Direct observation of depth-dependent atomic displacements associated with dislocations in gallium nitride.

We demonstrate that the aberration-corrected scanning transmission electron microscope has a sufficiently small depth of field to observe depth-dependent atomic displacements in a crystal. The depth-dependent displacements associated with the Eshelby twist of dislocations in GaN normal to the foil with a screw component of the Burgers vector are directly imaged. We show that these displacements are observed as a rotation of the lattice between images taken in a focal series. From the sense of the rotation, the sign of the screw component can be determined.

Probe integrated scattering cross sections in the analysis of atomic resolution HAADF STEM images.

The physical basis for using a probe-position integrated cross section (PICS) for a single column of atoms as an effective way to compare simulation and experiment in high-angle annular dark-field (HAADF) scanning transmission electron microscopy (STEM) is described, and the use of PICS in order to make quantitative use of image intensities is evaluated. It is based upon the calibration of the detector and the measurement of scattered intensities. Due to the predominantly incoherent nature of HAADF STEM, it is found to be robust to parameters that affect probe size and shape such as defocus and source coherence. The main imaging parameter dependencies are on detector angle and accelerating voltage, which are well known. The robustness to variation in other parameters allows for a quantitative comparison of experimental data and simulation without the need to fit parameters. By demonstrating the application of the PICS to the chemical identification of single atoms in a heterogeneous catalyst and in thin, layered-materials, we explore some of the experimental considerations when using this approach.

Defect structures in ZnO studied by high-resolution structural and spectroscopic imaging.

The formation of characteristic inversion domain structures in zinc oxide (ZnO) is triggered by the addition of trivalent Fe(3+) or In(3+) dopants. As-grown and inverted ZnO domains are separated by two types of inversion domain boundaries (IDBs): basal b-IDBs parallel to {0001}, and pyramidal p-IDBs parallel to {21¯1¯5} lattice planes in three equivalent variants. Cs-corrected analytical TEM/STEM is the method of choice for a comprehensive structural and compositional characterization of these materials. It is shown by electron and X-ray spectroscopic imaging in STEM that dopant species are essentially localized within both types of IDBs, whereas solid solubility of trivalent dopants within ZnO domains is rather low (<0.5at%). Under the assumption of one monolayer per IDB the relation between inversion domain structure and integral dopant concentration correlates well with integral EDS and EELS measurements in STEM over well defined sample regions. The presence of one close-packed monolayer of trivalent dopant ions within a b-IDB is unambiguously confirmed by atomic resolution STEM imaging. Columns of cations are clearly imaged in high-angle annular dark-field (HAADF) STEM imaging, whereas annular bright-field (ABF) STEM is capable of imaging both light and heavy atom columns simultaneously. It is shown that structural details in ABF images are directly interpretable even in specimen regions with thickness >50nm. The structural inversion associated with a stacking fault as a consequence of the presence of octahedrally coordinated In(3+) in the b-IDB is directly revealed by atomic resolution imaging. Column positions in atomic resolution ABF imaging in In2O3-ZnO nanorods show that the oxygen sub-lattice continues across the b-IDB with only marginal distortions, whereas the cation sub-lattice suffers a rigid shift relative to the oxygen lattice as a result of the coordination geometry of ZnO4 tetrahedrons sharing common oxygen ions with the InO6 coordination octahedrons.

Structural and elemental analysis of iron and indium doped zinc oxide by spectroscopic imaging in Cs-corrected STEM.

ZnO with additions of Fe2O3 or In2O3 shows characteristic inversion domain structures. ZnO domains are separated by two types of inversion domain boundaries (IDBs): basal b-IDBs parallel to (0001) planes, and complementary pairs of three possible variants of pyramidal p-IDBs parallel to {2115} lattice planes. The structure and composition of IDBs were investigated in a sophisticated aberration-corrected scanning transmission electron microscope (probe-corrected TEM/STEM). It is shown that Fe and In additions are essentially located in monolayers within the IDBs, and EELS electron spectroscopic imaging (ESI) as well as EDS spectroscopic imaging by X-rays (SIX) are capable of rapidly mapping the element distribution. With solid solubility of trivalent dopant species well below 1at.% within ZnO domains, the lateral spacings of b-IDBs are inversely proportional to the dopant concentration. Quantification of data acquired by ESI and SIX from well defined sample regions in STEM both confirm the assumption of one full monolayer of dopants per IDB. Atom columns of cations are well resolved in HAADF STEM imaging; experimental contrast intensities are approximately proportional to Z¹·6. Furthermore, annular bright-field (ABF)-STEM imaging is capable of resolving oxygen columns even in thick sample regions, thus providing highly localized information on atom positions and lattice distortions, and enables the construction of more reliable structure models of IDBs in doped ZnO.

Direct oxygen imaging within a ceramic interface, with some observations upon the dark contrast at the grain boundary.

Annular bright field scanning transmission electron microscopy, which has recently been established to produce directly interpretable images with both light and heavier atomic columns visible simultaneously, is shown to allow directly interpretable imaging of the oxygen columns within the Σ13[12¯10](101¯4) pyramidal twin grain boundary in α-Al(2)O(3). By using information in the high-angle annular dark field image and annular bright field images simultaneously, we estimate the specimen thickness and finite source size, and use them to explore in simulation the issue of dark contrast in the vicinity of the grain boundary in the annular dark field image.

Dynamics of annular bright field imaging in scanning transmission electron microscopy.

We explore the dynamics of image formation in the so-called annular bright field mode in scanning transmission electron microscopy, whereby an annular detector is used with detector collection range lying within the cone of illumination, i.e. the bright field region. We show that this imaging mode allows us to reliably image both light and heavy columns over a range of thickness and defocus values, and we explain the contrast mechanisms involved. The role of probe and detector aperture sizes is considered, as is the sensitivity of the method to intercolumn spacing and local disorder.

Lattice imaging in low-angle and high-angle bright-field scanning transmission electron microscopy.

Atomic resolution low-angle bright-field (LABF) scanning transmission electron-microscope (STEM) images and high-angle bright-field (HABF) STEM images of [011]-orientated Si have been experimentally obtained together with high-angle annular dark-field (HAADF) STEM images. The contrast formation mechanisms of the LABF STEM and HABF STEM images are examined in comparison with HAADF STEM images. The HABF STEM images independent of defocus and thickness have spatial resolution comparable with HAADF STEM images, and are shown to be given as a simple convolution under the non-dispersion approximation of localized Bloch waves.