Publications by authors named "Walt A de Heer"

Semiconducting graphene plays an important part in graphene nanoelectronics because of the lack of an intrinsic bandgap in graphene. In the past two decades, attempts to modify the bandgap either by quantum confinement or by chemical functionalization failed to produce viable semiconducting graphene. Here we demonstrate that semiconducting epigraphene (SEG) on single-crystal silicon carbide substrates has a band gap of 0.

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Graphene's original promise to succeed silicon faltered due to pervasive edge disorder in lithographically patterned deposited graphene and the lack of a new electronics paradigm. Here we demonstrate that the annealed edges in conventionally patterned graphene epitaxially grown on a silicon carbide substrate (epigraphene) are stabilized by the substrate and support a protected edge state. The edge state has a mean free path that is greater than 50 microns, 5000 times greater than the bulk states and involves a theoretically unexpected Majorana-like zero-energy non-degenerate quasiparticle that does not produce a Hall voltage.

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A cryogenic beam apparatus for studying neutral clusters has been built and tested. The lowest beam temperature reaches less than 9 K at a repetition rate of 20 Hz. Mechanical decoupling from the refrigerator avoids misalignment during temperature ramping.

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The realization of high-performance nanoelectronics requires control of materials at the nanoscale. Methods to produce high quality epitaxial graphene (EG) nanostructures on silicon carbide are known. The next step is to grow van der Waals semiconductors on top of EG nanostructures.

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The recent observation of non-classical electron transport regimes in two-dimensional materials has called for new high-resolution non-invasive techniques to locally probe electronic properties. We introduce a novel hybrid scanning probe technique to map the local resistance and electrochemical potential with nm- and μV resolution, and we apply it to study epigraphene nanoribbons grown on the sidewalls of SiC substrate steps. Remarkably, the potential drop is non-uniform along the ribbons, and μm-long segments show no potential variation with distance.

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The ultrafast dynamics of hot carriers in graphene are key to both understanding of fundamental carrier-carrier interactions and carrier-phonon relaxation processes in two-dimensional materials, and understanding of the physics underlying novel high-speed electronic and optoelectronic devices. Many recent experiments on hot carriers using terahertz spectroscopy and related techniques have interpreted the variety of observed signals within phenomenological frameworks, and sometimes invoke extrinsic effects such as disorder. Here, we present an integrated experimental and theoretical programme, using ultrafast time-resolved terahertz spectroscopy combined with microscopic modelling, to systematically investigate the hot-carrier dynamics in a wide array of graphene samples having varying amounts of disorder and with either high or low doping levels.

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In van der Waals bonded or rotationally disordered multilayer stacks of two-dimensional (2D) materials, the electronic states remain tightly confined within individual 2D layers. As a result, electron-phonon interactions occur primarily within layers and interlayer electrical conductivities are low. In addition, strong covalent in-plane intralayer bonding combined with weak van der Waals interlayer bonding results in weak phonon-mediated thermal coupling between the layers.

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Graphene nanoribbons grown on sidewall facets of SiC have demonstrated exceptional quantized ballistic transport up to 15 μm at room temperature. Angular-resolved photoemission spectroscopy (ARPES) has shown that the ribbons have the band structure of charge neutral graphene, while bent regions of the ribbon develop a bandgap. We present scanning tunneling microscopy and transmission electron microscopy of armchair nanoribbons grown on recrystallized sidewall trenches etched in SiC.

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Simultaneous magnetic and electric deflection measurements of rhodium clusters (Rh(N), 6 ≤ N ≤ 40) reveal ferromagnetism and ferroelectricity at low temperatures, while neither property exists in the bulk metal. Temperature-independent magnetic moments (up to 1 μ(B) per atom) are observed, and superparamagnetic blocking temperatures up to 20 K. Ferroelectric dipole moments on the order of 1D with transition temperatures up to 30 K are observed.

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A purely planar graphene/SiC field effect transistor is presented here. The horizontal current flow over one-dimensional tunneling barrier between planar graphene contact and coplanar two-dimensional SiC channel exhibits superior on/off ratio compared to conventional transistors employing vertical electron transport. Multilayer epitaxial graphene (MEG) grown on SiC(0001̅) was adopted as the transistor source and drain.

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Graphene nanoribbons will be essential components in future graphene nanoelectronics. However, in typical nanoribbons produced from lithographically patterned exfoliated graphene, the charge carriers travel only about ten nanometres between scattering events, resulting in minimum sheet resistances of about one kilohm per square. Here we show that 40-nanometre-wide graphene nanoribbons epitaxially grown on silicon carbide are single-channel room-temperature ballistic conductors on a length scale greater than ten micrometres, which is similar to the performance of metallic carbon nanotubes.

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Carbon-based magnetic materials and structures of mesoscopic dimensions may offer unique opportunities for future nanomagnetoelectronic/spintronic devices. To achieve their potential, carbon nanosystems must have controllable magnetic properties. We demonstrate that nitrophenyl functionalized graphene can act as a room-temperature 2D magnet.

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The maximum oscillation frequency (fmax) quantifies the practical upper bound for useful circuit operation. We report here an fmax of 70 GHz in transistors using epitaxial graphene grown on the C-face of SiC. This is a significant improvement over Si-face epitaxial graphene used in the prior high-frequency transistor studies, exemplifying the superior electronics potential of C-face epitaxial graphene.

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Despite theoretical predictions, the question of room-temperature magnetic order in graphene must be conclusively resolved before graphene can fully achieve its potential as a spintronic medium. Through scanning tunneling microscopy (STM) and point I-V measurements, the current study reveals that unlike pristine samples, graphene nanostructures, when functionalized with aryl radicals, can sustain magnetic order. STM images show 1-D and 2-D periodic super-lattices originating from the functionalization of a single sub-lattice of the bipartite graphene structure.

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After the pioneering investigations into graphene-based electronics at Georgia Tech, great strides have been made developing epitaxial graphene on silicon carbide (EG) as a new electronic material. EG has not only demonstrated its potential for large scale applications, it also has become an important material for fundamental two-dimensional electron gas physics. It was long known that graphene mono and multilayers grow on SiC crystals at high temperatures in ultrahigh vacuum.

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Homonuclear cobalt and iron clusters Co(N) and Fe(N) measured in a cryogenic molecular beam exist in two states with distinct magnetic moments (μ), polarizabilities, and ionization potentials, indicating distinct valences. The μ is approximately quantized: μ(N)∼2Nμ(B) in the ground states and μ(N)(*)∼Nμ(B) in the excited states for Co; μ(N)∼3Nμ(B) and μ(N)(*)∼Nμ(B) for Fe. At a large size, the average μ of the two states converges to the bulk value with diminishing ionization potential differences.

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Graphene's extraordinary physical properties and its planar geometry make it an ideal candidate for a wide array of applications, many of which require controlled chemical modification and the spatial organization of molecules on its surface. In particular, the ability to functionalize and micropattern graphene with proteins is relevant to bioscience applications such as biomolecular sensors, single-cell sensors, and tissue engineering. We report a general strategy for the noncovalent chemical modification of epitaxial graphene for protein immobilization and micropatterning.

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Electrons in a single sheet of graphene behave quite differently from those in traditional two-dimensional electron systems. Like massless relativistic particles, they have linear dispersion and chiral eigenstates. Furthermore, two sets of electrons centred at different points in reciprocal space ('valleys') have this dispersion, giving rise to valley degeneracy.

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In order to engineer a band gap into graphene, covalent bond-forming reactions can be used to change the hybridization of the graphitic atoms from sp(2) to sp(3), thereby modifying the conjugation length of the delocalized carbon lattice; similar side-wall chemistry has been shown to introduce a band gap into metallic single-walled carbon nanotubes. Here we demonstrate that the application of such covalent bond-forming chemistry modifies the periodicity of the graphene network thereby introducing a band gap (∼0.4 eV), which is observable in the angle-resolved photoelectron spectroscopy of aryl-functionalized graphene.

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The substrate-induced charge-density profile in carbon face epitaxial graphene is determined using nondegenerate ultrafast midinfrared pump-probe spectroscopy. Distinct zero crossings in the differential transmission spectra are used to identify the Fermi levels of layers within the multilayer stack. Probing within the transmission window of the SiC substrate, we find the Fermi levels of the first four heavily doped layers to be, respectively, 360, 215, 140, and 93 meV above the Dirac point.

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We report generation of ballistic electric currents in unbiased epitaxial graphene at 300 K via quantum interference between phase-controlled cross-polarized fundamental and second harmonic 220 fs pulses. The transient currents are detected via the emitted terahertz radiation. Because of graphene's special structure symmetry, the injected current direction can be well controlled by the polarization of the pump beam in epitaxial graphene.

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Application of a magnetic field to conductors causes the charge carriers to circulate in cyclotron orbits with quantized energies called Landau levels (LLs). These are equally spaced in normal metals and two-dimensional electron gases. In graphene, however, the charge carrier velocity is independent of their energy (like massless photons).

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The addition of nitrophenyl groups to the surface of few-layer epitaxial graphene (EG) by the formation of covalent carbon-carbon bonds changed the electronic structure and transport properties of the EG from near-metallic to semiconducting.

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