Marcel Tencé

Improving energy resolution of EELS spectra: an alternative to the monochromator solution

In this paper, we propose a numerical method which can routinely improve the energy resolution down to 0.2-0.3eV of electron energy-loss spectra acquired in a transmission electron microscope. The method involves measurement of the point-spread function (PSF) corresponding to the spectrometer aberration and to the incident energy spread, and then an inversion of this PSF so as to restore the spectrum. The chosen algorithm is based on an iterative calculation of the maximum likelihood solution known to be very robust against small errors in the PSF used. Restorations have been performed on diamond and graphite C-K edges acquired with an initial energy resolution of around 1eV. After reconstruction, the sharp core exciton lines become clearly visible for both compounds and the final energy resolution is estimated to be about 200-300meV. In the case of graphite, restorations involving both energy resolution and angular resolution have been successfully conducted. Finally, restorations of Fe L(2,3) and O-K edges measured for various iron oxides will be shown.

Nanometer Scale Spectral Imaging of Quantum Emitters in Nanowires and Its Correlation to Their Atomically Resolved Structure

We report the spectral imaging in the UV to visible range with nanometer scale resolution of closely packed GaN/AlN quantum disks in individual nanowires using an improved custom-made cathodoluminescence system. We demonstrate the possibility to measure full spectral features of individual quantum emitters as small as 1 nm and separated from each other by only a few nanometers and the ability to correlate their optical properties to their size, measured with atomic resolution. The direct correlation between the quantum disk size and emission wavelength provides evidence of the quantum confined Stark effect leading to an emission below the bulk GaN band gap for disks thicker than 2.6 nm. With the help of simulations, we show that the internal electric field in the studied quantum disks is smaller than what is expected in the quantum well case. We show evidence of a clear dispersion of the emission wavelengths of different quantum disks of identical size but different positions along the wire. This dispersion is systematically correlated to a change of the diameter of the AlN shell coating the wire and is thus attributed to the related strain variations along the wire. The present work opens the way both to fundamental studies of quantum confinement in closely packed quantum emitters and to characterizations of optoelectronic devices presenting carrier localization on the nanometer scale.

Electron energy loss spectrometry mapping

Among electron beam microanalytical techniques, electron energy loss spectrometry (EELS) offers unique advantages in terms of information content, sensitivity, limits of detection. This paper describes new methods and tools for acquiring families of spectra over many pixels on the specimen, i.e. spectrumimages, and for processing them. Applications in different fields of research, both in materials science and in life sciences, demonstrate the potential impact of the technique for characterizing nano-sized structures.

Unveiling Nanometer Scale Extinction and Scattering Phenomena through Combined Electron Energy Loss Spectroscopy and Cathodoluminescence Measurements

Plasmon modes of the exact same individual gold nanoprisms are investigated through combined nanometer-resolved electron energy-loss spectroscopy (EELS) and cathodoluminescence (CL) measurements. We show that CL only probes the radiative modes, in contrast to EELS, which additionally reveals dark modes. The combination of both techniques on the same particles thus provides complementary information and also demonstrates that although the radiative modes give rise to very similar spatial distributions when probed by EELS or CL, their resonant energies appear to be different. We trace this phenomenon back to plasmon dissipation, which affects in different ways the plasmon signatures probed by these techniques. Our experiments are in agreement with electromagnetic numerical simulations and can be further interpreted within the framework of a quasistatic analytical model. We therefore demonstrate that CL and EELS are closely related to optical scattering and extinction, respectively, with the addition of nanometer spatial resolution.

Multi-dot floating-gates for nonvolatile semiconductor memories: Their ion beam synthesis and morphology

Scalability and performance of current flash memories can be improved substantially by replacing the floating polycrystalline-silicon gate by a layer of Si dots. Here, we present both experimental and theoretical studies on ion beam synthesis of multi-dot layers consisting of Si nanocrystals (NCs) embedded in the gate oxide. Former studies have suffered from the weak Z contrast between Si and SiO2 in transmission electron microscopy (TEM). This letter maps Si plasmon losses with a scanning TEM equipped with a parallel electron energy loss spectroscopy system. Kinetic Monte Carlo simulations of Si phase separation have been performed and compared with Si plasmon maps. Predicted and measured Si morphologies agree remarkably well, both change with increasing ion fluence from isolated NCs to spinodal pattern. However, the predicted fluences are lower than the experimental ones. We identify as the main reason of this discrepancy the partial oxidation of implanted Si by atmospheric humidity, which penetrates in...

Electron energy-loss spectroscopy on individual nanotubes

Abstract Different spatially resolved electron energy-loss spectroscopy (EELS) experiments on individual nanotubes performed in the context of a scanning transmission electron microscope (STEM) are presented. The capabilities of EELS for probing the local anisotropy of the unoccupied electronic states are demonstrated and the effects of the graphite network curvature on the nature of the chemical bonding is investigated. The peculiarity of the valence electron excitation modes in carbon nanotubes due to the curved anisotropy is also pointed out through near-field EELS experiments.

Energy filtered STEM imaging of thick biological sections

Energy filtered imaging of thick biological specimens was analysed using a dedicated STEM fitted with an energy loss spectrometer and interfaced with a sophisticated data collection setup. All images were digital, thus permitting a quantitative analysis of the data. We also present a mathematical explanation of the data, which is useful in pradicting the quality of thick specimen images formed with energy filtered electrons.

Experimental investigation of the ultimate EELS spatial resolution

Abstract The spatial resolution of an inelastic scattering process, such as a core excitation, governs the ultimate spatial resolution of an EELS (electron energy loss spectroscopy) measurement. An experimental study of the attainable resolution has been made through a detailed analysis of the structure of energy-filtered images on a characteristic edge (uranium O 45 ), as compared to the simultaneously recorded annular dark field images. When it has been possible to select specimen areas with a suitable random distribution of point objects (subnanometer uranium clusters), an upper limit of the degradation of the resolution is of the order of 0.3-0.4 nm for a 100 eV loss.

Multi-dimensional and multi-signal approaches in scanning transmission electron microscopes

Developments in instrumentation are essential to open new fields of science. This clearly applies to electron microscopy, where recent progress in all hardware components and in digitally assisted data acquisition and processing has radically extended the domains of application. The demonstrated breakthroughs in electron optics, such as the successful design and practical realization and the use of correctors, filters and monochromators, and the permanent progress in detector efficiency have pushed forward the performance limits, in terms of spatial resolution in imaging, as well as for energy resolution in electron energy-loss spectroscopy (EELS) and for sensitivity to the identification of single atoms. As a consequence, the objects of the nanoworld, of natural or artificial origin, can now be explored at the ultimate atomic level. The improved energy resolution in EELS, which now encompasses the near-IR/visible/UV spectral domain, also broadens the range of available information, thus providing a powerful tool for the development of nanometre-level photonics. Furthermore, spherical aberration correctors offer an enlarged gap in the objective lens to accommodate nanolaboratory-type devices, while maintaining angström-level resolution for general characterization of the nano-object under study.

Capturing the signature of single atoms with the tiny probe of a STEM

With their first scanning transmission electron microscope (STEM), Albert Crewe and his collaborators have succeeded 40 years ago in bringing to reality a dream for all electron microscopists, to see individual atoms. In the derivation of Crewes pioneering work, the present review describes various historical and present steps, involving continuous instrumental and methodological developments as well as the preparation of suitable specimens. They have lead to the identification of individual atoms by electron energy-loss spectroscopy (EELS) and to the demonstration of atom-by-atom spectroscopy. Beyond these spectacular successes which open wide fields of use, most recent technical achievements, such as the introduction of monochromators on the incident electron beam or of optical spectrometers for recording spectra (in the visible as well as in the X-ray domain), will undoubtedly lead to refine the accessible signature of single atoms and molecules.