arXiv subjects

Hugo Lourenço-Martins

Publications and source records attributed to Hugo Lourenço-Martins.

17 recordsLinked to original sources

arXiv2026

Unveiling nanolaser physics: Non-Perturbative Measurement of the Lasing-Mode Photon Population at the Sub-Picoseconds and Nanometer Scale

Semiconducting nanowire lasers (NWLs) constitute nanometer-scale modular and tunable light sources hence an essential component for integrated opto-electronics. However, improving and optimizing NWL operation requires characterization of their near-field and dynamics at the nanometer scale, which is hampered by the light diffraction limit. In this article, we show how to non-perturbatively measure the absolute number of photons in the nanolaser cavity above the lasing threshold with sub-picosecond resolution using a GaN nanowire nanolaser, as well as map the lasing mode spatial profile at the nanoscale. This technique, based on the simultaneous measurements of the photon induced near-field electron microscopy (PINEM) and the photons far-field, allows for the complete nanoscale and time-resolved characterization of a NWL in operation while monitoring its macroscopic optical properties.

physics.optics↗

arXiv2026

Absolute measurement of the intrinsic helicity in nanophotonics

Helicity is a universal quantity describing the internal rotation of an object or a field. Whether it characterizes fundamental properties such as the spin of elementary particles or leads to practical consequences such as the toxicity or harmlessness of chiral molecules, defining and measuring it is essential. However, this remains ambiguous in the case of chiral photonic systems such as plasmonic nanoparticles or photonic metasurfaces, where contrary to common knowledge, the observation of circularly polarized dependent optical properties is not a relevant measure for the helicity. We demonstrate experimentally and theoretically that the helicity can be rigorously defined and measured in a nanophotonic system emitting circularly polarized light after excitation in the near-field by a focused electron beam. In the case of a model system composed of two plasmonic dipoles (Born-Kuhn systems), we show that the helicity of photonic modes takes on a very intuitive form and can be simply measured by symmetrizing the geometry of excitation and detection. The method could be extended to a variety of chiral photonic systems, whose locally enhanced properties make them promising for the engineering of local chirality.

physics.optics↗

arXiv2025

Morphologies of caustics studied by catastrophe charged-particle optics

This paper explores the topologies of caustics observed in instruments that employ charged particles, such as electron and ion microscopes. These geometrical figures are studied here using catastrophe theory. The application of this geometrical theory to our optical situation has enabled us to analytically reproduce the behaviours of various caustics. The interest lies mainly in the universal nature of these results since our treatment requires no prior knowledge of the optical configuration, but only a smart definition of the control space. This universal approach has finally made it possible to extract mathematical relationships between the aberration coefficients of any optical system, which were hidden by the complexity of optical trajectories but revealed by the set of catastrophes in the control space. These results provide a glimpse for future applications of caustics in the development of new corrected optical systems, especially for ions-based devices.

physics.optics↗

arXiv2025

Roadmap for Quantum Nanophotonics with Free Electrons

Over the past century, continuous advancements in electron microscopy have enabled the synthesis, control, and characterization of high-quality free-electron beams. These probes carry an evanescent electromagnetic field that can drive localized excitations and provide high-resolution information on material structures and their optical responses, currently reaching the sub-ångström and few-meV regime. Moreover, combining free electrons with pulsed light sources in ultrafast electron microscopy adds temporal resolution in the sub-femtosecond range while offering enhanced control of the electron wave function. Beyond their exceptional capabilities for time-resolved spectromicroscopy, free electrons are emerging as powerful tools in quantum nanophotonics, on par with photons in their ability to carry and transfer quantum information, create entanglement within and with a specimen, and reveal previously inaccessible details on nanoscale quantum phenomena. This Roadmap outlines the current state of this rapidly evolving field, highlights key challenges and opportunities, and discusses future directions through a collection of topical sections prepared by leading experts.

cond-mat.mes-hall↗

arXiv2024

Atomic-like selection rules in free electron scattering

Phase-shaped electron energy-loss spectroscopy (PSEELS) measures the scattering probability of structured free electron beams by a target. Over the last decade, it was shown that this scheme can be employed to emulate polarized optical spectroscopies with electrons, and therefore to transpose macroscopic optical concepts - such as dichroism - down to the deep sub-wavelength scale. In this work, we theoretically demonstrate that PSEELS can, in fact, go way further than mimicking optics and enables to map a plethora of so far inaccessible nano-optical quantities such as the electric quadrupolar momentum.

physics.optics↗

arXiv2024

Selective probing of longitudinal and transverse plasmon modes with electron phase-matching

The optical properties of metallic nanoparticles are dominated by localized surface plasmons (LSPs). Their properties only depend on the constituting material, the size and shape of the nano-object as well as its surrounding medium. In anisotropic structures, such as metallic nanorods, two families of modes generally exist, transverse and longitudinal. Their spectral and spatial overlaps usually impede their separate measurements in electron energy loss spectroscopy (EELS). In this work, we propose three different strategies enabling to overcome this difficulty and selectively probe longitudinal and transverse modes. The first strategy is numeric and relies on morphing of nano-structures, rooted in the geometrical nature of LSPs. The two other strategies exploit the relativistic and wave nature of the electrons in an EELS experiment. The first one is the phase-matching between the electron and the plasmon excitation to enhance their coupling by either tilting the sample and modifying the electron kinetic energy. The second one - polarized EELS (pEELS) - exploits the wave nature of electrons to mimic selection rules analogous to the one existing in light spectroscopies. The above-mentioned strategies are exemplified - either experimentally or numerically - on a canonical plasmonic toy model: the nano-rod. The goal of the paper is to bring together the state-of-the-art concepts of EELS for plasmonics to tackle a pedestrian problem in this field.

physics.optics↗

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

Photon induced near-field electron microscopy from nanostructured metallic films and membranes

We investigate - both experimentally and theoretically - the inelastic interaction between fast electrons and the electromagnetic field scattered by metallic apertures and nanostructures on dielectric membranes using photon induced near-field electron microscopy. The experiments - performed in a high brightness ultrafast transmission electron microscope - on gold apertures on silicon nitride membranes reveal strong modulations of the electron-light coupling strength. We demonstrates that this effect results from the combined action of the electric field scattered by the aperture edges and the reflection and transmission of the incident wave by the dielectric membrane. Moreover, when a nanostructure is added inside the metallic aperture, the new scattered field interferes with the previous contributions, thus imprinting the optical response of the nanostructure in additional modulations of the electron-light coupling strength. Using systematic electrodynamics simulations based on the Green dyadic method, we quantitatively analyze these different contributions to the electron-light coupling and propose further applications.

cond-mat.mtrl-sci↗

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↗

arXiv2020

Bridging nano-optics and condensed matter formalisms in a unified description of inelastic scattering of relativistic electron beams

In the last decades, the blossoming of experimental breakthroughs in the domain of electron energy loss spectroscopy (EELS) has triggered a variety of theoretical developments. Those have to deal with completely different situations, from atomically resolved phonon mapping to electron circular dichroism passing by surface plasmon mapping. All of them rely on very different physical approximations and have not yet been reconciled, despite early attempts to do so. As an effort in that direction, we report on the development of a scalar relativistic quantum electrodynamic (QED) approach of the inelastic scattering of fast electrons. This theory can be adapted to describe all modern EELS experiments, and under the relevant approximations, can be reduced to any of the last EELS theories. In that aim, we present in this paper the state of the art and the basics of scalar relativistic QED relevant to the electron inelastic scattering. We then give a clear relation between the two once antagonist descriptions of the EELS, the retarded green Dyadic, usually applied to describe photonic excitations and the quasi-static mixed dynamic form factor (MDFF), more adapted to describe core electronic excitations of material. We then use this theory to establish two important EELS-related equations. The first one relates the spatially resolved EELS to the imaginary part of the photon propagator and the incoming and outgoing electron beam wavefunction, synthesizing the most common theories developed for analyzing spatially resolved EELS experiments. The second one shows that the evolution of the electron beam density matrix is proportional to the mutual coherence tensor, proving that quite universally, the electromagnetic correlations in the target are imprinted in the coherence properties of the probing electron beam.

cond-mat.mes-hall↗

arXiv2020

Spontaneous and Stimulated Electron-Photon Interactions in Nanoscale Plasmonic Near Fields

We demonstrate spatially-resolved measurements of spontaneous and stimulated electron-photon interactions in nanoscale optical near fields using electron energy-loss spectroscopy (EELS), cathodoluminescence spectroscopy (CL), and photon-induced near-field electron microscopy (PINEM). Specifically, we study resonant surface plasmon modes that are tightly confined to the tip apexes of an Au nanostar, enabling a direct correlation of EELS, CL, and PINEM on the same physical structure at the nanometer length scale. Complemented by numerical electromagnetic boundary-element method calculations, we discuss the spontaneous and stimulated electron-photon interaction strength and spatial dependence of our EELS, CL and PINEM distributions. We demonstrate that in the limit of an isolated tip mode, spatial variations in the electron-near field coupling are fully determined by the modal electric field profile, irrespective of the spontaneous (in EELS and CL) or stimulated nature (in PINEM) of the process. Yet we show that coupling to the tip modes crucially depends on the incident electron energy with a maximum at a few keV, depending on the proximity of the interaction to the tip apex. Our results provide elementary insights into spontaneous and stimulated electron-light-matter interactions at the nanoscale that have key implications for research on (quantum) coherent optical phenomena in electron microscopy.

physics.optics↗

arXiv2020

Optical polarization analogue in free electrons beams

Fast electrons spectromicroscopies enable to measure quantitatively the optical response of excitations with unrivaled spatial resolution. However, due to their inherently scalar nature, electron waves cannot access to polarization-related quantities. In spite of promising attempts based on the conversion of concepts originating from singular optics (such as vortex beams), the definition of an optical polarization analogue for fast electrons has remained a dead letter. Here, we establish such an analogue as the dipole transition vector of the electron between two well-chosen singular wave states. We show that electron energy-loss spectroscopy (EELS) allows a direct measurement of the \textit{polarized} electromagnetic local density of states. In particular, in the case of circular polarization, it measures directly the local optical spin density. This work establishes EELS as a quantitative technique to tackle fundamental issues in nano-optics, such as super-chirality, the local polarization of dark excitations or polarization singularities at the nanoscale.

physics.optics↗

arXiv2019

Controlling free electrons with optical whispering-gallery modes

Free-electron beams serve as uniquely versatile probes of microscopic structure and composition, and have repeatedly revolutionized atomic-scale imaging, from solid-state physics to structural biology. Over the past decade, the manipulation and interaction of electrons with optical fields has seen significant progress, enabling novel imaging methods, schemes of near-field electron acceleration, and culminating in 4D microscopy techniques with both high temporal and spatial resolution. However, weak coupling strengths of electron beams to optical excitations are a standing issue for existing and emerging applications of optical free-electron control. Here, we demonstrate phase matched near-field coupling of a free-electron beam to optical whispering gallery modes of dielectric microresonators. The cavity-enhanced interaction with these optically excited modes imprints a strong phase modulation on co-propagating electrons, which leads to electron-energy sidebands up to hundreds of photon orders and a spectral broadening of 700 eV. Mapping the near-field interaction with ultrashort electron pulses in space and time, we trace the temporal ring-down of the microresonator following a femtosecond excitation and observe the cavity's resonant spectral response. Resonantly enhancing the coupling of electrons and light via optical cavities, with efficient injection and extraction, can open up novel applications such as continuous-wave acceleration, attosecond structuring, and real-time all-optical electron detection.

physics.optics↗

arXiv2019

Point defect states emergence in a plasmonic crystal

Plasmonic crystals are well known to have band structure including a bandgap, enabling the control of surface plasmon propagation and confinement. The band dispersion relation of bulk crystals has been generally measured by momentum-resolved spectroscopy using far field optical techniques while the defects introduced in the crystals have separately been investigated by near field imaging techniques so far. Particularly, defect related energy levels introduced in the plasmonic band gap have not been observed experimentally. In order to investigate such a localized mode, we performed electron energy-loss spectroscopy (EELS), on a point defect introduced in a plasmonic crystal made up of flat cylinders protruding out of a metal film and arranged on a triangular lattice. The energy level of the defect mode was observed to lie within the full band-gap energy range. This was confirmed by a momentum-resolved EELS measurement of the band gap performed on the same plasmonic crystal. Furthermore, we experimentally and theoretically investigated the emergence of the defect states by starting with a corral of flat cylinders protrusions and adding sequentially additional shells of those in order to eventually forming a plasmonic band-gap crystal encompassing a single point defect. It is demonstrated that a defect-like state already forms with a crystal made up of only two shells.

physics.optics↗

arXiv2019

Tailored nanoscale plasmon-enhanced vibrational electron spectroscopy

Vibrational optical spectroscopies can be enhanced by surface plasmons to reach molecular-sized limits of detection and characterization. The level of enhancement strongly depends on microscopic details of the sample that are generally missed by macroscopic techniques. Here we investigate phonons in h-BN by coupling them to silver-nanowire plasmons, whose energy is tuned by modifying the nanowire length. Specifically, we use electron beam milling to accurately and iteratively change the nanowire length, followed by electron energy-loss spectroscopy to reveal the plasmon-enhanced vibrational features of h-BN. This allows us to investigate otherwise hidden bulk phonons and observe strong plasmon-phonon coupling. The new milling-and-spectroscopy technique holds great potential for resolving vibrational features in material nanostructures.

cond-mat.mes-hall↗

arXiv2019

Visualizing plasmon-exciton polaritons at the nanoscale using electron microscopy

Polaritons are compositional light-matter quasiparticles that have recently enabled remarkable breakthroughs in quantum and nonlinear optics, as well as in material science. Despite the enormous progress, however, a direct nanometer-scale visualization of polaritons has remained an open challenge. Here, we demonstrate that plasmon-exciton polaritons, or plexcitons, generated by a hybrid system composed of an individual silver nanoparticle and a few-layer transition metal dichalcogenide can be spectroscopically mapped with nanometer spatial resolution using electron energy loss spectroscopy in a scanning transmission electron microscope. Our experiments reveal important insights about the coupling process, which have not been reported so far. These include nanoscale variation of Rabi splitting and plasmon-exciton detuning, as well as absorption-dominated extinction signals, which in turn provide the ultimate evidence for the plasmon-exciton hybridization in the strong coupling regime. These findings pioneer new possibilities for in-depth studies of polariton-related phenomena with nanometer spatial resolution.

physics.optics↗

arXiv2017

Vibrational surface EELS probes confined Fuchs-Kliewer modes

Recently, two reports have demonstrated the amazing possibility to probe vibrational excitations from nanoparticles with a spatial resolution much smaller than the corresponding free-space phonon wavelength using electron energy loss spectroscopy (EELS). While Lagos et al. evidenced a strong spatial and spectral modulation of the EELS signal over a nanoparticle, Krivanek et al. did not. Here, we show that discrepancies among different EELS experiments as well as their relation to optical near- and far-field optical experiments can be understood by introducing the concept of confined bright and dark Fuchs-Kliewer modes, whose density of states is probed by EELS. Such a concise formalism is the vibrational counterpart of the broadly used formalism for localized surface plasmons; it makes it straightforward to predict or interpret phenomena already known for localized surface plasmons such as environment-related energy shifts or the possibility of 3D mapping of the related surface charge densities.

cond-mat.mtrl-sci↗