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 templat

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

Far-Field Radiation of Three-Dimensional Plasmonic Gold Tapers near Apexes

International audienceThree-dimensional plasmonic gold tapers are widely used structures in nano-optics for achieving imaging at the nanometer scale, enhanced spectroscopy, confined light sources, and ultrafast photoelectron emission. To understand their radiation properties further, especially in the proximity of the apex at the nanoscale, we employ cathodoluminescence spectroscopy with high spatial and energy resolution. The plasmon-induced radiation in the visible spectral range from three-dimensional gold tapers with opening angles of 13°and 47°is investigated under local electron excitation. We observe a much weaker radiation from the apex of the 13°taper than from that of the 47°taper. By means of finite-difference time-domain simulations we show that for small opening angles plasmon modes that are created at the apex are efficiently guided along the taper shaft. In contrast for tapers with larger opening angles, generated plasmon polaritons experience larger radiation damping. Interestingly, we find for both tapers that the most intense radiation comes from locations a few hundreds of nanometers behind the apexes, instead of exactly at the apexes. Our findings provide useful details for the design of plasmonic gold tapers as confined light sources or light absorbers

Design and implementation of a device based on an off-axis parabolic mirror to perform luminescence experiments in a scanning tunneling microscope

We present the design, implementation, and illustrative results of a light collection/injection strategy based on an off-axis parabolic mirror collector for a low-temperature Scanning Tunneling Microscope (STM). This device allows us to perform STM induced Light Emission (STM-LE) and Cathodoluminescence (STM-CL) experiments and in situ Photoluminescence (PL) and Raman spectroscopy as complementary techniques. Considering the \'Etendue conservation and using an off-axis parabolic mirror, it is possible to design a light collection and injection system that displays 72% of collection efficiency (considering the hemisphere above the sample surface) while maintaining high spectral resolution and minimizing signal loss. The performance of the STM is tested by atomically resolved images and scanning tunneling spectroscopy results on standard sample surfaces. The capabilities of our system are demonstrated by performing STM-LE on metallic surfaces and two-dimensional semiconducting samples, observing both plasmonic and excitonic emissions. In addition, we carried out in situ PL measurements on semiconducting monolayers and quantum dots and in situ Raman on graphite and hexagonal boron nitride (h-BN) samples. Additionally, STM-CL and PL were obtained on monolayer h-BN gathering luminescence spectra that are typically associated with intragap states related to carbon defects. The results show that the flexible and efficient light injection and collection device based on an off-axis parabolic mirror is a powerful tool to study several types of nanostructures with multiple spectroscopic techniques in correlation with their morphology at the atomic scale and electronic structure.Comment: 19 pages, 14 Figure