Yukihito Kondo

Robust atomic resolution imaging of light elements using scanning transmission electron microscopy

We show that an annular detector placed within the bright field cone in scanning transmission electron microscopy allows direct imaging of light elements in crystals. In contrast to common high angle annular dark field imaging, both light and heavy atom columns are visible simultaneously. In contrast to common bright field imaging, the images are directly and robustly interpretable over a large range of thicknesses. We demonstrate this through systematic simulations and present a simple physical model to obtain some insight into the scattering dynamics.

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.

Visualization of Light Elements at Ultrahigh Resolution by STEM Annular Bright Field Microscopy

In the field of materials sciences such as studies on ceramics, semi-conducting material and metals, role of light elements is important, because it is one of mainly composing elements or determiner of character i. e. dopants. The light elements at high resolution have been observed by ultrahigh voltage electron microscopy or aberration corrected electron microscopy in Transmission Electron Microscopy (TEM), since the visualization of light requires highly resolving power. Recently, a high angle annular dark field (HAADF) scanning transmission electron microscopy (STEM) has become widely used in this field because of high-resolution capability and easily interpretable image contrast, which is roughly proportional to square of atomic number Z (Z). However, the HAADF image sometimes gives lack of light element because of excess contrast originated from Z, when the specimen contains the light and heavy elements. The TEM bright field imaging gives an image contrast roughly proportional to the Z, when the specimen is thin enough to be able to apply the ‘thin film approximation’. We have examined to apply an STEM annular bright field (ABF) imaging, which is equivalent to TEM hollow cone illumination imaging technique [1-2], to the oxide or nitride samples for simultaneous visualization of light and heavier elements. According to the article on hollow cone illumination in TEM [2], the contrast transfer in ABF expected to give better resolution than conventional BF STEM and to give non-oscillating contrast transfer, which gives easily-interpretable images unlike the BF STEM. This paper reports characteristics and the experimental result of the ABF imaging technique.

STEM imaging of 47-pm-separated atomic columns by a spherical aberration-corrected electron microscope with a 300-kV cold field emission gun

A spherical aberration-corrected electron microscope has been developed recently, which is equipped with a 300-kV cold field emission gun and an objective lens of a small chromatic aberration coefficient. A dumbbell image of 47 pm spacing, corresponding to a pair of atomic columns of germanium aligned along the [114] direction, is resolved in high-angle annular dark field (HAADF) scanning transmission electron microscopy (STEM) with a 0.4-eV energy spread of the electron beam. The observed image was compared with a simulated image obtained by dynamical calculation.

Direct imaging of lithium atoms in LiV2O4 by spherical aberration-corrected electron microscopy

We visualized lithium atom columns in LiV₂O₄ crystals by combining scanning transmission electron microscopy with annular bright field (ABF) imaging using a spherical aberration-corrected electron microscope (R005) viewed from the [110] direction. The incident electron beam was coherent with a convergent angle of 30 mrad (semi-angle), and the detector collected scattered electrons over 20-30 mrad (semi-angle). The ABF image showed dark dots corresponding to lithium, vanadium and oxygen columns.

Performance of low-voltage STEM/TEM with delta corrector and cold field emission gun

To reduce radiation damage caused by the electron beam and to obtain high-contrast images of specimens, we have developed a highly stabilized transmission electron microscope equipped with a cold field emission gun and spherical aberration correctors for image- and probe-forming systems, which operates at lower acceleration voltages than conventional transmission electron microscopes. A delta-type aberration corrector is designed to simultaneously compensate for third-order spherical aberration and fifth-order 6-fold astigmatism. Both were successfully compensated in both scanning transmission electron microscopy (STEM) and transmission electron microscopy (TEM) modes in the range 30-60 kV. The Fourier transforms of raw high-angle annular dark field (HAADF) images of a Si[110] sample revealed spots corresponding to lattice spacings of 111 and 96 pm at 30 and 60 kV, respectively, and those of raw TEM images of an amorphous Ge film with gold particles showed spots corresponding to spacings of 91 and 79 pm at 30 and 60 kV, respectively. Er@C(82)-doped single-walled carbon nanotubes, which are carbon-based samples, were successfully observed by HAADF-STEM imaging with an atomic-level resolution.

New area detector for atomic-resolution scanning transmission electron microscopy

A new area detector for atomic-resolution scanning transmission electron microscopy (STEM) is developed and tested. The circular detector is divided into 16 segments which are individually optically coupled with photomultiplier tubes. Thus, 16 atomic-resolution STEM images which are sensitive to the spatial distribution of scattered electrons on the detector plane can be simultaneously obtained. This new detector can be potentially used not only for the simultaneous formation of common bright-field, low-angle annular dark-field and high-angle annular dark-field images, but also for the quantification of images by detecting the full range of scattered electrons and even for exploring novel atomic-resolution imaging modes by post-processing combination of the individual images.

Measurement method of aberration from Ronchigram by autocorrelation function

Aberrations up to the fifth-order were successfully measured using an autocorrelation function of the segmental areas of a Ronchigram. The method applied to aberration measurement in a newly developed 300kV microscope that is equipped with a spherical aberration corrector for probe-forming systems. The experimental Ronchigram agreed well with the simulated Ronchigram that was calculated by using the measured aberrations. The Ronchigram had an infinite magnification area with a half-angle of 50mrad, corresponding to the convergence angle of a uniform phase.

Achieving 63 pm Resolution in Scanning Transmission Electron Microscope with Spherical Aberration Corrector

The performance of a newly developed high-resolution 300 kV microscope equipped with a spherical aberration corrector for probe-forming systems is reported. This microscope gave the highest resolution for the distance between atomic columns, as determined by a high-angle annular dark field imaging method using a GaN[211] crystalline specimen, where the distance between the neighboring columns of Ga was 63 pm.

Synthesis of carbon nanotubes from bulk polymer

Carbon nanotubes have been synthesized by heat treating the polymer at 400 °C in air which was obtained by polyesterification between citric acid and ethylene glycol. Transmission electron micrographs and an electron diffraction pattern showed the formation of carbon nanotubes. The diameter of the tubes ranged from 5 to 20 nm, whereas the lengths were less than 1 μm.