147 research outputs found
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
Probing Quantum Optical Excitations with Fast Electrons
Probing optical excitations with nanometer resolution is important for
understanding their dynamics and interactions down to the atomic scale.
Electron microscopes currently offer the unparalleled ability of rendering
spatially-resolved electron spectra with combined meV and sub-nm resolution,
while the use of ultrafast optical pulses enables fs temporal resolution and
exposure of the electrons to ultraintense confined optical fields. Here, we
theoretically investigate fundamental aspects of the interaction of fast
electrons with localized optical modes that are made possible by these
advances. We use a quantum-optics description of the optical field to predict
that the resulting electron spectra strongly depend on the statistics of the
sample excitations (bosonic or fermionic) and their population (Fock, coherent,
or thermal), whose autocorrelation functions are directly retrieved from the
ratios of electron gain intensities. We further explore feasible experimental
scenarios to probe the quantum characteristics of the sampled excitations and
their populations.Comment: 13 pages, 6 figures, 56 reference
Development of a high brightness ultrafast Transmission Electron Microscope based on a laser-driven cold field emission source
We report on the development of an ultrafast Transmission Electron Microscope
based on a cold field emission source which can operate in either DC or
ultrafast mode. Electron emission from a tungsten nanotip is triggered by
femtosecond laser pulses which are tightly focused by optical components
integrated inside a cold field emission source close to the cathode. The
properties of the electron probe (brightness, angular current density,
stability) are quantitatively determined. The measured brightness is the
largest reported so far for UTEMs. Examples of imaging, diffraction and
spectroscopy using ultrashort electron pulses are given. Finally, the potential
of this instrument is illustrated by performing electron holography in the
off-axis configuration using ultrashort electron pulses.Comment: 23 pages, 9 figure
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.Comment: Re-Submission to SciPost. Updated version: minor revisions, SciPost
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Modes propres plasmon de surface révélés par spectroscopies d'électrons rapides (de systèmes modèles simples vers des systèmes complexes)
Les plasmons de surface (SP) sont des excitations mêlant électrons et photons localisées aux surfaceset interfaces métalliques. On peut les voir classiquement comme les modes électromagnétiquespropres d un ensemble constitué d un métal et d un diélectrique. Cette thèse se base sur la capacitéofferte par les techniques de spectroscopie utilisant des électrons rapides disponibles dans un microscopeélectronique à balayage en transmission (STEM), de cartographier, dans une large gammespectrale et avec une résolution spatiale nanométrique, les modes propres SP. Une telle capacitéa été démontrée séparément, durant ces dernières années, par des expériences de spectroscopie depertes d énergie d électrons (EELS), qui mesurent l énergie perdue par des électrons rapides intéragissantavec un échantillon, et de cathodoluminescence (CL), qui mesurent l énergie réémisepar l échantillon par l intermédiaire de photons, toutes deux résolues spatialement. Dans le cas del EELS, ces résultats expérimentaux sont aujourd hui interprétables à l aide d analyses théoriquesconvaincantes tendant à prouver que la quantité mesurée dans une telle expérience peut être interprétéede façon sûre en terme de modes propres de surface de l échantillon. Afin d élargir une telleinterprétation aux techniques de spectroscopies utilisant des électrons rapides en général, j ai effectuédes expériences combinées d EELS et de CL résolues spatialement sur une nanoparticle uniquesimple (un nanoprisme d or). J ai montré que les résultats offerts par ces deux techniques présententde fortes similitudes mais également de légères différences, ce qui est confirmé par des simulationsnumériques. J ai étendu l analyse théorique du signal EELS au signal CL, et ai montré que la CLcartographie, tout comme l EELS, les modes de surface radiatifs du sytème, mais avec des propriétésspectrales légèrement différentes. Ce travail constitue une preuve de principe clarifiant les quantitésmesurées en EELS et CL sur des systèmes métal-dielectriques. Ces dernières sont démontrées êtrerespectivement des équivalents nanométriques des spectroscopies d extinction et de diffusion de lalumière. Basé sur cette interprétation, j ai utilisé l EELS pour dévoiler les modes propres SP demilieux métalliques aléatoires (dans notre cas, des films semicontinus métalliques avant le seuil depercolation). Ces modes propres constituent une problématique de longue date dans le domainede la nanooptique. J ai directement identifié ces modes par des mesures et le traitement de leursrésultats. J ai complètement caractérisé ces modes propres via les variations spatiales de l intensitéliée à leur champ électrique, une énergie propre et un taux de relaxation. Ce faisant, j ai montré quela géométrie fractale du milieu, dont la prédominance croit au fur et à mesure que l on s approchede la percolation, est responsable de l existence de modes propres de type aléatoire à basse énergie.Surface Plasmons (SP) are elementary excitations mixing electrons and photons at metal surfaces,which can be seen in a classical electrodynamics framework as electromagnetic surface eigenmodesof a metal-dielectric system. The present work bases on the ability of mapping SP eigenmodes withnanometric spatial resolution over a broad spectral range using spatially resolved fast electron basedspectroscopies in a Scanning Transmission Electron Microscope (STEM). Such an ability has beenseparately demonstrated during the last few years by many spatially resolved experiments of ElectronEnergy Loss Spectroscopy (EELS), which measures the energy lost by fast electrons interactingwith the sample, and CathodoLuminescence (CL), which measures the energy released by subsequentlyemitted photons. In the case of EELS, the experimental results are today well accountedfor by strong theory elements which tend to show that the quantity measured in an experiment canbe safely interpreted in terms of the surface eigenmodes of the sample. In order to broaden thisinterpretation to fast electron based spectroscopies in general, I have performed combined spatiallyresolved EELS and CL experiments on a simple single nanoparticle (a gold nanoprism). I have shownthat EELS and CL results bear strong similarities but also slight differences, which is confirmed bynumerical simulations. I have extended the theoretical analysis of EELS to CL to show that CLmaps equally well than EELS the radiative surface eigenmodes, yet with slightly different spectralfeatures. This work is a proof of principle clarifiying the quantities measured in EELS and CL,which are shown to be respectively some nanometric equivalent of extinction and scattering spectroscopieswhen applied to metal-dielectric systems. Based on this interpretation, I have applied EELSto reveal the SP eigenmodes of random metallic media (in our case, semicontinuous metal films beforethe percolation threshold). These SP eigenmodes constitute a long standing issue in nanooptics.I have directly identified the eigenmodes from measurements and data processing. I havefully characterized these eigenmodes experimentally through an electric field intensity pattern, aneigenenergy and a relaxation rate. Doing so, I have shown that the fractal geometry of the medium,which grows towards the percolation, induces random-like eigenmodes in the system at low energies.Keywords: Surface plasmons, fast electron based spectroscopies, scanning transmission electronmicroscopy, disordered mediaPARIS11-SCD-Bib. électronique (914719901) / SudocSudocFranceF
Plasmonic Oligomers with Tunable Conductive Nanojunctions
International audienceEngineering plasmonic hot-spots is essential for applications of plasmonic nanoparticles. A particularly appealing route is to weld plasmonic nanoparticles together to form more complex structures sustaining plasmons with symmetries targeted to given applications. However, thecontrol of the welding and subsequent hotspot characteristic is still challenging. Herein, we demonstrate an original method that connects gold particles to their neighbors by another metal of choice. We first assemble gold bipyramids in a tip-to-tip configuration, yielding short chainsof variable length and grow metallic junctions in a second step. We follow the chain formation and the deposition of the second metal (i.e. silver or palladium) via UV/Vis spectroscopy and we map the plasmonic properties using electron energy loss spectroscopy. The formation ofsilver bridges leads to a huge redshift of the longitudinal plasmon modes into the mid-infrared region, while the addition of palladium results in a redshift accompanied by significant plasmon damping
Excitons and stacking order in h-BN
The strong excitonic emission at 5.75 eV of hexagonal boron nitride (h-BN)
makes this material one of the most promising candidate for light emitting
devices in the far ultraviolet (UV). However, single excitons occur only in
perfect monocrystals that are extremely hard to synthesize, while regular h-BN
samples present a complex emission spectrum with several additional peaks. The
microscopic origin of these additional emissions has not yet been understood.
In this work we address this problem using an experimental and theoretical
approach that combines nanometric resolved cathodoluminescence, high resolution
transmission electron microscopy and state of the art theoretical spectroscopy
methods. We demonstrate that emission spectra are strongly inhomogeneus within
individual flakes and that additional excitons occur at structural
deformations, such as faceted plane folds, that lead to local changes of the
h-BN stacking order
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
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