Investigation of the Electric Field and Charge Density Distribution of pristine and defective 2D WSe2_2 by Differential Phase Contrast Imaging

Most properties of solid materials are defined by their internal electric field and charge density distributions which so far have been difficult to measure with sufficient spatial resolution. For 2D materials, the electric field at the atomic level in particular influences the optoelectronic properties. In this study, the atomic-scale electric field and charge density distribution of 2D WSe$_2$ are revealed by using an emerging microscopy technique, differential phase contrast (DPC) imaging in the scanning transmission electron microscope (STEM). Combined with high-angle annular dark-field imaging the charge density distribution of bi- and trilayers of WSe$_2$ is mapped. A measured higher positive charge density located at the selenium atomic columns compared to the tungsten atomic columns is reported, and possible reasons are discussed. Furthermore, the change in the electric field distribution of a selenium point defect in a trilayer is investigated exhibiting a characteristic electric field distribution in the vicinity of the defect: there are characteristic regions with locally enhanced and with locally reduced electric field magnitudes compared to the pristine lattice.Comment: 20 pages including the supplementary information, 3 figures in the main part and additional 2 figures in the supplementary informatio

Characterisation of the PS-PMMA Interfaces in Microphase Separated Block Copolymer Thin Films by Analytical (S)TEM

Block copolymer (BCP) self-assembly is a promising tool for next generation lithography as microphase separated polymer domains in thin films can act as templates for surface nanopatterning with sub-20 nm features. The replicated patterns can, however, only be as precise as their templates. Thus, the investigation of the morphology of polymer domains is of great importance. Commonly used analytical techniques (neutron scattering, scanning force microscopy) either lack spatial information or nanoscale resolution. Using advanced analytical (scanning) transmission electron microscopy ((S)TEM), we provide real space information on polymer domain morphology and interfaces between polystyrene (PS) and polymethylmethacrylate (PMMA) in cylinder- and lamellae-forming BCPs at highest resolution. This allows us to correlate the internal structure of polymer domains with line edge roughnesses, interface widths and domain sizes. STEM is employed for high-resolution imaging, electron energy loss spectroscopy and energy filtered TEM (EFTEM) spectroscopic imaging for material identification and EFTEM thickness mapping for visualisation of material densities at defects. The volume fraction of non-phase separated polymer species can be analysed by EFTEM. These methods give new insights into the morphology of polymer domains the exact knowledge of which will allow to improve pattern quality for nanolithography

Quality or Quantity? How Structural Parameters Affect Catalytic Activity of Iron Oxides for CO Oxidation

The replacement of noble metal catalysts by abundant iron as an active compound in CO oxidation is of ecologic and economic interest. However, improvement of their catalytic performance to the same level as state-of-the-art noble metal catalysts requires an in depth understanding of their working principle on an atomic level. As a contribution to this aim, a series of iron oxide catalysts with varying Fe loadings from 1 to 20 wt% immobilized on a γ-Al2O3 support is presented here, and a multidimensional structure–activity correlation is established. The CO oxidation activity is correlated to structural details obtained by various spectroscopic, diffraction, and microscopic methods, such as PXRD, PDF analysis, DRUVS, Mössbauer spectroscopy, STEM-EDX, and XAS. Low Fe loadings lead to less agglomerated but high percentual amounts of isolated, tetrahedrally coordinated iron oxide species, while the absolute amount of isolated species reaches its maximum at high Fe loadings. Consequently, the highest CO oxidation activity in terms of turnover frequencies can be correlated to small, finely dispersed iron oxide species with a large amount of tetrahedrally oxygen coordinated iron sites, while the overall amount of isolated iron oxide species correlates with a lower light-off temperature