Abstract: A decade ago, a statistics-based method was introduced to count the number of atoms from annular dark-field scanning transmission electron microscopy (ADF STEM) images. In the past years, this method was successfully applied to nanocrystals of arbitrary shape, size, and composition (and its high accuracy and precision has been demonstrated). However, the counting results obtained from this statistical framework are so far presented without a visualization of the actual uncertainty about this estimate. In this paper, we present three approaches that can be used to represent counting results together with their statistical error, and discuss which approach is most suited for further use based on simulations and an experimental ADF STEM image.

Abstract: Accurate geometrical calibration between the scan coordinates and the camera coordinates is critical in four-dimensional scanning transmission electron microscopy (4D-STEM) for both quantitative imaging and ptychographic reconstructions. For atomic-resolved, in-focus 4D-STEM datasets, we propose a hybrid method incorporating two sub-routines, namely a J-matrix method and a Fourier method, which can calibrate the uniform affine transformation between the scan-camera coordinates using raw data, without a priori knowledge about the crystal structure of the specimen. The hybrid method is found robust against scan distortions and residual probe aberrations. It is also effective even when defects are present in the specimen, or the specimen becomes relatively thick. We will demonstrate that a successful geometrical calibration with the hybrid method will lead to a more reliable recovery of both the specimen and the electron probe in a ptychographic reconstruction. We will also show that, although the elimination of local scan position errors still requires an iterative approach, the rate of convergence can be improved, and the residual errors can be further reduced if the hybrid method can be firstly applied for initial calibration. The code is made available as a simple-to-use tool to correct affine transformations of the scan-camera coordinates in 4D-STEM experiments.

Abstract: Fast pixelated detectors incorporating direct electron detection (DED) technology are increasingly being regarded as universal detectors for scanning transmission electron microscopy (STEM), capable of imaging under multiple modes of operation. However, several issues remain around the post-acquisition processing and visualization of the often very large multidimensional STEM datasets produced by them. We discuss these issues and present open source software libraries to enable efficient processing and visualization of such datasets. Throughout, we provide examples of the analysis methodologies presented, utilizing data from a 256 x 256 pixel Medipix3 hybrid DED detector, with a particular focus on the STEM characterization of the structural properties of materials. These include the techniques of virtual detector imaging; higher-order Laue zone analysis; nanobeam electron diffraction; and scanning precession electron diffraction. In the latter, we demonstrate a nanoscale lattice parameter mapping with a fractional precision <= 6 x 10(-4) (0.06%).

Abstract: Conventional glass-ionomer cements (GICs) are popular restorative materials, but their use is limited by their relatively low mechanical strength. This paper reports an attempt to improve these materials by incorporation of 10 wt% of three different types of nanoparticles, aluminum oxide, zirconium oxide, and titanium dioxide, into two commercial GICs (ChemFil((R)) Rock and EQUIA (TM) Fil). The results indicate that the nanoparticles readily dispersed into the cement matrix by hand mixing and reduced the porosity of set cements by filling the empty spaces between the glass particles. Both cements showed no significant difference in compressive strength with added alumina, and ChemFil((R)) Rock also showed no significant difference with zirconia. By contrast, ChemFil((R)) Rock showed significantly higher compressive strength with added titania, and EQUIA (TM) Fil showed significantly higher compressive strength with both zirconia and titania. Fewer air voids were observed in all nanoparticle-containing cements and this, in turn, reduced the development of cracks within the matrix of the cements. These changes in microstructure provide a likely reason for the observed increases in compressive strength, and overall the addition of nanoparticles appears to be a promising strategy for improving the physical properties of GICs.

Abstract: The characterization of biological and inorganic materials by determining their three-dimensional structure in conditions closer to their native state is a major challenge of technological research. Environmental scanning electron microscopy (ESEM) provides access to the observation of hydrated samples in water environments. Here, we present a specific device for ESEM in the scanning transmission electron microscopy mode, allowing the acquisition of tilt-series suitable for tomographic reconstructions. The resolution which can be obtained with this device is first determined. Then, we demonstrate the feasibility of tomography on wet materials. The example studied here is hydrophilic mesoporous silica (MCM-41). Finally, the minimum thickness of water which can be detected is calculated from Monte Carlo simulations and compared with the resolution expected in the tomograms.

Abstract: Imaging soft matter by transmission electron microscopy (TEM) is anything but straightforward. Recently, interest has grown in developing alternative imaging modes that generate contrast without additional staining. Here, we present a dark-field TEM technique based on the use of an annular objective aperture. Our experiments demonstrate an increase in both contrast and signal-to-noise ratio in comparison to conventional bright-field TEM. The proposed technique is easy to implement and offers an alternative imaging mode to investigate soft matter.

Abstract: Focused ion beam (FIB) induced damage in nanocrystalline Al thin films has been characterized using advanced transmission electron microscopy techniques. Electron tomography was used to analyze the three-dimensional distribution of point defect clusters induced by FIB milling, as well as their interaction with preexisting dislocations generated by internal stresses in the Al films. The atomic structure of interstitial Frank loops induced by irradiation, as well as the core structure of Frank dislocations, has been resolved with aberration-corrected high-resolution annular dark-field scanning TEM. The combination of both techniques constitutes a powerful tool for the study of the intrinsic structural properties of point defect clusters as well as the interaction of these defects with preexisting or deformation dislocations in irradiated bulk or nanostructured materials.

Abstract: The enamel of 20 Email Champlevé objects dating between the 12th and 19th centuries was investigated by means of microscopic and portable X-ray fluorescence analysis (μ-XRF and PXRF). Seven of these objects were microsampled and the fragments were analyzed with electron probe microanalysis (EPMA) and vacuum μ-XRF to obtain quantitative data about the composition of the glass used to produce these enameled objects. As a result of the evolution of the raw materials employed to produce the base glass, three different compositional groups could be discriminated. The first group consisted of soda-lime-silica glass with a sodium source of mineral origin (with low K content) that was opacified by addition of calcium antimonate crystals. This type of glass was only used in objects made in the 12th century. Email Champlevé objects from the beginning of the 13th century onward were enameled with soda-lime-silica glass with a sodium source of vegetal origin. This type of glass, which has a higher potassium content, was opacified with SnO2 crystals. The glass used for 19th century Email Champlevé artifacts was produced with synthetic and purified components resulting in a different chemical composition compared to the other groups. Although the four analytical techniques employed in this study have their own specific characteristics, they were all found to be suitable for classifying the objects into the different chronological categories.

Abstract: The three-dimensional (3D) distribution of carbon nanotubes (CNTs) grown inside semiconductor contact holes is studied by electron tomography. The use of a specialized tomography holder results in an angular tilt range of ±90°, which means that the so-called missing wedge is absent. The transmission electron microscopy (TEM) sample for this purpose consists of a micropillar that is prepared by a dedicated procedure using the focused ion beam (FIB) but keeping the CNTs intact. The 3D results are combined with energy dispersive X-ray spectroscopy (EDS) to study the relation between the CNTs and the catalyst particles used during their growth. The reconstruction, based on the full range of tilt angles, is compared with a reconstruction where a missing wedge is present. This clearly illustates that the missing wedge will lead to an unreliable interpretation and will limit quantitative studies