Michael Stöger-Pollach

Transmission electron microscopy at 20 kV for imaging and spectroscopy

The electron optical performance of a transmission electron microscope (TEM) is characterized for direct spatial imaging and spectroscopy using electrons with energies as low as 20 keV. The highly stable instrument is equipped with an electrostatic monochromator and a C(S)-corrector. At 20 kV it shows high image contrast even for single-layer graphene with a lattice transfer of 213 pm (tilted illumination). For 4 nm thick Si, the 200 reflections (271.5 pm) were directly transferred (axial illumination). We show at 20 kV that radiation-sensitive fullerenes (C(60)) within a carbon nanotube container withstand an about two orders of magnitude higher electron dose than at 80 kV. In spectroscopy mode, the monochromated low-energy electron beam enables the acquisition of EELS spectra up to very high energy losses with exceptionally low background noise. Using Si and Ge, we show that 20 kV TEM allows the determination of dielectric properties and narrow band gaps, which were not accessible by TEM so far. These very first results demonstrate that low kV TEM is an exciting new tool for determination of structural and electronic properties of different types of nano-materials.

Optical properties and bandgaps from low loss EELS: Pitfalls and solutions

We investigate the impacts of zero loss peak (ZLP) removal and retardation effects altering the electron energy loss spectrum on the optical properties obtained by using Kramers-Kronig analysis and on the determination of the bandgap. For this purpose we use amorphous SiN(x):H having a bandgap of Eg(SiNx:H)= 5.5 eV. We demonstrate that for bandgap determination not only the accurate removal of the ZLP is crucial, moreover also retardation losses have to be taken into account. The same is valid for an accurate determination of the optical properties of semiconductors which can be done if the retardation effects are treated correctly or avoided at all before Kramers-Kronig analysis is applied. Beside the detailed study on using SiN(x):H we discuss the impact of the retardation effects on several other semiconductors and insulators, like GaP.

Cation diffusion in La0.6Sr0.4CoO3−δ below 800 °C and its relevance for Sr segregation

Cation diffusion was investigated in La0.6Sr0.4CoO3-δ (LSC) thin films on (100) yttria stabilized zirconia in the temperature range 625-800 °C. Isotopic ((86)Sr) and elemental tracers (Fe, Sm) were used to establish diffusion profiles of the cations in bi- and multi-layered thin films. The profiles were analyzed by time of flight-secondary ion mass spectrometry (ToF-SIMS). Grain and grain boundary diffusion coefficients of the cations were determined for LSC thin films with columnar grains - diffusion along grain boundaries is shown to be about three orders of magnitude faster than in grains. This could be verified for thin films with different grain size. A- and B-site cations showed very similar temperature dependencies with activation energies of ∼3.5 eV for bulk and ∼4.1 eV for grain boundary diffusion. The importance of cation diffusivities for surface segregation of Sr and thus for a major degradation mechanism of LSC cathodes in solid oxide fuel cells is discussed.

Atomic scale electron vortices for nanoresearch

Electron vortex beams were only recently discovered and their potential as a probe for magnetism in materials was shown. Here we demonstrate a method to produce electron vortex beams with a diameter of less than 1.2 A. This unique way to prepare free electrons to a state resembling atomic orbitals is fascinating from a fundamental physics point of view and opens the road for magnetic mapping with atomic resolution in an electron microscope.

Is magnetic chiral dichroism feasible with electron vortices

We discuss the feasibility of detecting magnetic transitions with focused electron vortex probes, suggested by selection rules for the magnetic quantum number. We theoretically estimate the dichroic signal strength in the L2,3 edge of ferromagnetic d metals. It is shown that under realistic conditions, the dichroic signal is undetectable for nanoparticles larger than ∼1nm. This is confirmed by a key experiment with nanometer-sized vortices.

Novel vortex generator and mode converter for electron beams.

A mode converter for electron vortex beams is described. Numerical simulations, confirmed by experiment, show that the converter transforms a vortex beam with a topological charge m=±1 into beams closely resembling Hermite-Gaussian HG(10) and HG(01) modes. The converter can be used as a mode discriminator or filter for electron vortex beams. Combining the converter with a phase plate turns a plane wave into modes with topological charge m=±1. This combination serves as a generator of electron vortex beams of high brilliance.

Impact of the surface-near silicon substrate properties on the microstructure of sputter-deposited AlN thin films

In micro-/nanomachined devices and systems, aluminum nitride (AlN) thin films are widely used due to their piezoelectric properties. This work evaluates the potential of modifying the interface between the AlN thin film and the silicon (Si) wafer serving as bottom electrode for optimized crystallographic orientation and, hence, improved electrical and piezoelectric properties. The films were analyzed using temperature-dependant leakage current measurements, transmission electron microscopy, and x-ray diffraction. By preconditioning of the Si substrate surface applying sputter etching prior to film deposition, leakage current levels are substantially decreased and an increased (002) orientation of the AlN grains is observed.

Imaging the dynamics of free-electron Landau states

Landau levels and states of electrons in a magnetic field are fundamental quantum entities underlying the quantum Hall and related effects in condensed matter physics. However, the real-space properties and observation of Landau wave functions remain elusive. Here we report the real-space observation of Landau states and the internal rotational dynamics of free electrons. States with different quantum numbers are produced using nanometre-sized electron vortex beams, with a radius chosen to match the waist of the Landau states, in a quasi-uniform magnetic field. Scanning the beams along the propagation direction, we reconstruct the rotational dynamics of the Landau wave functions with angular frequency ~100 GHz. We observe that Landau modes with different azimuthal quantum numbers belong to three classes, which are characterized by rotations with zero, Larmor and cyclotron frequencies, respectively. This is in sharp contrast to the uniform cyclotron rotation of classical electrons, and in perfect agreement with recent theoretical predictions.

Circular dichroism in the electron microscope: Progress and applications "invited…

According to theory, x-ray magnetic circular dichroism in a synchrotron is equivalent to energy loss magnetic chiral dichroism (EMCD) in a transmission electron microscope (TEM). After a synopsis of the development of EMCD, the theoretical background is reviewed and recent results are presented, focusing on the study of magnetic nanoparticles for ferrofluids and Heusler alloys for spintronic devices. Simulated maps of the dichroic strength as a function of atom position in the crystal allow evaluating the influence of specimen thickness and sample tilt on the experimental EMCD signal. Finally, the possibility of direct observation of chiral electronic transitions with atomic resolution in a TEM is discussed.

Methane Decomposition and Carbon Growth on Y2O3, Yttria-Stabilized Zirconia, and ZrO2

Carbon deposition following thermal methane decomposition under dry and steam reforming conditions has been studied on yttria-stabilized zirconia (YSZ), Y2O3, and ZrO2 by a range of different chemical, structural, and spectroscopic characterization techniques, including aberration-corrected electron microscopy, Raman spectroscopy, electric impedance spectroscopy, and volumetric adsorption techniques. Concordantly, all experimental techniques reveal the formation of a conducting layer of disordered nanocrystalline graphite covering the individual grains of the respective pure oxides after treatment in dry methane at temperatures T ≥ 1000 K. In addition, treatment under moist methane conditions causes additional formation of carbon-nanotube-like architectures by partial detachment of the graphite layers. All experiments show that during carbon growth, no substantial reduction of any of the oxides takes place. Our results, therefore, indicate that these pure oxides can act as efficient nonmetallic substrates for methane-induced growth of different carbon species with potentially important implications regarding their use in solid oxide fuel cells. Moreover, by comparing the three oxides, we could elucidate differences in the methane reactivities of the respective SOFC-relevant purely oxidic surfaces under typical SOFC operation conditions without the presence of metallic constituents.