Scott D. Findlay

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.

Spectroscopic Imaging of Single Atoms Within a Bulk Solid

The ability to localize, identify, and measure the electronic environment of individual atoms will provide fundamental insights into many issues in materials science, physics, and nanotechnology. We demonstrate, using an aberration-corrected scanning transmission electron microscope, the spectroscopic imaging of single La atoms inside CaTiO3. Dynamical simulations confirm that the spectroscopic information is spatially confined around the scattering atom. Furthermore, we show how the depth of the atom within the crystal may be estimated.

Three-dimensional imaging of individual hafnium atoms inside a semiconductor device

The aberration-corrected scanning transmission electron microscope allows probes to be formed with less than 1-A diameter, providing sufficient sensitivity to observe individual Hf atoms within the SiO2 passivating layer of a HfO2∕SiO2∕Si alternative gate dielectric stack. Furthermore, the depth resolution is sufficient to localize the atom positions to half-nanometer precision in the third dimension. From a through-focal series of images, we demonstrate a three-dimensional reconstruction of the Hf atom sites, representing a three-dimensional map of potential breakdown sites within the gate dielectric.

Standardless atom counting in scanning transmission electron microscopy.

We demonstrate that high-angle annular dark-field imaging in scanning transmission electron microscopy allows for quantification of the number and location of all atoms in a three-dimensional, crystalline, arbitrarily shaped specimen without the need for a calibration standard. We show that the method also provides for an approach to directly measure the finite effective source size of a scanning transmission electron microscope.

Position averaged convergent beam electron diffraction: theory and applications.

A finely focused angstrom-sized coherent electron probe produces a convergent beam electron diffraction pattern composed of overlapping orders of diffracted disks that sensitively depends on the probe position within the unit cell. By incoherently averaging these convergent beam electron diffraction patterns over many probe positions, a pattern develops that ceases to depend on lens aberrations and effective source size, but remains highly sensitive to specimen thickness, tilt, and polarity. Through a combination of experiment and simulation for a wide variety of materials, we demonstrate that these position averaged convergent beam electron diffraction patterns can be used to determine sample thicknesses (to better than 10%), specimen tilts (to better than 1mrad) and sample polarity for the same electron optical conditions and sample thicknesses as used in atomic resolution scanning transmission electron microscopy imaging. These measurements can be carried out by visual comparison without the need to apply pattern-matching algorithms. The influence of thermal diffuse scattering on patterns is investigated by comparing the frozen phonon and absorptive model calculations. We demonstrate that the absorptive model is appropriate for measuring thickness and other specimen parameters even for relatively thick samples (>50nm).

Atomic Structure of a CeO2 Grain Boundary: The Role of Oxygen Vacancies

Determining both cation and oxygen sublattices of grain boundaries is essential to understand the properties of oxides. Here, with scanning transmission electron microscopy, electron energy-loss spectroscopy, and first-principles calculations, both the Ce and oxygen sublattices of a (210)Σ5 CeO(2) grain boundary were determined. Oxygen vacancies are shown to play a crucial role in the stable grain boundary structure. This finding paves the way for a comprehensive understanding of grain boundaries through the atomic scale determination of atom and defect locations.

Atomic-scale imaging of individual dopant atoms in a buried interface

Determining the atomic structure of internal interfaces in materials and devices is critical to understanding their functional properties. Interfacial doping is one promising technique for controlling interfacial properties at the atomic scale, but it is still a major challenge to directly characterize individual dopant atoms within buried crystalline interfaces. Here, we demonstrate atomic-scale plan-view observation of a buried crystalline interface (an yttrium-doped alumina high-angle grain boundary) using aberration-corrected Z-contrast scanning transmission electron microscopy. The focused electron beam transmitted through the off-axis crystals clearly highlights the individual yttrium atoms located on the monoatomic layer interface plane. Not only is their unique two-dimensional ordered positioning directly revealed with atomic precision, but local disordering at the single-atom level, which has never been detected by the conventional approaches, is also uncovered. The ability to directly probe individual atoms within buried interface structures adds new dimensions to the atomic-scale characterization of internal interfaces and other defect structures in many advanced materials and devices.

Direct Imaging of Reconstructed Atoms on TiO2 (110) Surfaces

Determining the atomic structures of oxide surfaces is critical for understanding their physical and chemical properties but also challenging because the breaking of atomic bonds in the formation of the surface termination can involve complex reconstructions. We used advanced transmission electron microscopy to directly observe the atomic structure of reduced titania (TiO2) (110) surfaces from directions parallel to the surface. In our direct atomic-resolution images, reconstructed titanium atoms at the top surface layer are clearly imaged and are found to occupy the interstitial sites of the TiO2 structure. Combining observations from two orthogonal directions, the three-dimensional positioning of the Ti interstitials is identified at atomic dimensions and allows a resolution of two previous models that differ in their oxygen stoichiometries.

Modelling the inelastic scattering of fast electrons

Imaging at atomic resolution based on the inelastic scattering of electrons has become firmly established in the last three decades. Harald Rose pioneered much of the early theoretical work on this topic, in particular emphasising the role of phase and the importance of a mixed dynamic form factor. In this paper we review how the modelling of inelastic scattering has subsequently developed and how numerical implementation has been achieved. A software package μSTEM is introduced, capable of simulating various imaging modes based on inelastic scattering in both scanning and conventional transmission electron microscopy.