Atomic resolution mapping of phonon excitations in STEM-EELS experiments

Atomically resolved electron energy-loss spectroscopy experiments are commonplace in modern aberrationcorrected transmission electron microscopes. Energy resolution has also been increasing steadily with the continuous improvement of electron monochromators. Electronic excitations however are known to be delocalised due to the long range interaction of the charged accelerated electrons with the electrons in a sample. This has made several scientists question the value of combined high spatial and energy resolution for mapping interband transitions and possibly phonon excitation in crystals. In this paper we demonstrate experimentally that atomic resolution information is indeed available at very low energy losses around 100 meV expressed as a modulation of the broadening of the zero loss peak. Careful data analysis allows us to get a glimpse of what are likely phonon excitations with both an energy loss and gain part. These experiments confirm recent theoretical predictions on the strong localisation of phonon excitations as opposed to electronic excitations and show that a combination of atomic resolution and recent developments in increased energy resolution will offer great benefit for mapping phonon modes in real space

Barrier efficiency of sponge-like La2Zr2O7 buffer layers for YBCO-coated conductors

Solution derived La2Zr2O7 films have drawn much attention for potential applications as thermal barriers or low-cost buffer layers for coated conductor technology. Annealing and coating parameters strongly affect the microstructure of La2Zr2O7, but different film processing methods can yield similar microstructural features such as nanovoids and nanometer-sized La2Zr2O7 grains. Nanoporosity is a typical feature found in such films and the implications for the functionality of the films is investigated by a combination of scanning transmission electron microscopy, electron energy-loss spectroscopy and quantitative electron tomography. Chemical solution based La2Zr2O7 films deposited on flexible Ni-5at.%W substrates with a {100} biaxial texture were prepared for an in-depth characterization. A sponge-like structure composed of nanometer sized voids is revealed by high-angle annular dark-field scanning transmission electron microscopy in combination with electron tomography. A three-dimensional quantification of nanovoids in the La2Zr2O7 film is obtained on a local scale. Mostly non-interconnected highly facetted nanovoids compromise more than one-fifth of the investigated sample volume. The diffusion barrier efficiency of a 170 nm thick La2Zr2O7 film is investigated by STEM-EELS yielding a 1.8 \pm 0.2 nm oxide layer beyond which no significant nickel diffusion can be detected and intermixing is observed. This is of particular significance for the functionality of YBa2Cu3O7-{\delta} coated conductor architectures based on solution derived La2Zr2O7 films as diffusion barriers.Comment: Accepted for publication in Superconductor Science and Technolog

Magnetic monopole field exposed by electrons

Magnetic monopoles have provided a rich field of study, leading to a wide area of research in particle physics, solid state physics, ultra-cold gases, superconductors, cosmology, and gauge theory. So far, no true magnetic monopoles were found experimentally. Using the Aharonov-Bohm effect, one of the central results of quantum physics, shows however, that an effective monopole field can be produced. Understanding the effects of such a monopole field on its surroundings is crucial to its observation and provides a better grasp of fundamental physical theory. We realize the diffraction of fast electrons at a magnetic monopole field generated by a nanoscopic magnetized ferromagnetic needle. Previous studies have been limited to theoretical semiclassical optical calculations of the motion of electrons in such a monopole field. Solid state systems like the recently studied 'spin ice' provide a constrained system to study similar fields, but make it impossible to separate the monopole from the material. Free space diffraction helps to understand the dynamics of the electron-monopole system without the complexity of a solid state system. The use of a simple object such as a magnetized needle will allow various areas of physics to use the general dynamical effects of monopole fields without requiring a monopole particle or specific solids which have internal monopole-like properties. The experiment performed here shows that even without a true magnetic monopole particle, the theoretical background on monopoles serves as a basis for experiments and can be applied to efficiently create electron vortices. Various predictions about angular momentum and general field effects can readily be studied using the available equipment. This realization provides insights for the scientific community on how to detect magnetic monopoles in high energy collisions, cosmological processes, or novel materials.Comment: 5 pages, 3 figures + 7 pages of supplementary information, 8 figure

Interplay of atomic displacements in the quantum magnet (CuCl)LaNb2O7

We report on the crystal structure of the quantum magnet (CuCl)LaNb2O7 that was controversially described with respect to its structural organization and magnetic behavior. Using high-resolution synchrotron powder x-ray diffraction, electron diffraction, transmission electron microscopy, and band structure calculations, we solve the room-temperature structure of this compound [alpha-(CuCl)LaNb2O7] and find two high-temperature polymorphs. The gamma-(CuCl)LaNb2O7 phase, stable above 640K, is tetragonal with a(sub) = 3.889 A, c(sub) = 11.738 A, and the space group P4/mmm. In the gamma-(CuCl)LaNb2O7 structure, the Cu and Cl atoms are randomly displaced from the special positions along the {100} directions. The beta-phase [a(sub) x 2a(sub) x c(sub), space group Pbmm] and the alpha-phase [2a(sub) x 2a(sub) x c(sub), space group Pbam] are stable between 640 K and 500 K and below 500 K, respectively. The structural changes at 500 K and 640 K are identified as order-disorder phase transitions. The displacement of the Cl atoms is frozen upon the gamma --> beta transformation, while a cooperative tilting of the NbO6 octahedra in the alpha-phase further eliminates the disorder of the Cu atoms. The low-temperature alpha-(CuCl)LaNb2O7 structure thus combines the two types of the atomic displacements that interfere due to the bonding between the Cu atoms and the apical oxygens of the NbO6 octahedra. The precise structural information resolves the controversy between the previous computation-based models and provides the long-sought input for understanding the magnetic properties of (CuCl)LaNb2O7.Comment: 12 pages, 10 figures, 5 tables; crystallographic information (cif files) include

Electronically coupled complementary interfaces between perovskite band insulators

Perovskite oxides exhibit a plethora of exceptional electronic properties, providing the basis for novel concepts of oxide-electronic devices. The interest in these materials is even extended by the remarkable characteristics of their interfaces. Studies on single epitaxial connections between the two wide-bandgap insulators LaAlO3 and SrTiO3 have revealed them to be either high-mobility electron conductors or insulating, depending on the atomic stacking sequences. In the latter case they are conceivably positively charged. For device applications, as well as for basic understanding of the interface conduction mechanism, it is important to investigate the electronic coupling of closely-spaced complementary interfaces. Here we report the successful realization of such electronically coupled complementary interfaces in SrTiO3 - LaAlO3 thin film multilayer structures, in which the atomic stacking sequence at the interfaces was confirmed by quantitative transmission electron microscopy. We found a critical separation distance of 6 perovskite unit cell layers, corresponding to approximately 2.3 nm, below which a decrease of the interface conductivity and carrier density occurs. Interestingly, the high carrier mobilities characterizing the separate electron doped interfaces are found to be maintained in coupled structures down to sub-nanometer interface spacing

Optimized fabrication of high quality La0.67Sr0.33MnO3 thin films considering all essential characteristics

In this article, an overview of the fabrication and properties of high quality La0.67Sr0.33MnO3 (LSMO) thin films is given. A high quality LSMO film combines a smooth surface morphology with a large magnetization and a small residual resistivity, while avoiding precipitates and surface segregation. In literature, typically only a few of these issues are adressed. We therefore present a thorough characterization of our films, which were grown by pulsed laser deposition. The films were characterized with reflection high energy electron diffraction, atomic force microscopy, x-ray diffraction, magnetization and transport measurements, x-ray photoelectron spectroscopy and scanning transmission electron microscopy. The films have a saturation magnetization of 4.0 {\mu}B/Mn, a Curie temperature of 350 K and a residual resistivity of 60 {\mu}{\Omega}cm. These results indicate that high quality films, combining both large magnetization and small residual resistivity, were realized. A comparison between different samples presented in literature shows that focussing on a single property is insufficient for the optimization of the deposition process. For high quality films, all properties have to be adressed. For LSMO devices, the thin film quality is crucial for the device performance. Therefore, this research is important for the application of LSMO in devices.Comment: Accepted for publication in Journal of Physics D - Applied Physic

The 0 and the pi phase Josephson coupling through an insulating barrier with magnetic impurities

We have studied temperature and field dependencies of the critical current $I_{C}$ in the Nb-Fe$_{0.1}$Si$_{0.9}$-Nb Josephson junction with tunneling barrier formed by paramagnetic insulator. We demonstrate that in these junctions the co-existence of both the 0 and the $\pi$ states within one tunnel junction takes place which leads to the appearance of a sharp cusp in the temperature dependence $I_{C}(T)$ similar to the $I_{C}(T)$ cusp found for the $0-\pi$ transition in metallic $\pi$ junctions. This cusp is not related to the $0-\pi$ temperature induced transition itself, but is caused by the different temperature dependencies of the opposing 0 and $\pi$ supercurrents through the barrier.Comment: Accepted in Physical Review

The tumor-associated antigen RHAMM (HMMR/CD168) is expressed by monocyte-derived dendritic cells and presented to T cells

We formerly demonstrated that vaccination with Wilms' tumor 1 (WT1)-loaded autologous monocyte-derived dendritic cells (mo-DCs) can be a well-tolerated effective treatment in acute myeloid leukemia (AML) patients. Here, we investigated whether we could introduce the receptor for hyaluronic acid-mediated motility (RHAMM/HMMR/CD168), another clinically relevant tumor-associated antigen, into these mo-DCs through mRNA electroporation and elicit RHAMM-specific immune responses. While RHAMM mRNA electroporation significantly increased RHAMM protein expression by mo-DCs, our data indicate that classical mo-DCs already express and present RHAMM at sufficient levels to activate RHAMM-specific T cells, regardless of electroporation. Moreover, we found that RHAMM-specific T cells are present at vaccination sites in AML patients. Our findings implicate that we and others who are using classical mo-DCs for cancer immunotherapy are already vaccinating against RHAMM

Effect of high temperature deposition on CoSi 2 phase formation

Abstract: This paper discusses the nucleation behaviour of the CoSi to CoSi2 transformation from cobalt silicide thin films grown by deposition at elevated substrate temperatures ranging from 375 °C to 600 °C. A combination of channelling, real-time Rutherford backscattering spectrometry, real-time x-ray diffraction, and transmission electron microscopy was used to investigate the effect of the deposition temperature on the subsequent formation temperature of CoSi2, its growth behaviour, and the epitaxial quality of the CoSi2 thus formed. The temperature at which deposition took place was observed to exert a significant and systematic influence on both the formation temperature of CoSi2 and its growth mechanism. CoSi films grown at the lowest temperatures were found to increase the CoSi2 nucleation temperature above that of CoSi2 grown by conventional solid phase reaction, whereas the higher deposition temperatures reduced the nucleation temperature significantly. In addition, a systematic change in growth mechanism of the subsequent CoSi2 growth occurs as a function of deposition temperature. First, the CoSi2 growth rate from films grown at the lower reactive deposition temperatures is substantially lower than that grown at higher reactive deposition temperatures, even though the onset of growth occurs at a higher temperature, Second, for deposition temperatures below 450 °C, the growth appears columnar, indicating nucleation controlled growth. Elevated deposition temperatures, on the other hand, render the CoSi2 formation process layer-by-layer which indicates enhanced nucleation of the CoSi2 and diffusion controlled growth. Our results further indicate that this observed trend is most likely related to stress and changes in microstructure introduced during reactive deposition of the CoSi film. The deposition temperature therefore provides a handle to tune the CoSi2 growth mechanism