High-angle Annular Dark-field Signal Research Articles

Characterization of Ordering in A-Site Deficient Perovskite Ca1-xLa2x/3TiO3 Using STEM/EELS.

The vacancy ordering behavior of an A-site deficient perovskite system, Ca1-xLa2x/3TiO3, was studied using atomic resolution scanning transmission electron microscopy (STEM) in conjunction with electron energy-loss spectroscopy (EELS), with the aim of determining the role of A-site composition changes. At low La content (x = 0.2), adopting Pbnm symmetry, there was no indication of long-range ordering. Domains, with clear boundaries, were observed in bright-field (BF) imaging, but were not immediately visible in the corresponding high-angle annular dark-field (HAADF) image. These boundaries, with the aid of displacement maps from A-site cations in the HAADF signal, are shown to be tilt boundaries. At the La-rich end of the composition (x = 0.9), adopting Cmmm symmetry, long-range ordering of vacancies and La3+ ions was observed, with alternating La-rich and La-poor layers on (001)p planes, creating a double perovskite lattice along the c axis. These highly ordered domains can be found isolated within a random distribution of vacancies/La3+, or within a large population, encompassing a large volume. In regions with a high number density of double perovskite domains, these highly ordered domains were separated by twin boundaries, with 90° or 180° lattice rotations across boundaries. The occurrence and characteristics of these ordered structures are discussed and compared with similar perovskite systems.

Interfacial Atomic Number Contrast in Thick Samples

A quantitative method to simulate the electron scattering at the interface of two material layers in thick samples is presented here. The samples are analyzed by Scanning Transmission Electron Microscopy (STEM) in a Tecnai F30 using a High Angle Annular Dark-Field (HAADF) detector with a collection range 55 mrad to 245 mrad. At the interface of a high-density and low-density material an increase in the HAADF signal for thick TEM samples can be observed. We report here the simulated HAADF detector intensity across the interface of two materials using Python programming language and its comparison with experimental results. The electron atomic scattering factor f e (s) for a complex potential is given by:

Experimental evaluation of interfaces using atomic-resolution high angle annular dark field (HAADF) imaging

Aberration-corrected high angle annular dark field (HAADF) imaging in scanning transmission electron microscopy (STEM) can now be performed at atomic-resolution. This is an important tool for the characterisation of the latest semiconductor devices that require individual layers to be grown to an accuracy of a few atomic layers. However, the actual quantification of interfacial sharpness at the atomic-scale can be a complicated matter. For instance, it is not clear how the use of the total, atomic column or background HAADF signals can affect the measured sharpness or individual layer widths. Moreover, a reliable and consistent method of measurement is necessary. To highlight these issues, two types of AlAs/GaAs interfaces were studied in-depth by atomic-resolution HAADF imaging. A method of analysis was developed in order to map the various HAADF signals across an image and to reliably determine interfacial sharpness. The results demonstrated that the level of perceived interfacial sharpness can vary significantly with specimen thickness and the choice of HAADF signal. Individual layer widths were also shown to have some dependence on the choice of HAADF signal. Hence, it is crucial to have an awareness of which part of the HAADF signal is chosen for analysis along with possible specimen thickness effects for future HAADF studies performed at the scale of a few atomic layers.

Quantitative Scanning Transmission Electron Microscopy for the Measurement of Thicknesses and Volumes of Individual Nanoparticles

AbstractIn Scanning Transmission Electron Microscopy (STEM) the High-Angle Annular Dark-Field (HAADF) signal increases with atomic number and sample thickness, while dynamic scattering effects and sample orientation have little influence on the contrast. The sensitivity of the HAADF detector for a FEI F30 transmission electron microscope has been calibrated. Additionally, a nearly linear relationship of the HAADF signal with the incident electron current is confirmed. Cross sections of multilayered samples for contrast calibration were obtained by focused ion-beam (FIB) preparation. These cross sections contained several layers with known composition. A database with several pure elements and compounds has been compiled, containing experimental data on the fraction of electrons scattered onto the HAADF detector for each nanometer of sample thickness. Contrast simulations are based on the multi-slice formalism and confirm the differences in HAADF-scattering contrast for the elements and compounds. TEM offers high lateral resolution, but contains little or no information on the thickness of samples. Thickness maps in energy-filtered transmission electron microscopy, convergent-beam electron diffraction and tilt series are so far the only methods to determine thicknesses of particles in a transmission electron microscope. We show that the calibrated HAADF contrast can be used to determine the thicknesses of individual nanoparticles deposited on carbon films. With this information the volumes of nanoparticles with known composition were determined.

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 Z 2 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.

Prospects of atomic resolution imaging with an aberration-corrected STEM

We investigated high-resolution scanning transmission electron microscope (STEM) images obtained from a microscope equipped with a spherical aberration corrector. The probe size (full-width at half-maximum) is reduced to 0.76 A at 200 kV by assuming the fifth-order spherical aberration coefficient C5 = 100 mm. For the simulation we have used the recently developed scheme for a STEM image simulation based on the Fast Fourier Transform (FFT) multislice algorithm. The peak-to-background (P/B) ratio of the high-angle annular dark-field (HAADF) image is significantly improved at a thin specimen region. Although the P/B ratio becomes worse at a thicker region, the resolution is kept high even at such a region. An almost true HAADF signal will be obtained even from a weak-scattering phosphorous column in InP [001] when the background is subtracted. In the bright-field image the coherent character of elastic scattering is suppressed by averaging over a large convergence angle, making the specimen effectively self-luminous. The claim that HAADF imaging is relatively insensitive to a defocus as well as a specimen thickness is valid only qualitatively, and a detailed image simulation will be required for a quantitative analysis as in the case of the conventional transmission electron microscope. It was noted that the delta function approximation for the object function may not be applicable for a very fine probe, and that the achievable resolution of the HAADF imaging will be limited by the widths of the high-angle thermal diffuse scattering potential.

Imaging dislocations with an annular dark-field detector

High-angle annular dark-field (HAADF) scanning transmission electron microscopy (STEM) has been recently the subject of active research because of its successful applications to the characterization of supported catalysts, interface problems in MBE grown semiconductors, superconductors and X-ray multilayers. The characteristics of HAADF images are different from those of the TEM images. For perfect single crystals the HAADF signal is mainly generated from thermal diffuse scattering. HAADF technique has also been used to study dopant contrast effects in semiconductors and dislocations have also been observed with an ADF detector. In this paper we report a study of dislocation contrasts and their dependence on the inner collection angle of the ADF detector.The STEM instrument used for the observations was the HB5 from VG Microscopes, Ld., modified by the addition of an ultra-high resolution pole piece (Cs = 0.8 mm) and a two-dimensional detector system. Post specimen lenses and various beam stops were used to change the inner (α) and outer (β) collection angles of the ADF detector.