentum of a free electron and studying coherent electron-matter interactions at the nanoscale.

cond-mat.mes-hall↗

arXiv2021

Inelastic Scattering of Electron Beams by Nonreciprocal Nanotructures

Probing optical excitations with high resolution is important for understanding their dynamics and controlling their interaction with other photonic elements. This can be done using state-of-the-art electron microscopes, which provide the means to sample optical excitations with combined meV--sub-nm energy--space resolution. For reciprocal photonic systems, electrons traveling in opposite directions produce identical signals, while this symmetry is broken in nonreciprocal structures. Here, we theoretically investigate this phenomenon by analyzing electron energy-loss spectroscopy (EELS) and cathodoluminescence (CL) in structures consisting of magnetically biased InAs as an instance of gyrotropic nonreciprocal material. We find that the spectral features associated with excitations of InAs films depend on the electron propagation direction in both EELS and CL, and can be tuned by varying the applied magnetic field within a relatively modest sub-tesla regime. The magnetic field modifies the optical field distribution of the sampled resonances, and this in turn produces a direction-dependent coupling to the electron. The present results pave the way to the use of electron microscope spectroscopies to explore the near-field characteristics of nonreciprocal systems with high spatial resolution.

cond-mat.mtrl-sci↗

arXiv2021

Nonlinear Tunable Vibrational Response in Hexagonal Boron Nitride

Nonlinear light-matter interactions in structured materials are the source of exciting properties and enable vanguard applications in photonics. However, the magnitude of nonlinear effects is generally small, thus requiring high optical intensities for their manifestation at the nanoscale. Here, we reveal a large nonlinear response of monolayer hexagonal boron nitride (hBN) in the mid-infrared phonon-polariton region, triggered by the strongly anharmonic potential associated with atomic vibrations in this material. We present robust first-principles theory predicting a threshold light field $\sim40\,$MV/m to produce order-unity effects in Kerr nonlinearities and harmonic generation, which are made possible by a combination of the long lifetimes exhibited by optical phonons and the strongly asymmetric landscape of the configuration energy in hBN. We further foresee polariton blockade at the few-quanta level in nanometer-sized structures. In addition, by mixing static and optical fields, the strong nonlinear response of monolayer hBN gives rise to substantial frequency shifts of optical phonon modes, exceeding their spectral width for in-plane DC fields that are attainable using lateral gating technology. We therefore predict a practical scheme for electrical tunability of the vibrational modes with potential interest in mid-infrared optoelectronics. The strong nonlinear response, low damping, and robustness of hBN polaritons set the stage for the development of applications in light modulation, sensing, and metrology, while triggering the search for intense vibrational nonlinear response in other ionic materials.

cond-mat.mtrl-sci↗

arXiv2021

Revealing Nanoscale Confinement Effects on Hyperbolic Phonon Polaritons with an Electron Beam

Hyperbolic phonon polaritons (HPhPs) in hexagonal boron nitride (hBN) enable the direct manipulation of mid-infrared light at nanometer scales, many orders of magnitude below the free-space light wavelength. High resolution monochromated electron energy-loss spectroscopy (EELS) facilitates measurement of excitations with energies extending into the mid-infrared while maintaining nanoscale spatial resolution, making it ideal for detecting HPhPs. The electron beam is a precise source and probe of HPhPs, that allows us to perform novel experiments to observe nanoscale confinement in HPhP structures and directly extract hBN polariton dispersions for both modes in the bulk of the flake and modes along the edge. Our measurements reveal technologically important non-trivial phenomena, such as localized polaritons induced by environmental heterogeneity, enhanced and suppressed excitation due to two-dimensional interference, and strong modification of high-momenta excitations of edge-confined polaritons by nanoscale heterogeneity on edge boundaries. Our work opens exciting prospects for the design of real-world optical mid-infrared devices based on hyperbolic polaritons.

physics.optics↗

arXiv2021

Modulation of Cathodoluminescence Emission by Interference with External Light

Spontaneous processes triggered in a sample by free electrons are commonly regarded as incoherent, and therefore unable to interfere with external light sources. Here, we challenge this concept by showing through first-principles theory that light and free-electron pulses can interfere when interacting with a nanostructure, giving rise to a modulation in the spectral distribution of the cathodoluminescence light emission that is strongly dependent on the electron wave function. Specifically, for a temporally focused electron, cathodoluminescence can be cancelled upon illumination with a spectrally modulated dimmed laser that is phase-locked relative to the electron density profile. We illustrate this idea with realistic simulations under attainable conditions in currently available ultrafast electron microscopes. We further argue that the interference between excitations produced by light and free electrons opens a new window to manipulate the ultrafast materials response by combining the spectral and temporal selectivity of the light with the atomic resolution of electron beams.

physics.optics↗

arXiv2021

Optical Excitations with Electron Beams: Challenges and Opportunities

Free electron beams such as those employed in electron microscopes have evolved into powerful tools to investigate photonic nanostructures with an unrivaled combination of spatial and spectral precision through the analysis of electron energy losses and cathodoluminescence light emission. In combination with ultrafast optics, the emerging field of ultrafast electron microscopy utilizes synchronized femtosecond electron and light pulses that are aimed at the sampled structures, holding the promise to bring simultaneous sub-Angstrom--sub-fs--sub-meV space-time-energy resolution to the study of material and optical-field dynamics. In addition, these advances enable the manipulation of the wave function of individual free electrons in unprecedented ways, opening sound prospects to probe and control quantum excitations at the nanoscale. Here, we provide an overview of photonics research based on free electrons, supplemented by original theoretical insights, and discussion of challenges and opportunities. In particular, we show that the excitation probability by a single electron is independent of its wave function, apart from a classical average over the transverse beam density profile, whereas the probability for two or more modulated electrons depends on their relative spatial arrangement, thus reflecting the quantum nature of their interactions. We derive first-principles analytical expressions that embody these results and have general validity for arbitrarily shaped electrons and any type of electron-sample interaction. We conclude with perspectives on various exciting directions for disruptive approaches to non-invasive spectroscopy and microscopy, the possibility of sampling the nonlinear optical response at the nanoscale, the manipulation of the density matrices associated with free electrons and optical sample modes, and applications in optical modulation of electron beams.

quant-ph↗

arXiv2021

Atomic-Scale Vibrational Mapping and Isotope Identification with Electron Beams

Transmission electron microscopy and spectroscopy currently enable the acquisition of spatially resolved spectral information from a specimen by focusing electron beams down to a sub-Angstrom spot and then analyzing the energy of the inelastically scattered electrons with few-meV energy resolution. This technique has recently been used to experimentally resolve vibrational modes in 2D materials emerging at mid-infrared frequencies. Here, based on first-principles theory, we demonstrate the possibility of identifying single isotope atom impurities in a nanostructure through the trace that they leave in the spectral and spatial characteristics of the vibrational modes. Specifically, we examine a hexagonal boron nitride molecule as an example of application, in which the presence of a single isotope impurity is revealed through dramatic changes in the electron spectra, as well as in the space-, energy-, and momentum-resolved inelastic electron signal. We compare these results with conventional far-field spectroscopy, showing that electron beams offer superior spatial resolution combined with the ability to probe the complete set of vibrational modes, including those that are optically dark. Our study is relevant for the atomic-scale characterization of vibrational modes in novel materials, including a detailed mapping of isotope distributions.

cond-mat.mtrl-sci↗

arXiv2021

Free-Electron Shaping Using Quantum Light

Controlling the wave function of free electrons is important to improve the spatial resolution of electron microscopes, the efficiency of electron interaction with sample modes of interest, and our ability to probe ultrafast materials dynamics at the nanoscale. In this context, attosecond electron compression has been recently demonstrated through interaction with the near fields created by scattering of ultrashort laser pulses at nanostructures followed by free electron propagation. Here, we show that control over electron pulse shaping, compression, and statistics can be improved by replacing coherent laser excitation by interaction with quantum light. We find that compression is accelerated for fixed optical intensity by using phase-squeezed light, while amplitude squeezing produces ultrashort double-pulse profiles. The generated electron pulses exhibit periodic revivals in complete analogy to the optical Talbot effect. We further reveal that the coherences created in a sample by interaction with the modulated electron are strongly dependent on the statistics of the modulating light, while the diagonal part of the sample density matrix reduces to a Poissonian distribution regardless of the type of light used to shape the electron. The present study opens a new direction toward the generation of free electron pulses with additional control over duration, shape, and statistics, which directly affect their interaction with a sample.

quant-ph↗

arXiv2020

Can Copper Nanostructures Sustain High-Quality Plasmons?

Silver is considered to be the king among plasmonic materials because it features low inelastic absorption in the visible and infrared (vis-IR) spectral regions compared to other metals. In contrast, copper is commonly regarded as being too lossy for plasmonic applications. Here, we experimentally demonstrate vis-IR plasmons in long copper nanowires (NWs) with quality factors that exceed a value of 60, as determined by spatially resolved, high-resolution electron energy-loss spectroscopy (EELS) measurements. We explain this counterintuitive result by the fact that plasmons in these metal wires have most of their electromagnetic energy outside the metal, and thus, they are less sensitive to inelastic losses in the material. We present an extensive set of data acquired on long silver and copper NWs of varying diameters supporting this conclusion and further allowing us to understand the relative roles played by radiative and nonradiative losses in plasmons that span a wide range of energies down to $<20\,$meV. At such small plasmon energies, thermal population of these modes becomes significant enough to enable the observation of electron energy gains associated with plasmon absorption events. Our results support the use of copper as an attractive cheap and abundant material platform for high quality plasmons in elongated nanostructures.

cond-mat.mtrl-sci↗

arXiv2020

Ultrafast Momentum-Resolved Probing of Plasmon Thermal Dynamics with Free Electrons

Current advances in ultrafast electron microscopy make it possible to combine optical pumping of a nanostructure and electron beam probing with subångstrom and femtosecond spatiotemporal resolution. We present a theory predicting that this technique can reveal a rich out-of-equilibrium dynamics of plasmon excitations in graphene and graphite samples. In a disruptive departure from the traditional probing of nanoscale excitations based on the identification of spectral features in the transmitted electrons, we show that measurement of angle-resolved, energy-integrated inelastic electron scattering can trace the temporal evolution of plasmons in these structures and provide momentum-resolved mode identification, thus avoiding the need for highly-monochromatic electron beams and the use of electron spectrometers. This previously unexplored approach to study the ultrafast dynamics of optical excitations can be of interest to understand and manipulate polaritons in 2D semiconductors and other materials exhibiting a strong thermo-optical response.

cond-mat.mtrl-sci↗

arXiv2020

Optical coherence transfer mediated by free electrons

We investigate theoretically the quantum-coherence properties of the cathodoluminescence (CL) emission produced by a temporally modulated electron beam. Specifically, we consider the quantum-optical correlations of CL from electrons that are previously shaped by a laser field. The main prediction here is the presence of phase correlations between the emitted CL field and the electron-modulating laser, even though the emission intensity and spectral profile are independent of the electron state. In addition, the coherence of the CL field extends to harmonics of the laser frequency. Since electron beams can be focused to below one Angstrom, their ability to transfer optical coherence could enable ultra precise excitation, manipulation, and spectroscopy of nanoscale quantum systems.

quant-ph↗