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Self-organized gold chains on vicinal Si(111) surfaces represent prototype examples of quasi-one-dimensional objects that are stabilized by hybridization with Si surface states. Their plasmons contain important information about the unoccupied bandstructure close to the Fermi level. Using Si(775)-Au as an example, we report here the modifications of the plasmon dispersion by the simple atomic adatom species H and O. Using a combination of low energy electron diffraction and high-resolution electron energy loss spectroscopy, we study the interconnection between plasmonic excitation and the corresponding local surface structure. Both adsorbates do not destroy metallicity, but, similar to Si(553)-Au, atomic hydrogen enhances dimerization of the Au chains, which at small concentrations counteracts the disorder introduced by random adsorption. This effect, most likely caused by electron donation of H to the surface states, is missing in case of adsorbed oxygen, so that only the effect of disorder is observed. For both adsorbates increasing disorder as a function of adsorbate concentration finally results in plasmon localization and opening of a band gap.
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Graphene was shown to reveal intriguing properties of its relativistic two-dimensional electron gas; however, its implementation to microelectronic applications is missing to date. In this work, we present a comprehensive study of epitaxial graphene on technologically relevant and in a standard CMOS process achievable Ge(100) epilayers grown on Si(100) substrates. Crystalline graphene monolayer structures were grown by means of chemical vapor deposition (CVD). Using angle-resolved photoemission spectroscopy and in situ surface transport measurements, we demonstrate their metallic character both in momentum and real space. Despite numerous crystalline imperfections, e.g., grain boundaries and strong corrugation, as compared to epitaxial graphene on SiC(0001), charge carrier mobilities of 1 × 104 cm2/Vs were obtained at room temperature, which is a result of the quasi-charge neutrality within the graphene monolayers on germanium and not dependent on the presence of an interface oxide. The interface roughness due to the facet structure of the Ge(100) epilayer, formed during the CVD growth of graphene, can be reduced via subsequent in situ annealing up to 850 °C coming along with an increase in the mobility by 30%. The formation of a Ge(100)-(2 × 1) structure demonstrates the weak interaction and effective delamination of graphene from the Ge/Si(100) substrate.
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Improving the graphitic structure in carbon nanofibers (CNFs) is important for exploiting their potential in mechanical, electrical and electrochemical applications. Typically, the synthesis of carbon fibers with a highly graphitized structure demands a high temperature of almost 2500 °C. Furthermore, to achieve an improved graphitic structure, the stabilization of a precursor fiber has to be assisted by the presence of tension in order to enhance the molecular orientation. Keeping this in view, herein we report on the fabrication of graphene nanoplatelets (GNPs) doped carbon nanofibers using electrospinning followed by oxidative stabilization and carbonization. The effect of doping GNPs on the graphitic structure was investigated by carbonizing them at various temperatures (1000 °C, 1200 °C, 1500 °C and 1700 °C). Additionally, a stabilization was achieved with and without constant creep stress (only shrinkage stress) for both pristine and doped precursor nanofibers, which were eventually carbonized at 1700 °C. Our findings reveal that the GNPs doping results in improving the graphitic structure of polyacrylonitrile (PAN). Further, in addition to the templating effect during the nucleation and growth of graphitic crystals, the GNPs encapsulated in the PAN nanofiber matrix act in-situ as micro clamp units performing the anchoring function by preventing the loss of molecular orientation during the stabilization stage, when no external tension is applied to nanofiber mats. The templating effect of the entire graphitization process is reflected by an increased electrical conductivity along the fibers. Simultaneously, the electrical anisotropy is reduced, i.e., the GNPs provide effective pathways with improved conductivity acting like bridges between the nanofibers resulting in an improved conductivity across the fiber direction compared to the pristine PAN system.
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The low-energy plasmonic excitations of the Ge(0 0 1)-Au close to one monolayer coverage of Au were investigated by momentum-resolved high resolution electron energy loss spectroscopy. A very weak plasmonic loss was identified dispersing along the chain direction of the [Formula: see text] formed at these Au coverages. The measured dispersion was compared with the Tomonaga-Luttinger-liquid (TLL) model and with a model for an anisotropic Fermi liquid. Using the TLL model both for single and arrays of wires, no consistent picture turned up that could describe all available data. On the contrary, a quasi-one-dimensional model of a confined 2D electron gas gave a satisfactorily consistent description of the data. From these results for the collective low-energy excitations we conclude that the Ge(0 0 1)-Au system is reasonably well described by a strongly anisotropic 2D Fermi liquid, but is incompatible with a TLL.
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Electromigration (EM) as a structuring tool was investigated in Ag nanowires (width 300 nm, thickness 25 nm) and partly in notched and bow-tie Ag structures on a Si(1 0 0) substrate in ultra-high vacuum using a four-tip scanning tunneling microscope in combination with a scanning electron microscope. From simulations of Ag nanowires we got estimates of temperature profiles, current density profiles, EM and thermal migration (TM) mass flux distributions within the nanowire induced by critical current densities of 108 A cm-2. At room temperature, the electron wind force at these current densities by far dominates over thermal diffusion, and is responsible for formation of voids at the cathode and hillocks at the anode side. For current densities that exceed the critical current densities necessary for EM, a new type of wire-like structure formation was found both at room temperature and at 100 K for notched and bow-tie structures. This suggests that the simultaneous action of EM and TM is structure forming, but with a very small influence of TM at low temperature.
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We report on electronic transport measurements in rotational square probe configuration in combination with scanning tunneling potentiometry of epitaxial graphene monolayers which were fabricated by polymer-assisted sublimation growth on SiC substrates. The absence of bilayer graphene on the ultralow step edges of below 0.75 nm scrutinized by atomic force microscopy and scanning tunneling microscopy result in a not yet observed resistance isotropy of graphene on 4H- and 6H-SiC(0001) substrates as low as 2%. We combine microscopic electronic properties with nanoscale transport experiments and thereby disentangle the underlying microscopic scattering mechanism to explain the remaining resistance anisotropy. Eventually, this can be entirely attributed to the resistance and the number of substrate steps which induce local scattering. Thereby, our data represent the ultimate limit for resistance isotropy of epitaxial graphene on SiC for the given miscut of the substrate.
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The photocatalytic performance of MoO3 is limited due to its weak visible light absorption ability and quick recombination of charge carriers. In the present work, we report the facile synthesis of Fe(iii)-grafted MoO3 nanorods using a hydrothermal method followed by an impregnation technique with the aim of enhancing the light harvesting ability and photocatalytic efficiency of MoO3. The prepared samples were characterized through the standard analytical techniques of XRD, SEM-EDS, TEM, XPS, UV-Vis-DRS, FT-IR, TG-DTA and PL spectrophotometry. XPS and TEM analyses reveal that Fe(iii) ions are successfully grafted onto the surface of the MoO3 nanorod with intimate interfacial contact. The photocatalytic performances of the prepared samples were investigated by studying the degradation of methylene blue (MB), rhodamine B (RhB) and 4-nitrophenol (4-NP) under visible light irradiation. The surface-modified MoO3 with Fe(iii) ions showed excellent photocatalytic activity towards the degradation of the above-mentioned pollutants, where Fe(iii) ions act as effective cocatalytic sites to produce hydroxyl radicals through multi-electron reduction of oxygen molecules. The improved photocatalytic activity could be ascribed to the effective separation of charge carriers and efficient production of hydroxyl radicals via the rapid capture of electrons by Fe(iii) through a well-known photoinduced interfacial charge transfer mechanism. Based on scavenger analysis study, a mechanism for the enhanced photocatalytic activity has been discussed and proposed. The concept of surface grafting onto large bandgap semiconductors with ubiquitous elements opens up a new avenue for the development of visible-light-responsive photocatalysts with excellent photocatalytic activity.
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In addition to the chemical and physical properties of nanostructures their successful utilization for applications is strongly triggered by economic aspects. Electrospinning of nanowires from solution followed by subsequent annealing steps is a comparably cheap technique to fabricate conductive carbon nanofibers (CNF) made from polyacrylonitrile (PAN) molecules in large quantities. In this work, we investigated the microscopic properties of the CNFs with diameters of 100-300 nm by means of Raman and x-ray photoelectron spectroscopy and correlated these results with transport measurements done with a 4-tip STM. In particular, we investigated the effect of fiber alignment and knot densities, which can be controlled by applying constant creep due to stress during the stabilization process. The comparison of the conductivity obtained from single CNFs revealed further that the fiber crossings within the ensemble structure act as scattering centers and proofs that the transport is along the surfaces of the CNFs.
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The practical difficulties to use graphene in microelectronics and optoelectronics is that the available methods to grow graphene are not easily integrated in the mainstream technologies. A growth method that could overcome at least some of these problems is chemical vapour deposition (CVD) of graphene directly on semiconducting (Si or Ge) substrates. Here we report on the comparison of the CVD and molecular beam epitaxy (MBE) growth of graphene on the technologically relevant Ge(001)/Si(001) substrate from ethene (C2H4) precursor and describe the physical properties of the films as well as we discuss the surface reaction and diffusion processes that may be responsible for the observed behavior. Using nano angle resolved photoemission (nanoARPES) complemented by transport studies and Raman spectroscopy as well as density functional theory (DFT) calculations, we report the direct observation of massless Dirac particles in monolayer graphene, providing a comprehensive mapping of their low-hole doped Dirac electron bands. The micrometric graphene flakes are oriented along two predominant directions rotated by 30° with respect to each other. The growth mode is attributed to the mechanism when small graphene "molecules" nucleate on the Ge(001) surface and it is found that hydrogen plays a significant role in this process.
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The properties of one-dimensional (1D) plasmons are rather unexplored. We investigated the plasmonic collective excitations, measured as one-dimensional plasmon dispersions with electron energy loss spectroscopy, highly resolved both in energy and lateral momentum, for both phases of Au induced chains on stepped Si(553) substrates. We observe 1D dispersions that are strongly influenced by the lateral chain width and by the interchain coupling. Indications for the existence of two different plasmons originating from two surface bands of the systems are given for the low coverage phase.
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The electrical conductivity of solid-state matter is a fundamental physical property and can be precisely derived from the resistance measured via the four-point probe technique excluding contributions from parasitic contact resistances. Over time, this method has become an interdisciplinary characterization tool in materials science, semiconductor industries, geology, physics, etc, and is employed for both fundamental and application-driven research. However, the correct derivation of the conductivity is a demanding task which faces several difficulties, e.g. the homogeneity of the sample or the isotropy of the phases. In addition, these sample-specific characteristics are intimately related to technical constraints such as the probe geometry and size of the sample. In particular, the latter is of importance for nanostructures which can now be probed technically on very small length scales. On the occasion of the 100th anniversary of the four-point probe technique, introduced by Frank Wenner, in this review we revisit and discuss various correction factors which are mandatory for an accurate derivation of the resistivity from the measured resistance. Among others, sample thickness, dimensionality, anisotropy, and the relative size and geometry of the sample with respect to the contact assembly are considered. We are also able to derive the correction factors for 2D anisotropic systems on circular finite areas with variable probe spacings. All these aspects are illustrated by state-of-the-art experiments carried out using a four-tip STM/SEM system. We are aware that this review article can only cover some of the most important topics. Regarding further aspects, e.g. technical realizations, the influence of inhomogeneities or different transport regimes, etc, we refer to other review articles in this field.
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Understanding acoustic surface plasmons (ASPs) in the presence of nanosized gratings is necessary for the development of future devices that couple light with ASPs. We show here by experiment and theory that two ASPs exist on Au(788), a vicinal surface with an ordered array of monoatomic steps. The ASPs propagate across the steps as long as their wavelength exceeds the terrace width, thereafter becoming localized. Our investigation identifies, for the first time, ASPs coupled with intersubband transitions involving multiple surface-state subbands.
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In this investigation we tested the role of Cr impurities on the strongly spin-polarized surface states of ultra-thin epitaxially grown Bi(1 1 1) films by measuring surface magnetoconductance and the Hall effect in conjunction with low-energy electron diffraction at a low temperature (10 K). Compared with Fe and Co, investigated recently, Cr atoms turned out to have scattering cross-sections that are about a factor of three higher than the former atoms. Nevertheless, only a small electron donation (0.03 e/atom) was found for Cr. It also exhibits strong spin-orbit scattering, as judged from quantitative analysis of weak localization effects. As a result, all spin-dependent selection rules are gradually relaxed with increasing Cr concentration, so that the initially observed weak anti-localization shifts towards weak localization. The non-monotonic decrease of conductance as a function of Cr concentration, even at 10 K, indicates high diffusivity and activated adsorption into its final optimal adsorption site.
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Bismuto/química , Cromo/química , Campos Magnéticos , Membranas Artificiais , Modelos Químicos , Nanoestruturas/química , Eletricidade Estática , Simulação por Computador , Transporte de Elétrons , Nanoestruturas/ultraestruturaRESUMO
The linear dispersion of the low-dimensional acoustic surface plasmon (ASP) opens perspectives in energy conversion, transport, and confinement far below optical frequencies. Although the ASP exists in a wide class of materials, ranging from metal surfaces and ultrathin films to graphene and topological insulators, its properties are still largely unexplored. Taking Au(111) as a model system, our combined experimental and theoretical study revealed an intriguing interplay between collective and single particle excitations, causing the ASP associated with the Shockley surface state to be embedded within the intraband transitions without losing its sharp character and linear dispersion.
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The interaction between adsorbate layers of transition metal atoms and strongly anisotropic surfaces can lead to various quasi-one-dimensional (1D) signatures, as demonstrated here for Ag adsorbed on Si(557). Using low energy electron diffraction in combination with scanning tunneling microscopy and electron energy loss spectroscopy, we correlated the structure with the properties of low dimensional collective excitations. Semiconducting structures with double periodicity along the chains are formed at Ag coverages below 0.3 ML. At higher coverages, the formation of wires with (â3 × â3) order sets in. Only these wires are metallic, as is evident from the appearance of plasmonic losses, which show 1D dispersion only along the wires. This 1D property even persists up to one monolayer, where a densely packed array of metallic (â3 × â3) stripes is formed. The triple steps between the wires are obviously insulating. Only plasmonic subband transitions are visible, which are characteristic for quasi-1D metallic stripes of finite width.
Assuntos
Nanopartículas Metálicas/química , Nanopartículas Metálicas/ultraestrutura , Semicondutores , Silício/química , Prata/química , Condutividade Elétrica , Teste de Materiais , Ressonância de Plasmônio de SuperfícieRESUMO
The mutual interplay between superlattice structures, band filling factors, and spin-orbit coupling results in a highly correlated electronic spin and charge state found for an array of atomic Pb wires grown on Si(557). By means of spin- and angle-resolved photoemission spectroscopy, the spin texture close to the Fermi surface was found to be alternating and equidistant; thus, Fermi nesting occurs in between bands with the same spin helicity, giving rise to spin-polarized charge-density waves in the direction across the wires. An out-of-phase superposition of both Rashba channels is manifested by an extraordinary large Rashba splitting of Δk0=0.2 Å(-1)=g/2, where g is a reciprocal lattice vector defined by the interwire distance and fits into the model of spin-density waves in antiferromagnetically ordered chain structures. The implications towards spin-polarized transport along the wires will be discussed.
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The quasiparticle dynamics of the sheet plasmons in epitaxially grown graphene layers on SiC(0001) has been studied systematically as a function of temperature, intrinsic defects, influence of multilayers and carrier density using electron energy loss spectroscopy with high energy and momentum resolution. The opening of an inter-band decay channel appears as an anomalous kink in the plasmon dispersion which we describe as a resonance effect in the formation of electron-hole pairs. Due to the inevitable strong coupling of plasmons with single particle excitations in reduced dimensions, such signatures are generally expected.
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Using monolayer graphene as a model system for a purely two-dimensional (2D) electron gas, we show by energy electron loss spectroscopy, highly resolved both in energy and momentum, that there is a significant probability for the excitation of not only one but two dispersing losses. The appearance of both losses is independent of the substrate (we tested graphene on the Si face of 6H-SiC(0001), and on Ir(111) without and with an intercalated Na layer), and the ratio of the slope in the dispersion curves varies between 1.4 (SiC) and 2. While the lower dispersion curve can be attributed to the excitation of the sheet plasmon, in agreement with theoretical model calculations, the upper dispersion branch has not been identified before for plasmonic excitations in a 2D electron gas, and we assign it tentatively to the excitation of a multipole sheet plasmon.
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The Pb/Si(557) system exhibits a strong anisotropy in conductance below 78 K, with the evolution of a characteristic chain structure. Here we show, using angle-resolved photoemission, that chain ordering results in complete Fermi-like nesting in the direction normal to the chains; in addition, the domain structure along the chains forms split-off valence bands with mesoscopic Fermi wavelengths which induce the 1D conductance without further instabilities at low temperatures.
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The interaction of ferrocene-1,1(')-dithiol (FDT) with two parallel Ag(111) surfaces has been theoretically studied at density-functional level. The effect of surface defects on the energetic and electronic structure was investigated. The electronic transport properties are studied with the nonequilibrium Green's function approach. The adsorption geometry has a strong effect on the electronic levels and conductivity. The presence of point defects strongly enhances the molecule-surface interaction but has a surprisingly small effect on the density of states near the Fermi energy. The FDT-surface bond is particularly strong near terraces or steps and leads to significant shifts of the molecular orbitals relative to the gas phase. For all considered defect types except the single adatom the electronic conductivity through the FDT molecule is decreased compared to adsorption on perfect surfaces.