Daniel Waldmann

Towards wafer-size graphene layers by atmospheric pressure graphitization of silicon carbide

Graphene, a single monolayer of graphite, has recently attracted considerable interest owing to its novel magneto-transport properties, high carrier mobility and ballistic transport up to room temperature. It has the potential for technological applications as a successor of silicon in the post Moores law era, as a single-molecule gas sensor, in spintronics, in quantum computing or as a terahertz oscillator. For such applications, uniform ordered growth of graphene on an insulating substrate is necessary. The growth of graphene on insulating silicon carbide (SiC) surfaces by high-temperature annealing in vacuum was previously proposed to open a route for large-scale production of graphene-based devices. However, vacuum decomposition of SiC yields graphene layers with small grains (30-200 nm; refs 14-16). Here, we show that the ex situ graphitization of Si-terminated SiC(0001) in an argon atmosphere of about 1 bar produces monolayer graphene films with much larger domain sizes than previously attainable. Raman spectroscopy and Hall measurements confirm the improved quality of the films thus obtained. High electronic mobilities were found, which reach mu=2,000 cm (2) V(-1) s(-1) at T=27 K. The new growth process introduced here establishes a method for the synthesis of graphene films on a technologically viable basis.

The quasi-free-standing nature of graphene on H-saturated SiC(0001)

We report on an investigation of quasi-free-standing graphene on 6H-SiC(0001) which was prepared by intercalation of hydrogen under the buffer layer. Using infrared absorption spectroscopy, we prove that the SiC(0001) surface is saturated with hydrogen. Raman spectra demonstrate the conversion of the buffer layer into graphene which exhibits a slight tensile strain and short range defects. The layers are hole doped (p = 5.0 − 6.5 × 1012 cm−2) with a carrier mobility of 3100 cm2/Vs at room temperature. Compared to graphene on the buffer layer, a strongly reduced temperature dependence of the mobility is observed for graphene on H-terminated SiC(0001) which justifies the term “quasi-free-standing.”

Quantum oscillations and quantum Hall effect in epitaxial graphene

Johannes Jobst, Daniel Waldmann, Florian Speck, Roland Hirner, Duncan K. Maude, Thomas Seyller, and Heiko B. Weber ∗ Lehrstuhl für Angewandte Physik, Universität Erlangen-Nürnberg, 91056 Erlangen, Germany Lehrstuhl für Technische Physik, Universität Erlangen-Nürnberg, 91056 Erlangen, Germany Laboratoire des Champs Magnétiques Intenses, 25 Avenue des Martyrs, 38042 Grenoble,France (Dated: August 14, 2009)

Dislocations in bilayer graphene

Dislocations represent one of the most fascinating and fundamental concepts in materials science. Most importantly, dislocations are the main carriers of plastic deformation in crystalline materials. Furthermore, they can strongly affect the local electronic and optical properties of semiconductors and ionic crystals. In materials with small dimensions, they experience extensive image forces, which attract them to the surface to release strain energy. However, in layered crystals such as graphite, dislocation movement is mainly restricted to the basal plane. Thus, the dislocations cannot escape, enabling their confinement in crystals as thin as only two monolayers. To explore the nature of dislocations under such extreme boundary conditions, the material of choice is bilayer graphene, the thinnest possible quasi-two-dimensional crystal in which such linear defects can be confined. Homogeneous and robust graphene membranes derived from high-quality epitaxial graphene on silicon carbide provide an ideal platform for their investigation. Here we report the direct observation of basal-plane dislocations in freestanding bilayer graphene using transmission electron microscopy and their detailed investigation by diffraction contrast analysis and atomistic simulations. Our investigation reveals two striking size effects. First, the absence of stacking-fault energy, a unique property of bilayer graphene, leads to a characteristic dislocation pattern that corresponds to an alternating AB  AC change of the stacking order. Second, our experiments in combination with atomistic simulations reveal a pronounced buckling of the bilayer graphene membrane that results directly from accommodation of strain. In fact, the buckling changes the strain state of the bilayer graphene and is of key importance for its electronic properties. Our findings will contribute to the understanding of dislocations and of their role in the structural, mechanical and electronic properties of bilayer and few-layer graphene.

Tailoring the graphene/silicon carbide interface for monolithic wafer-scale electronics

Graphene is an outstanding electronic material, predicted to have a role in post-silicon electronics. However, owing to the absence of an electronic bandgap, graphene switching devices with high on/off ratio are still lacking. Here in the search for a comprehensive concept for wafer-scale graphene electronics, we present a monolithic transistor that uses the entire material system epitaxial graphene on silicon carbide (0001). This system consists of the graphene layer with its vanishing energy gap, the underlying semiconductor and their common interface. The graphene/semiconductor interfaces are tailor-made for ohmic as well as for Schottky contacts side-by-side on the same chip. We demonstrate normally on and normally off operation of a single transistor with on/off ratios exceeding 10(4) and no damping at megahertz frequencies. In its simplest realization, the fabrication process requires only one lithography step to build transistors, diodes, resistors and eventually integrated circuits without the need of metallic interconnects.

Bottom-gated epitaxial graphene

High-quality epitaxial graphene on silicon carbide (SiC) is today available in wafer size. Similar to exfoliated graphene, its charge carriers are governed by the Dirac-Weyl Hamiltonian and it shows excellent mobilities. For many experiments with graphene, in particular for surface science, a bottom gate is desirable. Commonly, exfoliated graphene flakes are placed on an oxidized silicon wafer that readily provides a bottom gate. However, this cannot be applied to epitaxial graphene as the SiC provides the source material out of which graphene grows. Here, we present a reliable scheme for the fabrication of bottom-gated epitaxial graphene devices, which is based on nitrogen (N) implantation into a SiC wafer and subsequent graphene growth. We demonstrate working devices in a broad temperature range from 6 to 300  K. Two gating regimes can be addressed, which opens a wide engineering space for tailored devices by controlling the doping of the gate structure.

Electron-electron interaction in the magnetoresistance of graphene

We investigate the magnetotransport in large area graphene Hall bars epitaxially grown on silicon carbide. In the intermediate field regime between weak localization and Landau quantization, the observed temperature-dependent parabolic magnetoresistivity is a manifestation of the electron-electron interaction. We can consistently describe the data with a model for diffusive (magneto)transport that also includes magnetic-field-dependent effects originating from ballistic time scales. We find an excellent agreement between the experimentally observed temperature dependence of magnetoresistivity and the theory of electron-electron interaction in the diffusive regime. We can further assign a temperature-driven crossover to the reduction of the multiplet modes contributing to electron-electron interaction from 7 to 3 due to intervalley scattering. In addition, we find a temperature-independent ballistic contribution to the magnetoresistivity in classically strong magnetic fields.

Quasi-freestanding Graphene on SiC(0001)

We report on a comprehensive study of the properties of quasi-freestanding monolayer and bilayer graphene produced by conversion of the (6√3×6√3)R30° reconstruction into graphene via intercalation of hydrogen. The conversion is confirmed by photoelectron spectroscopy and Raman spectroscopy. By using infrared absorption spectroscopy we show that the underlying SiC(0001) surface is terminated by hydrogen in the form of Si-H bonds. Using Hall effect measurements we have determined the carrier concentration and type as well as the mobility which lies well above 1000 cm2/Vs despite a significant amount of short range scatterers detected by Raman spectroscopy.

Current annealing and electrical breakdown of epitaxial graphene

We report on epitaxial graphene on silicon carbide at high current densities. We observe two distinguished regimes, and a final breakdown. First for low current densities the conductance is enhanced due to desorption of adsorbates. Second with increasing bias the sample locally starts to glow and is strongly heated. The silicon carbide material decomposes, graphitic material is formed and thus additional current paths are created. The graphene layer breaks down, which is, however, not visible in high bias data. The final breakdown is a self-amplifying process resulting in a locally destroyed sample but surprisingly with better conductance than the original sample.

Robust graphene membranes in a silicon carbide frame.

We present a fabrication process for freely suspended membranes consisting of bi- and trilayer graphene grown on silicon carbide. The procedure, involving photoelectrochemical etching, enables the simultaneous fabrication of hundreds of arbitrarily shaped membranes with an area up to 500 μm(2) and a yield of around 90%. Micro-Raman and atomic force microscopy measurements confirm that the graphene layer withstands the electrochemical etching and show that the membranes are virtually unstrained. The process delivers membranes with a cleanliness suited for high-resolution transmission electron microscopy (HRTEM) at atomic scale. The membrane, and its frame, is very robust with respect to thermal cycling above 1000 °C as well as harsh acidic or alkaline treatment.