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 the photonic local density of states with electron energy loss spectroscopy

Electron energy-loss spectroscopy (EELS) performed in transmission electron microscopes is shown to directly render the photonic local density of states (LDOS) with unprecedented spatial resolution, currently below the nanometer. Two special cases are discussed in detail: (i) 2D photonic structures with the electrons moving along the translational axis of symmetry and (ii) quasi-planar plasmonic structures under normal incidence. Nanophotonics in general and plasmonics in particular should benefit from these results connecting the unmatched spatial resolution of EELS with its ability to probe basic optical properties like the photonic LDOS.Comment: 4 pages, 2 figure

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

Very low shot noise in carbon nanotubes

We have performed noise measurements on suspended ropes of single wall carbon nanotubes (SWNT) between 1 and 300 K for different values of dc current through the ropes. We find that the shot noise is suppressed by more than a factor 100 compared to the full shot noise 2eI. We have also measured an individual SWNT and found a level of noise which is smaller than the minimum expected. Another finding is the very low level of 1/f noise, which is significantly lower than previous observations. We propose two possible interpretations for this strong shot noise reduction: i) Transport within a rope takes place through a few nearly ballistic tubes within a rope and possibly involves non integer effective charges. ii) A substantial fraction of the tubes conduct with a strong reduction of effective charge (by more than a factor 50).Comment: Submitted to Eur. Phys. J. B (Jan. 2002) Higher resolution pictures are posted on http://www.lps.u-psud.fr/Collectif/gr_07/publications.htm

High-angular-resolution electron energy loss spectroscopy of hexagonal boron nitride

High-angular-resolution electron energy loss spectroscopy (EELS) is used to study the anisotropic behavior of the boron and nitrogen K ionization edges in h-BN. This work makes significant progress toward improving the anisotropy measurements. The authors show experimentally by EELS the vanishment of the p* peak existing in these K edges in agreement with electronic structure calculations and previous soft x-ray absorption spectroscopy measurements

Superconductivity in ropes of carbon nanotubes

Recent experimental and theoretical results on intrinsic superconductivity in ropes of single-wall carbon nanotubes are reviewed and compared. We find strong experimental evidence for superconductivity when the distance between the normal electrodes is large enough. This indicates the presence of attractive phonon-mediated interactions in carbon nanotubes, which can even overcome the repulsive Coulomb interactions. The effective low-energy theory of rope superconductivity explains the experimental results on the temperature-dependent resistance below the transition temperature in terms of quantum phase slips. Quantitative agreement with only one fit parameter can be obtained. Nanotube ropes thus represent superconductors in an extreme 1D limit never explored before.Comment: 19 pages, 9 figures, to appear in special issue of Sol. State Com

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