Katsuya Iwaya

Bottom-Up Graphene-Nanoribbon Fabrication Reveals Chiral Edges and Enantioselectivity

We produce precise chiral-edge graphene nanoribbons on Cu{111} using self-assembly and surface-directed chemical reactions. We show that, using specific properties of the substrate, we can change the edge conformation of the nanoribbons, segregate their adsorption chiralities, and restrict their growth directions at low surface coverage. By elucidating the molecular-assembly mechanism, we demonstrate that our method constitutes an alternative bottom-up strategy toward synthesizing defect-free zigzag-edge graphene nanoribbons.

Ca intercalated bilayer graphene as a thinnest limit of superconducting C6Ca

Success in isolating a 2D graphene sheet from bulky graphite has triggered intensive studies of its physical properties as well as its application in devices. Graphite intercalation compounds (GICs) have provided a platform of exotic quantum phenomena such as superconductivity, but it is unclear whether such intercalation is feasible in the thinnest 2D limit (i.e., bilayer graphene). Here we report a unique experimental realization of 2D GIC, by fabricating calcium-intercalated bilayer graphene C6CaC6 on silicon carbide. We have investigated the structure and electronic states by scanning tunneling microscopy and angle-resolved photoemission spectroscopy. We observed a free-electron–like interlayer band at the Brillouin-zone center, which is thought to be responsible for the superconductivity in 3D GICs, in addition to a large π* Fermi surface at the zone boundary. The present success in fabricating Ca-intercalated bilayer graphene would open a promising route to search for other 2D superconductors as well as to explore its application in devices.

Imaging Nanoscale Electronic Inhomogeneity in the Lightly Doped Mott Insulator Ca~2~-~xNa~xCuO~2Cl~2

The spatial variation of electronic states was imaged in the lightly doped Mott insulator Ca(2-x)NaxCuO2Cl2 using scanning tunneling microscopy or spectroscopy. We observed nanoscale domains with a high local density of states within an insulating background. The observed domains have a characteristic length scale of 2 nm (approximately 4-5a, a: lattice constant) with preferred orientations along the tetragonal [100] direction. We argue that such spatially inhomogeneous electronic states are inherent to slightly doped Mott insulators and play an important role for the insulator to metal transition.

Systematic analyses of vibration noise of a vibration isolation system for high-resolution scanning tunneling microscopes

We designed and constructed an effective vibration isolation system for stable scanning tunneling microscopy measurements using a separate foundation and two vibration isolation stages (i.e., a combination of passive and active vibration isolation dampers). Systematic analyses of vibration data along the horizontal and vertical directions are present, including the vibration transfer functions of each stage and the overall vibration isolation system. To demonstrate the performance of the system, tunneling current noise measurements are conducted with and without the vibration isolation. Combining passive and active vibration isolation dampers successfully removes most of the vibration noise in the tunneling current up to 100 Hz. These comprehensive vibration noise data, along with details of the entire system, can be used to establish a clear guideline for building an effective vibration isolation system for various scanning probe microscopes and electron microscopes.

Atomic-Scale Visualization of Initial Growth of Homoepitaxial SrTiO3 Thin Film on an Atomically Ordered Substrate

The initial homoepitaxial growth of SrTiO(3) on a (√13 × √13)-R33.7° SrTiO(3)(001) substrate surface, which can be prepared under oxide growth conditions, is atomically resolved by scanning tunneling microscopy. The identical (√13 × √13) atomic structure is clearly visualized on the deposited SrTiO(3) film surface as well as on the substrate. This result indicates the transfer of the topmost Ti-rich (√13 × √13) structure to the film surface and atomic-scale coherent epitaxy at the film/substrate interface. Such atomically ordered SrTiO(3) substrates can be applied to the fabrication of atom-by-atom controlled oxide epitaxial films and heterostructures.

Thickness-dependent local surface electronic structures of homoepitaxial SrTiO3 thin films

We have investigated the atomically-resolved substrate and homoepitaxial thin film surfaces of SrTiO3(001) using low-temperature scanning tunneling microscopy/scanning tunneling spectroscopy (STS) combined with pulsed laser deposition. It was found that a typical annealing treatment for preparation of SrTiO3 substrates, unexpectedly, resulted in a disordered surface on an atomic scale. In contrast, homoepitaxial SrTiO3 thin films grown on this disordered substrate exhibited a (2×2) surface reconstruction. The STS measurements revealed a number of surface defects in a 10 unit cell thick SrTiO3 film but much fewer in a 50 unit cell thick film, indicating nonuniform stoichiometry along the growth direction. These results suggest the possibility of using homoepitaxial SrTiO3 film surfaces as idealized substrates, opening a way to extract novel functionalities in complex oxides heterostructures.

Effect of oxygen deficiency on SrTiO3(001) surface reconstructions

The contribution of oxygen deficiencies to SrTiO3(001) surface reconstructions is studied using low-energy electron diffraction and scanning tunneling microscopy. We have prepared a SrTiO3 sample with spatially graded oxygen deficiencies, in which R33.7°-(13×13), (2×1), and R26.6°-(5×5) surface reconstructions are observed while increasing the amount of oxygen deficiencies. This indicates that oxygen nonstoichiometry has an influence on the formation of various surface reconstructions as one of the important factors. This concept is also applicable to other transition metal oxides to prepare atomically ordered surfaces in a reproducible manner.

Atomically Resolved Surface Structure of SrTiO3(001) Thin Films Grown in Step-Flow Mode by Pulsed Laser Deposition

The surface structure of SrTiO3(001) thin films homoepitaxially grown in step-flow mode by pulsed laser deposition was characterized using scanning tunneling microscopy. One-dimensional (1D) TiOx-based nanostructures were formed on the surface, and their density increased with increasing film thickness. Most of the 1D nanostructures disappeared after post-deposition annealing, and the resulting surface exhibited a domain structure with (2×1) and (1×2) reconstructions and fewer oxygen vacancies. These results imply that the step-flow growth is likely to produce a TiOx-rich surface and Ti deficiencies in the film, and that annealing can effectively reduce the density of atomic defects.

Visualizing Atomistic Formation Process of SrOx Thin Films on SrTiO3

Metallic conductivity observed in the heterostructure of LaAlO3/SrTiO3 has attracted great attention, triggering a debate over whether the origin is an intrinsic electronic effect or a defect-related phenomenon. One of the issues to be solved is the role of SrO layer, which turns the conductive interface into an insulator when inserted between LaAlO3 and SrTiO3. To understand the origins of this oxide interface phenomenon and to further explore unconventional functionalities, it is necessary to elucidate how SrO layers are formed during the initial growth process at the atomic level. Here, we atomically resolve growth processes of heteroepitaxial SrOx films on SrTiO3(001)-(√13×√13)-R33.7° substrate using scanning tunneling microscopy/spectroscopy. On the sub-unit-cell SrOx film surface, no periodic structure was observed as a result of random Ti incorporation into the SrOx islands, indicating the importance of the control of excess Ti atoms on the substrate prior to deposition. This random arrangement of Ti atoms is a marked contrast to the homoepitaxy on SrTiO3(001)-(√13×√13)-R33.7°. Furthermore, the formation of SrOx islands introduced defects in the surrounding SrTiO3 substrate surface. Such atom-by-atom engineering and characterizations of oxide heterostructures not only provide microscopic understanding of formation process of interfaces in metal-oxides, but also would lead to the creation of exotic electronic phenomena and novel functionalities at these interfaces.

Atomically resolved silicon donor states of β-Ga2O3

The electronic states of silicon donors in a wide gap semiconductor, β-Ga2O3(100), have been studied using low-temperature scanning tunneling microscopy. We observe one-dimensional rows along [010], as expected from the crystal structure. In addition, substitutional Si donors are identified up to the fourth subsurface layer with clear spectroscopic features at the bottom of the conduction band. The decay length of each subsurface Si donor is systematically measured, and reasonably agrees with a picture of the Si donor in bulk β-Ga2O3. These results strongly suggest that Si impurities are shallow donors and responsible for the high electrical conductivity of β-Ga2O3.