Deconvolution processing of HAADF STEM images

A deconvolution processing of high-resolution high-angle annular dark field (HAADF) scanning transmission electron microscopy (STEM) images, combined with maximum entropy method, is applied to two experimental [0 11]-Si images; one having unresolved dumbbells and the other having resolved dumbbells and artificial bright spots. The deconvoluted images for these images show bright spots corresponding to the projected atomic columns and no artificial bright spots. Thus, the deconvolution processing provides almost a real projected atomic structure by eliminating effects of the probe function from HAADF STEM images.     

A novel method for focus assessment in atomic resolution STEM HAADF experiments

Analysis of the Fourier components of through-focal images in scanning transmission electron microscopy with a high angle annular dark field detector is used to assess illumination defocus values. The method is based on a least squares fitting of the peculiar dependence of Fourier components of the high angle annular dark field image on defocus. The validity of the method has been checked against simulations and experiments obtaining a good level of accuracy on the defocus measurement (δf=2 nm) for simulated specimen thickness up to 40 nm. The difference between simulated and experimental Fourier coefficients for large defoci can be used to estimate the specimen thickness at least up to 30 nm but with decreasing precision for larger thickness.     

Quantitative structural analysis of twin boundary in alpha-Zn7Sb2O12 using HAADF STEM method

The structure and composition of the 1/4{110} twin boundary in alpha-Zn7Sb2O12 have been determined by using quantitative high-angle annular dark field scanning transmission electron microscopy (HAADF STEM) analysis. The noise in the experimental HAADF STEM images is reduced by using the maximum entropy method and average processing, and the parameters used in dynamical simulations are experimentally determined. From the analysis, it has been found that octahedral sites in the twin boundary slightly shift parallel to the [110] direction, and a reduction of the Sb concentration at the octahedral sites on the plane adjacent to the twin boundary was detected. The reduction was measured from three regions in the same twin boundary, and the Sb concentrations were 4 +/- 3, 8 +/- 3 and 19 +/-2 at% from 33 at%.     

Optimal scanning and image processing with the STEM

We have recently published a theory of an optimal scanning system which is particularly suited for the STEM. One concludes from the theory that the diffraction limit of the electron probe should be a fixed fraction of the full-scale deflection in order to avoid scanning artifacts. More recently, we have confirmed the value of this technique by direct experiments. Our program now is to combine the use of optimal scanning with the use of a programmable digital refresh memory for image analysis. Limited experience to date indicates that false color conversion is probably more useful than histogram equalization in black and white and that this system is particularly valuable for rotational averaging and selected area Fourier transforms.     

Bloch-wave-based STEM image simulation with layer-by-layer representation

In a dynamical STEM image simulation by the Bloch-wave method, Allen et al. formulated a framework for calculating the cross-section for any incoherent scattering process from the inelastic scattering coefficients: thermal diffuse scattering (TDS) for high-angle annular dark-field (HAADF) and back-scattered electron (BSE) STEM, and ionization for electron energy-loss spectroscopy (EELS) and energy-dispersive X-ray spectroscopy (EDX) STEM. Furthermore, their method employed a skilful approach for deriving the excitation amplitude and block diagonalization in the eigenvalue equation. In the present work, we extend their scheme to a layer-by-layer representation for application to inhomogeneous crystals that include precipitates, defects and atomic displacement. Calculations for a multi-layer sample of Si–Sb–Si were performed by multiplying Allen et al.'s block-diagonalized matrices. Electron intensities within the sample and EDX STEM images, as an example of the inelastic scattering, were calculated at various conditions. From the calculations, 3-dimensional STEM analysis was considered.     

Accurate structure determination from image reconstruction in ADF STEM

Annular dark-field (ADF) imaging in a scanning transmission electron microscope results in direct structure images of the atomic configuration of the specimen. Since such images are almost perfectly incoherent they can be treated as a convolution between a point-spread function, which is simply the intensity of the illuminating electron probe, and a sharply peaked object function that represents the projected structure of the specimen. Knowledge of the object function for an image region of perfect crystal allows the point-spread function to be directly determined for that image. We examine how the object function for an image can then be reconstructed using a Wiener filter, the CLEAN algorithm and a maximum entropy reconstruction. Prior information is required to perform a reconstruction, and we discuss what nature of prior information is suitable for ADF imaging.     

Thick specimens in the CEM and STEM. Resolution and image formation.

A theory of resolution and image formation is presented for thick amorphous specimens in transmission electron microscopes. Eight modes of operation are considered, four in the scanning transmission electron microscope (STEM) and four in the conventional electron microscope (CEM). A thick specimen is defined here as one in which the resolution of detail is limited by plural scattering of the electron beam. In practice this includes films on the order of a micron in thickness. An analytic theory of plural incoherent scattering is developed which is general with respect to material and beam voltage. The theory gives the distribution of elastically scattered electrons as a function of transverse coordinate and angles, and is directly applicable to optical systems. The theory applies to all thicknesses normally encountered, and includes thin specimens as well as thick specimens. Criteria are proposed for evaluation of the quality of microscope images, and the modulation transfer function is applied to determine some practical estimates of picture quality. The STEM is found to have distinct advantages over the CEM for thick specimens. For a carbon specimen one micron thick a STEM operating in bright field at 90 keV produces an image which is roughly equivalent to that of a CEM operating in bright field at 1 MeV. Improvement can be obtained in the CEM by filtering out eneryg-loss electrons which degrade resolution due to chromatic aberration. This results in a reduction in signal intensity and usable thickness, however.     

Application of image processing to STEM tomography of low-contrast materials

In this study, the effect of various image-processing techniques on the visibility of tomographic reconstructions is investigated for a low-contrast material system of non-uniform thickness containing complex features such as grain boundaries and nanoparticles. Starting with a tilt series of high-angle annular dark-field (HAADF) images from an area of Dy-doped YBa₂Cu₃O_7−x-coated superconductor obtained using a scanning transmission electron microscope, various image-processing techniques were applied. These can be classified as edge detection, contrast-enhancing methods for non-uniform thickness and image sharpening. Although the processing methods violate the projection criterion for tomographic reconstruction, they were found, at least in this case, to enhance contrast and define the correct shape and size of structural features with minimal artifacts. Enhancing the visibility of structural features in this way allows the spatial distribution of the nanoparticles, their size, number density and location relative to each other and grain boundaries to be determined, which are essential to understand the flux-pinning characteristics of these materials.     

Quantitative analysis of image contrast in phase contrast STEM for low dose imaging

This work quantitatively evaluates the contrast in phase contrast images of thin vermiculite crystals recorded by TEM and aberration-corrected bright-field STEM. Specimen movement induced by electron irradiation remains a major problem limiting the phase contrast in TEM images of radiation-sensitive specimens. While spot scanning improves the contrast, it does not eliminate the problem. One possibility is to utilise aberration-corrected scanning transmission electron microscopy (STEM) with an Ångstrom-sized probe to illuminate the sample, and thus further reduce irradiation-induced specimen movement. Vermiculite is relatively radiation insensitive in TEM to electron fluences below 100,000 e⁻/Ų and this is likely to be similar for STEM although different damage mechanisms could occur. We compare the performance of a TEM with a thermally assisted field emission electron gun (FEG) and charge coupled device (CCD) image capture to the performance of STEMs with spherical aberration correction, cold field emission electron sources and photomultiplier tube image capture at a range of electron fluences and similar illumination areas. We show that the absolute contrast of the phase contrast images obtained by aberration-corrected STEM is better than that obtained by TEM. Although the STEM contrast is higher, the efficiency of collection of electrons in bright field STEM is still much less than that in bright field TEM (where for thin samples virtually all the electrons contribute to the image), and the SNR of equivalent STEM images is three times lower. This is better than expected, probably due to the absence of a frequency dependent modulation transfer function in the STEM detection system. With optimisation of the STEM bright field collection angles, the efficiency may approach that of bright field TEM, and if reductions in beam-induced specimen movement are found, STEM could surpass the overall performance of TEM.     

An approach to the systematic distortion correction in aberration-corrected HAADF images

Systematic distortion has been analysed in high‐angle annular dark‐field (HAADF) images which may be caused by electrical interference. Strain mapping techniques have been applied to a strain‐free GaAs substrate in order to provide a broad analysis of the influence of this distortion on the determination of local strain in the heterostructure. We have developed a methodology for estimating the systematic distortion, and we correct the original images by using an algorithm that removes this systematic distortion.     

A practical approach for STEM image simulation based on the FFT multislice method

It has been demonstrated that a high-angle annular dark-field (HAADF) STEM technique gives an image resolving atomic columns. Due to the diffusion of this technique and an improvement of its resolution, a practical procedure for image simulation becomes important for a quantitative interpretation of the HAADF image. In this report a new practical scheme for a STEM image simulation is developed based on the FFT multislice algorithm. Here, a HAADF intensity due to thermal diffuse scattering (TDS) is calculated from the absorptive potential corresponding to high-angle TDS and the wave function equivalent to the propagating probe within the sample. Contrary to the commonly used Bloch wave method, a coherent bright-field intensity and a coherent HAADF intensity are also obtained straightforwardly. The HAADF image contrast calculated for GaAs is not simply proportional to Z2 as expected from the Rutherford scattering at high-angle, and the As/Ga contrast ratio depends on the specimen thickness. This suggests that the generation of the HAADF signal is appreciably affected by the coherent dynamical scattering. The developed procedure here will have a definitive advantage over the Bloch wave approach for simulating the HAADF images expected from a defect and interface or amorphous materials, and also the HAADF image obtained by using a Cs-corrected microscope. This is because the former requires a huge super cell, while the latter needs a large objective aperture including a large number of incident beam directions.     

Influence of detector geometry on image properties of the STEM for thick objects.

Plural electron scattering within thick objects broadens and smoothes the intensity distribution in the detector plane of a scanning transmission electron microscope. Detector arrangements have been determined which give maximum contrast and optimum S/N when the object details are large compared to the scanning spot. Asymptotic expressions for the optimum detector angles, specimen resolution, and S/N were obtained which are valid for objects thicker than approximately four elastic mean free path lengths. Exact calculations of the changes in contrast and S/N with thickness fluctuations in amorphous carbon foils were performed for atbitrary foil thicknesses. Elastic and inelastic electron scattering was taken into account.     

A method of combining STEM image with parallel beam diffraction and electron-optical conditions for diffractive imaging

We describe a method of combining STEM imaging functionalities with nanoarea parallel beam electron diffraction on a modern TEM. This facilitates the search for individual particles whose diffraction patterns are needed for diffractive imaging or structural studies of nanoparticles. This also lays out a base for 3D diffraction data collection.     

The use of array processors attached to minicomputers for multislice image calculations

The multislice algorithm is the dominant method in the computation of high resolution images from crystals. As the algorithm can be structured in terms of Fourier transforms and multiplications on large arrays, it is ideally suited to array processors. Computation times for various systems are compared, and it is shown that a minicomputer with an attached array processor is competitive with mainframe computers. This opens up the possibility of building interactive work stations for high resolution structure analysis.     

Surface studies in UHV SEM and STEM

Some recent advances in surface analyses with scanning electron microscopy techniques are reviewed. It is shown that secondary electron microscopy can image monatomic steps, emergent dislocations and the early growth of thin films and oxide nuclei. The chemical composition of inhomogeneous surfaces can, in some cases, be determined with nanometre resolution with Auger signals. Overlayer coverages can occasionally be monitored with the secondary electron signal if the change of work function with coverage has been determined previously. The interpretation of these secondary and Auger signals is discussed. The combination of angular electron spectroscopy with electron microscopy is potentially a powerful technique for determining atomic positions of surface atoms and one method for obtaining the experimental data is described. Several substrate/overlayer systems are used to illustrate the amount of information that can be obtained about surface processes with scanning electron microscopy.     

Fluctuation microscopy in the STEM

Fluctuation electron microscopy is a technique for studying medium-range order in disordered materials. We present an implementation of fluctuation microscopy using nanodiffraction in a scanning transmission electron microscope (STEM) at a spatial resolution varying from 0.8 to 5.0 nm. Compared to conventional TEM (CTEM), the STEM-based technique offers a denser scattering vector sampling at a reduced sample dose and easier access to variable resolution information. We have reproduced results on amorphous silicon previously obtained by CTEM-based fluctuation microscopy, and report initial variable-resolution measurements on amorphous germanium.     

HREM and STEM of defects in multiply-twinned particles

The structure of defects in multiply-twinned particles has been studied in detail using high-resolution lattice imaging, dark field and microdiffraction techniques. Icosahedral particles with sizes greater than about 15 nm were found to contain defects, in the form of stacking fault loops parallel with the external surface, which were extremely difficult to detect by conventional amplitude contrast techniques. Microdiffraction mappings correlated with these results, showing large rotations of the face-centred cubic segments. Results for decahedral particles indicated the presence of stacking faults running adjacent to, and parallel with, the twin boundaries. Microdiffraction maps confirmed that the particle structure was face-centred cubic, and also verified that the apparent epitaxy of these particles was highly variable. Models for the defects are proposed and discussed, and the relative merits of HREM and STEM for elucidating structural details in small particles is briefly considered. Finally, the potential for direct imaging at surfaces, as demonstrated by some recent images, is discussed.     

Channelling effects in atomic resolution STEM

A Bloch wave theory for incoherent scattering of an incident plane wave has proved successful in predicting the fine detail in 2-D zone axis channelling patterns formed by ADF, BSE and characteristic X-ray detection in beam rocking mode. A previously published example of polarity determination of GaAs by channelling contrast is compared with simulations in order to illustrate the applicability of the theory. Modification of boundary conditions for a focused coherent probe allows lattice-resolution incoherent contrast based on ADF and EELS detection as well as X-ray emissions to be catered for within a similar theoretical framework. Mixed dynamic form factors constitute an integral part of this theory, where quantum-mechanical phase is a core issue. Simulations of lattice-resolution ADF and EELS are discussed with reference to various zone axis projections of GaAs. Issues of single versus double channelling conditions, and local versus nonlocal interactions, are discussed in relation to X-ray, ADF and EELS detection.