Peter Christiaan Tiemeijer

Detection of Single Atoms and Buried Defects in Three Dimensions by Aberration-Corrected Electron Microscope with 0.5-Å Information Limit

The ability of electron microscopes to analyze all the atoms in individual nanostructures is limited by lens aberrations. However, recent advances in aberration-correcting electron optics have led to greatly enhanced instrument performance and new techniques of electron microscopy. The development of an ultrastable electron microscope with aberration-correcting optics and a monochromated high-brightness source has significantly improved instrument resolution and contrast. In the present work, we report information transfer beyond 50 pm and show images of single gold atoms with a signal-to-noise ratio as large as 10. The instruments new capabilities were exploited to detect a buried Sigma3 {112} grain boundary and observe the dynamic arrangements of single atoms and atom pairs with sub-angstrom resolution. These results mark an important step toward meeting the challenge of determining the three-dimensional atomic-scale structure of nanomaterials.

Electron energy-loss near-edge structures of 3d transition metal oxides recorded at high-energy resolution.

Near-edge fine structures of the metal L(2,3) and O K-edges in transition metal-oxides have been studied with a transmission electron microscope equipped with a monochromator and a high-resolution imaging filter. This system enables the recording of EELS spectra with an energy resolution of 0.1eV thus providing new near-edge fine structure details which could not be observed previously by EELS in conventional TEM instruments. EELS-spectra from well-defined oxides like titanium oxide (TiO(2)), vanadium oxide (V(2)O(5)), chromium oxide (Cr(2)O(3)), iron oxide (Fe(2)O(3)), cobalt oxide (CoO) and nickel oxide (NiO) have been measured with the new system. These spectra are compared with EELS data obtained from a conventional microscope and the main spectral features are interpreted. Additionally, the use of monochromised TEMs is discussed in view of the natural line widths of K and L(2,3) edges.

Precise beam-tilt alignment and collimation are required to minimize the phase error associated with coma in high-resolution cryo-EM.

Electron microscopy at a resolution of 0.4nm or better requires more careful adjustment of the illumination than is the case at a resolution of 0.8nm. The use of current-axis alignment is not always sufficient, for example, to avoid the introduction of large phase errors, at higher resolution, due to axial coma. In addition, one must also ensure that off-axis coma does not corrupt the data quality at the higher resolution. We particularly emphasize that the standard CTF correction does not account for the phase error associated with coma. We explain the cause of both axial coma and the typically most troublesome component of off-axis coma in terms of the well-known shift of the electron diffraction pattern relative to the optical axis that occurs when the illumination is not parallel to the axis. We review the experimental conditions under which coma causes unacceptably large phase errors, and we discuss steps that can be taken when setting up the conditions of illumination, so as to ensure that neither axial nor off-axis coma is a problem.

High resolution EELS using monochromator and high performance spectrometer: comparison of V2O5 ELNES with NEXAFS and band structure calculations.

Using single crystal V2O5 as a sample, we tested the performance of the new aberration corrected GATAN spectrometer on a monochromatised 200 kV FEG FEI (S)TEM. The obtained V L and O K ELNES were compared with that obtained in a common GATAN GIF and that in the new spectrometer, without monochromatised beam. The performance of the new instrumentation is impressive: recorded with an energy-resolution of 0.22 eV, the V L(3) edge reveals all the features due to the bulk electronic structure, that are also revealed in near-edge X-ray absorption fine structure (NEXAFS) with a much higher energy-resolution (0.08 eV). All features of the ELNES and NEXAFS are in line with a theoretical spectrum derived from band-structure calculations.

Using a monochromator to improve the resolution in TEM to below 0.5 Å. Part II: Application to focal series reconstruction

We apply monochromated illumination to improve the information transfer in focal series reconstruction to 0.5 Å at 300 kV. Contrary to single images, which can be taken arbitrarily close to Gaussian focus in a C(S)-corrected microscope, images in a focal series are taken at a certain defocus. This defocus poses limits on the spatial coherence of the illumination, and through this, limits on the brightness of the monochromated illumination. We derive an estimate for the minimum spatial coherence and the minimal brightness needed for a certain resolution at a certain defocus and apply this estimate to our focal series experiments. We find that the 0.5 Å information transfer would have been difficult and probably impossible to obtain without the exceptionally high brightness of the monochromated illumination.

Atomic Scale Analysis of Planar Defects in Polycrystalline Diamond

Planar defects in a polycrystalline diamond film were studied by high-resolution transmission electron microscopy (HRTEM) and high-resolution scanning transmission electron microscopy (STEM). In both modes, sub-Angstrom resolution was achieved by making use of two aberration-corrected systems; a TEM and a STEM C(s)-corrected microscope, each operated at 300 kV. For the first time, diamond in (110) zone-axis orientation was imaged in STEM mode at a resolution that allows for resolving the atomic dumbbells of carbon at a projected interatomic distance of 89 pm. Twin boundaries that show approximately the sigma3 CSL structure reveal at sub-Angstrom resolution imperfections; that is, local distortions, which break the symmetry of the ideal sigma3 type twin boundary, are likely present. In addition to these imperfect twin boundaries, voids on the atomic level were observed. It is proposed that both local distortions and small voids enhance the mechanical toughness of the film by locally increasing the critical stress intensity factor.

Atom size electron vortex beams with selectable orbital angular momentum

The decreasing size of modern functional magnetic materials and devices cause a steadily increasing demand for high resolution quantitative magnetic characterization. Transmission electron microscopy (TEM) based measurements of the electron energy-loss magnetic chiral dichroism (EMCD) may serve as the needed experimental tool. To this end, we present a reliable and robust electron-optical setup that generates and controls user-selectable single state electron vortex beams with defined orbital angular momenta. Our set-up is based on a standard high-resolution scanning TEM with probe aberration corrector, to which we added a vortex generating fork aperture and a miniaturized aperture for vortex selection. We demonstrate that atom size probes can be formed from these electron vortices and that they can be used for atomic resolution structural and spectroscopic imaging – both of which are prerequisites for future atomic EMCD investigations.

Using a monochromator to improve the resolution in focal-series reconstructed TEM down to 0.5Å

The resolution of present-day spherical-aberration corrected TEMs is limited by the chromatic aberration of the objective lens to about 0.7a at 300kV. The resolution can be improved by Cc correction or by reducing the energy spread in the illumination with a monochromator. We used TEAM 0.5, a special Titan column built within the TEAM project [1], and on this microscope we succeeded to improve the resolution to 0.5a by monochromation, not only in single images but also in images reconstructed from focal series. Such reconstructed images are free of possible contrast reversals due to incorrect focusing and possible artifacts due to non-linear interferences. However, focal series are more demanding to acquire than single images because of the higher demand on the stability of the column, and because they must be taken over some focus interval and this significantly increases the demands on the parallelness or coherence of the beam.

The Design and First Results of a Dedicated Corrector (S)TEM.

In all TEM imaging, the spatial resolution is predominantly limited by the spherical aberration and chromatic aberration of the objective lens [1, 2]. These aberrations cause the information in the image to be blurred. This information can be retrieved by through-focus series reconstruction or by holography. Alternatively, a more direct way is to correct the spherical aberration by incorporating a Cs corrector in the TEM column [3], thus making the point resolution equal to the information limit. For the situation where the aberrations are corrected on the image (Objective lens correction), a system shows enhancement of the resolution all the way down to the information limit. For the situation where the aberrations are corrected on the probe [4] (Condenser lens correction), the probe size can be improved however system stability starts to play a more and more important role in determining the final performance of the total system

First Applications of Electron Energy-Loss Spectroscopy with High Energy Resolution

A new transmission electron microscope equipped with a monochromator and a high resolution energy-filter was used for the first time to fully exploit the chemical bonding information contained in the near edge fine structures (ELNES) of electron energy-loss spectra. The instrument is capable of acquiring spectra with an energy resolution in the range of 0.1 eV, thus opening up the way for improved ELNES information. ELNES spectra of TiO 2 and CoO have been recorded and are compared with data obtained with a conventional microscope and with x-ray absorption spectroscopy. In case of the L 2,3 edges of the transition metals the new instrument revealed previously unobservable fine structure details, but for the O K edges the improved energy resolution does not result in more detailed structural features than observable in common microscopes. Furthermore, the potential of the new microscope to obtain chemical bonding information at the nanometer scale is discussed.