Jan Ingo Flege

Epitaxial graphene on ruthenium

Graphene has been used to explore the fascinating electronic properties of ideal two-dimensional carbon, and shows great promise for quantum device architectures. The primary method for isolating graphene, micromechanical cleavage of graphite, is difficult to scale up for applications. Epitaxial growth is an attractive alternative, but achieving large graphene domains with uniform thickness remains a challenge, and substrate bonding may strongly affect the electronic properties of epitaxial graphene layers. Here, we show that epitaxy on Ru(0001) produces arrays of macroscopic single-crystalline graphene domains in a controlled, layer-by-layer fashion. Whereas the first graphene layer indeed interacts strongly with the metal substrate, the second layer is almost completely detached, shows weak electronic coupling to the metal, and hence retains the inherent electronic structure of graphene. Our findings demonstrate a route towards rational graphene synthesis on transition-metal templates for applications in electronics, sensing or catalysis.

Growth mode and oxidation state analysis of individual cerium oxide islands on Ru(0001)

The growth of cerium oxide on Ru(0001) by reactive molecular beam epitaxy has been investigated using low-energy electron microscopy (LEEM) and diffraction as well as local valence band photoemission. The oxide islands are found to adopt a carpet-like growth mode, which depending on the local substrate morphology and misorientation leads to deviations from the otherwise almost perfect equilateral shape at a growth temperature of 850 °C. Furthermore, although even at this high growth temperature the micron-sized CeO₂(111) islands are found to exhibit different lattice registries with respect to the hexagonal substrate, the combination of dark-field LEEM and local intensity-voltage analysis reveals that the oxidation state of the islands is homogeneous down to the 10 nm scale.

Ultrathin, epitaxial cerium dioxide on silicon

It is shown that ultrathin, highly ordered, continuous films of cerium dioxide may be prepared on silicon following substrate prepassivation using an atomic layer of chlorine. The as-deposited, few-nanometer-thin Ce2O3 film may very effectively be converted at room temperature to almost fully oxidized CeO2 by simple exposure to air, as demonstrated by hard X-ray photoemission spectroscopy and X-ray diffraction. This post-oxidation process essentially results in a negligible loss in film crystallinity and interface abruptness.

Self-organized 2D nanopatterns after low-coverage Ga adsorption on Si (1 1 1)

The evolution of the Si(1 1 1) surface after submonolayer deposition of Ga has been observed in situ by low-energy electron microscopy and scanning tunnelling microscopy. A phase separation of Ga-terminated -R 30° reconstructed areas and bare Si(1 1 1)-7 × 7 regions leads to the formation of a two-dimensional nanopattern. The shape of this pattern can be controlled by the choice of the surface miscut direction, which is explained in terms of the anisotropy of the domain boundary line energy and a high kink-formation energy. A general scheme for the nanopattern formation, based on intrinsic properties of the Si(1 1 1) surface, is presented. Experiments performed with In instead of Ga support this scheme.

Surface resonances in electron reflection from overlayers

Electron scattering by oxygen monolayers on the Ru(0 0 0 1) surface is studied both experimentally and theoretically. Sharp transmission resonances at low energies are revealed and established to originate from critical points of a special kind in the complex band structure of the substrate. Electron reflection from the clean and oxidized Ru(0 0 0 1) is measured for kinetic energies up to 40 eV at normal incidence for oxygen coverages of 1/4, 1/2, 3/4, and one monolayer. The reflection spectra R(E) are analyzed using a Bloch-waves based ab initio scattering theory. In addition to the substrate-induced resonances the reconstructed (2 × 1) and (2 × 2) surfaces show surface resonances due to pre-emergent secondary diffraction beams. The R(E) spectra are shown to give unambiguous evidence of the hcp stacking of the oxygen layer.

Nanoscale Origin of Mesoscale Roughening: Real-Time Tracking and Identification of Three Distinct Ruthenium Oxide Phases in Ruthenium Oxidation

The structural modification of the Ru(0001) surface is followed in real-time using low-energy electron microscopy at elevated temperatures during exposure to molecular oxygen. We observe the nucleation and growth of three different RuO2 facets, which are unambiguously identified by single-domain microspot low-energy electron diffraction (μLEED) analysis from regions of 250 nm in diameter. Structural identification is then pushed to the true nanoscale by employing very-low-energy electron reflectivity spectra R(E) from regions down to 10 nm for structural fingerprinting of complex reactions such as the oxidation of metal surfaces. Calculations of R(E) with an ab initio scattering theory confirm the growth of (110), (100), and (101) orientations of RuO2 and explain the shape of the R(E) spectra in terms of the conducting band structure. This methodology is ideally suited to identify the structure of supported ultrathin films and dynamic transformations at multicomponent interfaces down to few nanometer lateral resolution at elevated temperature and in reactive environments.

Ultra-thin high-quality silicon nitride films on Si(111)

Ultra-thin silicon nitride films grown by exposure of Si(111) substrates to a flux of atomic nitrogen at temperatures between 700 °C and 1050 °C have been investigated by means of X-ray spectromicroscopy, atomic force microscopy, X-ray reflectivity, and X-ray photoemission spectroscopy. The films show a Si3N4 stoichiometry. For reactive nitride growth at temperatures below 800 °C, a smooth surface and interface morphology is found. Higher temperatures lead to the formation of rough films with holes and grooves of increasing size, approaching a lateral size of several hundred nanometers for growth temperatures above 900 °C. Nonetheless, X-ray spectromicroscopy shows that the bottom of the holes consists of Si3N4.

Surface Evolution of 4H-SiC(0001) during In Situ Surface Preparation and its Influence on Graphene Properties

The evolution of SiC surface morphology during graphene growth process has been studied through the comparison of substrate surface step structure after in-situ etching and graphene growth in vacuum. Influence of in-situ substrate surface preparation on the properties of graphene was studied through the comparison of graphene layers on etched and un-etched substrates grown under same conditions.

Improved epitaxy of ultrathin praseodymia films on chlorine passivated Si(111) reducing silicate interface formation

Ultrathin praseodymia films have been deposited on both Cl-passivated and nonpassivated Si(111) substrates by molecular beam epitaxy. Comparative studies on the crystallinity and stoichiometry are performed by x-ray photoelectron spectroscopy, x-ray standing waves, and x-ray reflectometry. On nonpassivated Si(111) an amorphous silicate film is formed. In contrast, praseodymia deposited on Cl-passivated Si(111) form a well-ordered crystalline film with cubic-Pr2O3 (bixbyite) structure. The vertical lattice constant of the praseodymia film is increased by 1.4% compared to the bulk value. Furthermore, the formation of an extended amorphous silicate interface layers is suppressed and confined to only one monolayer.

Cerium Oxide Epitaxial Nanostructures on Pt(111): Growth, Morphology and Structure

Cerium oxide in combination with metals is a very important material for catalysis. We present an in-depth characterization of the growth and morphology of cerium oxide in the form of an inverse model catalyst on Pt(111). Using state of the art low energy electron microscopy (LEEM) and microprobe low energy electron diffraction we provide a detailed in-situ insight into the nucleation and growth dynamics of this model system in different experimental conditions. By probing the unoccupied band structure of the sample during the growth process using intensity-voltage LEEM we also obtain information on the growth dynamics of the deposited ceria overlayer. The results represent an important basis in view of reactivity studies on well controlled ceria epitaxial systems.