Abstract: Accurate segmentation of nanoparticles within various matrix materials is a difficult problem in electron tomography. Due to artifacts related to image series acquisition and reconstruction, global thresholding of reconstructions computed by established algorithms, such as weighted backprojection or SIRT, may result in unreliable and subjective segmentations. In this paper, we introduce the Partially Discrete Algebraic Reconstruction Technique (PDART) for computing accurate segmentations of dense nanoparticles of constant composition. The particles are segmented directly by the reconstruction algorithm, while the surrounding regions are reconstructed using continuously varying gray levels. As no properties are assumed for the other compositions of the sample, the technique can be applied to any sample where dense nanoparticles must be segmented, regardless of the surrounding compositions. For both experimental and simulated data, it is shown that PDART yields significantly more accurate segmentations than those obtained by optimal global thresholding of the SIRT reconstruction.

Abstract: In the present work Cs aberration corrected and monochromated scanning transmission electron microscopy electron energy loss spectroscopy (STEM-EELS) has been used to explore experimental setups that allow bandgaps of high refractive index materials to be determined. Semi-convergence and collection angles in the mu rad range were combined with off-axis or dark field EELS to avoid relativistic losses and guided light modes in the low loss range to contribute to the acquired EEL spectra. Off-axis EELS further supressed the zero loss peak and the tail of the zero loss peak. The bandgap of several GaAs-based materials were successfully determined by simple regression analyses of the background subtracted EEL spectra. The presented set-up does not require that the acceleration voltage is set to below the. Cerenkov limit and can be applied over the entire acceleration voltage range of modern TEMs and for a wide range of specimen thicknesses. (C) 2017 Elsevier B.V. All rights reserved.

Abstract: Electron tomography is an essential imaging technique for the investigation of morphology and 3D structure of nanomaterials. This method, however, suffers from well-known missing wedge artifacts due to a restricted tilt range, which limits the objectiveness, repeatability and efficiency of quantitative structural analysis. Discrete tomography represents one of the promising reconstruction techniques for materials science, potentially capable of delivering higher fidelity reconstructions by exploiting the prior knowledge of the limited number of material compositions in a specimen. However, the application of discrete tomography to practical datasets remains a difficult task due to the underlying challenging mathematical problem. In practice, it is often hard to obtain consistent reconstructions from experimental datasets. In addition, numerous parameters need to be tuned manually, which can lead to bias and non-repeatability. In this paper, we present the application of a new
iterative reconstruction technique, named TVR-DART, for discrete electron tomography. The technique is capable of consistently delivering reconstructions with significantly reduced missing wedge artifacts for a variety of challenging data and imaging conditions, and can automatically estimate its key parameters. We describe the principles of the technique and apply it to datasets from three different types of samples acquired under diverse imaging modes. By further reducing the available tilt range and number of projections, we show that the
proposed technique can still produce consistent reconstructions with minimized missing wedge artifacts. This new development promises to provide the electron microscopy community with an easy-to-use and robust tool for high-fidelity 3D characterization of nanomaterials.

Abstract: In quantitative scanning transmission electron microscopy (STEM), scattering cross-sections have been shown to be very sensitive to the number of atoms in a column and its composition. They correspond to the integrated intensity over the atomic column and they outperform other measures. As compared to atomic column peak intensities, which saturate at a given thickness, scattering cross-sections increase monotonically. A study of the electron wave propagation is presented to explain the sensitivity of the scattering cross-sections. Based on the multislice algorithm, we analyse the wave propagation inside the crystal and its link to the scattered signal for the different probe positions contained in the scattering cross-section for detector collection in the low-, middle- and high-angle regimes. The influence to the signal from scattering of neighbouring columns is also discussed.

Abstract: A spiral holographic aperture is used in the condensor plane of a scanning transmission electron microscope to produce a focussed electron vortex probe carrying a topological charge of either −1, 0 or +1. The spiral aperture design has a major advantage over the previously used forked aperture in that the three beams with topological charge m=−1, 0, and 1 are not side by side in the specimen plane, but rather on top of each other, focussed at different heights. This allows us to have only one selected beam in focus on the sample while the others contribute only to a background signal. In this paper we describe the working principle as well as first experimental results demonstrating atomic resolution HAADF STEM images obtained with electron vortex probes. These results pave the way for atomic resolution magnetic information when combined with electron energy loss spectroscopy.

Abstract: 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 View the MathML source. This is confirmed by a key experiment with nanometer-sized vortices.

Abstract: This paper is the second part of a two-part paper on direct structure inversion from exit waves. In the first part, a method has been proposed to quantitatively determine structure parameters with atomic resolution such as atom column positions, surface profile and the number of atoms in the atom columns. In this part, the theory will be demonstrated by means of a Au[110] exit wave reconstructed from a set of focal-series images. The procedures to analyze the experimentally reconstructed exit wave in terms of quantitative structure information are described in detail.

Abstract: Transmission electron microscopy (TEM) is carried out in vacuum to minimize the interaction of the imaging electrons with gas molecules while passing through the microscope column. Nevertheless, in typical devices, the pressure remains at 10(-7) mbar or above, providing a large number of gas molecules for the electron beam to crack, which can lead to structural changes in the sample. Here, we describe experiments carried out in a modified scanning TEM (STEM) instrument, based on the Nion UltraSTEM 100. In this instrument, the base pressure at the sample is around 2 x 10(-10 )mbar, and can be varied up to 10(-6) mbar through introduction of gases directly into the objective area while maintaining atomic resolution imaging conditions. We show that air leaked into the microscope column during the experiment is efficient in cleaning graphene samples from contamination, but ineffective in damaging the pristine lattice. Our experiments also show that exposure to O(2 )and H2O lead to a similar result, oxygen providing an etching effect nearly twice as efficient as water, presumably due to the two 0 atoms per molecule. H(2 )and N-2 environments have no influence on etching. These results show that the residual gas environment in typical TEM instruments can have a large influence on the observations, and show that chemical etching of carbon-based structures can be effectively carried out with oxygen.

Abstract: Correlated noise is generally present in experimentally recorded electron energy loss spectra due to a non-ideal electron detector. In this contribution we describe a method to experimentally measure the noise properties of the detector as well as the consequences it has for model-based quantification using maximum likelihood. The effect of the correlated noise on the maximum likelihood fitting results can be shown to be negligible for the estimated (co)variance of the parameters while an experimentally obtained scaling factor is required to correct the likelihood ratio test for the reduction of noise power with frequency. Both effects are derived theoretically under a set of approximations and tested for a range of signal-to-noise values using numerical experiments. Finally, an experimental example shows that the correction for correlated noise is essential and should always be included in the fitting procedure. (c) 2007 Elsevier B.V. All rights reserved.

Abstract: Here, we study the effect of dynamic scattering on the projected geometric phase and strain maps reconstructed using dark-field electron holography (DFEH) for non-uniformly strained crystals. The investigated structure consists of a {SiGe/Si} superlattice grown on a (001)-Si substrate. The three dimensional strain held within the thin TEM lamella is modelled by the finite element method. The observed projected strain is simulated in two ways by multiplying the strain at each depth in the crystal by a weighting function determined from a recently developed analytical two-beam dynamical theory, and by simply taking the average value. We demonstrate that the experimental results need to be understood in terms of the dynamical theory and good agreement is found between the experimental and simulated results. Discrepancies do remain for certain cases and are likely to be from an imprecision in the actual two-beam diffraction conditions, notably the deviation parameter, and points to limitations in the 2-beam approximation. Finally, a route towards a 3D reconstruction of strain fields is proposed. (C) 2014 Elsevier B.V. All rights reserved.

Abstract: This study sheds light on the prerequisites, possibilities, limitations and interpretation of high-resolution differential phase contrast (DPC) imaging in scanning transmission electron microscopy (STEM). We draw particular attention to the well-established DPC technique based on segmented annular detectors and its relation to recent developments based on pixelated detectors. These employ the expectation value of the momentum transfer as a reliable measure of the angular deflection of the STEM beam induced by an electric field in the specimen. The influence of scattering and propagation of electrons within the specimen is initially discussed separately and then treated in terms of a two-state channeling theory. A detailed simulation study of GaN is presented as a function of specimen thickness and bonding. It is found that bonding effects are rather detectable implicitly, e.g., by characteristics of the momentum flux in areas between the atoms than by directly mapping electric fields and charge densities. For strontium titanate, experimental charge densities are compared with simulations and discussed with respect to experimental artifacts such as scan noise. Finally, we consider practical issues such as figures of merit for spatial and momentum resolution, minimum electron dose, and the mapping of larger-scale, built-in electric fields by virtue of data averaged over a crystal unit cell. We find that the latter is possible for crystals with an inversion center. Concerning the optimal detector design, this study indicates that a sampling of 5mrad per pixel is sufficient in typical applications, corresponding to approximately 10x10 available pixels.

Abstract: <script type='text/javascript'>document.write(unpmarked('HAADF-STEM tomography is a common technique for characterizing the three-dimensional morphology of nanomaterials. In conventional tomographic reconstruction algorithms, the image intensity is assumed to be a linear projection of a physical property of the specimen. However, this assumption of linearity is not completely valid due to the nonlinear damping of signal intensities. The nonlinear damping effects increase w.r.t the specimen thickness and lead to so-called \u0022cupping artifacts\u0022, due to a mismatch with the linear model used in the reconstruction algorithm. Moreover, nonlinear damping effects can strongly limit the applicability of advanced reconstruction approaches such as Total Variation Minimization and discrete tomography. In this paper, we propose an algorithm for automatically correcting the nonlinear effects and the subsequent cupping artifacts. It is applicable to samples in which chemical compositions can be segmented based on image gray levels. The correction is realized by iteratively estimating the nonlinear relationship between projection intensity and sample thickness, based on which the projections are linearized. The correction and reconstruction algorithms are tested on simulated and experimental data. (C) 2017 Elsevier B.V. All rights reserved.'));

Abstract: The concept of resolution in high-resolution electron microscopy (HREM) is the power to resolve neighboring atoms. Since the resolution is related to the width of the point spread function of the microscope, it could in principle be determined from the image of a point object. However, in electron microscopy there are no ideal point objects. The smallest object is an individual atom. If the width of an atom is much smaller than the resolution of the microscope, this atom can still be considered as a point object. As the resolution of the microscope enters the sub-Å regime, information about the microscope is strongly entangled with the information about the atoms in HREM images. Therefore, we need to find an alternative method to determine the resolution in an object-independent way. In this work we propose to use the image wave of a crystalline object in zone axis orientation. Under this condition, the atoms of a column act as small lenses so that the electron beam channels through the atom column periodically. Because of this focusing, the image wave of the column can be much more peaked than the constituting atoms and can thus be a much more sensitive probe to measure the resolution. Our approach is to use the peakiness of the image wave of the atom column to determine the resolution. We will show that the resolution can be directly linked to the total curvature of the atom column wave. Moreover, we can then directly obtain the resolution of the microscope given that the contribution from the object is known, which is related to the bounding energy of the atom. The method is applied on an experimental CaTiO3 image wave.