Si面4H-SiC衬底上外延石墨烯近平衡态制备

SiC热解法是制备大面积、高质量石墨烯的理想选择之一.外延石墨烯的晶体质量仍是制约其应用的关键因素之一.本文通过SiC热解法在4H-SiC(0001)衬底上制备单层外延石墨烯.通过引入氩气惰性气氛和硅蒸气,使SiC衬底表面的Si原子升华与返回概率接近平衡,外延石墨烯生长速率大大减慢,单层石墨烯的生长时间从15 min延长至75 min.测试分析表明,生长速率减慢,外延石墨烯中缺陷减少,晶体质量提高,使得外延石墨烯的电性能都得到改善,单层外延石墨烯的最高载流子迁移率达到1200 cm2/V·s,方阻604?/.以上结果表明,控制生长气氛,减慢生长速率是实现高质量外延石墨烯的可行途径之一.     

The physics of epitaxial graphene on SiC(0001)

Various physical properties of epitaxial graphene grown on SiC(0001) are studied. First, the electronic transport in epitaxial bilayer graphene on SiC(0001) and quasi-free-standing bilayer graphene on SiC(0001) is investigated. The dependences of the resistance and the polarity of the Hall resistance at zero gate voltage on the top-gate voltage show that the carrier types are electron and hole, respectively. The mobility evaluated at various carrier densities indicates that the quasi-free-standing bilayer graphene shows higher mobility than the epitaxial bilayer graphene when they are compared at the same carrier density. The difference in mobility is thought to come from the domain size of the graphene sheet formed. To clarify a guiding principle for controlling graphene quality, the mechanism of epitaxial graphene growth is also studied theoretically. It is found that a new graphene sheet grows from the interface between the old graphene sheets and the SiC substrate. Further studies on the energetics reveal the importance of the role of the step on the SiC surface. A first-principles calculation unequivocally shows that the C prefers to release from the step edge and to aggregate as graphene nuclei along the step edge rather than be left on the terrace. It is also shown that the edges of the existing graphene more preferentially absorb the isolated C atoms. For some annealing conditions, experiments can also provide graphene islands on SiC(0001) surfaces. The atomic structures are studied theoretically together with their growth mechanism. The proposed embedded island structures actually act as a graphene island electronically, and those with zigzag edges have a magnetoelectric effect. Finally, the thermoelectric properties of graphene are theoretically examined. The results indicate that reducing the carrier scattering suppresses the thermoelectric power and enhances the thermoelectric figure of merit. The fine control of the Fermi energy position is thought to be key for the practical use of graphene as a thermoelectric material, which could be achieved with epitaxial graphene. All of these results reveal that epitaxial graphene is physically interesting.     

Reactive chemical doping of the Bi2Se3 topological insulator

Using angular resolved photoemission spectroscopy we studied the evolution of the surface electronic structure of the topological insulator Bi(2)Se(3) as a function of water vapor exposure. We find that a surface reaction with water induces a band bending, which shifts the Dirac point deep into the occupied states and creates quantum well states with a strong Rashba-type splitting. The surface is thus not chemically inert, but the topological state remains protected. The band bending is traced back to Se abstraction, leaving positively charged vacancies at the surface. Because of the presence of water vapor, a similar effect takes place when Bi(2)Se(3) crystals are left in vacuum or cleaved in air, which likely explains the aging effect observed in the Bi(2)Se(3) band structure.     

The heterostructure and electrical properties of Sb2Se3/Bi2Se3 grown by molecular beam epitaxy

We report the growth and characterization of Sb₂Se₃/Bi₂Se₃ bilayer films fabricated by molecular beam epitaxy. High quality heterostructures are obtained as evidenced from the X-ray diffraction (XRD), atomic force microscopy and high-resolution transmission electron microscopic (HRTEM) analysis. Interestingly, Sb₂Se₃ grows as a (120) hexacrystal film in orthorhombic phase on rhombohedral Bi₂Se₃ (0001) plane, as verified by the out-of-plane and in-plane XRD scans. The cross-sectional TEM studies indicate a sharp interface between Sb₂Se₃ and Bi₂Se₃, which is important for the protection of surface states Bi₂Se₃. The ultraviolet photoelectron spectroscopy indicates that the Fermi level located 0.95 eV above the valence band maximum in Sb₂Se₃. The insulating nature of Sb₂Se₃ is confirmed by the nonlinear current-voltage curve via the vertical junction electrical measurement. By four point probe measurements, we confirm the charge transfer effect from Sb₂Se₃ into Bi₂Se₃, and such effect can be reduced in the Sb₂Se₃/(Bi_0.7Sb_0.3)₂Se₃ bilayer. This work opens a new avenue for the synthesis of multilayers consisting of topological insulators and ordinary insulator, which is important for harvesting of the multiple surface states for advanced electronic and spintronic applications.     

Influence of defects in SiC （0001） on epitaxial graphene

Defects in silicon carbide(SiC) substrate are crucial to the properties of the epitaxial graphene(EG) grown on it. Here we report the effect of defects in SiC on the crystalline quality of EGs through comparative studies of the characteristics of the EGs grown on SiC(0001) substrates with different defect densities. It is found that EGs on high quality SiC possess regular steps on the surface of the SiC and there is no discernible D peak in its Raman spectrum. Conversely, the EG on the SiC with a high density of defects has a strong D peak, irregular stepped morphology and poor uniformity in graphene layer numbers. It is the defects in the SiC that are responsible for the irregular stepped morphology and lead to the small domain size in the EG.     

High pressure transport properties of the topological insulator Bi2Se3

We report x-ray diffraction, electrical resistivity, and magnetoresistance measurements on Bi2Se3 under high pressure and low temperature conditions. Pressure induces profound changes in both the room temperature value of the electrical resistivity as well as the temperature dependence of the resistivity. Initially, pressure drives Bi2Se3 toward increasingly insulating behavior and then, at higher pressures, the sample appears to enter a fully metallic state coincident with a change in the crystal structure. Within the low pressure phase, Bi2Se3 exhibits an unusual field dependence of the transverse magnetoresistance Δρ(xx) that is positive at low fields and becomes negative at higher fields. Our results demonstrate that pressures below 8 GPa provide a non-chemical means to controllably reduce the bulk conductivity of Bi2Se3.     

Modulating doping and interface magnetism of epitaxial graphene on SiC(0001)

On the basis of first principles calculations, we report that the type and density of charge carriers of epitaxial graphene on Si C(0001) can be deliberately controlled by decorating the buffer layer with specific atoms(i.e., F, Cl, O, or N). More importantly, a fine tuning of the doping behavior from intrinsic n-type to charge neutrality to p-type and interface magnetism is achieved via increasing the doping concentration of F atoms on the buffer layer. Our results suggest an interesting avenue to the application of epitaxial graphene in nanoscale electronic and spintronic devices.     

Direct graphene growth on Co3O4(111) by molecular beam epitaxy

Direct growth of graphene on Co(3)O(4)(111) at 1000 K was achieved by molecular beam epitaxy from a graphite source. Auger spectroscopy shows a characteristic sp(2) carbon lineshape, at average carbon coverages from 0.4 to 3 ML. Low energy electron diffraction (LEED) indicates (111) ordering of the sp(2) carbon film with a lattice constant of 2.5(±0.1) ? characteristic of graphene. Sixfold symmetry of the graphene diffraction spots is observed at 0.4, 1 and 3 ML. The LEED data also indicate an average domain size of ~1800 ?, and show an incommensurate interface with the Co(3)O(4)(111) substrate, where the latter exhibits a lattice constant of 2.8(±0.1) ?. Core level photoemission shows a characteristically asymmetric C(1s) feature, with the expected π to π* satellite feature, but with a binding energy for the 3 ML film of 284.9(±0.1) eV, indicative of substantial graphene-to-oxide charge transfer. Spectroscopic ellipsometry data demonstrate broad similarity with graphene samples physically transferred to SiO(2) or grown on SiC substrates, but with the π to π* absorption blue-shifted, consistent with charge transfer to the substrate. The ability to grow graphene directly on magnetically and electrically polarizable substrates opens new opportunities for industrial scale development of charge- and spin-based devices.     

Rashba spin-splitting control at the surface of the topological insulator Bi2Se3

The electronic structure of Bi(2)Se(3) is studied by angle-resolved photoemission and density functional theory. We show that the instability of the surface electronic properties, observed even in ultrahigh-vacuum conditions, can be overcome via in situ potassium deposition. In addition to accurately setting the carrier concentration, new Rashba-like spin-polarized states are induced, with a tunable, reversible, and highly stable spin splitting. Ab initio slab calculations reveal that these Rashba states are derived from 5-quintuple-layer quantum-well states. While the K-induced potential gradient enhances the spin splitting, this may be present on pristine surfaces due to the symmetry breaking of the vacuum-solid interface.     

Molecular beam epitaxy of superconducting PdTe_2 films on topological insulator Bi_2Te_3

Majorana fermions have been observed in topological insulator/s-wave superconductor heterostructures. To manipulate Majorana fermions, superconducting materials should be deposited on the surfaces of topological insulators. In this study, highquality superconducting PdTe_2 films are deposited on the topological insulator Bi_2Te_3 surface using molecular beam epitaxy. The surface topography and electronic properties of PdTe_2/Bi_2Te_3 heterostructures are investigated via in situ scanning tunneling microscopy/spectroscopy. Under Te-rich conditions, the Pd atoms presumably form PdTe_2 film on Bi_2Te_3 surface rather than diffuse into Bi_2Te_3. The superconductivity of the PdTe_2/Bi_2Te_3 heterostructure is detected at a transition temperature of ～1.4 K using the two-coil mutual inductance technique. This study proposes a method for fabricating superconducting materials on topological insulator surfaces at low doping levels, paving ways for designing nanodevices that can manipulate Majorana fermions.     

Superconducting quantum interference devices made of Sb-doped Bi2Se3 topological insulator nanoribbons

We report the fabrication and characterization of superconducting quantum interference devices (SQUIDs) made of Sb-doped Bi₂Se₃ topological insulator (TI) nanoribbon (NR) contacted with PbIn superconducting electrodes. When an external magnetic field was applied along the NR axis, the TI NR exhibited periodic magneto-conductance oscillations, the so-called Aharonov-Bohm oscillations, owing to one-dimensional subbands. Below the superconducting transition temperature of PbIn electrodes, we observed supercurrent flow through TI NR-based SQUID. The critical current periodically modulates with a magnetic field perpendicular to the SQUID loop, revealing that the periodicity corresponds to the superconducting flux quantum. Our experimental observations can be useful to explore Majorana bound states (MBS) in TI NR, promising for developing topological quantum information devices.     

Surface scattering via bulk continuum states in the 3D topological insulator Bi2Se3

We have performed scanning tunneling microscopy and differential tunneling conductance (dI/dV) mapping for the surface of the three-dimensional topological insulator Bi(2)Se(3). The fast Fourier transformation applied to the dI/dV image shows an electron interference pattern near Dirac node despite the general belief that the backscattering is well suppressed in the bulk energy gap region. The comparison of the present experimental result with theoretical surface and bulk band structures shows that the electron interference occurs through the scattering between the surface states near the Dirac node and the bulk continuum states.     

Surface states of charge carriers in epitaxial films of the topological insulator Bi2Te3

The galvanomagnetic properties of p-type bismuth telluride heteroepitaxial films grown by the hot wall epitaxy method on oriented muscovite mica substrates have been investigated. Quantum oscillations of the magnetoresistance associated with surface electronic states in three-dimensional topological insulators have been studied in strong magnetic fields ranging from 6 to 14 T at low temperatures. The cyclotron effective mass, charge carrier mobility, and parameters of the Fermi surface have been determined based on the results of analyzing the magnetoresistance oscillations. The dependences of the cross-sectional area of the Fermi surface S(k _F), the wave vector k _F, and the surface concentration of charge carriers n _s on the frequency of magnetoresistance oscillations in p-type Bi₂Te₃ heteroepitaxial films have been obtained. The experimentally observed shift of the Landau level index is consistent with the value of the Berry phase, which is characteristic of topological surface states of Dirac fermions in the films. The properties of topological surface states of charge carriers in p-type Bi₂Te₃ films obtained by analyzing the magnetoresistance oscillations significantly expand fields of practical application and stimulate the investigation of transport properties of chalcogenide films.     

Layer by layer growth of ZnO on (0001) sapphire substrates by radical-source molecular beam epitaxy

Layer by layer growth of ZnO epilayers on (0001) Al₂O₃ substrates is achieved by radical-source molecular beam epitaxy. A thin MgO buffer, followed by a low-temperature ZnO buffer was used in order to accommodate the lattice mismatch between ZnO and sapphire. Reflection high-energy electron diffraction intensity was employed for the optimization of the ZnO growth. The surface morphology of the samples was studied with atomic force microscopy. Investigation of the nature of the influence of the MgO buffer layer on the formation of ZnO on sapphire substrate was carried out using Transmission Electron Microscopy. For the first time it was shown that a thin spinel (magnesium aluminum oxide) layer is formed on the interface of the sapphire substrate and MgO buffer layer leading to the crystalline quality improvement of the ZnO main layer. X-Ray diffractometry measurements of the obtained ZnO layers show excellent quality of the single crystalline ZnO heteroepitaxially grown on sapphire. The crystalline quality of the ZnO layers is even better than that of our previously reported layers grown employing hydrogen peroxide as an oxidant. The full width at half maximum of the XRD (0002) rocking curve is as low as 25 arc s. The influence of growth parameters (Zn/O flux ratio, temperature, etc.) on the structural properties as well as on the surface morphology of the zinc oxide layers on sapphire is investigated and discussed.     

Ultrafast optical excitation of a persistent surface-state population in the topological insulator Bi2Se3

Using femtosecond time- and angle-resolved photoemission spectroscopy, we investigated the nonequilibrium dynamics of the topological insulator Bi2Se3. We studied p-type Bi2Se3, in which the metallic Dirac surface state and bulk conduction bands are unoccupied. Optical excitation leads to a metastable population at the bulk conduction band edge, which feeds a nonequilibrium population of the surface state persisting for >10 ps. This unusually long-lived population of a metallic Dirac surface state with spin texture may present a channel in which to drive transient spin-polarized currents.     

Photoemission spectroscopy of magnetic and nonmagnetic impurities on the surface of the Bi2Se3 topological insulator

Dirac-like surface states on surfaces of topological insulators have a chiral spin structure that suppresses backscattering and protects the coherence of these states in the presence of nonmagnetic scatterers. In contrast, magnetic scatterers should open the backscattering channel via the spin-flip processes and degrade the state's coherence. We present angle-resolved photoemission spectroscopy studies of the electronic structure and the scattering rates upon the adsorption of various magnetic and nonmagnetic impurities on the surface of Bi2Se3, a model topological insulator. We reveal a remarkable insensitivity of the topological surface state to both nonmagnetic and magnetic impurities in the low impurity concentration regime. Scattering channels open up with the emergence of hexagonal warping in the high-doping regime, irrespective of the impurity's magnetic moment.     

Temperature dependence of the thickness and morphology of epitaxial graphene grown on SiC （0001） wafers

Epitaxial graphene is synthesized by silicon sublimation from the Si-terminated 6H–SiC substrate. The effects of graphitization temperature on the thickness and surface morphology of epitaxial graphene are investigated. X-ray photoelectron spectroscopy spectra and atomic force microscopy images reveal that the epitaxial graphene thickness increases and the epitaxial graphene roughness decreases with the increase in graphitization temperature. This means that the thickness and roughness of epitaxial graphene films can be modulated by varying the graphitization temperature. In addition, the electrical properties of epitaxial graphene film are also investigated by Hall effect measurement.     

Electron-phonon coupling on the surface of the topological insulator Bi2Se3 determined from surface-phonon dispersion measurements

In this Letter, we report measurements of the coupling between Dirac fermion quasiparticles (DFQs) and phonons on the (001) surface of the strong topological insulator Bi2Se3. While most contemporary investigations of this coupling have involved examining the temperature dependence of the DFQ self-energy via angle-resolved photoemission spectroscopy measurements, we employ inelastic helium-atom scattering to explore, for the first time, this coupling from the phonon perspective. Using a Hilbert transform, we are able to obtain the imaginary part of the phonon self-energy associated with a dispersive surface-phonon branch identified in our previous work [Phys. Rev. Lett. 107, 186102 (2011)] as having strong interactions with the DFQs. From this imaginary part of the self-energy we obtain a branch-specific electron-phonon coupling constant of 0.43, which is stronger than the values reported from the angle-resolved photoemission spectroscopy measurements.     

Adsorption and desorption of fullerene on graphene/SiC(0001)

Adsorption and desorption of fullerene on a single layer of graphene grown on SiC(0001) were investigated by photoemission spectroscopy (PES). No significant change in the band structure of graphene was observed after fullerene deposition on the graphene layer under vacuum conditions, and subsequent exposure to the air. After annealing the fullerene layer at 275 °C in a vacuum, complete desorption of fullerene was observed without any resulting damage to the graphene structure. The desorption temperature of fullerene was significantly higher than that of pentacene, indicating that fullerene layers show higher stability than pentacene as protection layers of graphene-based devices.     

Terahertz response and colossal Kerr rotation from the surface states of the topological insulator Bi2Se3

We report the THz response of thin films of the topological insulator Bi2Se3. At low frequencies, transport is essentially thickness independent showing the dominant contribution of the surface electrons. Despite their extended exposure to ambient conditions, these surfaces exhibit robust properties including narrow, almost thickness-independent Drude peaks, and an unprecedentedly large polarization rotation of linearly polarized light reflected in an applied magnetic field. This Kerr rotation can be as large as 65° and can be explained by a cyclotron resonance effect of the surface states.