Atomic Imaging Using Secondary Electrons in a Scanning Transmission Electron Microscope : Experimental Observations and Possible Mechanisms

We report our detailed investigation of high-resolution imaging using secondary electrons (SE) with a subnanometer probe in an aberration-corrected transmission electron microscope, Hitachi HD2700C. This instrument also allows us to acquire the corresponding annular-dark-field (ADF) images simultaneously and separately. We demonstrate that atomic SE imaging is achievable for a wide range of elements, from uranium to carbon. Using the ADF images as a reference, we study the SE image intensity and contrast as a function of applied bias, atomic number, crystal tilt and thickness to shed light on the origin of the unexpected ultrahigh resolution in SE imaging. We have also demonstrated that the SE signal is sensitive to the terminating species at a crystal surface. Possible mechanisms for atomicscale SE imaging are proposed. The ability to image both the surface and bulk of a sample at atomic scale is unprecedented, and could revolutionize the field of electron microscopy and imaging.

Optimized conditions for direct imaging of bonding charge density in electron microscopy

We report on the observability of valence bonding effects in aberration-corrected high resolution electron microscopy (HREM) images along the [010] projection of the mineral Forsterite(Mg2SiO4). We have also performed exit wave restorations using simulated noisy images and have determined that both the intensities of individual images and the modulus of the restored complex exit wave are most sensitive to bonding effects at a level of 25% for moderately thick samples of 20-25 nm. This relatively large thickness is due to dynamical amplification of bonding contrast arising from partial de-channeling of 1s states.

Structure and morphology of hydroxylated nickel oxide (111) surfaces

We report an experimental and theoretical analysis of the sqrt(3)x sqrt(3)-R30 and 2x2 reconstructions on the NiO (111) surface combining transmission electron microscopy, x-ray photoelectron spectroscopy, and reasonably accurate density functional calculations using the meta-GGA hybrid functional TPSSh. While the main focus here is on the surface structure, we also observe an unusual step morphology with terraces containing only even numbers of unit cells during annealing of the surfaces. The experimental data clearly shows that the surfaces contain significant coverage of hydroxyl terminations, and the surface structures are essentially the same as those reported on the MgO (111) surface implying an identical kinetically-limited water-driven structural transition pathway. The octapole structure can therefore be all but ruled out for single crystals of NiO annealed in or transported through humid air. . The theoretical analysis indicates, as expected, that simple density functional theory methods for such strongly-correlated oxide surfaces are marginal, while better consideration of the metal d-electrons has a large effect although, it is still not perfect.

Charge Density Refinement of the Si (111) 7x7 Surface

We report an experimental refinement of the local charge density at the Si (111) 7x7 surface utilizing a combination of x-ray and high energy electron diffraction. By perturbing about a bond-centered pseudoatom model, we find experimentally that the adatoms are in an anti-bonding state with the atoms directly below. We are also able to experimentally refine a charge transfer of 0.26(4) e- from each adatom site to the underlying layers. These results are compared with a full-potential all-electron density functional DFT calculation.