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Register a new userAtomic and Electronic Structure of Si Dangling Bonds in Quasi-Free-Standing Monolayer Graphene
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Si dangling bonds without H termination at the interface of quasi-free standing monolayer graphene (QFMLG) are known scattering centers that can severely affect carrier mobility. In this report, we study the atomic and electronic structure of Si dangling bonds in QFMLG using low-temperature scanning tunneling microscopy/spectroscopy (STM/STS), atomic force microscopy (AFM), and density functional theory (DFT) calculations. Two types of defects with different contrast were observed on a flat terrace by STM and AFM. Their STM contrast varies with bias voltage. In STS, they showed characteristic peaks at different energies, 1.1 and 1.4 eV. Comparison with DFT calculations indicates that they correspond to clusters of 3 and 4 Si dangling bonds, respectively. The relevance of these results for the optimization of graphene synthesis is discussed.
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With considering the great success of scanning tunnelling microscopy (STM) studies of graphene in the past few years, it is quite surprising to notice that there is still a fundamental contradiction about the reported tunnelling spectra of quasi-free-standing graphene monolayer. Many groups observed V-shape spectra with linearly vanishing density-of-state (DOS) at the Dirac point, whereas, the others reported spectra with a gap of 60 meV pinned to the Fermi level in the quasi-free-standing graphene monolayer. Here we systematically studied the two contradicted tunnelling spectra of the quasi-free-standing graphene monolayer on several different substrates and provided a consistent interpretation about the result. The gap in the spectra arises from the out-of-plane phonons in graphene, which mix the Dirac electrons at the Brillouin zone corners with the nearly free-electron states at the zone center. Our experiment indicated that interactions with substrates could effectively suppress effects of the out-of-plane phonons in graphene and enable us to detect only the DOS of the Dirac electrons in the spectra. We also show that it is possible to switch on and off the out-of-plane phonons of graphene at the nanoscale, i.e., the tunnelling spectra show switching between the two distinct features, through voltage pulses applied to the STM tip.
We present a study of quasi-free-standing monolayer graphene obtained by intercalation of Au atoms at the interface between the carbon buffer layer (Bu-L) and the silicon-terminated face (0001) of 4H-silicon carbide. Au intercalation is achieved by deposition of atomically thin Au on the Bu-L followed by annealing at 850 {deg}C in an Argon atmosphere. We explore the intercalation of Au and decoupling of the Bu-L into quasi-free-standing monolayer graphene by surface science characterizations and electron transport in top-gated electronic devices. By gate-dependent magnetotransport we find that the Au-intercalated buffer layer displays all properties of monolayer graphene, namely gate tunable ambipolar transport across the Dirac point, and n- or p-type doping depending on the Au content.
Bulk amorphous materials have been studied extensively and are widely used, yet their atomic arrangement remains an open issue. Although they are generally believed to be Zachariasen continuous random networks, recent experimental evidence favours the competing crystallite model in the case of amorphous silicon. In two-dimensional materials, however, the corresponding questions remain unanswered. Here we report the synthesis, by laser-assisted chemical vapour deposition, of centimetre-scale, free-standing, continuous and stable monolayer amorphous carbon, topologically distinct from disordered graphene. Unlike in bulk materials, the structure of monolayer amorphous carbon can be determined by atomic-resolution imaging. Extensive characterization by Raman and X-ray spectroscopy and transmission electron microscopy reveals the complete absence of long-range periodicity and a threefold-coordinated structure with a wide distribution of bond lengths, bond angles, and five-, six-, seven- and eight-member rings. The ring distribution is not a Zachariasen continuous random network, but resembles the competing (nano)crystallite model. We construct a corresponding model that enables density-functional-theory calculations of the properties of monolayer amorphous carbon, in accordance with observations. Direct measurements confirm that it is insulating, with resistivity values similar to those of boron nitride grown by chemical vapour deposition. Free-standing monolayer amorphous carbon is surprisingly stable and deforms to a high breaking strength, without crack propagation from the point of fracture. The excellent physical properties of this stable, free-standing monolayer amorphous carbon could prove useful for permeation and diffusion barriers in applications such as magnetic recording devices and flexible electronics.
By means of first-principles density functional theory calculations, we find that hydrogen-passivated ultrathin silicon nanowires (SiNWs) along [100] direction with symmetrical multiple surface dangling bonds (SDBs) and boron doping can have a half-metallic ground state with 100% spin polarization, where the half-metallicity is shown quite robust against external electric fields. Under the circumstances with various SDBs, the H-passivated SiNWs can also be ferromagnetic or antiferromagnetic semiconductors. The present study not only offers a possible route to engineer half-metallic SiNWs without containing magnetic atoms but also sheds light on manipulating spin-dependent properties of nanowires through surface passivation.
We investigate the morphology of quasi-free-standing monolayer graphene (QFMLG) formed at several temperatures by hydrogen intercalation and discuss its relationship with transport properties. Features corresponding to incomplete hydrogen intercalation at the graphene-substrate interface are observed by scanning tunneling microscopy on QFMLG formed at 600 and 800{deg}C. They contribute to carrier scattering as charged impurities. Voids in the SiC substrate and wrinkling of graphene appear at 1000{deg}C, and they decrease the carrier mobility significantly.
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