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Sample records for few-layer epitaxial graphene

  1. Vertically aligned GaAs nanowires on graphite and few-layer graphene: generic model and epitaxial growth.

    PubMed

    Munshi, A Mazid; Dheeraj, Dasa L; Fauske, Vidar T; Kim, Dong-Chul; van Helvoort, Antonius T J; Fimland, Bjørn-Ove; Weman, Helge

    2012-09-12

    By utilizing the reduced contact area of nanowires, we show that epitaxial growth of a broad range of semiconductors on graphene can in principle be achieved. A generic atomic model is presented which describes the epitaxial growth configurations applicable to all conventional semiconductor materials. The model is experimentally verified by demonstrating the growth of vertically aligned GaAs nanowires on graphite and few-layer graphene by the self-catalyzed vapor-liquid-solid technique using molecular beam epitaxy. A two-temperature growth strategy was used to increase the nanowire density. Due to the self-catalyzed growth technique used, the nanowires were found to have a regular hexagonal cross-sectional shape, and are uniform in length and diameter. Electron microscopy studies reveal an epitaxial relationship of the grown nanowires with the underlying graphitic substrates. Two relative orientations of the nanowire side-facets were observed, which is well explained by the proposed atomic model. A prototype of a single GaAs nanowire photodetector demonstrates a high-quality material. With GaAs being a model system, as well as a very useful material for various optoelectronic applications, we anticipate this particular GaAs nanowire/graphene hybrid to be promising for flexible and low-cost solar cells.

  2. Symmetry Breaking in Few Layer Graphene Films

    SciTech Connect

    Bostwick, A.; Ohta, T.; McChesney, J.L.; Emtsev, K.; Seyller,Th.; Horn, K.; Rotenberg, E.

    2007-05-25

    Recently, it was demonstrated that the quasiparticledynamics, the layer-dependent charge and potential, and the c-axisscreening coefficient could be extracted from measurements of thespectral function of few layer graphene films grown epitaxially on SiCusing angle-resolved photoemission spectroscopy (ARPES). In this articlewe review these findings, and present detailed methodology for extractingsuch parameters from ARPES. We also present detailed arguments againstthe possibility of an energy gap at the Dirac crossing ED.

  3. Ballistic electron propagation through periodic few-layer graphene nanostructures

    NASA Astrophysics Data System (ADS)

    Dragoman, Daniela; Mihalache, Iulia

    2016-10-01

    We have studied electron propagation in periodic structures containing mono- and few-layer graphene regions and/or semiconducting stripes. The calculation of the transmission coefficient in all cases has been performed using transfer matrices inside regions with the same material/potential energy, as well as interface matrices between regions in which the evolution laws of charge carriers differ. Numerical simulations of the transmission coefficient, as well as of the low-temperature conductance, suggest that different periodic structures modulate differently the electrical current. The obtained results can be used to model ballistic transport in all-graphene devices, in particular in few-layer graphene structures.

  4. Nonlocal thermal transport across embedded few-layer graphene sheets

    SciTech Connect

    Liu, Ying; Huxtable, Scott T.; Yang, Bao; Sumpter, Bobby G.; Qiao, Rui

    2014-11-13

    Thermal transport across the interfaces between few-layer graphene sheets and soft materials exhibits intriguing anomalies when interpreted using the classical Kapitza model, e.g., the conductance of the same interface differs greatly for different modes of interfacial thermal transport. Using atomistic simulations, we show that such thermal transport follows a nonlocal flux-temperature drop constitutive law and is characterized jointly by a quasi-local conductance and a nonlocal conductance instead of the classical Kapitza conductance. Lastly, the nonlocal model enables rationalization of many anomalies of the thermal transport across embedded few-layer graphene sheets and should be used in studies of interfacial thermal transport involving few-layer graphene sheets or other ultra-thin layered materials.

  5. Nonlocal thermal transport across embedded few-layer graphene sheets

    DOE PAGESBeta

    Liu, Ying; Huxtable, Scott T.; Yang, Bao; Sumpter, Bobby G.; Qiao, Rui

    2014-11-13

    Thermal transport across the interfaces between few-layer graphene sheets and soft materials exhibits intriguing anomalies when interpreted using the classical Kapitza model, e.g., the conductance of the same interface differs greatly for different modes of interfacial thermal transport. Using atomistic simulations, we show that such thermal transport follows a nonlocal flux-temperature drop constitutive law and is characterized jointly by a quasi-local conductance and a nonlocal conductance instead of the classical Kapitza conductance. Lastly, the nonlocal model enables rationalization of many anomalies of the thermal transport across embedded few-layer graphene sheets and should be used in studies of interfacial thermal transportmore » involving few-layer graphene sheets or other ultra-thin layered materials.« less

  6. Characterization of few-layered graphene grown by carbon implantation

    SciTech Connect

    Lee, Kin Kiong; McCallum, Jeffrey C.; Jamieson, David N.

    2014-02-21

    Graphene is considered to be a very promising material for applications in nanotechnology. The properties of graphene are strongly dependent on defects that occur during growth and processing. These defects can be either detrimental or beneficial to device performance depending on defect type, location and device application. Here we present experimental results on formation of few-layered graphene by carbon ion implantation into nickel films and characteristics of graphene devices formed by graphene transfer and lithographic patterning. Micro-Raman spectroscopy was used to determine the number of graphene layers formed and identify defects arising from the device processing. The graphene films were cleaned by annealing in vacuum. Transport properties of cleaned graphene films were investigated by fabrication of back-gated field-effect transistors, which exhibited high hole and electron mobility of 1935 and 1905 cm2/Vs, respectively.

  7. Interfacial Atomic Structure of Twisted Few-Layer Graphene.

    PubMed

    Ishikawa, Ryo; Lugg, Nathan R; Inoue, Kazutoshi; Sawada, Hidetaka; Taniguchi, Takashi; Shibata, Naoya; Ikuhara, Yuichi

    2016-02-18

    A twist in bi- or few-layer graphene breaks the local symmetry, introducing a number of intriguing physical properties such as opening new bandgaps. Therefore, determining the twisted atomic structure is critical to understanding and controlling the functional properties of graphene. Combining low-angle annular dark-field electron microscopy with image simulations, we directly determine the atomic structure of twisted few-layer graphene in terms of a moiré superstructure which is parameterized by a single twist angle and lattice constant. This method is shown to be a powerful tool for accurately determining the atomic structure of two-dimensional materials such as graphene, even in the presence of experimental errors. Using coincidence-site-lattice and displacement-shift-complete theories, we show that the in-plane translation state between layers is not a significant structure parameter, explaining why the present method is adequate not only for bilayer graphene but also a few-layered twisted graphene.

  8. Interfacial Atomic Structure of Twisted Few-Layer Graphene

    PubMed Central

    Ishikawa, Ryo; Lugg, Nathan R.; Inoue, Kazutoshi; Sawada, Hidetaka; Taniguchi, Takashi; Shibata, Naoya; Ikuhara, Yuichi

    2016-01-01

    A twist in bi- or few-layer graphene breaks the local symmetry, introducing a number of intriguing physical properties such as opening new bandgaps. Therefore, determining the twisted atomic structure is critical to understanding and controlling the functional properties of graphene. Combining low-angle annular dark-field electron microscopy with image simulations, we directly determine the atomic structure of twisted few-layer graphene in terms of a moiré superstructure which is parameterized by a single twist angle and lattice constant. This method is shown to be a powerful tool for accurately determining the atomic structure of two-dimensional materials such as graphene, even in the presence of experimental errors. Using coincidence-site-lattice and displacement-shift-complete theories, we show that the in-plane translation state between layers is not a significant structure parameter, explaining why the present method is adequate not only for bilayer graphene but also a few-layered twisted graphene. PMID:26888259

  9. Detection of interlayer interaction in few-layer graphene

    NASA Astrophysics Data System (ADS)

    Wu, Zefei; Han, Yu; Lin, Jiangxiazi; Zhu, Wei; He, Mingquan; Xu, Shuigang; Chen, Xiaolong; Lu, Huanhuan; Ye, Weiguang; Han, Tianyi; Wu, Yingying; Long, Gen; Shen, Junying; Huang, Rui; Wang, Lin; He, Yuheng; Cai, Yuan; Lortz, Rolf; Su, Dangsheng; Wang, Ning

    2015-08-01

    Bernal-stacked few-layer graphene has been investigated by analyzing its Landau-level spectra through quantum capacitance measurements. We find that surface relaxation, which is insignificant in trilayer graphene, starts to manifest in Bernal-stacked tetralayer graphene. In trilayer graphene, the interlayer interaction parameters are generally similar to those of graphite. However, in tetralayer graphene, the hopping parameters of the two bulk layers are quite different from those of the two outer layers. This represents direct evidence of the surface relaxation phenomenon. Traditionally, the van der Waals interaction between the carbon layers is thought to be insignificant. However, we suggest that the interlayer interaction is an important factor in explaining the observed results, and the symmetry-breaking effects in graphene sublattice are not negligible.

  10. Extreme ultraviolet induced defects on few-layer graphene

    NASA Astrophysics Data System (ADS)

    Gao, A.; Rizo, P. J.; Zoethout, E.; Scaccabarozzi, L.; Lee, C. J.; Banine, V.; Bijkerk, F.

    2013-07-01

    We use Raman spectroscopy to show that exposing few-layer graphene to extreme ultraviolet (EUV, 13.5 nm) radiation, i.e., relatively low photon energy, results in an increasing density of defects. Furthermore, exposure to EUV radiation in a H2 background increases the graphene dosage sensitivity, due to reactions caused by the EUV induced hydrogen plasma. X-ray photoelectron spectroscopy results show that the sp2 bonded carbon fraction decreases while the sp3 bonded carbon and oxide fraction increases with exposure dose. Our experimental results confirm that even in reducing environment oxidation is still one of the main source of inducing defects.

  11. Few layer epitaxial germanene: a novel two-dimensional Dirac material.

    PubMed

    Dávila, María Eugenia; Le Lay, Guy

    2016-01-01

    Monolayer germanene, a novel graphene-like germanium allotrope akin to silicene has been recently grown on metallic substrates. Lying directly on the metal surfaces the reconstructed atom-thin sheets are prone to lose the massless Dirac fermion character and unique associated physical properties of free standing germanene. Here, we show that few layer germanene, which we create by dry epitaxy on a gold template, possesses Dirac cones thanks to a reduced interaction. This finding established on synchrotron-radiation-based photoemission, scanning tunneling microscopy imaging and surface electron diffraction places few layer germanene among the rare two-dimensional Dirac materials. Since germanium is currently used in the mainstream Si-based electronics, perspectives of using germanene for scaling down beyond the 5 nm node appear very promising. Other fascinating properties seem at hand, typically the robust quantum spin Hall effect for applications in spintronics and the engineering of Floquet Majorana fermions by light for quantum computing.

  12. Few layer epitaxial germanene: a novel two-dimensional Dirac material.

    PubMed

    Dávila, María Eugenia; Le Lay, Guy

    2016-01-01

    Monolayer germanene, a novel graphene-like germanium allotrope akin to silicene has been recently grown on metallic substrates. Lying directly on the metal surfaces the reconstructed atom-thin sheets are prone to lose the massless Dirac fermion character and unique associated physical properties of free standing germanene. Here, we show that few layer germanene, which we create by dry epitaxy on a gold template, possesses Dirac cones thanks to a reduced interaction. This finding established on synchrotron-radiation-based photoemission, scanning tunneling microscopy imaging and surface electron diffraction places few layer germanene among the rare two-dimensional Dirac materials. Since germanium is currently used in the mainstream Si-based electronics, perspectives of using germanene for scaling down beyond the 5 nm node appear very promising. Other fascinating properties seem at hand, typically the robust quantum spin Hall effect for applications in spintronics and the engineering of Floquet Majorana fermions by light for quantum computing. PMID:26860590

  13. Few layer epitaxial germanene: a novel two-dimensional Dirac material

    PubMed Central

    Dávila, María Eugenia; Le Lay, Guy

    2016-01-01

    Monolayer germanene, a novel graphene-like germanium allotrope akin to silicene has been recently grown on metallic substrates. Lying directly on the metal surfaces the reconstructed atom-thin sheets are prone to lose the massless Dirac fermion character and unique associated physical properties of free standing germanene. Here, we show that few layer germanene, which we create by dry epitaxy on a gold template, possesses Dirac cones thanks to a reduced interaction. This finding established on synchrotron-radiation-based photoemission, scanning tunneling microscopy imaging and surface electron diffraction places few layer germanene among the rare two-dimensional Dirac materials. Since germanium is currently used in the mainstream Si-based electronics, perspectives of using germanene for scaling down beyond the 5 nm node appear very promising. Other fascinating properties seem at hand, typically the robust quantum spin Hall effect for applications in spintronics and the engineering of Floquet Majorana fermions by light for quantum computing. PMID:26860590

  14. Long Spin Diffusion Length in Few-Layer Graphene Flakes

    NASA Astrophysics Data System (ADS)

    Yan, W.; Phillips, L. C.; Barbone, M.; Hämäläinen, S. J.; Lombardo, A.; Ghidini, M.; Moya, X.; Maccherozzi, F.; van Dijken, S.; Dhesi, S. S.; Ferrari, A. C.; Mathur, N. D.

    2016-09-01

    We report a spin valve with a few-layer graphene flake bridging highly spin-polarized La0.67Sr0.33MnO3 electrodes, whose surfaces are kept clean during lithographic definition. Sharp magnetic switching is verified using photoemission electron microscopy with x-ray magnetic circular dichroism contrast. A naturally occurring high interfacial resistance ˜12 M Ω facilitates spin injection, and a large resistive switching (0.8 M Ω at 10 K) implies a 70 - 130 μ m spin diffusion length that exceeds previous values obtained with sharp-switching electrodes.

  15. Extreme ultraviolet induced defects on few-layer graphene

    SciTech Connect

    Gao, A.; Zoethout, E.; Lee, C. J.; Rizo, P. J.; Scaccabarozzi, L.; Banine, V.; Bijkerk, F.

    2013-07-28

    We use Raman spectroscopy to show that exposing few-layer graphene to extreme ultraviolet (EUV, 13.5 nm) radiation, i.e., relatively low photon energy, results in an increasing density of defects. Furthermore, exposure to EUV radiation in a H{sub 2} background increases the graphene dosage sensitivity, due to reactions caused by the EUV induced hydrogen plasma. X-ray photoelectron spectroscopy results show that the sp{sup 2} bonded carbon fraction decreases while the sp{sup 3} bonded carbon and oxide fraction increases with exposure dose. Our experimental results confirm that even in reducing environment oxidation is still one of the main source of inducing defects.

  16. Synthesis and characterization of intercalated few-layer graphenes

    NASA Astrophysics Data System (ADS)

    Sato, Shogo; Ichikawa, Hiroaki; Iwata, Nobuyuki; Yamamoto, Hiroshi

    2014-02-01

    Toward achieving room-temperature superconductivity, FeCl3-intercalated few-layer graphenes (FeCl3-FLGs) and Ca-intercalated few-layer graphenes (Ca-FLGs) were synthesized. FeCl3-FLGs were synthesized by the two-zone method and Ca-FLGs were synthesized using Ca-Li alloy. The Raman spectra of the FeCl3-FLGs showed a lower-intensity peak at 1607 cm-1 than that of the corresponding bare G. The peak at 1607 cm-1 suggested that the sample was stage 4-5 FeCl3-FLGs. The room-temperature electrical resistivity of FeCl3-FLGs was 2.65 × 10-5 Ω·m, which linearly decreased with decreasing temperature with a marked change occurring at approximately 200 K. From a XRD pattern of Ca-FLGs, we concluded that Ca is intercalated in FLGs. The room-temperature resistivity of Ca-FLGs was 3.45 × 10-5 Ω·m, which increased with decreasing temperature.

  17. Structural distortions in few-layer graphene creases.

    PubMed

    Robertson, Alex W; Bachmatiuk, Alicja; Wu, Yimin A; Schäffel, Franziska; Büchner, Bernd; Rümmeli, Mark H; Warner, Jamie H

    2011-12-27

    Folds and creases are frequently found in graphene grown by chemical vapor deposition (CVD), due to the differing thermal expansion coefficients of graphene from the growth catalyst and the flexibility of the sheet during transfer from the catalyst. The structure of a few-layer graphene (FLG) crease is examined by aberration-corrected high-resolution transmission electron microscopy (AC-HRTEM). A study of 2D fast Fourier transforms (FFTs) taken about the region of the crease allowed for the crystal stacking structure of the system to be elucidated. It was found that strain-induced stacking faults were created in the AB Bernal-stacked FLG bulk around the region proximal to the crease termination; this is of interest as the stacking order of FLG is known to have an effect on its electronic properties and thus should be considered when transferring CVD-grown FLG to alternate substrates for electronic device fabrication. The FFTs, along with analysis of the real space images, were used to determine the configuration of the layers in the crease itself and were corroborated by multislice atomistic TEM simulations. The termination of the crease part way through the FLG sheet is also examined and is found to show strong out of plane distortions in the area about it. PMID:22122696

  18. Raman Scattering from few-layer Graphene Films

    NASA Astrophysics Data System (ADS)

    Gupta, A.; Joshi, P.; Srinivas, T.; Eklund, Peter

    2006-03-01

    Few layer-graphene sheet (nGL's) films, where n is the number of graphene layers, are new two-dimensional sp^2 carbon systems that have been shown to produce exciting Fractional Quantum Hall phenomena. We report here on the first Raman scattering (RS) results of nGLs. nGLs with lateral dimensions of ˜1-3 μm were prepared by chemical delamination of graphite flake or HOPG and then transferred from solution onto substrates (mica, pyrex,In/pyrex and Au/pyrex). RS spectra have been collected on nGL's with n=1, 2, 3 and compared with the graphite. Graphite exhibits two E2g interlayer modes at 42 cm-1 and 1582 cm-1. The Raman spectra of (n=1-3) nGLs were found to exhibit peaks at 1350 cm-1 and 1620 cm-1, i.e., near frequencies associated with high phonon density of states. The high frequency E2g band is found to split into two bands when the nGL is supported on metallic substrates (In,Au). In both these cases, we observe bands at 1583 cm-1, ˜1592 cm-1 rather than one band at 1581 cm-1 when the nGL is on insulating pyrex. The splitting of the interlayer band when on metallic substrates is identified with charge transfer between the nGL and the substrate. The phonon density of states scattering observed does not appear to be due to disorder in the basal plane.

  19. Epitaxial deposition of silver ultra-fine nano-clusters on defect-free surfaces of HOPG-derived few-layer graphene in a UHV multi-chamber by in situ STM, ex situ XPS, and ab initio calculations.

    PubMed

    Ndlovu, Gebhu F; Roos, Wiets D; Wang, Zhiming M; Asante, Joseph Ko; Mashapa, Matete G; Jafta, Charl J; Mwakikunga, Bonex W; Hillie, Kenneth T

    2012-01-01

    The growth of three-dimensional ultra-fine spherical nano-particles of silver on few layers of graphene derived from highly oriented pyrolytic graphite in ultra-high vacuum were characterized using in situ scanning tunneling microscopy (STM) in conjunction with X-ray photoelectron spectroscopy. The energetics of the Ag clusters was determined by DFT simulations. The Ag clusters appeared spherical with size distribution averaging approximately 2 nm in diameter. STM revealed the preferred site for the position of the Ag atom in the C-benzene ring of graphene. Of the three sites, the C-C bridge, the C-hexagon hollow, and the direct top of the C atom, Ag prefers to stay on top of the C atom, contrary to expectation of the hexagon-close packing. Ab initio calculations confirm the lowest potential energy between Ag and the graphene structure to be at the exact site determined from STM imaging.

  20. Epitaxial deposition of silver ultra-fine nano-clusters on defect-free surfaces of HOPG-derived few-layer graphene in a UHV multi-chamber by in situ STM, ex situ XPS, and ab initio calculations

    PubMed Central

    2012-01-01

    The growth of three-dimensional ultra-fine spherical nano-particles of silver on few layers of graphene derived from highly oriented pyrolytic graphite in ultra-high vacuum were characterized using in situ scanning tunneling microscopy (STM) in conjunction with X-ray photoelectron spectroscopy. The energetics of the Ag clusters was determined by DFT simulations. The Ag clusters appeared spherical with size distribution averaging approximately 2 nm in diameter. STM revealed the preferred site for the position of the Ag atom in the C-benzene ring of graphene. Of the three sites, the C-C bridge, the C-hexagon hollow, and the direct top of the C atom, Ag prefers to stay on top of the C atom, contrary to expectation of the hexagon-close packing. Ab initio calculations confirm the lowest potential energy between Ag and the graphene structure to be at the exact site determined from STM imaging. PMID:22395057

  1. Understanding Graphene Coatings: Characterization of Solvent Exfoliated Few-Layer Graphene by Raman Scattering

    NASA Astrophysics Data System (ADS)

    Camacho, Jorge; Lampert, Lester; Arifin, Willson; Flaig, Robby; Rue, Timothy; Krisko, Tyler; Hamilton, James

    2011-03-01

    Graphene has unique properties like its ballistic transport at room temperature combined with chemical and mechanical stability and these properties can be extended to few-layer of graphene. Potential large-area applications that include transparent conductive coatings and fuel cell electrodes require dispersing graphene in a fluid phase. Graphene nano-platelets can be synthesized by dispersion and exfoliation of graphite in organic solvents such N-methyl-pyrrolidine (NMP) and cyclohexylpyrrolidone (CHP). However, liquid-phase exfoliation produces graphene with defects that can disrupt the electronic properties. One of the remaining questions is whether the defects created during synthesis can be minimized. We report a Raman spectroscopic study showing that defects in few-layer graphene produced by liquid-phase exfoliation of graphite can be controlled by the type or mixture of solvents used.

  2. Few layer graphene synthesis via SiC decomposition at low temperature and low vacuum

    NASA Astrophysics Data System (ADS)

    Kayali, Emre; Mercan, Elif; Emre Oren, Ersin; Cambaz Buke, Goknur

    2016-04-01

    Based on the large-scale availability and good electrical properties, the epitaxial graphene (EG) on SiC exhibits a big potential for future electronic devices. However, it is still necessary to work continuously on lowering the formation temperature and vacuum values of EG while improving the quality and increasing the lateral size to fabricate high-performance electronic devices at reduced processing costs. In this study, we investigated the effect of the presence of Mo plate and hydrogen atmosphere as well as the vacuum annealing durations on SiC decomposition. Our studies showed that the graphene layers can be produced at lower annealing temperatures (1200 °C) and vacuum values (10-4 Torr) in the presence of Mo plate and hydrogen. For high quality continuous graphene formation, Mo plate should be in contact with SiC. If there is a gap between Mo and SiC, non-wetting oxide droplets on few layer graphene (FLG) are recorded. Moreover, it is found that the morphology of these islands can be controlled by changing the annealing time and atmosphere conditions, and applying external disturbances such as vibration.

  3. Tribological characteristics of few-layer graphene over Ni grain and interface boundaries

    NASA Astrophysics Data System (ADS)

    Tripathi, Manoj; Awaja, Firas; Paolicelli, Guido; Bartali, Ruben; Iacob, Erica; Valeri, Sergio; Ryu, Seunghwa; Signetti, Stefano; Speranza, Giorgio; Pugno, Nicola Maria

    2016-03-01

    The tribological properties of metal-supported few-layered graphene depend strongly on the grain topology of the metal substrate. Inhomogeneous distribution of graphene layers at such regions led to variable landscapes with distinguishable roughness. This discrepancy in morphology significantly affects the frictional and wetting characteristics of the FLG system. We discretely measured friction characteristics of FLG covering grains and interfacial grain boundaries of polycrystalline Ni metal substrate via an atomic force microscopy (AFM) probe. The friction coefficient of FLG covered at interfacial grain boundaries is found to be lower than that on grains in vacuum (at 10-5 Torr pressure) and similar results were obtained in air condition. Sliding history with AFM cantilever, static and dynamic pull-in and pull-off adhesion forces were addressed in the course of friction measurements to explain the role of the out-of-plane deformation of graphene layer(s). Finite element simulations showed good agreement with experiments and led to a rationalization of the observations. Thus, with interfacial grain boundaries the FLG tribology can be effectively tuned.The tribological properties of metal-supported few-layered graphene depend strongly on the grain topology of the metal substrate. Inhomogeneous distribution of graphene layers at such regions led to variable landscapes with distinguishable roughness. This discrepancy in morphology significantly affects the frictional and wetting characteristics of the FLG system. We discretely measured friction characteristics of FLG covering grains and interfacial grain boundaries of polycrystalline Ni metal substrate via an atomic force microscopy (AFM) probe. The friction coefficient of FLG covered at interfacial grain boundaries is found to be lower than that on grains in vacuum (at 10-5 Torr pressure) and similar results were obtained in air condition. Sliding history with AFM cantilever, static and dynamic pull-in and pull

  4. Direct Synthesis of Few-Layer Graphene on NaCl Crystals.

    PubMed

    Shi, Liurong; Chen, Ke; Du, Ran; Bachmatiuk, Alicja; Rümmeli, Mark Hermann; Priydarshi, Manish Kumar; Zhang, Yanfeng; Manivannan, Ayyakkannu; Liu, Zhongfan

    2015-12-16

    Chemical vapor deposition is used to synthesize few-layer graphene on micro crystalline sodium chloride (NaCl) powder. The water-soluble nature of NaCl makes it convenient to produce free standing graphene layers via a facile and low-cost approach. Unlike traditional metal-catalyzed or oxygen-aided growth, the micron-size NaCl crystal planes play an important role in the nucleation and growth of few-layer graphene. Moreover, the possibility of synthesizing cuboidal graphene is also demonstrated in the present approach for the first time. Raman spectroscopy, optical microscopy, scanning electron microscopy, transmission electron microscopy, and atomic force microscopy are used to evaluate the quality and structure of the few-layer graphene along with cuboidal graphene obtained in this process. The few-layer graphene synthesized using the present method has an adsorption ability for anionic and cationic dye molecules in water. The present synthesis method may pave a facile way for manufacturing few-layer graphene on a large scale. PMID:26524105

  5. Facile Large Scale Production of Few-Layer Graphene Sheets by Shear Exfoliation in Volatile Solvent.

    PubMed

    Akhtar, M Wasim; Park, Chan Woo; Kim, Youn Sop; Kim, Jong Seok

    2015-12-01

    Few layer graphene sheets were synthesized from natural graphite through mechanical shear mixer in 1-butanol as solvent. The liquid phase exfoliation of graphite through the shear mixer generated incising forces for 20 minutes which changed the large amount of graphite's flake into few layer graphene. The removal of solvent from the deposited dispersion was performed immediately by keeping at the room temperature. The deposited graphene thin films were characterized by AFM, HR-TEM, XRD, FT-IR and Raman Spectroscopy. The HR-TEM results showed the formation of few layers and well dispersed graphene. The Raman spectroscopy and XRD characterization confirmed the good quality and non-oxidized state of graphene. PMID:26682388

  6. Synthesis of few layer graphene by non-transferred arc plasma system.

    PubMed

    Baek, Jong-Jun; Kim, Tae-Hee; Park, Dong-Wha

    2013-11-01

    Graphene has recently been the focus of a great deal of attention owing to its outstanding properties, which include high mobility, high thermal conductivity and high structural stability. In this study, a few layer graphene was successfully synthesized from methane gas using a non-transferred direct current arc plasma system. Non-transferred thermal plasma offers high temperature, steep temperature gradient and high enthalpy to enhance the reaction kinetics of graphene synthesis. In order to prepare high quality few layer graphene, graphene products synthesized under several conditions was analyzed comparatively. Effects of gap distance between the plasma torch and graphite substrate, the flow rate of additional reactant gas, and different types of plasma forming gas on the synthesis of few layer graphene were investigated. Methane gas was injected into the plasma jet as a carbon source for the synthesis of graphene and a thermal plasma jet was generated by pure argon or a mixture of argon-hydrogen. The results revealed that hydrogen gas improved the quality of few layer graphene by inducing surface etching and increasing plasma power. PMID:24245266

  7. Synthesis of few layer graphene by non-transferred arc plasma system.

    PubMed

    Baek, Jong-Jun; Kim, Tae-Hee; Park, Dong-Wha

    2013-11-01

    Graphene has recently been the focus of a great deal of attention owing to its outstanding properties, which include high mobility, high thermal conductivity and high structural stability. In this study, a few layer graphene was successfully synthesized from methane gas using a non-transferred direct current arc plasma system. Non-transferred thermal plasma offers high temperature, steep temperature gradient and high enthalpy to enhance the reaction kinetics of graphene synthesis. In order to prepare high quality few layer graphene, graphene products synthesized under several conditions was analyzed comparatively. Effects of gap distance between the plasma torch and graphite substrate, the flow rate of additional reactant gas, and different types of plasma forming gas on the synthesis of few layer graphene were investigated. Methane gas was injected into the plasma jet as a carbon source for the synthesis of graphene and a thermal plasma jet was generated by pure argon or a mixture of argon-hydrogen. The results revealed that hydrogen gas improved the quality of few layer graphene by inducing surface etching and increasing plasma power.

  8. Functionalization of graphene and few-layer graphene with aqueous solution of hydrofluoric acid

    NASA Astrophysics Data System (ADS)

    Nebogatikova, N. A.; Antonova, I. V.; Volodin, V. A.; Prinz, V. Ya.

    2013-08-01

    In the present study, conditions suitable for efficient modification of graphene and few-layer graphene (FLG) films with aqueous solutions of hydrofluoric acid (HF) and for local protection of the graphene against such modification in isopropyl alcohol were identified. A combination of the two treatments gives one a key to nanodesign of graphene-based 2D devices. It was found that a few-minute treatment of graphene or FLG in HF aqueous solutions (∼1 min for graphene and ∼5 min for FLG films about 5 nm thick) leads to strong changes in the structural and electrical properties of graphene involving a step-like increase in resistivity (up to 1011 Ω/□). Two types of materials were obtained after different times of treatment: (i) promising for electronic applications of the material due to a combination of high carrier mobility, high conductivity, and strong current modulation by gate voltage (up to four orders of magnitude); (ii) a material with insulating properties and graphene quantum dots embedded in an insulating matrix.

  9. Contribution of Dielectric Screening to the Total Capacitance of Few-Layer Graphene Electrodes.

    PubMed

    Zhan, Cheng; Jiang, De-en

    2016-03-01

    We apply joint density functional theory (JDFT), which treats the electrode/electrolyte interface self-consistently, to an electric double-layer capacitor (EDLC) based on few-layer graphene electrodes. The JDFT approach allows us to quantify a third contribution to the total capacitance beyond quantum capacitance (CQ) and EDL capacitance (CEDL). This contribution arises from the dielectric screening of the electric field by the surface of the few-layer graphene electrode, and we therefore term it the dielectric capacitance (CDielec). We find that CDielec becomes significant in affecting the total capacitance when the number of graphene layers in the electrode is more than three. Our investigation sheds new light on the significance of the electrode dielectric screening on the capacitance of few-layer graphene electrodes. PMID:26884129

  10. Contribution of dielectric screening to the total capacitance of few-layer graphene electrodes

    DOE PAGESBeta

    Zhan, Cheng; Jiang, De-en

    2016-02-17

    We apply joint density functional theory (JDFT), which treats the electrode/electrolyte interface self-consistently, to an electric double-layer capacitor (EDLC) based on few-layer graphene electrodes. The JDFT approach allows us to quantify a third contribution to the total capacitance beyond quantum capacitance (CQ) and EDL capacitance (CEDL). This contribution arises from the dielectric screening of the electric field by the surface of the few-layer graphene electrode, and we therefore term it the dielectric capacitance (CDielec). We find that CDielec becomes significant in affecting the total capacitance when the number of graphene layers in the electrode is more than three. In conclusion,more » our investigation sheds new light on the significance of the electrode dielectric screening on the capacitance of few-layer graphene electrodes.« less

  11. Reversible Loss of Bernal Stacking during the Deformation of Few-Layer Graphene in Nanocomposites

    PubMed Central

    2013-01-01

    The deformation of nanocomposites containing graphene flakes with different numbers of layers has been investigated with the use of Raman spectroscopy. It has been found that there is a shift of the 2D band to lower wavenumber and that the rate of band shift per unit strain tends to decrease as the number of graphene layers increases. It has been demonstrated that band broadening takes place during tensile deformation for mono- and bilayer graphene but that band narrowing occurs when the number of graphene layers is more than two. It is also found that the characteristic asymmetric shape of the 2D Raman band for the graphene with three or more layers changes to a symmetrical shape above about 0.4% strain and that it reverts to an asymmetric shape on unloading. This change in Raman band shape and width has been interpreted as being due to a reversible loss of Bernal stacking in the few-layer graphene during deformation. It has been shown that the elastic strain energy released from the unloading of the inner graphene layers in the few-layer material (∼0.2 meV/atom) is similar to the accepted value of the stacking fault energies of graphite and few layer graphene. It is further shown that this loss of Bernal stacking can be accommodated by the formation of arrays of partial dislocations and stacking faults on the basal plane. The effect of the reversible loss of Bernal stacking upon the electronic structure of few-layer graphene and the possibility of using it to modify the electronic structure of few-layer graphene are discussed. PMID:23899378

  12. Reversible loss of Bernal stacking during the deformation of few-layer graphene in nanocomposites.

    PubMed

    Gong, Lei; Young, Robert J; Kinloch, Ian A; Haigh, Sarah J; Warner, Jamie H; Hinks, Jonathan A; Xu, Ziwei; Li, Li; Ding, Feng; Riaz, Ibtsam; Jalil, Rashid; Novoselov, Kostya S

    2013-08-27

    The deformation of nanocomposites containing graphene flakes with different numbers of layers has been investigated with the use of Raman spectroscopy. It has been found that there is a shift of the 2D band to lower wavenumber and that the rate of band shift per unit strain tends to decrease as the number of graphene layers increases. It has been demonstrated that band broadening takes place during tensile deformation for mono- and bilayer graphene but that band narrowing occurs when the number of graphene layers is more than two. It is also found that the characteristic asymmetric shape of the 2D Raman band for the graphene with three or more layers changes to a symmetrical shape above about 0.4% strain and that it reverts to an asymmetric shape on unloading. This change in Raman band shape and width has been interpreted as being due to a reversible loss of Bernal stacking in the few-layer graphene during deformation. It has been shown that the elastic strain energy released from the unloading of the inner graphene layers in the few-layer material (~0.2 meV/atom) is similar to the accepted value of the stacking fault energies of graphite and few layer graphene. It is further shown that this loss of Bernal stacking can be accommodated by the formation of arrays of partial dislocations and stacking faults on the basal plane. The effect of the reversible loss of Bernal stacking upon the electronic structure of few-layer graphene and the possibility of using it to modify the electronic structure of few-layer graphene are discussed. PMID:23899378

  13. Robust adhesion of flower-like few-layer graphene nanoclusters.

    PubMed

    Tian, Shibing; Li, Lin; Sun, Wangning; Xia, Xiaoxiang; Han, Dong; Li, Junjie; Gu, Changzhi

    2012-01-01

    Nanostructured surface possessing ultrahigh adhesion like "gecko foot" or "rose petal" can offer more opportunities for bionic application. We grow flower-like few-layer graphene on silicon nanocone arrays to form graphene nanoclusters, showing robust adhesion. Their contact angle (CA) is 164° with a hysteresis CA of 155° and adhesive force for a 5 μL water droplet is about 254 μN that is far larger than present reported results. We bring experimental evidences that this great adhesion depends on large-area plentiful edges of graphene nanosheets tuned by conical nanostructure and intrinsic wetting features of graphene. Such new hierarchical few-layer graphene nanostructure provides a feasible strategy to understand the ultra-adhesive mechanism of the "gecko effect" or "rose effect" and enhance the wettability of graphene for many practical applications.

  14. Few-layer graphene characterization by near-field scanning microwave microscopy.

    PubMed

    Talanov, Vladimir V; Del Barga, Christopher; Wickey, Lee; Kalichava, Irakli; Gonzales, Edward; Shaner, Eric A; Gin, Aaron V; Kalugin, Nikolai G

    2010-07-27

    Near-field scanning microwave microscopy is employed for quantitative imaging at 4 GHz of the local impedance for monolayer and few-layer graphene. The microwave response of graphene is found to be thickness dependent and determined by the local sheet resistance of the graphene flake. Calibration of the measurement system and knowledge of the probe geometry allows evaluation of the AC impedance for monolayer and few-layer graphene, which is found to be predominantly active. The use of localized evanescent electromagnetic field in our experiment provides a promising tool for investigations of plasma waves in graphene with wave numbers determined by the spatial spectrum of the near-field. By using near-field microwave microscopy one can perform simultaneous imaging of location, geometry, thickness, and distribution of electrical properties of graphene without a need for device fabrication. PMID:20536187

  15. Robust adhesion of flower-like few-layer graphene nanoclusters

    NASA Astrophysics Data System (ADS)

    Tian, Shibing; Li, Lin; Sun, Wangning; Xia, Xiaoxiang; Han, Dong; Li, Junjie; Gu, Changzhi

    2012-07-01

    Nanostructured surface possessing ultrahigh adhesion like ``gecko foot'' or ``rose petal'' can offer more opportunities for bionic application. We grow flower-like few-layer graphene on silicon nanocone arrays to form graphene nanoclusters, showing robust adhesion. Their contact angle (CA) is 164° with a hysteresis CA of 155° and adhesive force for a 5 μL water droplet is about 254 μN that is far larger than present reported results. We bring experimental evidences that this great adhesion depends on large-area plentiful edges of graphene nanosheets tuned by conical nanostructure and intrinsic wetting features of graphene. Such new hierarchical few-layer graphene nanostructure provides a feasible strategy to understand the ultra-adhesive mechanism of the ``gecko effect'' or ``rose effect'' and enhance the wettability of graphene for many practical applications.

  16. Thermoacoustic and photoacoustic characterizations of few-layer graphene by pulsed excitations

    NASA Astrophysics Data System (ADS)

    Wang, Xiong; Witte, Russell S.; Xin, Hao

    2016-04-01

    We characterized the thermoacoustic and photoacoustic properties of large-area, few-layer graphene by pulsed microwave and optical excitations. Due to its high electric conductivity and low heat capacity per unit area, graphene lends itself to excellent microwave and optical energy absorption and acoustic signal emanation due to the thermoacoustic effect. When exposed to pulsed microwave or optical radiation, distinct thermoacoustic and photoacoustic signals generated by the few-layer graphene are obtained due to microwave and laser absorption of the graphene, respectively. Clear thermoacoustic and photoacoustic images of large-area graphene sample are achieved. A numerical model is developed and the simulated results are in good accordance with the measured ones. This characterization work may find applications in ultrasound generator and detectors for microwave and optical radiation. It may also become an alternative characterization approach for graphene and other types of two-dimensional materials.

  17. Monolayer and/or few-layer graphene on metal or metal-coated substrates

    DOEpatents

    Sutter, Peter Werner; Sutter, Eli Anguelova

    2015-04-14

    Disclosed is monolayer and/or few-layer graphene on metal or metal-coated substrates. Embodiments include graphene mirrors. In an example, a mirror includes a substrate that has a surface exhibiting a curvature operable to focus an incident beam onto a focal plane. A graphene layer conformally adheres to the substrate, and is operable to protect the substrate surface from degradation due to the incident beam and an ambient environment.

  18. Few layered graphene Sheet decorated by ZnO Nanoparticles for anti-bacterial application

    NASA Astrophysics Data System (ADS)

    Bykkam, Satish; Narsingam, Sowmya; Ahmadipour, Mohsen; Dayakar, T.; Venkateswara Rao, K.; Shilpa Chakra, Ch.; Kalakotla, Shanker

    2015-07-01

    A widely soluble few layered graphene (FLG) sheets decorated by ZnO nano particles were prepared through hydrothermal method using ethylene glycol as a solvent and a reducing agent. The obtained FLG/ZnO composite material was characterized by X-ray diffraction (XRD), Transmission electron microscopy (TEM) and Raman spectroscopy. The anti-bacterial properties of ZnO nano particles decorated few layered graphenes were tested against Escherichia coli and Salmonella typhi by using well diffusion method. The results confirmed that FLG/ZnO has significant antibacterial activity more against S. typhi than E. coli. The obtained results from the current research work conclusively states that the ZnO nano particles which were decorated by few layered graphene possess a significant anti-bacterial activity.

  19. Few-layer graphene shells and nonmagnetic encapsulates: a versatile and nontoxic carbon nanomaterial.

    PubMed

    Bachmatiuk, Alicja; Mendes, Rafael G; Hirsch, Cordula; Jähne, Carsten; Lohe, Martin R; Grothe, Julia; Kaskel, Stefan; Fu, Lei; Klingeler, Rüdiger; Eckert, Jürgen; Wick, Peter; Rümmeli, Mark H

    2013-12-23

    In this work a simple and scalable approach to coat nonmagnetic nanoparticles with few-layer graphene is presented. In addition, the easy processing of such nanoparticles to remove their core, leaving only the 3D graphene nanoshell, is demonstrated. The samples are comprehensively characterized, as are their versatility in terms of functionalization and as a material for electrochemical storage. Indeed, these 3D graphene nanostructures are easily functionalized much as is found with carbon nanotubes and planar graphene. Electrochemical investigations indicate these nanostructures are promising for stable long-life battery applications. Finally, initial toxicological investigations suggest no acute health risk from these 3D graphene nanostructures.

  20. Roller-style electrostatic printing of prepatterned few-layer-graphenes

    NASA Astrophysics Data System (ADS)

    Liang, Xiaogan; Giacometti, Valentina; Ismach, Ariel; Harteneck, Bruce D.; Olynick, Deirdre L.; Cabrini, Stefano

    2010-01-01

    Electrostatic exfoliation of patterned few-layer-graphenes was demonstrated using a method compatible with high throughput roll-to-roll manufacturing. A patterned graphite template was placed on a roller and used to exfoliate patterned graphene on a planar substrate. The exfoliated graphene features were subsequently characterized by Raman spectroscopy. In comparison with previously demonstrated planar electrostatic exfoliation approach, the roller-style method can create a narrower distribution of thickness of few-layer-graphenes, which is attributed to the combinational action of tangential rolling friction and electrostatic forces. This roller-style electrostatic printing technique could be applied for roll-to-roll manufacturing of graphene-based devices in the future.

  1. Magneto-transport properties of a random distribution of few-layer graphene patches

    NASA Astrophysics Data System (ADS)

    Iacovella, Fabrice; Trinsoutrot, Pierre; Mitioglu, Anatolie; Conédéra, Véronique; Pierre, Mathieu; Raquet, Bertrand; Goiran, Michel; Vergnes, Hugues; Caussat, Brigitte; Plochocka, Paulina; Escoffier, Walter

    2014-11-01

    In this study, we address the electronic properties of conducting films constituted of an array of randomly distributed few layer graphene patches and investigate on their most salient galvanometric features in the moderate and extreme disordered limit. We demonstrate that, in annealed devices, the ambipolar behaviour and the onset of Landau level quantization in high magnetic field constitute robust hallmarks of few-layer graphene films. In the strong disorder limit, however, the magneto-transport properties are best described by a variable-range hopping behaviour. A large negative magneto-conductance is observed at the charge neutrality point, in consistency with localized transport regime.

  2. Hexagonal single crystal domains of few-layer graphene on copper foils.

    PubMed

    Robertson, Alex W; Warner, Jamie H

    2011-03-01

    Hexagonal-shaped single crystal domains of few layer graphene (FLG) are synthesized on copper foils using atmospheric pressure chemical vapor deposition with a high methane flow. Scanning electron microscopy reveals that the graphene domains have a hexagonal shape and are randomly orientated on the copper foil. However, the sites of graphene nucleation exhibit some correlation by forming linear rows. Transmission electron microscopy is used to examine the folded edges of individual domains and reveals they are few-layer graphene consisting of approximately 5-10 layers in the central region and thinning out toward the edges of the domain. Selected area electron diffraction of individual isolated domains reveals they are single crystals with AB Bernal stacking and free from the intrinsic rotational stacking faults that are associated with turbostratic graphite. We study the time-dependent growth dynamics of the domains and show that the final continuous FLG film is polycrystalline, consisting of randomly connected single crystal domains.

  3. Designed nitrogen doping of few-layer graphene functionalized by selective oxygenic groups

    PubMed Central

    2014-01-01

    Few-layer nitrogen doped graphene was synthesized originating from graphene oxide functionalized by selective oxygenic functional groups (hydroxyl, carbonyl, carboxyl etc.) under hydrothermal conditions, respectively. Transmission electron microscopy (TEM) and atomic force microscopy (AFM) observation evidenced few-layer feature of the graphene oxide. X-ray diffraction (XRD) pattern confirmed phase structure of the graphene oxide and reduced graphene oxide. Nitrogen doping content and bonding configuration of the graphene was determined by X-ray photoelectron spectroscopy (XPS), which indicated that different oxygenic functional groups were evidently different in affecting the nitrogen doping process. Compared with other oxygenic groups, carboxyl group played a crucial role in the initial stage of nitrogen doping while hydroxyls exhibited more evident contribution to the doping process in the late stage of the reaction. Formation of graphitic-like nitrogen species was controlled by a synergistic effect of the involved oxygenic groups (e.g., -COOH, -OH, C-O-C, etc.). The doping mechanism of nitrogen in the graphene was scrutinized. The research in this work may not only contribute to the fundamental understandings of nitrogen doping within graphene but promote the development of producing novel graphene-based devices with designed surface functionalization. PMID:25520594

  4. Single adatom dynamics at monatomic steps of free-standing few-layer reduced graphene

    PubMed Central

    Chang, Haixin; Saito, Mitsuhiro; Nagai, Takuro; Liang, Yunye; Kawazoe, Yoshiyuki; Wang, Zhongchang; Wu, Hongkai; Kimoto, Koji; Ikuhara, Yuichi

    2014-01-01

    Steps and their associated adatoms extensively exist and play prominent roles in affecting surface properties of materials. Such impacts should be especially pronounced in two-dimensional, atomically-thin membranes like graphene. However, how single adatom behaves at monatomic steps of few-layer graphene is still illusive. Here, we report dynamics of individual adatom at monatomic steps of free-standing few-layer reduced graphene under the electron beam radiations, and demonstrate the prevalent existence of monatomic steps even down to unexpectedly ultrasmall lateral size of a circular diameter of ~5 Å. Single adatom prefers to stay at the edges of the atomic steps of few-layer reduced graphene and evolve with the steps. Moreover, we also find that how the single adatom behaves at atomic step edges can be remarkably influenced by the type of adatoms and step edges. Such single adatoms at monatomic steps and ultrasmall atomic steps open up a new window for surface physics and chemistry for graphene-based as well as other two-dimensional materials. PMID:25113125

  5. A 3D insight on the catalytic nanostructuration of few-layer graphene

    PubMed Central

    Melinte, G.; Florea, I.; Moldovan, S.; Janowska, I.; Baaziz, W.; Arenal, R.; Wisnet, A.; Scheu, C.; Begin-Colin, S.; Begin, D.; Pham-Huu, C.; Ersen, O.

    2014-01-01

    The catalytic cutting of few-layer graphene is nowadays a hot topic in materials research due to its potential applications in the catalysis field and the graphene nanoribbons fabrication. We show here a 3D analysis of the nanostructuration of few-layer graphene by iron-based nanoparticles under hydrogen flow. The nanoparticles located at the edges or attached to the steps on the FLG sheets create trenches and tunnels with orientations, lengths and morphologies defined by the crystallography and the topography of the carbon substrate. The cross-sectional analysis of the 3D volumes highlights the role of the active nanoparticle identity on the trench size and shape, with emphasis on the topographical stability of the basal planes within the resulting trenches and channels, no matter the obstacle encountered. The actual study gives a deep insight on the impact of nanoparticles morphology and support topography on the 3D character of nanostructures built up by catalytic cutting. PMID:24916201

  6. Synthesis of few layer graphene by direct exfoliation of graphite and a Raman spectroscopic study

    NASA Astrophysics Data System (ADS)

    Gayathri, S.; Jayabal, P.; Kottaisamy, M.; Ramakrishnan, V.

    2014-02-01

    The exfoliation of graphene from pristine graphite in a liquid phase was achieved successfully via sonication followed by centrifugation method. Ultraviolet-visible (UV-vis) spectra of the obtained graphene dispersions at different exfoliation time indicated that the concentration of graphene dispersion increased markedly with increasing exfoliation time. The sheet-like morphology of the exfoliated graphene was revealed by Scanning Electron Microscopy (SEM) image. Further, the morphological change in different exfoliation time was investigated by Atomic Force Microscopy (AFM). A complete structural and defect characterization was probed using micro-Raman spectroscopic technique. The shape and position of the 2D band of Raman spectra revealed the formation of bilayer to few layer graphene. Also, Raman mapping confirmed the presence of uniformly distributed bilayer graphene sheets on the substrate.

  7. Synthesis of Few-Layer Graphene Using DC PE-CVD

    NASA Astrophysics Data System (ADS)

    Kim, Jeong Hyuk; Castro, Edward Joseph D.; Hwang, Yong Gyoo; Lee, Choong Hun

    2011-12-01

    Few layer graphene (FLG) had been successfully grown on polycrystalline Ni films or foils on a large scale using DC Plasma Enhanced Chemical Vapor Deposition (DC PE-CVD) as a result of the Raman spectra drawn out of the sample. The size of graphene films is dependent on the area of the Ni film as well as the DC PE-CVD chamber size. Synthesis time has an effect on the quality of graphene produced. However, further analysis and experiments must be pursued to further identify the optimum settings and conditions of producing better quality graphene. Applied plasma voltage on the other hand, had an influence on the minimization of defects in the graphene grown. It has also presented a method of producing a free standing PMMA/graphene membrane on a FeCl3(aq) solution which could then be transferred to a desired substrate.

  8. A novel mechanical cleavage method for synthesizing few-layer graphenes

    PubMed Central

    2011-01-01

    A novel method to synthesize few layer graphene from bulk graphite by mechanical cleavage is presented here. The method involves the use of an ultrasharp single crystal diamond wedge to cleave a highly ordered pyrolytic graphite sample to generate the graphene layers. Cleaving is aided by the use of ultrasonic oscillations along the wedge. Characterization of the obtained layers shows that the process is able to synthesize graphene layers with an area of a few micrometers. Application of oscillation enhances the quality of the layers produced with the layers having a reduced crystallite size as determined from the Raman spectrum. Interesting edge structures are observed that needs further investigation. PMID:21711598

  9. Hydrothermal synthesis of highly nitrogen-doped few-layer graphene via solid–gas reaction

    SciTech Connect

    Liang, Xianqing; Zhong, Jun; Shi, Yalin; Guo, Jin; Huang, Guolong; Hong, Caihao; Zhao, Yidong

    2015-01-15

    Highlights: • A novel approach to synthesis of N-doped few-layer graphene has been developed. • The high doping levels of N in products are achieved. • XPS and XANES results reveal a thermal transformation of N bonding configurations. • The developed method is cost-effective and eco-friendly. - Abstract: Nitrogen-doped (N-doped) graphene sheets with high doping concentration were facilely synthesized through solid–gas reaction of graphene oxide (GO) with ammonia vapor in a self-designed hydrothermal system. The morphology, surface chemistry and electronic structure of N-doped graphene sheets were investigated by TEM, AFM, XRD, XPS, XANES and Raman characterizations. Upon hydrothermal treatment, up to 13.22 at% of nitrogen could be introduced into the crumpled few-layer graphene sheets. Both XPS and XANES analysis reveal that the reaction between oxygen functional groups in GO and ammonia vapor produces amide and amine species in hydrothermally treated GO (HTGO). Subsequent thermal annealing of the resultant HTGO introduces a gradual transformation of nitrogen bonding configurations in graphene sheets from amine N to pyridinic and graphitic N with the increase of annealing temperature. This study provides a simple but cost-effective and eco-friendly method to prepare N-doped graphene materials in large-scale for potential applications.

  10. Stacking sequence and interlayer coupling in few-layer graphene revealed by in situ imaging

    PubMed Central

    Wang, Zhu-Jun; Dong, Jichen; Cui, Yi; Eres, Gyula; Timpe, Olaf; Fu, Qiang; Ding, Feng; Schloegl, R.; Willinger, Marc-Georg

    2016-01-01

    In the transition from graphene to graphite, the addition of each individual graphene layer modifies the electronic structure and produces a different material with unique properties. Controlled growth of few-layer graphene is therefore of fundamental interest and will provide access to materials with engineered electronic structure. Here we combine isothermal growth and etching experiments with in situ scanning electron microscopy to reveal the stacking sequence and interlayer coupling strength in few-layer graphene. The observed layer-dependent etching rates reveal the relative strength of the graphene–graphene and graphene–substrate interaction and the resulting mode of adlayer growth. Scanning tunnelling microscopy and density functional theory calculations confirm a strong coupling between graphene edge atoms and platinum. Simulated etching confirms that etching can be viewed as reversed growth. This work demonstrates that real-time imaging under controlled atmosphere is a powerful method for designing synthesis protocols for sp2 carbon nanostructures in between graphene and graphite. PMID:27759024

  11. Resistance and rupture analysis of single- and few-layer graphene nanosheets impacted by various projectiles

    NASA Astrophysics Data System (ADS)

    Sadeghzadeh, Sadegh; Liu, Ling

    2016-09-01

    In this paper, a quasi-classical model for the collision of various nanoparticles with single- and few-layer graphene nanosheets was introduced as a multi-scale approach that couples non-equilibrium molecular dynamics with the Finite Element Method. As a resistance criterion, it was observed that the coefficient of restitution and the induced stresses depend on the impact velocity of projectile. These parameters were evaluated computationally, and it was revealed that certain resulting behaviors differ from behaviors at the macro scale. By obtaining an out-of-plane yield stress limit of 1.0 TPa for graphene, the stress analysis of single- and multi-layer graphene sheets revealed that the limit projectile velocity needed for the yielding of graphene sheets increases with the increase in the number of layers. For aluminum nanoparticles, this increase is almost linear, and for other metals, it slightly deviates from the linear trend. It was also observed that the graphene sheets have a different rupture form when impacted by gaseous molecules than by metal particles. Considering the very high momentum of gas molecules and their shock-like behavior during high-speed collisions with a graphene sheet, pores with a size of one carbon atom can be created in graphene sheets. Since a single-layer graphene sheet can withstand a projectile which is 3.64 times larger than a projectile impacting a 20-layer graphene sheet, spaced graphene sheets seem to be more effective in absorbing the impact energy of projectiles than conventional few-layer graphene sheets.

  12. Few-layer graphene as a support film for transmission electron microscopy imaging of nanoparticles.

    PubMed

    McBride, James R; Lupini, Andrew R; Schreuder, Michael A; Smith, Nathanael J; Pennycook, Stephen J; Rosenthal, Sandra J

    2009-12-01

    One consistent limitation for high-resolution imaging of small nanoparticles is the high background signal from the amorphous carbon support film. With interest growing for smaller and smaller nanostructures, state of the art electron microscopes are becoming necessary for rudimentary tasks, such as nanoparticle sizing. As a monolayer of carbon, free-standing graphene represents the ultimate support film for nanoparticle imaging. In this work, conventional high-resolution transmission electron microscopy (HRTEM) and aberration-corrected scanning transmission electron microscopy (STEM) were used to assess the benefits and feasibility of few-layer graphene support films. Suspensions of few-layer graphene to produce the support films were prepared by simple sonication of exfoliated graphite. The greatest benefit was observed for conventional HRTEM, where lattice resolved imaging of sub 2 nm CdSe nanocrystals was achieved. The few-layer graphene films were also used as a support film for C(s)-corrected STEM and electron energy loss spectroscopy of CuInSe(2) nanocrystals. PMID:20356171

  13. Few-layer graphene growth from polystyrene as solid carbon source utilizing simple APCVD method

    NASA Astrophysics Data System (ADS)

    Ahmadi, Shahrokh; Afzalzadeh, Reza

    2016-07-01

    This research article presents development of an economical, simple, immune and environment friendly process to grow few-layer graphene by controlling evaporation rate of polystyrene on copper foil as catalyst and substrate utilizing atmospheric pressure chemical vapor deposition (APCVD) method. Evaporation rate of polystyrene depends on molecular structure, amount of used material and temperature. We have found controlling rate of evaporation of polystyrene by controlling the source temperature is easier than controlling the material weight. Atomic force microscopy (AFM) as well as Raman Spectroscopy has been used for characterization of the layers. The frequency of G‧ to G band ratio intensity in some samples varied between 0.8 and 1.6 corresponding to few-layer graphene. Topography characterization by atomic force microscopy confirmed Raman results.

  14. Synthesis of transparent vertically aligned TiO2 nanotubes on a few-layer graphene (FLG) film.

    PubMed

    Cottineau, Thomas; Albrecht, Arnaud; Janowska, Izabela; Macher, Nicolas; Bégin, Dominique; Ledoux, Marc Jacques; Pronkin, Sergey; Savinova, Elena; Keller, Nicolas; Keller, Valérie; Pham-Huu, Cuong

    2012-01-30

    Novel transparent 1D-TiO(2)/few-layer graphene electrodes are realised by the anodic growth of vertically aligned TiO(2) nano-tubes on a few-layer graphene film coated on a glass substrate. PMID:22057023

  15. Environmental Synthesis of Few Layers Graphene Sheets Using Ultrasonic Exfoliation with Enhanced Electrical and Thermal Properties.

    PubMed

    Noroozi, Monir; Zakaria, Azmi; Radiman, Shahidan; Abdul Wahab, Zaidan

    2016-01-01

    In this paper, we report how few layers graphene that can be produced in large quantity with low defect ratio from exfoliation of graphite by using a high intensity probe sonication in water containing liquid hand soap and PVP. It was founded that the graphene powder obtained by this simple exfoliation method after the heat treatment had an excellent exfoliation into a single or layered graphene sheets. The UV-visible spectroscopy, FESEM, TEM, X-ray powder diffraction and Raman spectroscopy was used to analyse the graphene product. The thermal diffusivity of the samples was analysed using a highly accurate thermal-wave cavity photothermal technique. The data obtained showed excellent enhancement in the thermal diffusivity of the graphene dispersion. This well-dispersed graphene was then used to fabricate an electrically conductive polymer-graphene film composite. The results demonstrated that this low cost and environmental friendly technique allowed to the production of high quality layered graphene sheets, improved the thermal and electrical properties. This may find use in the wide range of applications based on graphene. PMID:27064575

  16. Environmental Synthesis of Few Layers Graphene Sheets Using Ultrasonic Exfoliation with Enhanced Electrical and Thermal Properties.

    PubMed

    Noroozi, Monir; Zakaria, Azmi; Radiman, Shahidan; Abdul Wahab, Zaidan

    2016-01-01

    In this paper, we report how few layers graphene that can be produced in large quantity with low defect ratio from exfoliation of graphite by using a high intensity probe sonication in water containing liquid hand soap and PVP. It was founded that the graphene powder obtained by this simple exfoliation method after the heat treatment had an excellent exfoliation into a single or layered graphene sheets. The UV-visible spectroscopy, FESEM, TEM, X-ray powder diffraction and Raman spectroscopy was used to analyse the graphene product. The thermal diffusivity of the samples was analysed using a highly accurate thermal-wave cavity photothermal technique. The data obtained showed excellent enhancement in the thermal diffusivity of the graphene dispersion. This well-dispersed graphene was then used to fabricate an electrically conductive polymer-graphene film composite. The results demonstrated that this low cost and environmental friendly technique allowed to the production of high quality layered graphene sheets, improved the thermal and electrical properties. This may find use in the wide range of applications based on graphene.

  17. Environmental Synthesis of Few Layers Graphene Sheets Using Ultrasonic Exfoliation with Enhanced Electrical and Thermal Properties

    PubMed Central

    Noroozi, Monir; Zakaria, Azmi; Radiman, Shahidan; Abdul Wahab, Zaidan

    2016-01-01

    In this paper, we report how few layers graphene that can be produced in large quantity with low defect ratio from exfoliation of graphite by using a high intensity probe sonication in water containing liquid hand soap and PVP. It was founded that the graphene powder obtained by this simple exfoliation method after the heat treatment had an excellent exfoliation into a single or layered graphene sheets. The UV-visible spectroscopy, FESEM, TEM, X-ray powder diffraction and Raman spectroscopy was used to analyse the graphene product. The thermal diffusivity of the samples was analysed using a highly accurate thermal-wave cavity photothermal technique. The data obtained showed excellent enhancement in the thermal diffusivity of the graphene dispersion. This well-dispersed graphene was then used to fabricate an electrically conductive polymer-graphene film composite. The results demonstrated that this low cost and environmental friendly technique allowed to the production of high quality layered graphene sheets, improved the thermal and electrical properties. This may find use in the wide range of applications based on graphene. PMID:27064575

  18. The effect of spin-orbit coupling in band structure of few-layer graphene

    SciTech Connect

    Sahdan, Muhammad Fauzi Darma, Yudi

    2014-03-24

    Topological insulators are electronic materials that have a bulk band gap like an ordinary insulator but have protected conducting states on their edge or surface. This can be happened due to spin-orbit coupling and time-reversal symmetry. Moreover, the edge current flows through their edge or surface depends on its spin orientation and also it is robust against non-magnetic impurities. Therefore, topological insulators are predicted to be useful ranging from spintronics to quantum computation. Graphene was first predicted to be the precursor of topological insulator by Kane-Mele. They developed a Hamiltonian model to describe the gap opening in graphene. In this work, we investigate the band structure of few-layer graphene by using this model with analytical approach. The results of our calculations show that the gap opening occurs at K and K’ point, not only in single layer, but also in bilayer and trilayer graphene.

  19. Synthesis of few-layered graphene by H{sub 2}O{sub 2} plasma etching of graphite

    SciTech Connect

    Zhao Guixia; Shao Dadong; Chen Changlun; Wang Xiangke

    2011-05-02

    Herein, we reported an approach to synthesize few-layered graphene by etching of the graphite using H{sub 2}O{sub 2} plasma technique. The synthesized few-layered graphene was characterized by scanning electron microscopy, atomic force microscopy, Raman spectroscopy, and x-ray photoelectron spectroscopy (XPS). The analysis showed that few-layered graphene was formed in high quality level. The XPS analysis suggested that H{sub 2}O{sub 2} plasma etching of graphite could oxidize graphene and generated -C-OH and >C=O groups on the graphene surfaces. The H{sub 2}O{sub 2} plasma technique is an easy and environmental friendly method to synthesize few-layered graphene from the graphite.

  20. Controlling single and few-layer graphene crystals growth in a solid carbon source based chemical vapor deposition

    SciTech Connect

    Papon, Remi; Sharma, Subash; Shinde, Sachin M.; Vishwakarma, Riteshkumar; Tanemura, Masaki; Kalita, Golap

    2014-09-29

    Here, we reveal the growth process of single and few-layer graphene crystals in the solid carbon source based chemical vapor deposition (CVD) technique. Nucleation and growth of graphene crystals on a polycrystalline Cu foil are significantly affected by the injection of carbon atoms with pyrolysis rate of the carbon source. We observe micron length ribbons like growth front as well as saturated growth edges of graphene crystals depending on growth conditions. Controlling the pyrolysis rate of carbon source, monolayer and few-layer crystals and corresponding continuous films are obtained. In a controlled process, we observed growth of large monolayer graphene crystals, which interconnect and merge together to form a continuous film. On the other hand, adlayer growth is observed with an increased pyrolysis rate, resulting few-layer graphene crystal structure and merged continuous film. The understanding of monolayer and few-layer crystals growth in the developed CVD process can be significant to grow graphene with controlled layer numbers.

  1. Structural and optical properties of cobalt slanted nanopillars conformally coated with few-layer graphene

    SciTech Connect

    Wilson, Peter M.; Lipatov, Alexey; Schmidt, Daniel; Schubert, Eva; Schubert, Mathias; Hofmann, Tino E-mail: thofmann@engr.unl.edu; Sinitskii, Alexander E-mail: thofmann@engr.unl.edu

    2015-06-08

    Optical characterization of anisotropic multicomponent nanostructures is generally not a trivial task, since the relation between a material's structural properties and its permittivity tensor is nonlinear. In this regard, an array of slanted cobalt nanopillars that are conformally coated with few-layer graphene is a particularly challenging object for optical characterization, as it has a complex anisotropic geometry and comprises several materials with different topologies and filling fractions. Normally, a detailed characterization of such complex nanostructures would require a combination of several microscopic and spectroscopic techniques. In this letter, we demonstrate that the important structural parameters of these graphene-coated sculptured thin films can be determined using a fast and simple generalized spectroscopic ellipsometry test combined with an anisotropic Bruggeman effective medium approximation. The graphene coverage as well as structural parameters of nanostructured thin films agree excellently with electron microscopy and Raman spectroscopy observations. The demonstrated optical approach may also be applied to the characterization of other nanostructured materials.

  2. Electronic Raman scattering in graphite and single-layer and few-layer graphene

    NASA Astrophysics Data System (ADS)

    Ponosov, Yu. S.; Ushakov, A. V.; Streltsov, S. V.

    2015-05-01

    We investigated polarization-resolved electronic Raman scattering in different graphitic structures, including bulk graphite and single-layer and few-layer graphene. For all investigated samples, the broad continua of interband electronic transitions were detected at an energy ˜0.35 eV, while they were expected to be at ˜6 eV [Phys. Rev. B 88, 085416 (2013), 10.1103/PhysRevB.88.085416]. The symmetry of the observed excitations corresponds to the A2 g irreducible representation. A quasilinear behavior of the Raman response is observed at low energies in all cases at room temperature, in agreement with performed tight-binding calculations. High-energy features at ˜0.8 eV are detected in the spectra of graphite and few-layer graphene. They are attributed to interband transitions in the vicinity of the K point, which involve electronic bands split by interlayer interaction. The effects of the substrate type, defect amount, and doping on the continuum line shape and symmetry are discovered. The silent layer-breathing mode is observed in a single-layer graphene. The results evidence that the electronic light scattering in graphitic structures without an external magnetic field is a powerful tool, which provides a variety of data on the structure and symmetry of low-energy electronic excitations.

  3. Few layer graphene-polypropylene nanocomposites: the role of flake diameter.

    PubMed

    Vallés, Cristina; Abdelkader, Amr M; Young, Robert J; Kinloch, Ian A

    2014-01-01

    Graphene shows excellent potential as a structural reinforcement in polymer nanocomposites due to its exceptional mechanical properties. We have shown previously that graphene composites can be analysed using conventional composite theory with the graphene flakes acting as short fillers which have a critical length of ∼3 μm which is required for good reinforcement. Herein, polypropylene (PP) nanocomposites were prepared using electrochemically-exfoliated few layer graphene (FLG) with two different flake diameters (5 μm and 20 μm). The crystallization temperature and degree of crystallinity of the PP were found to increase with the loading of FLG, which suggests that the flakes acted as crystallisation nucleation sites. Mechanical testing showed that the 5 μm flakes behaved as short fillers and reinforced the PP matrix poorly. The modulus of the 20 μm flake composites, however, increased linearly with loading up to 20 wt%, without any of the detrimental aggregation effects seen in other graphene systems. The mechanical data were compared with our previous work on other graphene composite systems and the apparent need to balance the degree of functionalization to improve matrix compatibility whilst not encouraging aggregation is discussed.

  4. Significant thickness dependence of the thermal resistance between few-layer graphenes

    NASA Astrophysics Data System (ADS)

    Ni, Yuxiang; Chalopin, Yann; Volz, Sebastian

    2013-08-01

    The inter-layer resistance in few layer graphene (FLG) is an unknown intrinsic property that affects the heat removal efficiency of FLG-based thermal devices. Here we present data that demonstrates the layer number dependence of the resistance between FLGs, by using molecular dynamics simulations. The resistance was found to decrease as the layer number increases. FLGs with larger thicknesses are proposed to be advantageous in heat spreading owing to their lower contact resistances. The observed properties do not depend on temperature, which is crucial for FLG based structures to retain a stable heat removal efficiency while working at a large temperature range.

  5. Influence of irradiation upon few-layered graphene using electron-beams and gamma-rays

    SciTech Connect

    Wang, Yuqing; Feng, Yi Mo, Fei; Qian, Gang; Chen, Yangming; Yu, Dongbo; Wang, Yang; Zhang, Xuebin

    2014-07-14

    Few-layered graphene (FLG) is irradiated by electron beams and gamma rays. After 100 keV electron irradiation, the edges of FLG start bending, shrinking, and finally generate gaps and carbon onions due to sputtering and knock-on damage mechanism. When the electron beam energy is increased further to 200 keV, FLG suffers rapid and catastrophic destruction. Unlike electron irradiation, Compton effect is the dominant damage mechanism in gamma irradiation. The irradiation results indicate the crystallinity of FLG decreases first, then restores as increasing irradiation doses, additionally, the ratio (O/C) of FLG surface and the relative content of oxygen groups increases after irradiation.

  6. Self-organized arrays of graphene and few-layer graphene quantum dots in fluorographene matrix: Charge transient spectroscopy

    SciTech Connect

    Antonova, Irina V.; Nebogatikova, Nadezhda A.; Prinz, Victor Ya.

    2014-05-12

    Arrays of graphene or few-layer graphene quantum dots (QDs) embedded in a partially fluorinated graphene matrix were created by chemical functionalization of layers. Charge transient spectroscopy employed for investigation of obtained QD systems (size 20–70 nm) has allowed us to examine the QD energy spectra and the time of carrier emission (or charge relaxation) from QDs as a function of film thickness. It was found that the characteristic time of carrier emission from QDs decreased markedly (by about four orders of magnitude) on increasing the QD thickness from one graphene monolayer to 3 nm. Daylight-assisted measurements also demonstrate a strong decrease of the carrier emission time.

  7. High-yield synthesis of few-layer graphene flakes through electrochemical expansion of graphite in propylene carbonate electrolyte.

    PubMed

    Wang, Junzhong; Manga, Kiran Kumar; Bao, Qiaoliang; Loh, Kian Ping

    2011-06-15

    High-yield production of few-layer graphene flakes from graphite is important for the scalable synthesis and industrial application of graphene. However, high-yield exfoliation of graphite to form graphene sheets without using any oxidation process or super-strong acid is challenging. Here we demonstrate a solution route inspired by the lithium rechargeable battery for the high-yield (>70%) exfoliation of graphite into highly conductive few-layer graphene flakes (average thickness <5 layers). A negative graphite electrode can be electrochemically charged and expanded in an electrolyte of Li salts and organic solvents under high current density and exfoliated efficiently into few-layer graphene sheets with the aid of sonication. The dispersible graphene can be ink-brushed to form highly conformal coatings of conductive films (15 ohm/square at a graphene loading of <1 mg/cm(2)) on commercial paper. PMID:21557613

  8. Few layers isolated graphene domains grown on copper foils by microwave surface wave plasma CVD using camphor as a precursor

    NASA Astrophysics Data System (ADS)

    Ram Aryal, Hare; Adhikari, Sudip; Uchida, Hideo; Wakita, Koichi; Umeno, Masayoshi

    2016-03-01

    Few layers isolated graphene domains were grown by microwave surface wave plasma CVD technique using camphor at low temperature. Graphene nucleation centers were suppressed on pre-annealed copper foils by supplying low dissociation energy. Scanning electron microscopy study of time dependent growth reveals that graphene nucleation centers were preciously suppressed, which indicates the possibility of controlled growth of large area single crystal graphene domains by plasma processing. Raman spectroscopy revealed that the graphene domains are few layered which consist of relatively low defects.

  9. Chemical Vapor Deposited Few-Layer Graphene as an Electron Field Emitter.

    PubMed

    Behural, Sanjay K; Nayak, Sasmita; Yang, Qiaoqin; Hirose, Akira; Janil, Omkar

    2016-01-01

    Chemical vapor deposition (CVD) growth of graphene on polycrystalline copper (Cu) foil in a low pressure conditions has been presented, aiming to achieve the highest quality with large-scale fabrications, which requires comprehensive understanding and effective controlling of the growth process. Herein, few-layer graphene (FLG) films with large-domain sizes were grown on Cu metal catalyst substrates using a vertical mass-flow hot-filament CVD reactor, with the intention of large scale production, by optimizing the CVD system and three of the process parameters: (i) gas flow compositions, (ii) substrate annealing time and (iii) graphene deposition time. The detailed scanning electron microscope and Raman spectroscopy analysis indicate that all the above mentioned process parameters affect growth of FLG film on Cu substrate. The presence of two intense peaks, G and 2D-band at 1583.6 and 2702.6 cm⁻¹ for synthesized sample at optimized conditions (H₂/CH₄ ratio of 50:1 at graphene deposition time of 10 minutes and substrate annealed time for 20 minutes) revealed the formation of FLG films with large domain size. These graphene films on Cu have shown the room temperature field electron emission characteristics, hence appears to be prospective candidate for vacuum nanoelectronics. PMID:27398456

  10. Thermal transport in three-dimensional foam architectures of few-layer graphene and ultrathin graphite.

    PubMed

    Pettes, Michael Thompson; Ji, Hengxing; Ruoff, Rodney S; Shi, Li

    2012-06-13

    At a very low solid concentration of 0.45 ± 0.09 vol %, the room-temperature thermal conductivity (κ(GF)) of freestanding graphene-based foams (GF), comprised of few-layer graphene (FLG) and ultrathin graphite (UG) synthesized through the use of methane chemical vapor deposition on reticulated nickel foams, was increased from 0.26 to 1.7 W m(-1) K(-1) after the etchant for the sacrificial nickel support was changed from an aggressive hydrochloric acid solution to a slow ammonium persulfate etchant. In addition, κ(GF) showed a quadratic dependence on temperature between 11 and 75 K and peaked at about 150 K, where the solid thermal conductivity (κ(G)) of the FLG and UG constituents reached about 1600 W m(-1) K(-1), revealing the benefit of eliminating internal contact thermal resistance in the continuous GF structure.

  11. Temperature-activated layer-breathing vibrations in few-layer graphene.

    PubMed

    Lui, Chun Hung; Ye, Zhipeng; Keiser, Courtney; Xiao, Xun; He, Rui

    2014-08-13

    We investigated the low-frequency Raman spectra of freestanding few-layer graphene (FLG) at varying temperatures (400-900 K) controlled by laser heating. At high temperature, we observed the fundamental Raman mode for the lowest-frequency branch of rigid-plane layer-breathing mode (LBM) vibration. The mode frequency redshifts dramatically from 81 cm(-1) for bilayer to 23 cm(-1) for 8-layer. The thickness dependence is well described by a simple model of coupled oscillators. Notably, the LBM Raman response is unobservable at room temperature, and it is turned on at higher temperature (>600 K) with a steep increase of Raman intensity. The observation suggests that the LBM vibration is strongly suppressed by molecules adsorbed on the graphene surface but is activated as desorption occurs at high temperature.

  12. Carrier lifetime in exfoliated few-layer graphene determined from intersubband optical transitions.

    PubMed

    Limmer, Thomas; Feldmann, Jochen; Da Como, Enrico

    2013-05-24

    We report a femtosecond transient spectroscopy study in the near to middle infrared range, 0.8-0.35 eV photon energy, on graphene and few layer graphene single flakes. The spectra show an evolving structure of photoinduced absorption bands superimposed on the bleaching caused by Pauli blocking of the interband optically coupled states. Supported by tight-binding model calculations, we assign the photoinduced absorption features to intersubband transitions as the number of layers is increased. Interestingly, the intersubband photoinduced resonances show a longer dynamics than the interband bleaching, because of their independence from the absolute energy of the carriers with respect to the Dirac point. The dynamic of these intersubband transitions reflects the lifetime of the hot carriers and provides an elegant method to access it in this important class of semimetals.

  13. Carrier Lifetime in Exfoliated Few-Layer Graphene Determined from Intersubband Optical Transitions

    NASA Astrophysics Data System (ADS)

    Limmer, Thomas; Feldmann, Jochen; Da Como, Enrico

    2013-05-01

    We report a femtosecond transient spectroscopy study in the near to middle infrared range, 0.8-0.35 eV photon energy, on graphene and few layer graphene single flakes. The spectra show an evolving structure of photoinduced absorption bands superimposed on the bleaching caused by Pauli blocking of the interband optically coupled states. Supported by tight-binding model calculations, we assign the photoinduced absorption features to intersubband transitions as the number of layers is increased. Interestingly, the intersubband photoinduced resonances show a longer dynamics than the interband bleaching, because of their independence from the absolute energy of the carriers with respect to the Dirac point. The dynamic of these intersubband transitions reflects the lifetime of the hot carriers and provides an elegant method to access it in this important class of semimetals.

  14. Interlayer catalytic exfoliation realizing scalable production of large-size pristine few-layer graphene.

    PubMed

    Geng, Xiumei; Guo, Yufen; Li, Dongfang; Li, Weiwei; Zhu, Chao; Wei, Xiangfei; Chen, Mingliang; Gao, Song; Qiu, Shengqiang; Gong, Youpin; Wu, Liqiong; Long, Mingsheng; Sun, Mengtao; Pan, Gebo; Liu, Liwei

    2013-01-01

    Mass production of reduced graphene oxide and graphene nanoplatelets has recently been achieved. However, a great challenge still remains in realizing large-quantity and high-quality production of large-size thin few-layer graphene (FLG). Here, we create a novel route to solve the issue by employing one-time-only interlayer catalytic exfoliation (ICE) of salt-intercalated graphite. The typical FLG with a large lateral size of tens of microns and a thickness less than 2 nm have been obtained by a mild and durative ICE. The high-quality graphene layers preserve intact basal crystal planes owing to avoidance of the degradation reaction during both intercalation and ICE. Furthermore, we reveal that the high-quality FLG ensures a remarkable lithium-storage stability (>1,000 cycles) and a large reversible specific capacity (>600 mAh g(-1)). This simple and scalable technique acquiring high-quality FLG offers considerable potential for future realistic applications.

  15. Interlayer catalytic exfoliation realizing scalable production of large-size pristine few-layer graphene

    NASA Astrophysics Data System (ADS)

    Geng, Xiumei; Guo, Yufen; Li, Dongfang; Li, Weiwei; Zhu, Chao; Wei, Xiangfei; Chen, Mingliang; Gao, Song; Qiu, Shengqiang; Gong, Youpin; Wu, Liqiong; Long, Mingsheng; Sun, Mengtao; Pan, Gebo; Liu, Liwei

    2013-01-01

    Mass production of reduced graphene oxide and graphene nanoplatelets has recently been achieved. However, a great challenge still remains in realizing large-quantity and high-quality production of large-size thin few-layer graphene (FLG). Here, we create a novel route to solve the issue by employing one-time-only interlayer catalytic exfoliation (ICE) of salt-intercalated graphite. The typical FLG with a large lateral size of tens of microns and a thickness less than 2 nm have been obtained by a mild and durative ICE. The high-quality graphene layers preserve intact basal crystal planes owing to avoidance of the degradation reaction during both intercalation and ICE. Furthermore, we reveal that the high-quality FLG ensures a remarkable lithium-storage stability (>1,000 cycles) and a large reversible specific capacity (>600 mAh g-1). This simple and scalable technique acquiring high-quality FLG offers considerable potential for future realistic applications.

  16. MgO-decorated few-layered graphene as an anode for li-ion batteries.

    PubMed

    Petnikota, Shaikshavali; Rotte, Naresh K; Reddy, M V; Srikanth, Vadali V S S; Chowdari, B V R

    2015-02-01

    Combustion of magnesium in dry ice and a simple subsequent acid treatment step resulted in a MgO-decorated few-layered graphene (FLG) composite that has a specific surface area of 393 m(2)/g and an average pore volume of 0.9 cm(3)/g. As an anode material in Li-ion batteries, the composite exhibited high reversible capacity and excellent cyclic performance in spite of high first-cycle irreversible capacity loss. A reversible capacity as high as 1052 mAh/g was measured during the first cycle. Even at the end of the 60th cycle, more than 83% of the capacity could be retained. Cyclic voltammetry results indicated pseudocapacitance behavior due to electrochemical absorption and desorption of lithium ions onto graphene. An increase in the capacity has been observed during long-term cycling owing to electrochemical exfoliation of graphene sheets. Owing to its good thermal stability and superior cyclic performance with high reversible capacities, MgO-decked FLG can be an excellent alternative to graphite as an anode material in Li-ion batteries, after suitable modifications. PMID:25559260

  17. Direct Preparation of Few Layer Graphene Epoxy Nanocomposites from Untreated Flake Graphite.

    PubMed

    Throckmorton, James; Palmese, Giuseppe

    2015-07-15

    The natural availability of flake graphite and the exceptional properties of graphene and graphene-polymer composites create a demand for simple, cost-effective, and scalable methods for top-down graphite exfoliation. This work presents a novel method of few layer graphite nanocomposite preparation directly from untreated flake graphite using a room temperature ionic liquid and laminar shear processing regimen. The ionic liquid serves both as a solvent and initiator for epoxy polymerization and is incorporated chemically into the matrix. This nanocomposite shows low electrical percolation (0.005 v/v) and low thickness (1-3 layers) graphite/graphene flakes by TEM. Additionally, the effect of processing conditions by rheometry and comparison with solvent-free conditions reveal the interactions between processing and matrix properties and provide insight into the theory of the chemical and physical exfoliation of graphite crystals and the resulting polymer matrix dispersion. An interaction model that correlates the interlayer shear physics of graphite flakes and processing parameters is proposed and tested.

  18. Electrostatic force microscopy and electrical isolation of etched few-layer graphene nano-domains

    SciTech Connect

    Hunley, D. Patrick; Sundararajan, Abhishek; Boland, Mathias J.; Strachan, Douglas R.

    2014-12-15

    Nanostructured bi-layer graphene samples formed through catalytic etching are investigated with electrostatic force microscopy. The measurements and supporting computations show a variation in the microscopy signal for different nano-domains that are indicative of changes in capacitive coupling related to their small sizes. Abrupt capacitance variations detected across etch tracks indicates that the nano-domains have strong electrical isolation between them. Comparison of the measurements to a resistor-capacitor model indicates that the resistance between two bi-layer graphene regions separated by an approximately 10 nm wide etch track is greater than about 1×10{sup 12} Ω with a corresponding gap resistivity greater than about 3×10{sup 14} Ω⋅nm. This extremely large gap resistivity suggests that catalytic etch tracks within few-layer graphene samples are sufficient for providing electrical isolation between separate nano-domains that could permit their use in constructing atomically thin nanogap electrodes, interconnects, and nanoribbons.

  19. Identifying active functionalities on few-layered graphene catalysts for oxidative dehydrogenation of isobutane.

    PubMed

    Dathar, Gopi Krishna Phani; Tsai, Yu-Tung; Gierszal, Kamil; Xu, Ye; Liang, Chengdu; Rondinone, Adam J; Overbury, Steven H; Schwartz, Viviane

    2014-02-01

    The general consensus in the studies of nanostructured carbon catalysts for oxidative dehydrogenation (ODH) of alkanes to olefins is that the oxygen functionalities generated during synthesis and reaction are responsible for the catalytic activity of these nanostructured carbons. Identification of the highly active oxygen functionalities would enable engineering of nanocarbons for ODH of alkanes. Few-layered graphenes were used as model catalysts in experiments to synthesize reduced graphene oxide samples with varying oxygen concentrations, to characterize oxygen functionalities, and to measure the activation energies for ODH of isobutane. Periodic density functional theory calculations were performed on graphene nanoribbon models with a variety of oxygen functionalities at the edges to calculate their thermal stability and to model reaction mechanisms for ODH of isobutane. Comparing measured and calculated thermal stability and activation energies leads to the conclusion that dicarbonyls at the zigzag edges and quinones at armchair edges are appropriately balanced for high activity, relative to other model functionalities considered herein. In the ODH of isobutane, both dehydrogenation and regeneration of catalytic sites are relevant at the dicarbonyls, whereas regeneration is facile compared with dehydrogenation at quinones. The catalytic mechanism involves weakly adsorbed isobutane reducing functional oxygen and leaving as isobutene, and O2 in the feed, weakly adsorbed on the hydrogenated functionality, reacting with that hydrogen and regenerating the catalytic sites.

  20. MgO-decorated few-layered graphene as an anode for li-ion batteries.

    PubMed

    Petnikota, Shaikshavali; Rotte, Naresh K; Reddy, M V; Srikanth, Vadali V S S; Chowdari, B V R

    2015-02-01

    Combustion of magnesium in dry ice and a simple subsequent acid treatment step resulted in a MgO-decorated few-layered graphene (FLG) composite that has a specific surface area of 393 m(2)/g and an average pore volume of 0.9 cm(3)/g. As an anode material in Li-ion batteries, the composite exhibited high reversible capacity and excellent cyclic performance in spite of high first-cycle irreversible capacity loss. A reversible capacity as high as 1052 mAh/g was measured during the first cycle. Even at the end of the 60th cycle, more than 83% of the capacity could be retained. Cyclic voltammetry results indicated pseudocapacitance behavior due to electrochemical absorption and desorption of lithium ions onto graphene. An increase in the capacity has been observed during long-term cycling owing to electrochemical exfoliation of graphene sheets. Owing to its good thermal stability and superior cyclic performance with high reversible capacities, MgO-decked FLG can be an excellent alternative to graphite as an anode material in Li-ion batteries, after suitable modifications.

  1. Tribological characteristics of few-layer graphene over Ni grain and interface boundaries.

    PubMed

    Tripathi, Manoj; Awaja, Firas; Paolicelli, Guido; Bartali, Ruben; Iacob, Erica; Valeri, Sergio; Ryu, Seunghwa; Signetti, Stefano; Speranza, Giorgio; Pugno, Nicola Maria

    2016-03-28

    The tribological properties of metal-supported few-layered graphene depend strongly on the grain topology of the metal substrate. Inhomogeneous distribution of graphene layers at such regions led to variable landscapes with distinguishable roughness. This discrepancy in morphology significantly affects the frictional and wetting characteristics of the FLG system. We discretely measured friction characteristics of FLG covering grains and interfacial grain boundaries of polycrystalline Ni metal substrate via an atomic force microscopy (AFM) probe. The friction coefficient of FLG covered at interfacial grain boundaries is found to be lower than that on grains in vacuum (at 10(-5) Torr pressure) and similar results were obtained in air condition. Sliding history with AFM cantilever, static and dynamic pull-in and pull-off adhesion forces were addressed in the course of friction measurements to explain the role of the out-of-plane deformation of graphene layer(s). Finite element simulations showed good agreement with experiments and led to a rationalization of the observations. Thus, with interfacial grain boundaries the FLG tribology can be effectively tuned. PMID:26948836

  2. Few layers graphene as thermally activated optical modulator in the visible-near IR spectral range.

    PubMed

    Benítez, J L; Hernández-Cordero, Juan; Muhl, S; Mendoza, D

    2016-01-01

    We report the temperature modulation of the optical transmittance of a few layers of graphene (FLG). The FLG was heated either by the Joule effect of the current flowing between coplanar electrodes or by the absorption of a continuous-wave 532 nm laser. The optical signals used to evaluate the modulation of the FLG were at 633, 975, and 1550 nm; the last wavelengths are commonly used in optical communications. We also evaluated the effect of the substrate on the modulation effect by comparing the performance of a freely suspended FLG sample with one mounted on a glass substrate. Our results show that the modulation of the optical transmittance of FLG can be from millihertz to kilohertz. PMID:26696185

  3. Field emission properties of hybrid few-layer graphene-carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Lei Qi, Jun; Zhang, Fu; Xia Zhang, Li; Cao, Jian; Cai Feng, Ji

    2014-04-01

    Few-layer graphene (FLG) and carbon nanotube (CNT) hybrid is prepared by in situ growth of FLG on the walls of CNTs, using PECVD, without catalyst. The amount and size of FLG can be controlled by total gas pressure and growth time. The field emission (FE) characteristics of CNTs coated with different-density FLG were studied, and an FE phenomenon schematic and electrostatic field equipotential model of these FLG-CNTs were proposed. These results show that the geometrical morphology of FLG plays an important role in the FE property of hybrid FLG-CNTs. The medium-density FLG on the CNTs exhibits excellent FE properties, with a low turn-on electric field and threshold field, as well as large field enhancement factor, which are much better than those of the as-grown CNTs. The excellent FE properties of the FLG-CNT hybrids make them promising candidates for high-performance FE emitters.

  4. Oil lubricant tribological behaviour improvement through dispersion of few layer graphene oxide.

    PubMed

    Sarno, Maria; Senatore, Adolfo; Cirillo, Claudia; Petrone, Vincenzo; Ciambelli, Paolo

    2014-07-01

    Few layer graphene oxide (GO) nanosheets were prepared by a very fast modified Hummers method and widely characterized. Avoiding further chemical reactions, trying to take advantage of the easy exfoliation of GO favoring the formation of a tribofilm, and using a methodology well known to the lubricant industry, they were added to a mineral oil by the help of a dispersant. The tribological behaviour of GO in mineral oil was investigated under a wide spectrum of conditions, from boundary and mixed lubrication to elastohydrodynamic regimes. A ball on disc setup tribometer has been used to verify the friction reduction due to nanosheets dispersed in mineral oil. Their good friction and anti-wear properties may possibly be attributed to the small and extremely thin laminated structure, which offer lower shear stress and prevent interaction between metal interfaces. Furthermore, the results clearly prove that graphene platelets in oil easily form a protective film to prevent the direct contact between steel surfaces and, thereby, improving the frictional behaviour of the base oil. This evidence is also related to the frictional coefficient trend in boundary regime.

  5. Stacking Structures of Few-Layer Graphene Revealed by Phase-Sensitive Infrared Nanoscopy.

    PubMed

    Kim, Deok-Soo; Kwon, Hyuksang; Nikitin, Alexey Yu; Ahn, Seongjin; Martín-Moreno, Luis; García-Vidal, Francisco J; Ryu, Sunmin; Min, Hongki; Kim, Zee Hwan

    2015-07-28

    The stacking orders in few-layer graphene (FLG) strongly influences the electronic properties of the material. To explore the stacking-specific properties of FLG in detail, one needs powerful microscopy techniques that visualize stacking domains with sufficient spatial resolution. We demonstrate that infrared (IR) scattering scanning near-field optical microscopy (sSNOM) directly maps out the stacking domains of FLG with a nanometric resolution, based on the stacking-specific IR conductivities of FLG. The intensity and phase contrasts of sSNOM are compared with the sSNOM contrast model, which is based on the dipolar tip-sample coupling and the theoretical conductivity spectra of FLG, allowing a clear assignment of each FLG domain as Bernal, rhombohedral, or intermediate stacks for tri-, tetra-, and pentalayer graphene. The method offers 10-100 times better spatial resolution than the far-field Raman and infrared spectroscopic methods, yet it allows far more experimental flexibility than the scanning tunneling microscopy and electron microscopy.

  6. Few layer graphene to graphitic films: infrared photoconductive versus bolometric response

    NASA Astrophysics Data System (ADS)

    Kurra, Narendra; Bhadram, Venkata Srinu; Narayana, Chandrabhas; Kulkarni, Giridhar U.

    2012-12-01

    We report a comparative study of the performance of infrared (IR) photoconductive and bolometric detectors fabricated from few layer graphene (FLG) to graphitic films obtained by different methods. FLG films grown directly on insulating substrates with the aid of residual hydrocarbons and polymethylmethacrylate (PMMA) carbon sources show an IR photoresponse of 73% which is far higher compared to the FLG films (6-14%) obtained by CVD and Scotch tape methods. The photoconductive nature of FLG films is due to generation of photoexcited charge carriers. On the other hand, the photoresponse of the bulk graphitic films is bolometric in nature where the resistance changes are due to thermal effects. The IR photoresponse from these graphitic films is correlated with the Raman peak intensities which are very sensitive to the nature of the FLG.We report a comparative study of the performance of infrared (IR) photoconductive and bolometric detectors fabricated from few layer graphene (FLG) to graphitic films obtained by different methods. FLG films grown directly on insulating substrates with the aid of residual hydrocarbons and polymethylmethacrylate (PMMA) carbon sources show an IR photoresponse of 73% which is far higher compared to the FLG films (6-14%) obtained by CVD and Scotch tape methods. The photoconductive nature of FLG films is due to generation of photoexcited charge carriers. On the other hand, the photoresponse of the bulk graphitic films is bolometric in nature where the resistance changes are due to thermal effects. The IR photoresponse from these graphitic films is correlated with the Raman peak intensities which are very sensitive to the nature of the FLG. Electronic supplementary information (ESI) available: The Raman spectrum of the FLG on the Ni surface (before etching) is shown in Fig. S1. The thickness and mobility of the FLG films are provided in Fig. S2 and S3 respectively. The sensitivity of the RHC-FLG towards the IR radiation emitted by an

  7. Salt-assisted direct exfoliation of graphite into high-quality, large-size, few-layer graphene sheets.

    PubMed

    Niu, Liyong; Li, Mingjian; Tao, Xiaoming; Xie, Zhuang; Zhou, Xuechang; Raju, Arun P A; Young, Robert J; Zheng, Zijian

    2013-08-21

    We report a facile and low-cost method to directly exfoliate graphite powders into large-size, high-quality, and solution-dispersible few-layer graphene sheets. In this method, aqueous mixtures of graphite and inorganic salts such as NaCl and CuCl2 are stirred, and subsequently dried by evaporation. Finally, the mixture powders are dispersed into an orthogonal organic solvent solution of the salt by low-power and short-time ultrasonication, which exfoliates graphite into few-layer graphene sheets. We find that the as-made graphene sheets contain little oxygen, and 86% of them are 1-5 layers with lateral sizes as large as 210 μm(2). Importantly, the as-made graphene can be readily dispersed into aqueous solution in the presence of surfactant and thus is compatible with various solution-processing techniques towards graphene-based thin film devices. PMID:23824229

  8. Salt-assisted direct exfoliation of graphite into high-quality, large-size, few-layer graphene sheets.

    PubMed

    Niu, Liyong; Li, Mingjian; Tao, Xiaoming; Xie, Zhuang; Zhou, Xuechang; Raju, Arun P A; Young, Robert J; Zheng, Zijian

    2013-08-21

    We report a facile and low-cost method to directly exfoliate graphite powders into large-size, high-quality, and solution-dispersible few-layer graphene sheets. In this method, aqueous mixtures of graphite and inorganic salts such as NaCl and CuCl2 are stirred, and subsequently dried by evaporation. Finally, the mixture powders are dispersed into an orthogonal organic solvent solution of the salt by low-power and short-time ultrasonication, which exfoliates graphite into few-layer graphene sheets. We find that the as-made graphene sheets contain little oxygen, and 86% of them are 1-5 layers with lateral sizes as large as 210 μm(2). Importantly, the as-made graphene can be readily dispersed into aqueous solution in the presence of surfactant and thus is compatible with various solution-processing techniques towards graphene-based thin film devices.

  9. Tribological properties of few-layer graphene oxide sheets as oil-based lubricant additives

    NASA Astrophysics Data System (ADS)

    Chen, Zhe; Liu, Yuhong; Luo, Jianbin

    2016-03-01

    The performance of a lubricant largely depends on the additives it involves. However, currently used additives cause severe pollution if they are burned and exhausted. Therefore, it is necessary to develop a new generation of green additives. Graphene oxide (GO) consists of only C, H and O and thus is considered to be environmentally friendly. So the tribological properties of the few-layer GO sheet as an additive in hydrocarbon base oil are investigated systematically. It is found that, with the addition of GO sheets, both the coefficient of friction (COF) and wear are decreased and the working temperature range of the lubricant is expanded in the positive direction. Moreover, GO sheets has better performance under higher sliding speed and the optimized concentration of GO sheets is determined to be 0.5wt%. After rubbing, GO is detected on the wear scars through Raman spectroscopy. And it is believed that, during the rubbing, GO sheets adhere to the sliding surfaces, behaving like protective films and preventing the sliding surfaces from contacting with each other directly. This paper proves that the GO sheet is an effective lubricant additive, illuminates the lubrication mechanism, and provides some critical parameters for the practical application of GO sheets in lubrication.

  10. In situ nitrogenated graphene-few-layer WS2 composites for fast and reversible Li+ storage.

    PubMed

    Chen, Dongyun; Ji, Ge; Ding, Bo; Ma, Yue; Qu, Baihua; Chen, Weixiang; Lee, Jim Yang

    2013-09-01

    Two-dimensional nanosheets can leverage on their open architecture to support facile insertion and removal of Li(+) as lithium-ion battery electrode materials. In this study, two two-dimensional nanosheets with complementary functions, namely nitrogen-doped graphene and few-layer WS2, were integrated via a facile surfactant-assisted synthesis under hydrothermal conditions. The layer structure and morphology of the composites were confirmed by X-ray diffraction, scanning electron microscopy and high-resolution transmission microscopy. The effects of surfactant amount on the WS2 layer number were investigated and the performance of the layered composites as high energy density lithium-ion battery anodes was evaluated. The composite formed with a surfactant : tungsten precursor ratio of 1 : 1 delivered the best cyclability (average of only 0.08% capacity fade per cycle for 100 cycles) and good rate performance (80% capacity retention with a 50-fold increase in current density from 100 mA g(-1) to 5000 mA g(-1)), and may find uses in power-oriented applications.

  11. Optical reflectivity and Raman scattering in few-layer-thick graphene highly doped by K and Rb.

    PubMed

    Jung, Naeyoung; Kim, Bumjung; Crowther, Andrew C; Kim, Namdong; Nuckolls, Colin; Brus, Louis

    2011-07-26

    We report the optical reflectivity and Raman scattering of few layer (L) graphene exposed to K and Rb vapors. Samples many tens of layers thick show the reflectivity and Raman spectra of the stage 1 bulk alkali intercalation compounds (GICs) KC(8) and RbC(8). However, these bulk optical and Raman properties only begin to appear in samples more than about 15 graphene layers thick. The 1 L to 4 L alkali exposed graphene Raman spectra are profoundly different than the Breit-Wigner-Fano (BWF) spectra of the bulk stage 1 compounds. Samples less than 10 layers thick show Drude-like plasma edge reflectivity dip in the visible; alkali exposed few layer graphenes are significantly more transparent than intrinsic graphene. Simulations show the in-plane free electron density is lower than in the bulk stage 1 GICs. In few layer graphenes, alkalis both intercalate between layers and adsorb on the graphene surfaces. Charge transfer electrically dopes the graphene sheets to densities near and above 10(+14) electrons/cm(2). New intrinsic Raman modes at 1128 and 1264 cm(-1) are activated by in-plane graphene zone folding caused by strongly interacting, locally crystalline alkali adlayers. The K Raman spectra are independent of thickness for L = 1-4, indicating that charge transfer from adsorbed and intercalated K layers are similar. The Raman G mode is downshifted and significantly broadened from intrinsic graphene. In contrast, the Rb spectra vary strongly with L and show increased doping by intercalated alkali as L increases. Rb adlayers appear to be disordered liquids, while intercalated layers are locally crystalline solids. A significant intramolecular G mode electronic resonance Raman enhancement is observed in K exposed graphene, as compared with intrinsic graphene. PMID:21682332

  12. Magnetotransport properties of a few-layer graphene-ferromagnetic metal junctions in vertical spin valve devices

    SciTech Connect

    Entani, Shiro Naramoto, Hiroshi; Sakai, Seiji

    2015-05-07

    Magnetotransport properties were studied for the vertical spin valve devices with two junctions of permalloy electrodes and a few-layer graphene interlayer. The graphene layer was directly grown on the bottom electrode by chemical vapor deposition. X-ray photoelectron spectroscopy showed that the permalloy surface fully covered with a few-layer graphene is kept free from oxidation and contamination even after dispensing and removing photoresist. This enabled fabrication of the current perpendicular to plane spin valve devices with a well-defined interface between graphene and permalloy. Spin-dependent electron transport measurements revealed a distinct spin valve effect in the devices. The magnetotransport ratio was 0.8% at room temperature and increased to 1.75% at 50 K. Linear current-voltage characteristics and resistance increase with temperature indicated that ohmic contacts are realized at the relevant interfaces.

  13. Structural Analysis and Direct Imaging of Rotational Stacking Faults in Few-Layer Graphene Synthesized from Solid Botanical Precursor

    NASA Astrophysics Data System (ADS)

    Kalita, Golap; Wakita, Koichi; Umeno, Masayoshi

    2011-07-01

    Here, we report the structural analysis and rotational stacking faults of few-layer graphene sheets derived by the controlled pyrolysis of the solid botanical derivative camphor (C10H16O). The second-order Raman spectra of the sheets show that the graphene layers are more than one single layer, and the numbers of layers can be controlled by adjusting the amount of camphor pyrolyzed. Transmission electron microscopy images show a minimum of 3 layers for thinner graphene sheets and a maximum of 12 layers for thicker graphene sheets. Low-voltage aberration-corrected high-resolution transmission electron microscopy is also carried out to gain insight into the hexagonal structure and stacking of graphene layers. The transmission electron microscopy study showed the presence of moiré patterns with a relative rotation between graphene layers.

  14. Tunable Electrical and Optical Characteristics in Monolayer Graphene and Few-Layer MoS2 Heterostructure Devices.

    PubMed

    Rathi, Servin; Lee, Inyeal; Lim, Dongsuk; Wang, Jianwei; Ochiai, Yuichi; Aoki, Nobuyuki; Watanabe, Kenji; Taniguchi, Takashi; Lee, Gwan-Hyoung; Yu, Young-Jun; Kim, Philip; Kim, Gil-Ho

    2015-08-12

    Lateral and vertical two-dimensional heterostructure devices, in particular graphene-MoS2, have attracted profound interest as they offer additional functionalities over normal two-dimensional devices. Here, we have carried out electrical and optical characterization of graphene-MoS2 heterostructure. The few-layer MoS2 devices with metal electrode at one end and monolayer graphene electrode at the other end show nonlinearity in drain current with drain voltage sweep due to asymmetrical Schottky barrier height at the contacts and can be modulated with an external gate field. The doping effect of MoS2 on graphene was observed as double Dirac points in the transfer characteristics of the graphene field-effect transistor (FET) with a few-layer MoS2 overlapping the middle part of the channel, whereas the underlapping of graphene have negligible effect on MoS2 FET characteristics, which showed typical n-type behavior. The heterostructure also exhibits a strongest optical response for 520 nm wavelength, which decreases with higher wavelengths. Another distinct feature observed in the heterostructure is the peak in the photocurrent around zero gate voltage. This peak is distinguished from conventional MoS2 FETs, which show a continuous increase in photocurrent with back-gate voltage. These results offer significant insight and further enhance the understanding of the graphene-MoS2 heterostructure.

  15. The influence of few-layer graphene on the gas permeability of the high-free-volume polymer PIM-1

    PubMed Central

    Althumayri, Khalid; Harrison, Wayne J.; Shin, Yuyoung; Gardiner, John M.; Casiraghi, Cinzia; Bernardo, Paola; Clarizia, Gabriele

    2016-01-01

    Gas permeability data are presented for mixed matrix membranes (MMMs) of few-layer graphene in the polymer of intrinsic microporosity PIM-1, and the results compared with previously reported data for two other nanofillers in PIM-1: multiwalled carbon nanotubes functionalized with poly(ethylene glycol) (f-MWCNTs) and fused silica. For few-layer graphene, a significant enhancement in permeability is observed at very low graphene content (0.05 vol.%), which may be attributed to the effect of the nanofiller on the packing of the polymer chains. At higher graphene content permeability decreases, as expected for the addition of an impermeable filler. Other nanofillers, reported in the literature, also give rise to enhancements in permeability, but at substantially higher loadings, the highest measured permeabilities being at 1 vol.% for f-MWCNTs and 24 vol.% for fused silica. These results are consistent with the hypothesis that packing of the polymer chains is influenced by the curvature of the nanofiller surface at the nanoscale, with an increasingly pronounced effect on moving from a more-or-less spherical nanoparticle morphology (fused silica) to a cylindrical morphology (f-MWCNT) to a planar morphology (graphene). While the permeability of a high-free-volume polymer such as PIM-1 decreases over time through physical ageing, for the PIM-1/graphene MMMs a significant permeability enhancement was retained after eight months storage. PMID:26712643

  16. The influence of few-layer graphene on the gas permeability of the high-free-volume polymer PIM-1.

    PubMed

    Althumayri, Khalid; Harrison, Wayne J; Shin, Yuyoung; Gardiner, John M; Casiraghi, Cinzia; Budd, Peter M; Bernardo, Paola; Clarizia, Gabriele; Jansen, Johannes C

    2016-02-13

    Gas permeability data are presented for mixed matrix membranes (MMMs) of few-layer graphene in the polymer of intrinsic microporosity PIM-1, and the results compared with previously reported data for two other nanofillers in PIM-1: multiwalled carbon nanotubes functionalized with poly(ethylene glycol) (f-MWCNTs) and fused silica. For few-layer graphene, a significant enhancement in permeability is observed at very low graphene content (0.05 vol.%), which may be attributed to the effect of the nanofiller on the packing of the polymer chains. At higher graphene content permeability decreases, as expected for the addition of an impermeable filler. Other nanofillers, reported in the literature, also give rise to enhancements in permeability, but at substantially higher loadings, the highest measured permeabilities being at 1 vol.% for f-MWCNTs and 24 vol.% for fused silica. These results are consistent with the hypothesis that packing of the polymer chains is influenced by the curvature of the nanofiller surface at the nanoscale, with an increasingly pronounced effect on moving from a more-or-less spherical nanoparticle morphology (fused silica) to a cylindrical morphology (f-MWCNT) to a planar morphology (graphene). While the permeability of a high-free-volume polymer such as PIM-1 decreases over time through physical ageing, for the PIM-1/graphene MMMs a significant permeability enhancement was retained after eight months storage. PMID:26712643

  17. Evolution of surface morphology and electronic structure of few layer graphene after low energy Ar{sup +} ion irradiation

    SciTech Connect

    Al-Harthi, S. H.; Kara'a, A.; Elzain, M.; Hysen, T.; Al-Hinai, A. T.; Myint, M. T. Z.

    2012-11-19

    We report on co-existing dual anisotropy ripple formation, sp bonding transformation, and variation in the delocalized {pi} electron system in 1 keV Ar{sup +} ion irradiated few-layer graphene surfaces. Ripples in directions, perpendicular and parallel to the ion beam were found. The irradiation effect and the transition from the sp{sup 2}-bonding to sp{sup 3}-hybridized state were analyzed from the deconvolution of the C (1s) peak and from the shape of the derivative of the Auger transition spectra. The results suggest a plausible mechanism for tailoring of few-layer graphene electronic band structure with interlayer coupling tuned by the ion irradiation.

  18. Thermal conductivity of giant mono- to few-layered CVD graphene supported on an organic substrate.

    PubMed

    Liu, Jing; Wang, Tianyu; Xu, Shen; Yuan, Pengyu; Xu, Xu; Wang, Xinwei

    2016-05-21

    The thermal conductivity (k) of supported graphene is a critical property that reflects the graphene-substrate interaction, graphene structure quality, and is needed for thermal design of a graphene device. Yet the related k measurement has never been a trivial work and very few studies are reported to date, only at the μm level. In this work, for the first time, the k of giant chemical vapor decomposition (CVD) graphene supported on poly(methyl methacrylate) (PMMA) is characterized using our transient electro-thermal technique based on a differential concept. Our graphene size is ∼mm, far above the samples studied in the past. This giant graphene measurement eliminates the thermal contact resistance problems and edge phonon scattering encountered in μm-scale graphene k measurement. Such mm-scale measurement is critical for device/system-level thermal design since it reflects the effect of abundant grains in graphene. The k of 1.33-layered, 1.53-layered, 2.74-layered and 5.2-layered supported graphene is measured as 365 W m(-1) K(-1), 359 W m(-1) K(-1), 273 W m(-1) K(-1) and 33.5 W m(-1) K(-1), respectively. These values are significantly lower than the k of supported graphene on SiO2, and are about one order of magnitude lower than the k of suspended graphene. We speculate that the abundant C atoms in the PMMA promote more ready energy and momentum exchange with the supported graphene, and give rise to more phonon scattering than the SiO2 substrate. This leads to a lower k of CVD graphene on PMMA than that on SiO2. We attribute the existence of disorder in the sp(2) domain, graphene oxide (GO) and stratification in the 5.2-layered graphene to its more k reduction. The Raman linewidth (G peak) of the 5.2-layered graphene is also twice larger than that of the other three kinds of graphene, indicating the much more phonon scattering and shorter phonon lifetime in it. Also the electrical conductivity of the 5.2-layered graphene is about one-fifth of that for the

  19. Thermal conductivity of giant mono- to few-layered CVD graphene supported on an organic substrate

    NASA Astrophysics Data System (ADS)

    Liu, Jing; Wang, Tianyu; Xu, Shen; Yuan, Pengyu; Xu, Xu; Wang, Xinwei

    2016-05-01

    The thermal conductivity (k) of supported graphene is a critical property that reflects the graphene-substrate interaction, graphene structure quality, and is needed for thermal design of a graphene device. Yet the related k measurement has never been a trivial work and very few studies are reported to date, only at the μm level. In this work, for the first time, the k of giant chemical vapor decomposition (CVD) graphene supported on poly(methyl methacrylate) (PMMA) is characterized using our transient electro-thermal technique based on a differential concept. Our graphene size is ~mm, far above the samples studied in the past. This giant graphene measurement eliminates the thermal contact resistance problems and edge phonon scattering encountered in μm-scale graphene k measurement. Such mm-scale measurement is critical for device/system-level thermal design since it reflects the effect of abundant grains in graphene. The k of 1.33-layered, 1.53-layered, 2.74-layered and 5.2-layered supported graphene is measured as 365 W m-1 K-1, 359 W m-1 K-1, 273 W m-1 K-1 and 33.5 W m-1 K-1, respectively. These values are significantly lower than the k of supported graphene on SiO2, and are about one order of magnitude lower than the k of suspended graphene. We speculate that the abundant C atoms in the PMMA promote more ready energy and momentum exchange with the supported graphene, and give rise to more phonon scattering than the SiO2 substrate. This leads to a lower k of CVD graphene on PMMA than that on SiO2. We attribute the existence of disorder in the sp2 domain, graphene oxide (GO) and stratification in the 5.2-layered graphene to its more k reduction. The Raman linewidth (G peak) of the 5.2-layered graphene is also twice larger than that of the other three kinds of graphene, indicating the much more phonon scattering and shorter phonon lifetime in it. Also the electrical conductivity of the 5.2-layered graphene is about one-fifth of that for the other three. This

  20. Mechanical Deformation of Single- and Few- Layer Graphene on Micro-Scale-Grooved PDMS

    NASA Astrophysics Data System (ADS)

    Rocklin, David; Scharfenberg, Scott; Chialvo, Cesar; Weaver, Richard; Goldbart, Paul; Mason, Nadya

    2009-11-01

    The physical properties of the material graphene are currently of wide interest. To explore their mechanical aspects, we placed graphene flakes, of thicknesses ranging from one to seven layers, on a rubbery PDMS (polydimethylsiloxane) substrate containing microgrooves. We used Atomic Force Microscopy (AFM) imaging techniques to study the resulting deformations of the surface, and found that the graphene adhered to the sample and substantially flattened the profile of the grooves. We have examined this flattening effect within a model based on linear elasticity theory. Thus, we have been able to identify, at least tentatively, the point at which shear stress breaks the interlayer coupling and causes the graphene layers to slide against each other.

  1. The photoelectric characteristics of a few-layer graphene/Si Schottky junction solar cell

    NASA Astrophysics Data System (ADS)

    Ma, Xiying; Gu, Weixia

    2015-10-01

    We present a study of the photovoltaic effects of a graphene/n- Si Schottky junction solar cell. The graphene/Si solar cell was prepared by means of rapid chemical vapor deposition, while the graphene films were grown with a CH4/Ar mixed gas under a constant flow at 950°C and then annealed at 1000°C. It was found that the junction between the graphene film and the n-Si structure played an important role in determining the device performance. An energy conversion efficiency of 2.1% was achieved under an optical illumination of 100 mW. The strong photovoltaic effects of the cell were due to device junction's ability to efficiently generate and separate electron-hole pairs.

  2. Co3O4 nanocubes homogeneously assembled on few-layer graphene for high energy density lithium-ion batteries

    NASA Astrophysics Data System (ADS)

    Xu, Junming; Wu, Jinsong; Luo, Langli; Chen, Xinqi; Qin, Huibin; Dravid, Vinayak; Mi, Shaobo; Jia, Chunlin

    2015-01-01

    Graphene-based nanocomposites have been synthesized and tested as electrode materials for high power lithium-ion batteries. In the synthesis of such nanocomposites, graphene is generally introduced by either thermally or chemically reduced graphite oxide (GO), which has poorer electric conductivity and crystallinity than mechanically exfoliated graphene. Here, we prepare few-layer graphene sheet (FLGS) with high electric conductivity, by sonicating expanded graphite in DMF solvent, and develop a simple one-pot hydrothermal method to fabricate monodispersed and ultrasmall Co3O4 nanocubes (about 4 nm in size) on the FLGS. This composite, consisting of homogeneously assembled and high crystalline Co3O4 nanocubes on the FLGS, has shown higher capacity and much better cycling stability than counterparts synthesized using GO as a precursor. The products in different synthesis stages have been characterized by TEM, FTIR and XPS to investigate the nanocube growth mechanism. We find that Co(OH)2 initially grew homogeneously on the graphene surface, then gradually oxidized to form Co3O4 nanoparticle seeds, and finally converted to Co3O4 nanocubes with caboxylated anion as surfactant. This work explores the mechanism of nanocrystal growth and its impact on electrochemical properties to provide further insights into the development of nanostructured electrode materials for high power energy storage.

  3. Powder, paper and foam of few-layer graphene prepared in high yield by electrochemical intercalation exfoliation of expanded graphite.

    PubMed

    Wu, Liqiong; Li, Weiwei; Li, Peng; Liao, Shutian; Qiu, Shengqiang; Chen, Mingliang; Guo, Yufen; Li, Qi; Zhu, Chao; Liu, Liwei

    2014-04-01

    A facile and high-yield approach to the preparation of few-layer graphene (FLG) by electrochemical intercalation exfoliation (EIE) of expanded graphite in sulfuric acid electrolyte is reported. Stage-1 H2SO4-graphite intercalation compound is used as a key intermediate in EIE to realize the efficient exfoliation. The yield of the FLG sheets (<7 layers) with large lateral sizes (tens of microns) is more than 75% relative to the total amount of starting expanded graphite. A low degree of oxygen functionalization existing in the prepared FLG flakes enables them to disperse effectively, which contributes to the film-forming characteristics of the FLG flakes. These electrochemically exfoliated FLG flakes are integrated into several kinds of macroscopic graphene structures. Flexible and freestanding graphene papers made of the FLG flakes retain excellent conductivity (≈24,500 S m(-1)). Three-dimensional (3D) graphene foams with light weight are fabricated from the FLG flakes by the use of Ni foams as self-sacrifice templates. Furthermore, 3D graphene/Ni foams without any binders, which are used as supercapacitor electrodes in aqueous electrolyte, provide the specific capacitance of 113.2 F g(-1) at a current density of 0.5 A g(-1), retaining 90% capacitance after 1000 cycles.

  4. Surface-enhanced Raman scattering studies of few-layer graphene on silver substrate with 514 nm excitation

    NASA Astrophysics Data System (ADS)

    Ouyang, Yu; Chen, Li

    2011-04-01

    Few-layer graphene was prepared by deoxidizing graphite oxide. Surface-enhanced Raman scattering (SERS) spectrum of graphene on Ag substrate was presented with 514 nm excitation. More than nine Raman lines are shown in the 100-3200 cm -1. The intensities of all lines are enhanced. Besides D mode at 1347 cm -1, G peak at 1581 cm -1, G ∗ band at ˜2458 cm -1, and G' band at ˜2691 cm -1, there are two features in low frequency area at about 239 cm -1 and 992 cm -1 separately, one line in high frequency area at about 2900 cm -1 with a shoulder appearing at ˜2860 cm -1. According to SERS, the structure of graphene was analyzed. Furthermore, the increase of D/G intensity ratio in SERS shows the SERS has much potential to be applied in controlling synthesis quality of graphene. In addition, low frequency Raman lines presented in SERS show application potential in analyzing the layer number, stacked style and edge of graphene.

  5. Electron Hopping Through Single-to-Few-Layer Graphene Oxide Films. Side-Selective Photocatalytic Deposition of Metal Nanoparticles.

    PubMed

    Lightcap, Ian V; Murphy, Sean; Schumer, Timothy; Kamat, Prashant V

    2012-06-01

    Single- to few-layer graphene oxide (GO) sheets have been successfully anchored onto TiO2 films using electrophoretic deposition. Upon UV illumination of TiO2-GO films, photogenerated electrons from TiO2 are captured by GO. These electrons are initially used in GO's reduction, while additional electron transfer results in storage across its sp(2) network. In the presence of silver ions, deposition of silver nanoparticles (NPs) is accomplished on the GO surface opposite the TiO2, thus confirming the ability of GO to transport electrons through its plane. Illumination-controlled reduction of silver ions allows for simple selection of particle size and loading, making these semiconductor-graphene-metal (SGM) films ideal for custom catalysis and sensor applications. Initial testing of SGM films as surface-enhanced resonance Raman (SERRS) sensors produced significant target molecule signal enhancements, enabling detection of nanomolar concentrations. PMID:26285621

  6. Towards Lego Snapping; Integration of Carbon Nanotubes and Few-Layer Graphene

    NASA Astrophysics Data System (ADS)

    Nasseri, Mohsen; Boland, Mathias; Farrokhi, M. Javad; Strachan, Douglas

    Integration of semiconducting, conducting, and insulating nanomaterials into precisely aligned complicated systems is one of the main challenges to the ultimate size scaling of electronic devices, which is a key goal in nanoscience and nanotechnology. This integration could be made more effective through controlled alignment of the crystallographic lattices of the nanoscale components. Of the vast number of materials of atomically-thin materials, two of the sp2 bonded carbon structures, graphene and carbon nanotubes, are ideal candidates for this type of application since they are built from the same backbone carbon lattice. Here we report carbon nanotube and graphene hybrid nanostructures fabricated through their catalytic synthesis and etching. The growth formations we have investigated through various high-resolution microscopy techniques provide evidence of lego-snapped interfaces between nanotubes and graphene into device-relevant orientations. We will finish with a discussion of the various size and energy regimes relevant to these lego-snapped interfaces and their implications on developing these integrated formations.

  7. Vacancies in epitaxial graphene

    SciTech Connect

    Davydov, S. Yu.

    2015-08-15

    The coherent-potential method is used to consider the problem of the influence of a finite concentration of randomly arranged vacancies on the density of states of epitaxial graphene. To describe the density of states of the substrate, simple models (the Anderson model, Haldane-Anderson model, and parabolic model) are used. The electronic spectrum of free single-sheet graphene is considered in the low-energy approximation. Charge transfer in the graphene-substrate system is discussed. It is shown that, in all cases, the density of states of epitaxial graphene decreases proportionally to the vacancy concentration. At the same time, the average charge transferred from graphene to the substrate increases.

  8. Observation of spin-glass behavior in nickel adsorbed few layer graphene

    SciTech Connect

    Mitra, Sreemanta; Mondal, Oindrila; Banerjee, Sourish; Chakravorty, Dipankar

    2013-01-14

    Nickel-adsorbed graphene was prepared by first synthesizing graphite oxide (GO) by modified Hummers' method and then reducing a solution containing both GO and Ni{sup 2+}. Energy dispersive X-ray spectroscopy analysis showed 31 at. % nickel was present. Magnetization measurements under both dc and ac magnetic fields were carried out in the temperature range 2 K to 300 K. The zero field cooled and field cooled magnetization data showed a pronounced irreversibility at a temperature around 20 K. The analysis of the ac susceptibility data was carried out by both Vogel-Fulcher as well as power law. From dynamic scaling analysis, the microscopic flipping time {tau}{sub 0}{approx}10{sup -13}s and critical exponent z{nu}=5.9{+-}0.1 were found, indicating the presence of conventional spin glass in the system. The spin glass transition temperature was estimated as 19.5 K. Decay of thermoremanent magnetization was explained by stretched exponential function with a value of the exponent as 0.6. From the results, it is concluded that nickel adsorbed graphene behaves like a spin-glass.

  9. Nanoscale measurements of unoccupied band dispersion in few-layer graphene

    PubMed Central

    Jobst, Johannes; Kautz, Jaap; Geelen, Daniël; Tromp, Rudolf M.; van der Molen, Sense Jan

    2015-01-01

    The properties of any material are fundamentally determined by its electronic band structure. Each band represents a series of allowed states inside a material, relating electron energy and momentum. The occupied bands, that is, the filled electron states below the Fermi level, can be routinely measured. However, it is remarkably difficult to characterize the empty part of the band structure experimentally. Here, we present direct measurements of unoccupied bands of monolayer, bilayer and trilayer graphene. To obtain these, we introduce a technique based on low-energy electron microscopy. It relies on the dependence of the electron reflectivity on incidence angle and energy and has a spatial resolution ∼10 nm. The method can be easily applied to other nanomaterials such as van der Waals structures that are available in small crystals only. PMID:26608712

  10. Synthesis of ethanol-soluble few-layer graphene nanosheets for flexible and transparent conducting composite films.

    PubMed

    Nguyen, D D; Tai, N H; Chueh, Y L; Chen, S Y; Chen, Y J; Kuo, W S; Chou, T W; Hsu, C S; Chen, L J

    2011-07-22

    We report a facile method of preparing few-layer graphene nanosheets (FLGs), which can be soluble in ethanol. Atomic force microscopy and high-resolution transmission electron microscopy studies reveal that FLGs have average thicknesses in the range of 2.6-2.8 nm, corresponding to 8-9 layers. A graphene/nafion composite film has a sheet resistance of 9.70 kΩ/sq at the transmittance of 74.5% (at 550 nm) while the nafion film on polyethylene terephthalate has a sheet resistance of 128 kΩ/sq at transmittance of 90.0%. For the cycling/bending test, almost no change in resistance was exhibited when the film was bent at an angle up to 140°, and no obvious deviation in resistance could be found after 100 bending cycles was applied. In addition, an FLGs-poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) composite layer was demonstrated as the effective hole transporting layer to improve the hole transporting ability in an organic photovoltaic device, with which the power conversion efficiency was enhanced from 3.10% to 3.70%. The results demonstrated the promising applications of FLGs on graphene-based electronics, such as transparent electrode and flexible conducting film.

  11. Synthesis of ethanol-soluble few-layer graphene nanosheets for flexible and transparent conducting composite films

    NASA Astrophysics Data System (ADS)

    Nguyen, D. D.; Tai, N. H.; Chueh, Y. L.; Chen, S. Y.; Chen, Y. J.; Kuo, W. S.; Chou, T. W.; Hsu, C. S.; Chen, L. J.

    2011-07-01

    We report a facile method of preparing few-layer graphene nanosheets (FLGs), which can be soluble in ethanol. Atomic force microscopy and high-resolution transmission electron microscopy studies reveal that FLGs have average thicknesses in the range of 2.6-2.8 nm, corresponding to 8-9 layers. A graphene/nafion composite film has a sheet resistance of 9.70 kΩ/sq at the transmittance of 74.5% (at 550 nm) while the nafion film on polyethylene terephthalate has a sheet resistance of 128 kΩ/sq at transmittance of 90.0%. For the cycling/bending test, almost no change in resistance was exhibited when the film was bent at an angle up to 140°, and no obvious deviation in resistance could be found after 100 bending cycles was applied. In addition, an FLGs-poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) composite layer was demonstrated as the effective hole transporting layer to improve the hole transporting ability in an organic photovoltaic device, with which the power conversion efficiency was enhanced from 3.10% to 3.70%. The results demonstrated the promising applications of FLGs on graphene-based electronics, such as transparent electrode and flexible conducting film.

  12. Temperature Dependence of Electric Transport in Few-layer Graphene under Large Charge Doping Induced by Electrochemical Gating

    PubMed Central

    Gonnelli, R. S.; Paolucci, F.; Piatti, E.; Sharda, Kanudha; Sola, A.; Tortello, M.; Nair, Jijeesh R.; Gerbaldi, C.; Bruna, M.; Borini, S.

    2015-01-01

    The temperature dependence of electric transport properties of single-layer and few-layer graphene at large charge doping is of great interest both for the study of the scattering processes dominating the conductivity at different temperatures and in view of the theoretically predicted possibility to reach the superconducting state in such extreme conditions. Here we present the results obtained in 3-, 4- and 5-layer graphene devices down to 3.5 K, where a large surface charge density up to about 6.8·1014 cm−2 has been reached by employing a novel polymer electrolyte solution for the electrochemical gating. In contrast with recent results obtained in single-layer graphene, the temperature dependence of the sheet resistance between 20 K and 280 K shows a low-temperature dominance of a T2 component – that can be associated with electron-electron scattering – and, at about 100 K, a crossover to the classic electron-phonon regime. Unexpectedly, this crossover does not show any dependence on the induced charge density, i.e. on the large tuning of the Fermi energy. PMID:25906088

  13. Liquid-Phase Exfoliation of Graphite into Single- and Few-Layer Graphene with α-Functionalized Alkanes.

    PubMed

    Haar, Sébastien; Bruna, Matteo; Lian, Jian Xiang; Tomarchio, Flavia; Olivier, Yoann; Mazzaro, Raffaello; Morandi, Vittorio; Moran, Joseph; Ferrari, Andrea C; Beljonne, David; Ciesielski, Artur; Samorì, Paolo

    2016-07-21

    Graphene has unique physical and chemical properties, making it appealing for a number of applications in optoelectronics, sensing, photonics, composites, and smart coatings, just to cite a few. These require the development of production processes that are inexpensive and up-scalable. These criteria are met in liquid-phase exfoliation (LPE), a technique that can be enhanced when specific organic molecules are used. Here we report the exfoliation of graphite in N-methyl-2-pyrrolidinone, in the presence of heneicosane linear alkanes terminated with different head groups. These molecules act as stabilizing agents during exfoliation. The efficiency of the exfoliation in terms of the concentration of exfoliated single- and few-layer graphene flakes depends on the functional head group determining the strength of the molecular dimerization through dipole-dipole interactions. A thermodynamic analysis is carried out to interpret the impact of the termination group of the alkyl chain on the exfoliation yield. This combines molecular dynamics and molecular mechanics to rationalize the role of functionalized alkanes in the dispersion and stabilization process, which is ultimately attributed to a synergistic effect of the interactions between the molecules, graphene, and the solvent. PMID:27349897

  14. Spectroscopic metrics allow in situ measurement of mean size and thickness of liquid-exfoliated few-layer graphene nanosheets.

    PubMed

    Backes, Claudia; Paton, Keith R; Hanlon, Damien; Yuan, Shengjun; Katsnelson, Mikhail I; Houston, James; Smith, Ronan J; McCloskey, David; Donegan, John F; Coleman, Jonathan N

    2016-02-21

    Liquid phase exfoliation is a powerful and scalable technique to produce defect-free mono- and few-layer graphene. However, samples are typically polydisperse and control over size and thickness is challenging. Notably, high throughput techniques to measure size and thickness are lacking. In this work, we have measured the extinction, absorption, scattering and Raman spectra for liquid phase exfoliated graphene nanosheets of various lateral sizes (90 ≤ 〈L〉 ≤ 810 nm) and thicknesses (2.7 ≤ 〈N〉 ≤ 10.4). We found all spectra to show well-defined dependences on nanosheet dimensions. Measurements of extinction and absorption spectra of nanosheet dispersions showed both peak position and spectral shape to vary with nanosheet thickness in a manner consistent with theoretical calculations. This allows the development of empirical metrics to extract the mean thickness of liquid dispersed nanosheets from an extinction (or absorption) spectrum. While the scattering spectra depended on nanosheet length, poor signal to noise ratios made the resultant length metric unreliable. By analyzing Raman spectra measured on graphene nanosheet networks, we found both the D/G intensity ratio and the width of the G-band to scale with mean nanosheet length allowing us to establish quantitative relationships. In addition, we elucidate the variation of 2D/G band intensities and 2D-band shape with the mean nanosheet thickness, allowing us to establish quantitative metrics for mean nanosheet thickness from Raman spectra.

  15. Thermal conductivity measurement of few layer graphene film by a micropipette sensor with laser point heating source

    NASA Astrophysics Data System (ADS)

    Jeong, J. Y.; Lee, K. M.; Shrestha, R.; Horne, K.; Das, S.; Choi, W.; Kim, M.; Choi, T. Y.

    2016-05-01

    We report a thermal characterization method for a large-scale free-standing chemical vapor deposited few layer graphene (FLG), in which a micropipette temperature sensor with an inbuilt laser point heating source was used. The technique is unique as it exhibits in general the characteristic features of high accuracy measurement of thermal conductivity of free-standing ultrathin films. Using the micropipette sensor we successfully implemented the characterization technique to show high thermal transport behavior in free-standing graphene. For accurate and successful measurement of thermal conductivity, FLG grown on Ni was transferred to a polycarbonate (PC) membrane with holes (average diameter of 100 μm) in order to isolate the graphene film from heat spreading through the bottom of the film by the laser point heating. The thermal conductivity of FLG by this method was measured at 2868 ± 932 W/m °C. The large uncertainty of 32% in thermal conductivity measurement is mainly due to the non-uniform (∼30% deviation) thickness of the film.

  16. Liquid-Phase Exfoliation of Graphite into Single- and Few-Layer Graphene with α-Functionalized Alkanes.

    PubMed

    Haar, Sébastien; Bruna, Matteo; Lian, Jian Xiang; Tomarchio, Flavia; Olivier, Yoann; Mazzaro, Raffaello; Morandi, Vittorio; Moran, Joseph; Ferrari, Andrea C; Beljonne, David; Ciesielski, Artur; Samorì, Paolo

    2016-07-21

    Graphene has unique physical and chemical properties, making it appealing for a number of applications in optoelectronics, sensing, photonics, composites, and smart coatings, just to cite a few. These require the development of production processes that are inexpensive and up-scalable. These criteria are met in liquid-phase exfoliation (LPE), a technique that can be enhanced when specific organic molecules are used. Here we report the exfoliation of graphite in N-methyl-2-pyrrolidinone, in the presence of heneicosane linear alkanes terminated with different head groups. These molecules act as stabilizing agents during exfoliation. The efficiency of the exfoliation in terms of the concentration of exfoliated single- and few-layer graphene flakes depends on the functional head group determining the strength of the molecular dimerization through dipole-dipole interactions. A thermodynamic analysis is carried out to interpret the impact of the termination group of the alkyl chain on the exfoliation yield. This combines molecular dynamics and molecular mechanics to rationalize the role of functionalized alkanes in the dispersion and stabilization process, which is ultimately attributed to a synergistic effect of the interactions between the molecules, graphene, and the solvent.

  17. Direct Synthesis of Few-Layer F-Doped Graphene Foam and Its Lithium/Potassium Storage Properties.

    PubMed

    Ju, Zhicheng; Zhang, Shuai; Xing, Zheng; Zhuang, Quanchao; Qiang, Yinghuai; Qian, Yitai

    2016-08-17

    Heteroatom-doped graphene is considered a potential electrode materials for lithium-ion batteries (LIBs). However, potassium-ion batteries (PIBs) systems are possible alternatives due to the comparatively higher abundance. Here, a practical solid-state method is described for the preparation of few-layer F-doped graphene foam (FFGF) with thickness of about 4 nm and high surface area (874 m(2)g(-1)). As anode material for LIBs, FFGF exhibits 800 mAh·g(-1) after 50 cycles at a current density of 100 mA·g(-1) and 555 mAh·g(-1) after 100 cycles at 200 mA·g(-1) as well as remarkable rate capability. FFGF also shows 165.9 mAh·g(-1) at 500 mA·g(-1) for 200 cycles for PIBs. Research suggests that the multiple synergistic effects of the F-modification, high surface area, and mesoporous membrane structures endow the ions and electrons throughout the electrode matrix with fast transportation as well as offering sufficient active sites for lithium and potassium storage, resulting in excellent electrochemical performance. Furthermore, the insights obtained will be of benefit to the design of reasonable electrode materials for alkali metal ion batteries. PMID:27467782

  18. Coulomb screening effects on the optoelectronic far-infrared properties of spatially separated few-layer graphene

    NASA Astrophysics Data System (ADS)

    Yang, C. H.; Wan, P.; Li, Q. F.; Ao, Z. M.

    2016-10-01

    We investigate the longitudinal optical conductivity of spatially separated few-layer graphene analytically and numerically. Each layer could be monolayer or bilayer graphene. The density-density correlation function has been screened by the dielectric function using the random phase approximation, which includes the inter-layer Coulomb coupling. In the presence of the potential function between the layers, the carrier densities in each layer can be tuned respectively. In these two-dimensional layered structures, the main contributions to the optical conductivity are from the intra- and inter-band transition channels in a same layer. In the infrared region, the Drude optical conductivity was observed by the unscreened intra-band transition process. But in the presence of the inter-layer Coulomb interaction, one peak structure of the optical conductivity is observed which can be modified by the dielectric environment. From the number of turning points and the turning positions, the carrier density, the Fermi wavevector, and the layered structure can be determined.

  19. Cationic surfactant-assisted hydrothermal synthesis of few-layer molybdenum disulfide/graphene composites: Microstructure and electrochemical lithium storage

    NASA Astrophysics Data System (ADS)

    Ma, Lin; Huang, Guochuang; Chen, Weixiang; Wang, Zhen; Ye, Jianbo; Li, Haiyang; Chen, Dongyun; Lee, Jim Yang

    2014-10-01

    Few-layer molybdenum disulfide/graphene (FL-MoS2/GNS) composites are fabricated by a facile hydrothermal route and a post-annealing with the assistance of various cationic surfactants (dodecyltrimethylammonium bromide, DTAB; octyltrimethylammonium bromide, OTAB; and tetrabutylammonium bromide, TBAB), which have different alkyl-chain lengths and stereo configurations. The effects of these cationic surfactants on the microstructures and electrochemical performances of the FL-MoS2/GNS for lithium storage are investigated. It is demonstrated the cationic surfactants show some ability to control the microstructure (layer number) of FL-MoS2 in composites. The electrochemical performances of FL-MoS2/GNS composites for lithium storage are greatly improved compared to the bare MoS2. Especially, FL-MoS2/GNS with ∼6 MoS2 layers prepared with the assistance of OTAB exhibits very high reversible capacity of ∼1200 mAh g-1 with excellent cycle stability and enhanced rate capability. Electrochemical impedance spectrum also confirms that the FL-MoS2/GNS composite electrodes exhibit much lower electron-transfer resistance than the MoS2. The remarkable electrochemical performances of FL-MoS2/GNS composites can be attributed to the synergistic interaction between FL-MoS2 and graphene and their quasi-3D architectures, which promote lithium diffusion, electron transfer and electrolyte access.

  20. Microwave-Assisted Synthesis of Highly-Crumpled, Few-Layered Graphene and Nitrogen-Doped Graphene for Use as High-Performance Electrodes in Capacitive Deionization

    PubMed Central

    Amiri, Ahmad; Ahmadi, Goodarz; Shanbedi, Mehdi; Savari, Maryam; Kazi, S. N.; Chew, B. T.

    2015-01-01

    Capacitive deionization (CDI) is a promising procedure for removing various charged ionic species from brackish water. The performance of graphene-based material in capacitive deionization is lower than the expectation of the industry, so highly-crumpled, few-layered graphene (HCG) and highly-crumpled nitrogen-doped graphene (HCNDG) with high surface area have been introduced as promising candidates for CDI electrodes. Thus, HCG and HCNDG were prepared by exfoliation of graphite in the presence of liquid-phase, microwave-assisted methods. An industrially-scalable, cost-effective, and simple approach was employed to synthesize HCG and HCNDG, resulting in few-layered graphene and nitrogen-doped graphene with large specific surface area. Then, HCG and HCNDG were utilized for manufacturing a new class of carbon nanostructure-based electrodes for use in large-scale CDI equipment. The electrosorption results indicated that both the HCG and HCNDG have fairly large specific surface areas, indicating their huge potential for capacitive deionization applications. PMID:26643279

  1. Free-standing few-layered graphene oxide films: selective, steady and lasting permeation of organic molecules with adjustable speeds

    NASA Astrophysics Data System (ADS)

    Huang, Tao; An, Qi; Luan, Xinglong; Zhang, Qian; Zhang, Yihe

    2016-01-01

    A variety of small molecules with diameters around 1 nm possess a range of functions, such as antibiotic, antimicrobic, anticoagulant, pesticidal and chemotherapy effects, making these molecules especially useful in various applications ranging from medical treatment to environmental microbiological control. However, the long-term steady delivery (release or permeation) of these small molecules with adjustable and controllable speeds has remained an especially challenging task. In this study, we prepared covalently cross-linked free-standing few-layered GO films using a layer-by-layer technique in combination with photochemical cross-linkages, and achieved a controlled release of positively charged, negatively charged, and zwitterionic small molecules with adjustable and controllable speeds. The steady delivery of the small molecule lasted up to 9 days. Other functionalities, such as graphene-enhanced Raman spectra and electrochemical properties that could also be integrated or employed in delivery systems, were also studied for our films. We expect the special molecular delivery properties of our films to lead to new possibilities in drug/fertilizer delivery and environmental microbiological control applications.A variety of small molecules with diameters around 1 nm possess a range of functions, such as antibiotic, antimicrobic, anticoagulant, pesticidal and chemotherapy effects, making these molecules especially useful in various applications ranging from medical treatment to environmental microbiological control. However, the long-term steady delivery (release or permeation) of these small molecules with adjustable and controllable speeds has remained an especially challenging task. In this study, we prepared covalently cross-linked free-standing few-layered GO films using a layer-by-layer technique in combination with photochemical cross-linkages, and achieved a controlled release of positively charged, negatively charged, and zwitterionic small molecules with

  2. Epitaxial growth of large area single-crystalline few-layer MoS2 with high space charge mobility of 192 cm2 V-1 s-1

    NASA Astrophysics Data System (ADS)

    Ma, Lu; Nath, Digbijoy N.; Lee, Edwin W.; Lee, Choong Hee; Yu, Mingzhe; Arehart, Aaron; Rajan, Siddharth; Wu, Yiying

    2014-08-01

    We report on the vapor-solid growth of single crystalline few-layer MoS2 films on (0001)-oriented sapphire with excellent structural and electrical properties over centimeter length scale. High-resolution X-ray diffraction scans indicated that the films had good out-of-plane ordering and epitaxial registry. A carrier density of ˜2 × 1011 cm-2 and a room temperature mobility of 192 cm2/Vs were extracted from space-charge limited transport regime in the films. The electron mobility was found to exhibit in-plane anisotropy with a ratio of ˜1.8. Theoretical estimates of the temperature-dependent electron mobility including optical phonon, acoustic deformation potential, and remote ionized impurity scattering were found to satisfactorily match the measured data. The synthesis approach reported here demonstrates the feasibility of device quality few-layer MoS2 films with excellent uniformity and high quality.

  3. Local solid phase growth of few-layer graphene on silicon carbide from nickel silicide supersaturated with carbon

    SciTech Connect

    Escobedo-Cousin, Enrique; Vassilevski, Konstantin; Hopf, Toby; Wright, Nick; O'Neill, Anthony; Horsfall, Alton; Goss, Jonathan; Cumpson, Peter

    2013-03-21

    Patterned few-layer graphene (FLG) films were obtained by local solid phase growth from nickel silicide supersaturated with carbon, following a fabrication scheme, which allows the formation of self-aligned ohmic contacts on FLG and is compatible with conventional SiC device processing methods. The process was realised by the deposition and patterning of thin Ni films on semi-insulating 6H-SiC wafers followed by annealing and the selective removal of the resulting nickel silicide by wet chemistry. Raman spectroscopy and X-ray photoelectron spectroscopy (XPS) were used to confirm both the formation and subsequent removal of nickel silicide. The impact of process parameters such as the thickness of the initial Ni layer, annealing temperature, and cooling rates on the FLG films was assessed by Raman spectroscopy, XPS, and atomic force microscopy. The thickness of the final FLG film estimated from the Raman spectra varied from 1 to 4 monolayers for initial Ni layers between 3 and 20 nm thick. Self-aligned contacts were formed on these patterned films by contact photolithography and wet etching of nickel silicide, which enabled the fabrication of test structures to measure the carrier concentration and mobility in the FLG films. A simple model of diffusion-driven solid phase chemical reaction was used to explain formation of the FLG film at the interface between nickel silicide and silicon carbide.

  4. Free-standing few-layered graphene oxide films: selective, steady and lasting permeation of organic molecules with adjustable speeds.

    PubMed

    Huang, Tao; An, Qi; Luan, Xinglong; Zhang, Qian; Zhang, Yihe

    2016-01-28

    A variety of small molecules with diameters around 1 nm possess a range of functions, such as antibiotic, antimicrobic, anticoagulant, pesticidal and chemotherapy effects, making these molecules especially useful in various applications ranging from medical treatment to environmental microbiological control. However, the long-term steady delivery (release or permeation) of these small molecules with adjustable and controllable speeds has remained an especially challenging task. In this study, we prepared covalently cross-linked free-standing few-layered GO films using a layer-by-layer technique in combination with photochemical cross-linkages, and achieved a controlled release of positively charged, negatively charged, and zwitterionic small molecules with adjustable and controllable speeds. The steady delivery of the small molecule lasted up to 9 days. Other functionalities, such as graphene-enhanced Raman spectra and electrochemical properties that could also be integrated or employed in delivery systems, were also studied for our films. We expect the special molecular delivery properties of our films to lead to new possibilities in drug/fertilizer delivery and environmental microbiological control applications. PMID:26698634

  5. Synthesis of few-layered, high-purity graphene oxide sheets from different graphite sources for biology

    NASA Astrophysics Data System (ADS)

    Jasim, Dhifaf A.; Lozano, Neus; Kostarelos, Kostas

    2016-03-01

    This work aimed to interrogate the role that the starting graphitic material played on the physicochemical properties of graphene oxide (GO) sheets and their impact on mammalian cell viability following exposure to those flakes. Three different GO thin sheets were synthesised from three starting graphite material: flakes (GO-f), ground (GO-g) and powder (GO-p) using a modified Hummers’ method. The synthetic yield of this methodology was found to differ according to type of starting material, with GO-p resulting in most efficient yields. Structural and morphological comparison of the three GO sheet types were carried out using transmission electron microscopy and atomic force microscopy. Optical properties were measured using UV/visible and fluorescence spectroscopy. Surface characteristics and chemistry were determined using a battery of techniques. Exposure to human cells was studied using the human A549 lung epithelial cultures. Our results revealed that all three GO samples were composed of few-layer sheets with similar physicochemical and surface characteristics. However, significant differences were observed in terms of their lateral dimensions with GO-p, prepared from graphite powder, being the largest among the GOs. No cytotoxicity was detected for any of the GO samples following exposure onto A549 cells up to 48 h. In conclusion, the form and type of the starting graphite material is shown to be an important factor that can determine the synthetic yield and the structural characteristics of the resulting GO sheets.

  6. Understanding the role of few-layer graphene nanosheets in enhancing the hydrogen sorption kinetics of magnesium hydride.

    PubMed

    Liu, Guang; Wang, Yijing; Jiao, Lifang; Yuan, Huatang

    2014-07-23

    The catalytic effects of few-layer, highly wrinkled graphene nanosheet (GNS) addition on the dehydrogenation/rehydrogenation performance of MgH2 were investigated. It was found that MgH2-5 wt %GNSs nanocomposites prepared by ball milling exhibit relatively lower sorption temperature, faster sorption kinetics, and more stable cycling performance than that of pure-milled MgH2. The dehydrogenation step confirms that the Avrami exponent n increases from 1.22 to 2.20 by the Johnson-Mehl-Avrami (JMA) formalism when the desorption temperature is reduced from 350 °C to 320 °C and 300 °C, implying that a change in the decomposition temperature can alter the mechanism during the dehydrogenation process. For rehydrogenation, the Avrami value n is close to 1; further study by several models coincident with n = 1 reveals that the absorption process of the MgH2-5 wt %GNSs sample conforms to the Mampel equation formulated through the random nucleation approach and that the nature of the absorption mechanism does not change within the temperature range studied. Furthermore, microstructure analysis demonstrated that the defective GNSs are distributed uniformly among the MgH2 particles and that the grain size of the MgH2-5 wt %GNSs nanocomposite is approximately 5-9 nm. The efficient metal-free catalytic dehydrogenation/rehydrogenation of MgH2 can be attributed to the coupling of the nanosize effect and defective GNSs.

  7. Ultrafine nickel oxide quantum dots enbedded with few-layer exfoliative graphene for an asymmetric supercapacitor: Enhanced capacitances by alternating voltage

    NASA Astrophysics Data System (ADS)

    Jing, Mingjun; Wang, Chiwei; Hou, Hongshuai; Wu, Zhibin; Zhu, Yirong; Yang, Yingchang; Jia, Xinnan; Zhang, Yan; Ji, Xiaobo

    2015-12-01

    A green and one-step method of electrochemical alternating voltage has been utilized to form NiO quantum dots/graphene flakes (NiO-dots/Gh) for supercapacitor applications. NiO quantum dots (∼3 nm) are uniformly deposited on few-layer graphene surfaces by oxygen functional groups on graphene surface that is naturally utilized to bridge NiO and graphene through Ni-O-C bands, which exhibits outstanding specific capacitance 1181.1 F g-1 at a current density of 2.1 A g-1 and rate behavior 66.2% at 42 A g-1 as NiO dots can be fleetly wired up to current collector through the underlying graphene two-dimensional layers. The NiO-dots/Gh composite is further undertaken in asymmetric supercapacitors with high energy density (27.3 Wh kg-1 at 1562.6 W kg-1).

  8. Phosphorus and nitrogen dual-doped few-layered porous graphene: a high-performance anode material for lithium-ion batteries.

    PubMed

    Ma, Xinlong; Ning, Guoqing; Qi, Chuanlei; Xu, Chenggen; Gao, Jinsen

    2014-08-27

    Few-layered graphene networks composed of phosphorus and nitrogen dual-doped porous graphene (PNG) are synthesized via a MgO-templated chemical vapor deposition (CVD) using (NH4)3PO4 as N and P source. P and N atoms have been substitutionally doped in graphene networks since the doping takes place at the same time with the graphene growth in the CVD process. Raman spectra show that the amount of defects or disorders increases after P and N atoms are incorporated into graphene frameworks. The doping levels of P and N measured by X-ray photoelectron spectroscopy are 0.6 and 2.6 at %, respectively. As anodes for Li ion batteries (LIBs), the PNG electrode exhibits high reversible capacity (2250 mA h g(-1) at the current density of 50 mA g(-1)), excellent rate capability (750 mA h g(-1) at 1000 mA g(-1)), and satisfactory cycling stability (no capacity decay after 1500 cycles), showing much enhanced electrode performance as compared to the undoped few-layered porous graphene. Our results show that the PNG is a promising candidate for anode materials in high-rate LIBs.

  9. Direct physical exfoliation of few-layer graphene from graphite grown on a nickel foil using polydimethylsiloxane with tunable elasticity and adhesion.

    PubMed

    Yoo, Kwanghyun; Takei, Yusuke; Kim, Sungjin; Chiashi, Shohei; Maruyama, Shigeo; Matsumoto, Kiyoshi; Shimoyama, Isao

    2013-05-24

    We firstly introduce a facile method for the site-specific direct physical exfoliation of few-layer graphene sheets from cheap and easily enlargeable graphite grown on a Ni foil using an optimized polydimethylsiloxane (PDMS) stamp. By decreasing the PDMS cross-linking time, the PDMS elasticity is reduced to ∼52 kPa, similar to that of a typical gel. As a result of this process, the PDMS becomes more flexible yet remains in a handleable state as a stamp. Furthermore, the PDMS adhesion to a graphite/Ni surface, as measured by the peel strength, increases to ∼5.1 N m⁻¹, which is approximately 17 times greater than that of typical PDMS. These optimized properties allow the PDMS stamp to have improved contact with the graphite/Ni surface, including the graphite wrinkles. This process is verified, and changes in surface morphology are observed using a 3D laser scanning microscope. Under conformal contact, the optimized PDMS stamp demonstrates the site-specific direct physical exfoliation of few-layer graphene sheets including mono- and bi-layer graphene sheets from the graphite/Ni substrate without the use of special equipment, conditions or chemicals. The number of layers of the exfoliated graphene and its high quality are revealed by the measured Raman spectroscopy. The exfoliation method using tunable elasticity and adhesion of the PDMS stamp can be used not only for cost-effective mass production of defect-less few-layer graphene from the graphite substrate for micro/nano device arrays but also for nano-contact printing of various structures, devices and cells.

  10. Direct physical exfoliation of few-layer graphene from graphite grown on a nickel foil using polydimethylsiloxane with tunable elasticity and adhesion

    NASA Astrophysics Data System (ADS)

    Yoo, Kwanghyun; Takei, Yusuke; Kim, Sungjin; Chiashi, Shohei; Maruyama, Shigeo; Matsumoto, Kiyoshi; Shimoyama, Isao

    2013-05-01

    We firstly introduce a facile method for the site-specific direct physical exfoliation of few-layer graphene sheets from cheap and easily enlargeable graphite grown on a Ni foil using an optimized polydimethylsiloxane (PDMS) stamp. By decreasing the PDMS cross-linking time, the PDMS elasticity is reduced to ˜52 kPa, similar to that of a typical gel. As a result of this process, the PDMS becomes more flexible yet remains in a handleable state as a stamp. Furthermore, the PDMS adhesion to a graphite/Ni surface, as measured by the peel strength, increases to ˜5.1 N m-1, which is approximately 17 times greater than that of typical PDMS. These optimized properties allow the PDMS stamp to have improved contact with the graphite/Ni surface, including the graphite wrinkles. This process is verified, and changes in surface morphology are observed using a 3D laser scanning microscope. Under conformal contact, the optimized PDMS stamp demonstrates the site-specific direct physical exfoliation of few-layer graphene sheets including mono- and bi-layer graphene sheets from the graphite/Ni substrate without the use of special equipment, conditions or chemicals. The number of layers of the exfoliated graphene and its high quality are revealed by the measured Raman spectroscopy. The exfoliation method using tunable elasticity and adhesion of the PDMS stamp can be used not only for cost-effective mass production of defect-less few-layer graphene from the graphite substrate for micro/nano device arrays but also for nano-contact printing of various structures, devices and cells.

  11. Imaging layer number and stacking order through formulating Raman fingerprints obtained from hexagonal single crystals of few layer graphene

    NASA Astrophysics Data System (ADS)

    Hwang, Jih-Shang; Lin, Yu-Hsiang; Hwang, Jeong-Yuan; Chang, Railing; Chattopadhyay, Surojit; Chen, Chang-Jiang; Chen, Peilin; Chiang, Hai-Pang; Tsai, Tsong-Ru; Chen, Li-Chyong; Chen, Kuei-Hsien

    2013-01-01

    Quantitative mapping of layer number and stacking order for CVD-grown graphene layers is realized by formulating Raman fingerprints obtained on two stepwise stacked graphene single-crystal domains with AB Bernal and turbostratic stacking (with ˜30°interlayer rotation), respectively. The integrated peak area ratio of the G band to the Si band, AG/ASi, is proven to be a good fingerprint for layer number determination, while the area ratio of the 2D and G bands, A2D/AG, is shown to differentiate effectively between the two different stacking orders. The two fingerprints are well formulated and resolve, quantitatively, the layer number and stacking type of various graphene domains that used to rely on tedious transmission electron microscopy for structural analysis. The approach is also noticeable in easy discrimination of the turbostratic graphene region (˜30° rotation), the structure of which resembles the well known high-mobility graphene R30/R2± fault pairs found on the vacuum-annealed C-face SiC and suggests an electron mobility reaching 14 700 cm3 V-1 s-1. The methodology may shed light on monitoring and control of high-quality graphene growth, and thereby facilitate future mass production of potential high-speed graphene applications.

  12. Tunable plasmons in few-layer nitrogen-doped graphene nanostructures: A time-dependent density functional theory study

    NASA Astrophysics Data System (ADS)

    Shu, Xiao-qin; Zhang, Hong; Cheng, Xin-lu; Miyamoto, Yoshiyuki

    2016-05-01

    Compared with conventional metal plasmonic materials, surface plasmons in graphene are advantageous in terms of higher confinement, relative low loss, flexible featuring, and good tunability. However, the working frequencies of the pristine graphene (undoped graphene) surface plasmons are located in the terahertz and infrared regions, which limit their applications. Here we show high-frequency plasmons in nitrogen (N)-doped graphene nanostructures investigated by time-dependent density functional theory. We found the optical absorption strength of systems containing two layers to be more than twofold stronger than that of systems with monolayers. The optical absorption strength increases as the interlayer distance increases, and the absorption spectra are red-shifted for impulse excitations polarized in the armchair edge direction (x axis). For microstructures of more than two layers, the optical absorption strength increases as number of layers of the N-doped graphene nanostructures increases. In addition, when the number of layers becomes elevated at low-energy resonances, the absorption spectra are seen to blue-shift. The plasmon energy resonance points are located in the visible and ultraviolet regions. The N-doped graphene provides an effective strategy for nanoscale plasmon devices in the visible and ultraviolet regions, despite their weaker absorption intensities when compared with the pristine graphene.

  13. CVD synthesis of mono- and few-layer graphene using alcohols at low hydrogen concentration and atmospheric pressure

    NASA Astrophysics Data System (ADS)

    Campos-Delgado, Jessica; Botello-Méndez, Andrés R.; Algara-Siller, Gerardo; Hackens, Benoit; Pardoen, Thomas; Kaiser, Ute; Dresselhaus, Mildred S.; Charlier, Jean-Christophe; Raskin, Jean-Pierre

    2013-10-01

    An original and easy route to produce mono-, bi- and tri-layer graphene is proposed using the chemical vapor deposition technique. The synthesis is carried out at atmospheric pressure using liquid precursors, copper as catalyst, and a single gas injection line consisting of a very diluted mixture of H2 in Argon (H2: 5%). Two different alcohols are investigated as possible sources of carbon: 2-phenylethanol and ethanol. The characterization of the samples with SEM, TEM and Raman spectroscopy confirms the presence of graphene on top of copper, and yields a detailed picture of the structure of the produced graphene layers.

  14. Few-layer MoS2-anchored graphene aerogel paper for free-standing electrode materials.

    PubMed

    Lee, Wee Siang Vincent; Peng, Erwin; Loh, Tamie Ai Jia; Huang, Xiaolei; Xue, Jun Min

    2016-04-21

    To reduce the reliance on polymeric binders, conductive additives, and metallic current collectors during the electrode preparation process, as well as to assess the true performance of lithium ion battery (LIB) anodes, a free-standing electrode has to be meticulously designed. Graphene aerogel is a popular scaffolding material that has been widely used with embedded nanoparticles for application in LIB anodes. However, the current graphene aerogel/nanoparticle composite systems still involve decomposition into powder and the addition of additives during electrode preparation because of the thick aerogel structure. To further enhance the capacity of the system, MoS2 was anchored onto a graphene aerogel paper and the composite was used directly as an LIB anode. The resultant additive-free MoS2/graphene aerogel paper composite exhibited long cyclic performance with 101.1% retention after 700 cycles, which demonstrates the importance of free-standing electrodes in enhancing cyclic stability. PMID:27020143

  15. Few-layer MoS2-anchored graphene aerogel paper for free-standing electrode materials.

    PubMed

    Lee, Wee Siang Vincent; Peng, Erwin; Loh, Tamie Ai Jia; Huang, Xiaolei; Xue, Jun Min

    2016-04-21

    To reduce the reliance on polymeric binders, conductive additives, and metallic current collectors during the electrode preparation process, as well as to assess the true performance of lithium ion battery (LIB) anodes, a free-standing electrode has to be meticulously designed. Graphene aerogel is a popular scaffolding material that has been widely used with embedded nanoparticles for application in LIB anodes. However, the current graphene aerogel/nanoparticle composite systems still involve decomposition into powder and the addition of additives during electrode preparation because of the thick aerogel structure. To further enhance the capacity of the system, MoS2 was anchored onto a graphene aerogel paper and the composite was used directly as an LIB anode. The resultant additive-free MoS2/graphene aerogel paper composite exhibited long cyclic performance with 101.1% retention after 700 cycles, which demonstrates the importance of free-standing electrodes in enhancing cyclic stability.

  16. Few-layer MoS2-anchored graphene aerogel paper for free-standing electrode materials

    NASA Astrophysics Data System (ADS)

    Lee, Wee Siang Vincent; Peng, Erwin; Loh, Tamie Ai Jia; Huang, Xiaolei; Xue, Jun Min

    2016-04-01

    To reduce the reliance on polymeric binders, conductive additives, and metallic current collectors during the electrode preparation process, as well as to assess the true performance of lithium ion battery (LIB) anodes, a free-standing electrode has to be meticulously designed. Graphene aerogel is a popular scaffolding material that has been widely used with embedded nanoparticles for application in LIB anodes. However, the current graphene aerogel/nanoparticle composite systems still involve decomposition into powder and the addition of additives during electrode preparation because of the thick aerogel structure. To further enhance the capacity of the system, MoS2 was anchored onto a graphene aerogel paper and the composite was used directly as an LIB anode. The resultant additive-free MoS2/graphene aerogel paper composite exhibited long cyclic performance with 101.1% retention after 700 cycles, which demonstrates the importance of free-standing electrodes in enhancing cyclic stability.To reduce the reliance on polymeric binders, conductive additives, and metallic current collectors during the electrode preparation process, as well as to assess the true performance of lithium ion battery (LIB) anodes, a free-standing electrode has to be meticulously designed. Graphene aerogel is a popular scaffolding material that has been widely used with embedded nanoparticles for application in LIB anodes. However, the current graphene aerogel/nanoparticle composite systems still involve decomposition into powder and the addition of additives during electrode preparation because of the thick aerogel structure. To further enhance the capacity of the system, MoS2 was anchored onto a graphene aerogel paper and the composite was used directly as an LIB anode. The resultant additive-free MoS2/graphene aerogel paper composite exhibited long cyclic performance with 101.1% retention after 700 cycles, which demonstrates the importance of free-standing electrodes in enhancing cyclic

  17. Layer Number Dependence of Li(+) Intercalation on Few-Layer Graphene and Electrochemical Imaging of Its Solid-Electrolyte Interphase Evolution.

    PubMed

    Hui, Jingshu; Burgess, Mark; Zhang, Jiarui; Rodríguez-López, Joaquín

    2016-04-26

    A fundamental question facing electrodes made out of few layers of graphene (FLG) is if they display chemical properties that are different to their bulk graphite counterpart. Here, we show evidence that suggests that lithium ion intercalation on FLG, as measured via stationary voltammetry, shows a strong dependence on the number of layers of graphene that compose the electrode. Despite its extreme thinness and turbostratic structure, Li ion intercalation into FLG still proceeds through a staging process, albeit with different signatures than bulk graphite or multilayer graphene. Single-layer graphene does not show any evidence of ion intercalation, while FLG with four graphene layers displays limited staging peaks, which broaden and increase in number as the layer number increases to six. Despite these mechanistic differences on ion intercalation, the formation of a solid-electrolyte interphase (SEI) was observed on all electrodes. Scanning electrochemical microscopy (SECM) in the feedback mode was used to demonstrate changes in the surface conductivity of FLG during SEI evolution. Observation of ion intercalation on large area FLG was conditioned to the fabrication of "ionic channels" on the electrode. SECM measurements using a recently developed Li-ion sensitive imaging technique evidenced the role of these channels in enabling Li-ion intercalation through localized flux measurements. This work highlights the impact of nanostructure and microstructure on macroscopic electrochemical behavior and provides guidance to the mechanistic control of ion intercalation using graphene, an atomically thin interface where surface and bulk reactivity converge. PMID:26943950

  18. Fabrication of few-layer graphene film based field effect transistor and its application for trace-detection of herbicide atrazine

    NASA Astrophysics Data System (ADS)

    Thanh Cao, Thi; Chuc Nguyen, Van; Binh Nguyen, Hai; Thang Bui, Hung; Thu Vu, Thi; Phan, Ngoc Hong; Thang Phan, Bach; Hoang, Le; Bayle, Maxime; Paillet, Matthieu; Sauvajol, Jean Louis; Phan, Ngoc Minh; Tran, Dai Lam

    2016-09-01

    We describe the fabrication of highly sensitive graphene-based field effect transistor (FET) enzymatic biosensor for trace-detection of atrazine. The few-layers graphene films were prepared on polycrystalline copper foils by atmospheric pressure chemical vapor deposition method using an argon/hydrogen/methane mixture. The characteristics of graphene films were investigated by scanning electron microscopy, transmission electron microscopy and Raman spectroscopy. The results indicated low uniformity of graphene layers, which is probably induced by heterogeneous distribution of graphene nucleation sites on the Cu surface. The pesticide detection is accomplished through the measurement of the drain-source current variations of the FET sensor upon the urea enzymatic hydrolysis reaction. The obtained biosensor is able to detect atrazine with a sensitivity of 56 μA/logCATZ in range between 2 × 10-4 and 20 ppb and has a limit of detection as low as 0.05 ppt. The elaboration of such highly sensitive biosensors will provide better biosensing performances for the detection of biochemical targets.

  19. Fabrication of few-layer graphene film based field effect transistor and its application for trace-detection of herbicide atrazine

    NASA Astrophysics Data System (ADS)

    Thanh Cao, Thi; Chuc Nguyen, Van; Binh Nguyen, Hai; Thang Bui, Hung; Thu Vu, Thi; Phan, Ngoc Hong; Thang Phan, Bach; Hoang, Le; Bayle, Maxime; Paillet, Matthieu; Sauvajol, Jean Louis; Phan, Ngoc Minh; Tran, Dai Lam

    2016-09-01

    We describe the fabrication of highly sensitive graphene-based field effect transistor (FET) enzymatic biosensor for trace-detection of atrazine. The few-layers graphene films were prepared on polycrystalline copper foils by atmospheric pressure chemical vapor deposition method using an argon/hydrogen/methane mixture. The characteristics of graphene films were investigated by scanning electron microscopy, transmission electron microscopy and Raman spectroscopy. The results indicated low uniformity of graphene layers, which is probably induced by heterogeneous distribution of graphene nucleation sites on the Cu surface. The pesticide detection is accomplished through the measurement of the drain-source current variations of the FET sensor upon the urea enzymatic hydrolysis reaction. The obtained biosensor is able to detect atrazine with a sensitivity of 56 μA/logCATZ in range between 2 × 10‑4 and 20 ppb and has a limit of detection as low as 0.05 ppt. The elaboration of such highly sensitive biosensors will provide better biosensing performances for the detection of biochemical targets.

  20. One-Minute Room-Temperature Transfer-Free Production of Mono- and Few-Layer Polycrystalline Graphene on Various Substrates

    PubMed Central

    Jiang, Shenglin; Zeng, Yike; Zhou, Wenli; Miao, Xiangshui; Yu, Yan

    2016-01-01

    Graphene deposited on various substrates has attracted the attention of the scientific and technical communities for use in a wide range of applications. Graphene on substrates is commonly produced by two types of methods, namely, methods that require a transfer step and transfer-free methods. Compared with methods that require a transfer step, transfer-free methods have a simpler procedure and a lower cost. Thus, transfer-free methods have considerable potential to meet the industrial and commercial demands of production methods. However, some limitations of the current transfer-free methods must be overcome, such as the high temperatures encountered during production, the relatively long manufacturing times, incompatibilities for both rigid and flexible substrates, and an inability to extend the process to other two-dimensional (2-D) atomic crystals. In this work, a room-temperature rubbing method is developed for the rapid transfer-free production of defect-free polycrystalline graphene on rigid and flexible substrates. Starting with inexpensive commercially obtained graphite powder, mono- and few-layer graphene can be fabricated directly on various substrates, with an average production time of less than one minute (from raw graphite to graphene on the substrate). Importantly, this method can be extended to other 2-D atomic crystals. PMID:26763292

  1. One-Minute Room-Temperature Transfer-Free Production of Mono- and Few-Layer Polycrystalline Graphene on Various Substrates.

    PubMed

    Jiang, Shenglin; Zeng, Yike; Zhou, Wenli; Miao, Xiangshui; Yu, Yan

    2016-01-01

    Graphene deposited on various substrates has attracted the attention of the scientific and technical communities for use in a wide range of applications. Graphene on substrates is commonly produced by two types of methods, namely, methods that require a transfer step and transfer-free methods. Compared with methods that require a transfer step, transfer-free methods have a simpler procedure and a lower cost. Thus, transfer-free methods have considerable potential to meet the industrial and commercial demands of production methods. However, some limitations of the current transfer-free methods must be overcome, such as the high temperatures encountered during production, the relatively long manufacturing times, incompatibilities for both rigid and flexible substrates, and an inability to extend the process to other two-dimensional (2-D) atomic crystals. In this work, a room-temperature rubbing method is developed for the rapid transfer-free production of defect-free polycrystalline graphene on rigid and flexible substrates. Starting with inexpensive commercially obtained graphite powder, mono- and few-layer graphene can be fabricated directly on various substrates, with an average production time of less than one minute (from raw graphite to graphene on the substrate). Importantly, this method can be extended to other 2-D atomic crystals. PMID:26763292

  2. Few-layer and symmetry-breaking effects on the electrical properties of ordered CF3Cl phases on graphene

    NASA Astrophysics Data System (ADS)

    Morales-Cifuentes, Josue; Wang, Yilin; Reutt-Robey, Janice; Einstein, T. L.

    2014-03-01

    An effective pseudopotential mechanism for breaking the inherent sub-lattice symmetry of graphene has been studied using DFT calculations on hexagonal boron nitride. Electrical detection of CF3Cl phase transitions on graphene shows the existence of a commensurate ordered phase in which this can be tested. We study the electronic properties of this phase using VASP ver 5.3.3, with ab initio van der Waals density functionals (vdW-DF1 and vdW-DF2). Consistent with a physisorbed phase, binding energies and charge transfer per CF3Cl molecule are calculated to be on the order of 280meV and 0.01e, respectively. By exploring different coverages and orientations of this ordered phase we are able to open a band gap in some configurations; said gap is in the range of 8 to 80meV depending on the strength of the effective pseudopotential. Furthermore, we calculate the screening of these effects in bi-layer and tri-layer graphene. Work supported by NSF-MRSEC at UMD, grant DMR 05-20471 and NSF-CHE 13-05892.

  3. CO2 enhanced chemical vapor deposition growth of few-layer graphene over NiO(x).

    PubMed

    Son, In Hyuk; Song, Hyun Jae; Kwon, Soonchul; Bachmatiuk, Alicja; Lee, Seung Jae; Benayad, Anass; Park, Jong Hwan; Choi, Jae-Young; Chang, Hyuk; Rümmeli, Mark H

    2014-09-23

    The use of mild oxidants in chemical vapor deposition (CVD) reactions has proven enormously useful. This was also true for the CVD growth of carbon nanotubes. As yet though, the use of mild oxidants in the CVD of graphene has remained unexplored. Here we explore the use of CO2 as a mild oxidant during the growth of graphene over Ni with CH4 as the feedstock. Both our experimental and theoretical findings provide in-depth insight into the growth mechanisms and point to the mild oxidants playing multiple roles. Mild oxidants lead to the formation of a suboxide in the Ni, which suppresses the bulk diffusion of C species suggesting a surface growth mechanism. Moreover, the formation of a suboxide leads to enhanced catalytic activity at the substrate surface, which allows reduced synthesis temperatures, even as low as 700 °C. Even at these low temperatures, the quality of the graphene is exceedingly high as indicated by a negligible D mode in the Raman spectra. These findings suggest the use of mild oxidants in the CVD fabrication as a whole could have a positive impact. PMID:25171048

  4. Dissolution-and-reduction CVD synthesis of few-layer graphene on ultra-thin nickel film lifted off for mode-locking fiber lasers

    PubMed Central

    Peng, Kaung-Jay; Lin, Yung-Hsiang; Wu, Chung-Lun; Lin, Sheng-Fong; Yang, Chun-Yu; Lin, Shih-Meng; Tsai, Din-Ping; Lin, Gong-Ru

    2015-01-01

    The in-situ dissolution-and-reduction CVD synthesized few-layer graphene on ultra-thin nickel catalyst film is demonstrated at temperature as low as 550 °C, which can be employed to form transmission-type or reflection-type saturable absorber (SA) for mode-locking the erbium-doped fiber lasers (EDFLs). With transmission-type graphene SA, the EDFL shortens its pulsewidth from 483 to 441 fs and broadens its spectral linewidth from 4.2 to 6.1 nm with enlarging the pumping current from 200 to 900 mA. In contrast, the reflection-type SA only compresses the pulsewidth from 875 to 796 fs with corresponding spectral linewidth broadened from 2.2 to 3.3 nm. The reflection-type graphene mode-locker increases twice of its equivalent layer number to cause more insertion loss than the transmission-type one. Nevertheless, the reflection-type based saturable absorber system can generate stabilized soliton-like pulse easier than that of transmission-type system, because the nonlinearity induced self-amplitude modulation depth is simultaneously enlarged when passing through the graphene twice under the retro-reflector design. PMID:26328535

  5. Sulfur and nitrogen co-doped, few-layered graphene oxide as a highly efficient electrocatalyst for the oxygen-reduction reaction.

    PubMed

    Xu, Jiaoxing; Dong, Guofa; Jin, Chuanhong; Huang, Meihua; Guan, Lunhui

    2013-03-01

    S and N co-doped, few-layered graphene oxide is synthesized by using pyrimidine and thiophene as precursors for the application of the oxygen reduction reaction (ORR). The dual-doped catalyst with pyrrolic/graphitic N-dominant structures exhibits competitive catalytic activity (10.0 mA cm(-2) kinetic-limiting current density at -0.25 V) that is superior to that for mono N-doped carbon nanomaterials. This is because of a synergetic effect of N and S co-doping. Furthermore, the dual-doped catalyst also shows an efficient four-electron-dominant ORR process, which has excellent methanol tolerance and improved durability in comparison to commercial Pt/C catalysts. PMID:23404829

  6. Unusual surface and edge morphologies, sp2 to sp3 hybridized transformation and electronic damage after Ar+ ion irradiation of few-layer graphene surfaces.

    PubMed

    Al-Harthi, Salim Hamood; Elzain, Mohammed; Al-Barwani, Muataz; Kora'a, Amal; Hysen, Thomas; Myint, Myo Tay Zar; Anantharaman, Maliemadom Ramaswamy

    2012-01-01

    Roughness and defects induced on few-layer graphene (FLG) irradiated by Ar+ ions at different energies were investigated using X-ray photoemission spectroscopy (XPS) and atomic force microscopy techniques. The results provide direct experimental evidence of ripple formation, sp2 to sp3 hybridized carbon transformation, electronic damage, Ar+ implantation, unusual defects and edge reconstructions in FLG, which depend on the irradiation energy. In addition, shadowing effects similar to those found in oblique-angle growth of thin films were seen. Reliable quantification of the transition from the sp2-bonding to sp3-hybridized state as a result of Ar+ ion irradiation is achieved from the deconvolution of the XPS C (1s) peak. Although the ion irradiation effect is demonstrated through the shape of the derivative of the Auger transition C KVV spectra, we show that the D parameter values obtained from these spectra which are normally used in the literature fail to account for the sp2 to sp3 hybridization transition. In contrast to what is known, it is revealed that using ion irradiation at large FLG sample tilt angles can lead to edge reconstructions. Furthermore, FLG irradiation by low energy of 0.25 keV can be a plausible way of peeling graphene layers without the need of Joule heating reported previously. PMID:22901368

  7. Binder free three-dimensional sulphur/few-layer graphene foam cathode with enhanced high-rate capability for rechargeable lithium sulphur batteries.

    PubMed

    Xi, Kai; Kidambi, Piran R; Chen, Renjie; Gao, Chenlong; Peng, Xiaoyu; Ducati, Caterina; Hofmann, Stephan; Kumar, R Vasant

    2014-06-01

    A novel ultra-lightweight three-dimensional (3-D) cathode system for lithium sulphur (Li-S) batteries has been synthesised by loading sulphur on to an interconnected 3-D network of few-layered graphene (FLG) via a sulphur solution infiltration method. A free-standing FLG monolithic network foam was formed as a negative of a Ni metallic foam template by CVD followed by etching away of Ni. The FLG foam offers excellent electrical conductivity, an appropriate hierarchical pore structure for containing the electro-active sulphur and facilitates rapid electron/ion transport. This cathode system does not require any additional binding agents, conductive additives or a separate metallic current collector thus decreasing the weight of the cathode by typically ∼20-30 wt%. A Li-S battery with the sulphur-FLG foam cathode shows good electrochemical stability and high rate discharge capacity retention for up to 400 discharge/charge cycles at a high current density of 3200 mA g(-1). Even after 400 cycles the capacity decay is only ∼0.064% per cycle relative to the early (e.g. the 5th cycle) discharge capacity, while yielding an average columbic efficiency of ∼96.2%. Our results indicate the potential suitability of graphene foam for efficient, ultra-light and high-performance batteries.

  8. Binder free three-dimensional sulphur/few-layer graphene foam cathode with enhanced high-rate capability for rechargeable lithium sulphur batteries

    NASA Astrophysics Data System (ADS)

    Xi, Kai; Kidambi, Piran R.; Chen, Renjie; Gao, Chenlong; Peng, Xiaoyu; Ducati, Caterina; Hofmann, Stephan; Kumar, R. Vasant

    2014-05-01

    A novel ultra-lightweight three-dimensional (3-D) cathode system for lithium sulphur (Li-S) batteries has been synthesised by loading sulphur on to an interconnected 3-D network of few-layered graphene (FLG) via a sulphur solution infiltration method. A free-standing FLG monolithic network foam was formed as a negative of a Ni metallic foam template by CVD followed by etching away of Ni. The FLG foam offers excellent electrical conductivity, an appropriate hierarchical pore structure for containing the electro-active sulphur and facilitates rapid electron/ion transport. This cathode system does not require any additional binding agents, conductive additives or a separate metallic current collector thus decreasing the weight of the cathode by typically ~20-30 wt%. A Li-S battery with the sulphur-FLG foam cathode shows good electrochemical stability and high rate discharge capacity retention for up to 400 discharge/charge cycles at a high current density of 3200 mA g-1. Even after 400 cycles the capacity decay is only ~0.064% per cycle relative to the early (e.g. the 5th cycle) discharge capacity, while yielding an average columbic efficiency of ~96.2%. Our results indicate the potential suitability of graphene foam for efficient, ultra-light and high-performance batteries.A novel ultra-lightweight three-dimensional (3-D) cathode system for lithium sulphur (Li-S) batteries has been synthesised by loading sulphur on to an interconnected 3-D network of few-layered graphene (FLG) via a sulphur solution infiltration method. A free-standing FLG monolithic network foam was formed as a negative of a Ni metallic foam template by CVD followed by etching away of Ni. The FLG foam offers excellent electrical conductivity, an appropriate hierarchical pore structure for containing the electro-active sulphur and facilitates rapid electron/ion transport. This cathode system does not require any additional binding agents, conductive additives or a separate metallic current collector

  9. Dielectric properties of novel composites prepared with few layered graphene (FLG)-lithium triniobate (LiNb{sub 3}O{sub 8})

    SciTech Connect

    Tumuluri, Anil; Raju, K. C. James; Marka, Sandeep Kumar; Srikanth, V. V. S. S.

    2015-08-28

    Lithium triniobate (LiNb{sub 3}O{sub 8}) has been prepared using microwave assisted combustion synthesis at a low temperature of 400 °C. Graphite oxide is synthesized using Hummers method and thereafter it is thermally exfoliated at 500 and 700 °C to obtain two samples of Few Layered Graphene (FLG). Then, FLG-LiNb{sub 3}O{sub 8} composites prepared through a simple ultra-sonication assisted solution mixing process. The obtained samples are named as FLN5 and FLN7 based on the temperature used to obtain FLG. Low frequency dielectric measurements are recorded for both the samples and the measured dielectric constant is observed to be more for FLN5 (250 at 60 Hz) than FLN7 (115 at 60 Hz) whilst the dielectric loss is less in case of FLN5 (1.525 at 60 Hz). The enhancement in dielectric properties for FLN5 is explained in terms of polarization in FLG-LiNb{sub 3}O{sub 8} composites.

  10. Resonant orbitals in fluorinated epitaxial graphene.

    PubMed

    Gunasinghe, R N; Samarakoon, D K; Arampath, A B; Shashikala, H B M; Vilus, J; Hall, J H; Wang, X-Q

    2014-09-21

    Fluorinated epitaxial graphene has potential applications in organic electronics. We present the calculation results by means of first-principles density-functional-theory for various fluorination patterns. Our results indicate that semi-fluorinated graphene conformations follow the same energetic order as the corresponding hydrogenated graphene counterparts. The distinctive electronic properties between semi-hydrogenated graphene and semi-fluorinated graphene are attributed to the polar covalent C-F bond in contrast to the covalent C-H bond. The partial ionic character of the C-F bond results in the hyperconjugation of C-F σ-bonds with an sp(2) network of graphene. Resonant orbitals stabilize the stirrup conformation via the gauche effect. Resonant orbitals also lead to electron doping of the sp(2) network and enhanced excitonic effect. The implications of resonant-orbital-induced doping for the electronic and magnetic properties of fluorinated epitaxial graphene are discussed.

  11. Epitaxial graphene: the material for graphene electronics

    SciTech Connect

    Sprinkle, M.; Soukiassian, P.; de Heer, W.A.; Berger, C.; Conrad, E.H.

    2009-12-10

    The search for an ideal graphene sheet has been a quest driving graphene research. While most research has focused on exfoliated graphene, intrinsic substrate interactions and mechanical disorder have precluded the observation of a number of graphene's expected physical properties in this material. The only graphene candidate that has demonstrated all the essential properties of an ideal sheet is multilayer graphene grown on the SiC(000) surface. Its unique stacking allows nearly all the sheets in the stack to behave like isolated graphene, while the weak graphene-graphene interaction prevents any significant doping or distortion in the band near the Fermi level.

  12. Selective epitaxial growth of graphene on SiC

    SciTech Connect

    Camara, N.; Rius, G.; Godignon, P.; Huntzinger, J.-R.; Tiberj, A.; Camassel, J.

    2008-09-22

    We present a method of selective epitaxial growth of few layers graphene (FLG) on a ''prepatterned'' silicon carbide (SiC) substrate. The methods involves, successively, the sputtering of a thin aluminium nitride (AlN) layer on top of a monocrystalline SiC substrate and, then, patterning it with e-beam lithography and wet etching. The sublimation of few atomic layers of Si from the SiC substrate occurs only through the selectively etched AlN layer. The presence of the Raman G-band at {approx}1582 cm{sup -1} in the AlN-free areas is used to validate the concept. It gives absolute evidence of selective FLG growth.

  13. Selective epitaxial growth of graphene on SiC

    NASA Astrophysics Data System (ADS)

    Camara, N.; Rius, G.; Huntzinger, J.-R.; Tiberj, A.; Mestres, N.; Godignon, P.; Camassel, J.

    2008-09-01

    We present a method of selective epitaxial growth of few layers graphene (FLG) on a "prepatterned" silicon carbide (SiC) substrate. The methods involves, successively, the sputtering of a thin aluminium nitride (AlN) layer on top of a monocrystalline SiC substrate and, then, patterning it with e-beam lithography and wet etching. The sublimation of few atomic layers of Si from the SiC substrate occurs only through the selectively etched AlN layer. The presence of the Raman G-band at ˜1582cm-1 in the AlN-free areas is used to validate the concept. It gives absolute evidence of selective FLG growth.

  14. Epitaxial growth of large area single-crystalline few-layer MoS{sub 2} with high space charge mobility of 192 cm{sup 2} V{sup −1} s{sup −1}

    SciTech Connect

    Ma, Lu; Yu, Mingzhe; Wu, Yiying E-mail: wu@chemistry.ohio-state.edu; Nath, Digbijoy N.; Lee, Edwin W.; Lee, Choong Hee; Arehart, Aaron; Rajan, Siddharth E-mail: wu@chemistry.ohio-state.edu

    2014-08-18

    We report on the vapor-solid growth of single crystalline few-layer MoS{sub 2} films on (0001)-oriented sapphire with excellent structural and electrical properties over centimeter length scale. High-resolution X-ray diffraction scans indicated that the films had good out-of-plane ordering and epitaxial registry. A carrier density of ∼2 × 10{sup 11 }cm{sup −2} and a room temperature mobility of 192 cm{sup 2}/Vs were extracted from space-charge limited transport regime in the films. The electron mobility was found to exhibit in-plane anisotropy with a ratio of ∼1.8. Theoretical estimates of the temperature-dependent electron mobility including optical phonon, acoustic deformation potential, and remote ionized impurity scattering were found to satisfactorily match the measured data. The synthesis approach reported here demonstrates the feasibility of device quality few-layer MoS{sub 2} films with excellent uniformity and high quality.

  15. New X-ray insight into oxygen intercalation in epitaxial graphene grown on 4H-SiC(0001)

    SciTech Connect

    Kowalski, G. Tokarczyk, M.; Dąbrowski, P.; Ciepielewski, P.; Możdżonek, M.; Strupiński, W.; Baranowski, J. M.

    2015-03-14

    Efficient control of intercalation of epitaxial graphene by specific elements is a way to change properties of the graphene. Results of several experimental techniques, such as X-ray photoelectron spectroscopy, micro-Raman mapping, reflectivity, attenuated total reflection, X-ray diffraction, and X-ray reflectometry, gave a new insight into the intercalation of oxygen in the epitaxial graphene grown on 4H-SiC(0001). These results confirmed that oxygen intercalation decouples the graphene buffer layer from the 4H-SiC surface and converts it into the graphene layer. However, in contrast to the hydrogen intercalation, oxygen does not intercalate between carbon planes (in the case of few layer graphene) and the interlayer spacing stays constant at the level of 3.35–3.32 Å. Moreover, X-ray reflectometry showed the presence of an oxide layer having the thickness of about 0.8 Å underneath the graphene layers. Apart from the formation of the nonuniform thin oxide layer, generation of defects in graphene caused by oxygen was also evidenced. Last but not least, water islands underneath defected graphene regions in both intercalated and non-intercalated samples were most probably revealed. These water islands are formed in the case of all the samples stored under ambient laboratory conditions. Water islands can be removed from underneath the few layer graphene stacks by relevant thermal treatment or by UV illumination.

  16. Exfoliating and Dispersing Few-Layered Graphene in Low-Boiling-Point Organic Solvents towards Solution-Processed Optoelectronic Device Applications.

    PubMed

    Zhang, Lu; Miao, Zhongshuo; Hao, Zhen; Liu, Jun

    2016-05-01

    With normal organic surfactants, graphene can only be dispersed in water and cannot be dispersed in low-boiling-point organic solvents, which hampers its application in solution-processed organic optoelectronic devices. Herein, we report the exfoliation of graphite into graphene in low-boiling-point organic solvents, for example, methanol and acetone, by using edge-carboxylated graphene quantum dots (ECGQD) as the surfactant. The great capability of ECGQD for graphene dispersion is due to its ultralarge π-conjugated unit that allows tight adhesion on the graphene surface through strong π-π interactions, its edge-carboxylated structure that diminishes the steric effects of the oxygen-containing functional groups on the basal plane of ECGQD, and its abundance of carboxylic acid groups for solubility. The graphene dispersion in methanol enables the application of graphene:ECGQD as a cathode interlayer in polymer solar cells (PSCs). Moreover, the PSC device performance of graphene:ECGQD is better than that of Ca, the state-of-the-art cathode interlayer material.

  17. Exfoliating and Dispersing Few-Layered Graphene in Low-Boiling-Point Organic Solvents towards Solution-Processed Optoelectronic Device Applications.

    PubMed

    Zhang, Lu; Miao, Zhongshuo; Hao, Zhen; Liu, Jun

    2016-05-01

    With normal organic surfactants, graphene can only be dispersed in water and cannot be dispersed in low-boiling-point organic solvents, which hampers its application in solution-processed organic optoelectronic devices. Herein, we report the exfoliation of graphite into graphene in low-boiling-point organic solvents, for example, methanol and acetone, by using edge-carboxylated graphene quantum dots (ECGQD) as the surfactant. The great capability of ECGQD for graphene dispersion is due to its ultralarge π-conjugated unit that allows tight adhesion on the graphene surface through strong π-π interactions, its edge-carboxylated structure that diminishes the steric effects of the oxygen-containing functional groups on the basal plane of ECGQD, and its abundance of carboxylic acid groups for solubility. The graphene dispersion in methanol enables the application of graphene:ECGQD as a cathode interlayer in polymer solar cells (PSCs). Moreover, the PSC device performance of graphene:ECGQD is better than that of Ca, the state-of-the-art cathode interlayer material. PMID:26957045

  18. Exceptional ballistic transport in epitaxial graphene nanoribbons.

    PubMed

    Baringhaus, Jens; Ruan, Ming; Edler, Frederik; Tejeda, Antonio; Sicot, Muriel; Taleb-Ibrahimi, Amina; Li, An-Ping; Jiang, Zhigang; Conrad, Edward H; Berger, Claire; Tegenkamp, Christoph; de Heer, Walt A

    2014-02-20

    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. This is equivalent to sheet resistances below 1 ohm per square, surpassing theoretical predictions for perfect graphene by at least an order of magnitude. In neutral graphene ribbons, we show that transport is dominated by two modes. One is ballistic and temperature independent; the other is thermally activated. Transport is protected from back-scattering, possibly reflecting ground-state properties of neutral graphene. At room temperature, the resistance of both modes is found to increase abruptly at a particular length--the ballistic mode at 16 micrometres and the other at 160 nanometres. Our epitaxial graphene nanoribbons will be important not only in fundamental science, but also--because they can be readily produced in thousands--in advanced nanoelectronics, which can make use of their room-temperature ballistic transport properties.

  19. Superconductivity in Ca-intercalated epitaxial graphene on silicon carbide

    NASA Astrophysics Data System (ADS)

    Li, Kang; Feng, Xiao; Zhang, Wenhao; Ou, Yunbo; Chen, Lianlian; He, Ke; Wang, Li-Li; Guo, Liwei; Liu, Guodong; Xue, Qi-Kun; Ma, Xucun

    2013-08-01

    We have prepared Ca-intercalated multilayer epitaxial graphene films on silicon carbide and observed superconductivity in them with both magnetic and transport measurements. Superconducting transition has been detected at temperature up to 7 K in Ca-intercalated epitaxial graphene with the thickness down to 10 layers grown on both Si-face and C-face of silicon carbide. The result demonstrates intercalated epitaxial graphene as a good platform to study graphene-based superconductivity.

  20. Exfoliation of graphite with triazine derivatives under ball-milling conditions: preparation of few-layer graphene via selective noncovalent interactions.

    PubMed

    León, Verónica; Rodriguez, Antonio M; Prieto, Pilar; Prato, Maurizio; Vázquez, Ester

    2014-01-28

    A ball-milling treatment can be employed to exfoliate graphite through interactions with commercially available melamine under solid conditions. This procedure allows the fast production of relatively large quantities of material with a low presence of defects. The milling treatment can be modulated in order to achieve graphene flakes with different sizes. Once prepared, the graphene samples can be redispersed in organic solvents, water, or culture media, forming stable dispersions that can be used for multiple purposes. In the present work, we have screened electron-rich benzene derivatives along with triazine derivatives in their respective ability to exfoliate graphite. The results suggest that the formation of a hydrogen-bonding network is important for the formation of multipoint interactions with the surfaces of graphene, which can be used for the exfoliation of graphite and the stabilization of graphene in different solvents. Aminotriazine systems were found to be the best partners in the preparation and stabilization of graphene layers in different solvents, while the equivalent benzene derivatives did not show comparable exfoliation ability. Computational studies have also been performed to rationalize the experimental results. The results provide also the basis for further work in the preparation of noncovalently modified graphene, where derivatives of aminotriazines can be designed to form extensive hydrogen-bond 2D networks on the graphene surface with the aim of manipulating their electronic and chemical properties.

  1. Scattering and interference in epitaxial graphene.

    PubMed

    Rutter, G M; Crain, J N; Guisinger, N P; Li, T; First, P N; Stroscio, J A

    2007-07-13

    A single sheet of carbon, graphene, exhibits unexpected electronic properties that arise from quantum state symmetries, which restrict the scattering of its charge carriers. Understanding the role of defects in the transport properties of graphene is central to realizing future electronics based on carbon. Scanning tunneling spectroscopy was used to measure quasiparticle interference patterns in epitaxial graphene grown on SiC(0001). Energy-resolved maps of the local density of states reveal modulations on two different length scales, reflecting both intravalley and intervalley scattering. Although such scattering in graphene can be suppressed because of the symmetries of the Dirac quasiparticles, we show that, when its source is atomic-scale lattice defects, wave functions of different symmetries can mix.

  2. On the density of states of disordered epitaxial graphene

    SciTech Connect

    Davydov, S. Yu.

    2015-05-15

    The study is concerned with two types of disordered epitaxial graphene: (i) graphene with randomly located carbon vacancies and (ii) structurally amorphous graphene. The former type is considered in the coherent potential approximation, and for the latter type, a model of the density of states is proposed. The effects of two types of substrates, specifically, metal and semiconductor substrates are taken into account. The specific features of the density of states of epitaxial graphene at the Dirac point and the edges of the continuous spectrum are analyzed. It is shown that vacancies in epitaxial graphene formed on the metal substrate bring about logarithmic nulling of the density of states of graphene at the Dirac point and the edges of the continuous spectrum. If the Dirac point corresponds to the middle of the band gap of the semiconductor substrate, the linear trend of the density of states to zero in the vicinity of the Dirac point in defect-free graphene transforms into a logarithmic decrease in the presence of vacancies. In both cases, the graphene-substrate interaction is assumed to be weak (quasi-free graphene). In the study of amorphous epitaxial graphene, a simple model of free amorphous graphene is proposed as the initial model, in which account is taken of the nonzero density of states at the Dirac point, and then the interaction of the graphene sheet with the substrate is taken into consideration. It is shown that, near the Dirac point, the quadratic behavior of the density of states of free amorphous graphene transforms into a linear dependence for amorphous epitaxial graphene. In the study, the density of states of free graphene corresponds to the low-energy approximation of the electron spectrum.

  3. Epitaxy of GaN Nanowires on Graphene.

    PubMed

    Kumaresan, Vishnuvarthan; Largeau, Ludovic; Madouri, Ali; Glas, Frank; Zhang, Hezhi; Oehler, Fabrice; Cavanna, Antonella; Babichev, Andrey; Travers, Laurent; Gogneau, Noelle; Tchernycheva, Maria; Harmand, Jean-Christophe

    2016-08-10

    Epitaxial growth of GaN nanowires on graphene is demonstrated using molecular beam epitaxy without any catalyst or intermediate layer. Growth is highly selective with respect to silica on which the graphene flakes, grown by chemical vapor deposition, are transferred. The nanowires grow vertically along their c-axis and we observe a unique epitaxial relationship with the ⟨21̅1̅0⟩ directions of the wurtzite GaN lattice parallel to the directions of the carbon zigzag chains. Remarkably, the nanowire density and height decrease with increasing number of graphene layers underneath. We attribute this effect to strain and we propose a model for the nanowire density variation. The GaN nanowires are defect-free and they present good optical properties. This demonstrates that graphene layers transferred on amorphous carrier substrates is a promising alternative to bulk crystalline substrates for the epitaxial growth of high quality GaN nanostructures.

  4. Epitaxy of GaN Nanowires on Graphene.

    PubMed

    Kumaresan, Vishnuvarthan; Largeau, Ludovic; Madouri, Ali; Glas, Frank; Zhang, Hezhi; Oehler, Fabrice; Cavanna, Antonella; Babichev, Andrey; Travers, Laurent; Gogneau, Noelle; Tchernycheva, Maria; Harmand, Jean-Christophe

    2016-08-10

    Epitaxial growth of GaN nanowires on graphene is demonstrated using molecular beam epitaxy without any catalyst or intermediate layer. Growth is highly selective with respect to silica on which the graphene flakes, grown by chemical vapor deposition, are transferred. The nanowires grow vertically along their c-axis and we observe a unique epitaxial relationship with the ⟨21̅1̅0⟩ directions of the wurtzite GaN lattice parallel to the directions of the carbon zigzag chains. Remarkably, the nanowire density and height decrease with increasing number of graphene layers underneath. We attribute this effect to strain and we propose a model for the nanowire density variation. The GaN nanowires are defect-free and they present good optical properties. This demonstrates that graphene layers transferred on amorphous carrier substrates is a promising alternative to bulk crystalline substrates for the epitaxial growth of high quality GaN nanostructures. PMID:27414518

  5. Electronic states in epitaxial graphene fabricated on silicon carbide

    SciTech Connect

    Davydov, S. Yu.

    2011-08-15

    An analytical expression for the density of states of a graphene monolayer interacting with a silicon carbide surface (epitaxial graphene) is derived. The density of states of silicon carbide is described within the Haldane-Anderson model. It is shown that the graphene-substrate interaction results in a narrow gap of {approx}0.01-0.06 eV in the density of states of graphene. The graphene atom charge is estimated; it is shown that the charge transfer from the substrate is {approx}10{sup -3}-10{sup -2}e per graphene atom.

  6. On the kinetic barriers of graphene homo-epitaxy

    SciTech Connect

    Zhang, Wei; Yu, Xinke; Xie, Ya-Hong; Cahyadi, Erica; Ratsch, Christian

    2014-12-01

    The diffusion processes and kinetic barriers of individual carbon adatoms and clusters on graphene surfaces are investigated to provide fundamental understanding of the physics governing epitaxial growth of multilayer graphene. It is found that individual carbon adatoms form bonds with the underlying graphene whereas the interaction between graphene and carbon clusters, consisting of 6 atoms or more, is very weak being van der Waals in nature. Therefore, small carbon clusters are quite mobile on the graphene surfaces and the diffusion barrier is negligibly small (∼6 meV). This suggests the feasibility of high-quality graphene epitaxial growth at very low growth temperatures with small carbon clusters (e.g., hexagons) as carbon source. We propose that the growth mode is totally different from 3-dimensional bulk materials with the surface mobility of carbon hexagons being the highest over graphene surfaces that gradually decreases with further increase in cluster size.

  7. Scanning Tunneling Spectroscopy of Proximity Superconductivity in Epitaxial Multilayer Graphene

    PubMed Central

    Natterer, Fabian D.; Ha, Jeonghoon; Baek, Hongwoo; Zhang, Duming; Cullen, William; Zhitenev, Nikolai B.; Kuk, Young; Stroscio, Joseph A.

    2016-01-01

    We report on spatial measurements of the superconducting proximity effect in epitaxial graphene induced by a graphene-superconductor interface. Superconducting aluminum films were grown on epitaxial multilayer graphene on SiC. The aluminum films were discontinuous with networks of trenches in the film morphology reaching down to exposed graphene terraces. Scanning tunneling spectra measured on the graphene terraces show a clear decay of the superconducting energy gap with increasing separation from the graphene-aluminum edges. The spectra were well described by Bardeen-Cooper-Schrieffer (BCS) theory. The decay length for the superconducting energy gap in graphene was determined to be greater than 400 nm. Deviations in the exponentially decaying energy gap were also observed on a much smaller length scale of tens of nanometers. PMID:27088134

  8. Growth of Epitaxial Oxide Thin Films on Graphene

    NASA Astrophysics Data System (ADS)

    Zou, Bin; Walker, Clementine; Wang, Kai; Tileli, Vasiliki; Shaforost, Olena; Harrison, Nicholas M.; Klein, Norbert; Alford, Neil M.; Petrov, Peter K.

    2016-08-01

    The transfer process of graphene onto the surface of oxide substrates is well known. However, for many devices, we require high quality oxide thin films on the surface of graphene. This step is not understood. It is not clear why the oxide should adopt the epitaxy of the underlying oxide layer when it is deposited on graphene where there is no lattice match. To date there has been no explanation or suggestion of mechanisms which clarify this step. Here we show a mechanism, supported by first principles simulation and structural characterisation results, for the growth of oxide thin films on graphene. We describe the growth of epitaxial SrTiO3 (STO) thin films on a graphene and show that local defects in the graphene layer (e.g. grain boundaries) act as bridge-pillar spots that enable the epitaxial growth of STO thin films on the surface of the graphene layer. This study, and in particular the suggestion of a mechanism for epitaxial growth of oxides on graphene, offers new directions to exploit the development of oxide/graphene multilayer structures and devices.

  9. Growth of Epitaxial Oxide Thin Films on Graphene

    PubMed Central

    Zou, Bin; Walker, Clementine; Wang, Kai; Tileli, Vasiliki; Shaforost, Olena; Harrison, Nicholas M.; Klein, Norbert; Alford, Neil M.; Petrov, Peter K.

    2016-01-01

    The transfer process of graphene onto the surface of oxide substrates is well known. However, for many devices, we require high quality oxide thin films on the surface of graphene. This step is not understood. It is not clear why the oxide should adopt the epitaxy of the underlying oxide layer when it is deposited on graphene where there is no lattice match. To date there has been no explanation or suggestion of mechanisms which clarify this step. Here we show a mechanism, supported by first principles simulation and structural characterisation results, for the growth of oxide thin films on graphene. We describe the growth of epitaxial SrTiO3 (STO) thin films on a graphene and show that local defects in the graphene layer (e.g. grain boundaries) act as bridge-pillar spots that enable the epitaxial growth of STO thin films on the surface of the graphene layer. This study, and in particular the suggestion of a mechanism for epitaxial growth of oxides on graphene, offers new directions to exploit the development of oxide/graphene multilayer structures and devices. PMID:27515496

  10. Growth of Epitaxial Oxide Thin Films on Graphene.

    PubMed

    Zou, Bin; Walker, Clementine; Wang, Kai; Tileli, Vasiliki; Shaforost, Olena; Harrison, Nicholas M; Klein, Norbert; Alford, Neil M; Petrov, Peter K

    2016-01-01

    The transfer process of graphene onto the surface of oxide substrates is well known. However, for many devices, we require high quality oxide thin films on the surface of graphene. This step is not understood. It is not clear why the oxide should adopt the epitaxy of the underlying oxide layer when it is deposited on graphene where there is no lattice match. To date there has been no explanation or suggestion of mechanisms which clarify this step. Here we show a mechanism, supported by first principles simulation and structural characterisation results, for the growth of oxide thin films on graphene. We describe the growth of epitaxial SrTiO3 (STO) thin films on a graphene and show that local defects in the graphene layer (e.g. grain boundaries) act as bridge-pillar spots that enable the epitaxial growth of STO thin films on the surface of the graphene layer. This study, and in particular the suggestion of a mechanism for epitaxial growth of oxides on graphene, offers new directions to exploit the development of oxide/graphene multilayer structures and devices. PMID:27515496

  11. The physics of epitaxial graphene on SiC(0001).

    PubMed

    Kageshima, H; Hibino, H; Tanabe, S

    2012-08-01

    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

  12. Localized States Influence Spin Transport in Epitaxial Graphene

    NASA Astrophysics Data System (ADS)

    Maassen, T.; van den Berg, J. J.; Huisman, E. H.; Dijkstra, H.; Fromm, F.; Seyller, T.; van Wees, B. J.

    2013-02-01

    We developed a spin transport model for a diffusive channel with coupled localized states that result in an effective increase of spin precession frequencies and a reduction of spin relaxation times in the system. We apply this model to Hanle spin precession measurements obtained on monolayer epitaxial graphene on SiC(0001). Combined with newly performed measurements on quasi-free-standing monolayer epitaxial graphene on SiC(0001) our analysis shows that the different values for the diffusion coefficient measured in charge and spin transport measurements on monolayer epitaxial graphene on SiC(0001) and the high values for the spin relaxation time can be explained by the influence of localized states arising from the buffer layer at the interface between the graphene and the SiC surface.

  13. Photoinduced topological phase transition in epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Zhai, Xuechao; Jin, Guojun

    2014-06-01

    In epitaxial graphene irradiated by an off-resonance circularly polarized light, we demonstrate a phase transition taking place between the band insulator and Floquet topological insulator. Considering the competition between staggered sublattice potential and photon dressing, we derive the dynamical energy gap and phase diagram in the tight-binding approximation. It is found that a threshold value of light intensity is necessary to realize a Floquet topological insulator. At the phase boundary, for each set of parameters, there is a special state with only one valley that is Dirac cone gapless, but the other remains gapped; in the band insulating phase, only one valley provides low-energy electrons, and it could be switched to the other by reversing the polarization direction of light. From these results, two electronic devices are designed: one is an optical-sensing np junction, where the photodriven unusual intervalley tunneling exhibits a stronger detectable signal than the intravalley tunneling, and the other is a topological field-effect transistor, where polarized light is used to turn on or turn off a nonequilibrium current.

  14. Raman spectra of epitaxial graphene on SiC and of epitaxial graphene transferred to SiO2.

    PubMed

    Lee, Dong Su; Riedl, Christian; Krauss, Benjamin; von Klitzing, Klaus; Starke, Ulrich; Smet, Jurgen H

    2008-12-01

    Raman spectra were measured for mono-, bi-, and trilayer graphene grown on SiC by solid state graphitization, whereby the number of layers was preassigned by angle-resolved ultraviolet photoemission spectroscopy. It was found that the only unambiguous fingerprint in Raman spectroscopy to identify the number of layers for graphene on SiC(0001) is the line width of the 2D (or D*) peak. The Raman spectra of epitaxial graphene show significant differences as compared to micromechanically cleaved graphene obtained from highly oriented pyrolytic graphite crystals. The G peak is found to be blue-shifted. The 2D peak does not exhibit any obvious shoulder structures, but it is much broader and almost resembles a single-peak even for multilayers. Flakes of epitaxial graphene were transferred from SiC onto SiO2 for further Raman studies. A comparison of the Raman data obtained for graphene on SiC with data for epitaxial graphene transferred to SiO2 reveals that the G peak blue-shift is clearly due to the SiC substrate. The broadened 2D peak however stems from the graphene structure itself and not from the substrate.

  15. Spin transport in epitaxial graphene on SiC (0001)

    NASA Astrophysics Data System (ADS)

    Du, Yuchen; Neal, Adam T.; Capano, Mike; Ye, Peide

    2013-03-01

    Graphene has been identified as a promising material for future spintronics devices due to its low spin orbit coupling and long spin diffusion lengths, even at room temperature. However, any device application requires the use of large-area graphene compatible with wafer-scale manufacturing methods, such as graphene grown epitaxially on SiC. We study spin transport in epitaxial graphene grown on SiC (0001) as a step toward future spintronics devices. A non-local spin valve signal of 200m Ω is observed at 77K, with a signal of 50m Ω resolved at 145K. Assuming a contact polarization of 10%, the measured signal corresponds to a spin diffusion length of 130nm at T =77K. Hanle effect spin precession measurements are ongoing.

  16. Argon-assisted growth of epitaxial graphene on Cu(111)

    NASA Astrophysics Data System (ADS)

    Robinson, Zachary R.; Tyagi, Parul; Mowll, Tyler R.; Ventrice, Carl A., Jr.; Hannon, James B.

    2012-12-01

    The growth of graphene by catalytic decomposition of ethylene on Cu(111) in an ultrahigh vacuum system was investigated with low-energy electron diffraction, low-energy electron microscopy, and atomic force microscopy. Attempts to form a graphene overlayer using ethylene at pressures as high as 10 mTorr and substrate temperatures as high as 900 ∘C resulted in almost no graphene growth. By using an argon overpressure, the growth of epitaxial graphene on Cu(111) was achieved. The suppression of graphene growth without the use of an argon overpressure is attributed to Cu sublimation at elevated temperatures. During the initial stages of growth, a random distribution of rounded graphene islands is observed. The predominant rotational orientation of the islands is within ±1∘ of the Cu(111) substrate lattice.

  17. Growth and Features of Epitaxial Graphene on SiC

    NASA Astrophysics Data System (ADS)

    Kusunoki, Michiko; Norimatsu, Wataru; Bao, Jianfeng; Morita, Koichi; Starke, Ulrich

    2015-12-01

    Recent progress of epitaxial graphene on SiC was reviewed, focusing on its growth and structural and electronic features. Homogeneous graphene can be grown on SiC(0001) on a wafer scale, however on SiC(000bar{1}) multilayer but rotationally stacked graphene with monolayer like electronic property grows. HRTEM revealed the formation mechanism and structural features of graphene on the both surfaces. The high structural and electronic quality of the grown graphene is monitored by Raman spectroscopy and magneto-transport characterization. High-resolution ARPES measurements of the electronic dispersion around the bar{K}-point retrieved the ABA and ABC stacked trilayer graphene. The measurements also directly revealed that electronic structures of graphene were manipulated by transfer doping and atomic intercalation. In particular, p- and n-doped regions on a meso-scale and the p-n junctions prepared on SiC via controlling intercalation of Ge exhibited ballistic transport and Klein tunneling, which predicted novel potentials on to epitaxial graphene on SiC.

  18. Extraordinary epitaxial alignment of graphene islands on Au(111)

    NASA Astrophysics Data System (ADS)

    Wofford, Joseph M.; Starodub, Elena; Walter, Andrew L.; Nie, Shu; Bostwick, Aaron; Bartelt, Norman C.; Thürmer, Konrad; Rotenberg, Eli; McCarty, Kevin F.; Dubon, Oscar D.

    2012-05-01

    Pristine, single-crystalline graphene displays a unique collection of remarkable electronic properties that arise from its two-dimensional, honeycomb structure. Using in situ low-energy electron microscopy, we show that when deposited on the (111) surface of Au carbon forms such a structure. The resulting monolayer, epitaxial film is formed by the coalescence of dendritic graphene islands that nucleate at a high density. Over 95% of these islands can be identically aligned with respect to each other and to the Au substrate. Remarkably, the dominant island orientation is not the better lattice-matched 30° rotated orientation but instead one in which the graphene [01] and Au [011] in-plane directions are parallel. The epitaxial graphene film is only weakly coupled to the Au surface, which maintains its reconstruction under the slightly p-type doped graphene. The linear electronic dispersion characteristic of free-standing graphene is retained regardless of orientation. That a weakly interacting, non-lattice matched substrate is able to lock graphene into a particular orientation is surprising. This ability, however, makes Au(111) a promising substrate for the growth of single crystalline graphene films.

  19. Charged nano-domes and bubbles in epitaxial graphene.

    PubMed

    Trabelsi, A Ben Gouider; Kusmartsev, F V; Robinson, B J; Ouerghi, A; Kusmartseva, O E; Kolosov, O V; Mazzocco, R; Gaifullin, Marat B; Oueslati, M

    2014-04-25

    For the first time, new epitaxial graphene nano-structures resembling charged 'bubbles' and 'domes' are reported. A strong influence, arising from the change in morphology, on the graphene layer's electronic, mechanical and optical properties has been shown. The morphological properties of these structures have been studied with atomic force microscopy (AFM), ultrasonic force microscopy (UFM) and Raman spectroscopy. After initial optical microscopy observation of the graphene, a detailed description of the surface morphology, via AFM and nanomechanical UFM measurements, was obtained. Here, graphene nano-structures, domes and bubbles, ranging from a few tens of nanometres (150–200 nm) to a few μm in size have been identified. The AFM topographical and UFM stiffness data implied the freestanding nature of the graphene layer within the domes and bubbles, with heights on the order of 5–12 nm. Raman spectroscopy mappings of G and 2D bands and their ratio confirm not only the graphene composition of these structures but also the existence of step bunching, defect variations and the carrier density distribution. In particular, inside the bubbles and substrate there arises complex charge redistribution; in fact, the graphene bubble–substrate interface forms a charged capacitance. We have determined the strength of the electric field inside the bubble–substrate interface, which may lead to a minigap of the order of 5 meV opening for epitaxial graphene grown on 4H-SiC face-terminated carbon.

  20. Substrate-induced magnetism in epitaxial graphene buffer layers.

    PubMed

    Ramasubramaniam, A; Medhekar, N V; Shenoy, V B

    2009-07-01

    Magnetism in graphene is of fundamental as well as technological interest, with potential applications in molecular magnets and spintronic devices. While defects and/or adsorbates in freestanding graphene nanoribbons and graphene sheets have been shown to cause itinerant magnetism, controlling the density and distribution of defects and adsorbates is in general difficult. We show from first principles calculations that graphene buffer layers on SiC(0001) can also show intrinsic magnetism. The formation of graphene-substrate chemical bonds disrupts the graphene pi-bonds and causes localization of graphene states near the Fermi level. Exchange interactions between these states lead to itinerant magnetism in the graphene buffer layer. We demonstrate the occurrence of magnetism in graphene buffer layers on both bulk-terminated as well as more realistic adatom-terminated SiC(0001) surfaces. Our calculations show that adatom density has a profound effect on the spin distribution in the graphene buffer layer, thereby providing a means of engineering magnetism in epitaxial graphene.

  1. Weak Localization in few layer Black Phosphorus

    NASA Astrophysics Data System (ADS)

    Gillgren, Nathaniel; Shi, Yanmeng; Espiritu, Timothy; Watanabe, Kenji; Taniguchi, Takahashi; Lau, Chun Ning (Jeanie)

    Few-layer black phosphorus has recently attracted interest from the scientific community due to its high mobility, tunable band gap, and large anisotropy. Recent experiments have demonstrated that black phosphorus provides a promising candidate to explore the physics of 2D semiconductors. In this study we explore the magnetotransport of few-layer black phosphorus-boron nitride hetereostructure devices at low magnetic fields. Weak localization is observed at low temperatures. We extract the dephasing length and measure its dependence on temperature, carrier density and electric field.

  2. The effect of adsorption on static conductivity of epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Davydov, S. Yu.

    2014-12-01

    An analytical expression for adsorption-induced changes in the static conductivity of the adlayer-single-sheet-graphene-substrate system has been obtained using the Kubo-Greenwood formalism with allowance for the dipole-dipole repulsion in the adlayer. The cases of both metal and semiconductor substrates have been considered. The results are applied to description of the hydrogen monolayer-single-sheet-graphene-tungsten substrate system. Numerical estimations show that the magnitude of the effect of the adsorbed hydrogen monolayer on the static conductivity σeg of epitaxial graphene on tungsten is on the order of the σeg value.

  3. Electron heat conductivity of epitaxial graphene on silicon carbide

    NASA Astrophysics Data System (ADS)

    Alisultanov, Z. Z.; Meilanov, R. P.

    2016-08-01

    The diagonal component of the electron heat conductivity tensor of epitaxial graphene formed in a semiconductor has been investigated within a simple analytical model. It is shown that the heat conductivity sharply changes at a chemical potential close to the substrate band gap edge. Low-temperature expressions for the heat conductivity are derived.

  4. Terahertz and mid-infrared reflectance of epitaxial graphene

    PubMed Central

    Santos, Cristiane N.; Joucken, Frédéric; De Sousa Meneses, Domingos; Echegut, Patrick; Campos-Delgado, Jessica; Louette, Pierre; Raskin, Jean-Pierre; Hackens, Benoit

    2016-01-01

    Graphene has emerged as a promising material for infrared (IR) photodetectors and plasmonics. In this context, wafer scale epitaxial graphene on SiC is of great interest in a variety of applications in optics and nanoelectronics. Here we present IR reflectance spectroscopy of graphene grown epitaxially on the C-face of 6H-SiC over a broad optical range, from terahertz (THz) to mid-infrared (MIR). Contrary to the transmittance, reflectance measurements are not hampered by the transmission window of the substrate, and in particular by the SiC Reststrahlen band in the MIR. This allows us to present IR reflectance data exhibiting a continuous evolution from the regime of intraband to interband charge carrier transitions. A consistent and simultaneous analysis of the contributions from both transitions to the optical response yields precise information on the carrier dynamics and the number of layers. The properties of the graphene layers derived from IR reflection spectroscopy are corroborated by other techniques (micro-Raman and X-ray photoelectron spectroscopies, transport measurements). Moreover, we also present MIR microscopy mapping, showing that spatially-resolved information can be gathered, giving indications on the sample homogeneity. Our work paves the way for a still scarcely explored field of epitaxial graphene-based THz and MIR optical devices. PMID:27102827

  5. Terahertz and mid-infrared reflectance of epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Santos, Cristiane N.; Joucken, Frédéric; de Sousa Meneses, Domingos; Echegut, Patrick; Campos-Delgado, Jessica; Louette, Pierre; Raskin, Jean-Pierre; Hackens, Benoit

    2016-04-01

    Graphene has emerged as a promising material for infrared (IR) photodetectors and plasmonics. In this context, wafer scale epitaxial graphene on SiC is of great interest in a variety of applications in optics and nanoelectronics. Here we present IR reflectance spectroscopy of graphene grown epitaxially on the C-face of 6H-SiC over a broad optical range, from terahertz (THz) to mid-infrared (MIR). Contrary to the transmittance, reflectance measurements are not hampered by the transmission window of the substrate, and in particular by the SiC Reststrahlen band in the MIR. This allows us to present IR reflectance data exhibiting a continuous evolution from the regime of intraband to interband charge carrier transitions. A consistent and simultaneous analysis of the contributions from both transitions to the optical response yields precise information on the carrier dynamics and the number of layers. The properties of the graphene layers derived from IR reflection spectroscopy are corroborated by other techniques (micro-Raman and X-ray photoelectron spectroscopies, transport measurements). Moreover, we also present MIR microscopy mapping, showing that spatially-resolved information can be gathered, giving indications on the sample homogeneity. Our work paves the way for a still scarcely explored field of epitaxial graphene-based THz and MIR optical devices.

  6. The invention of graphene electronics and the physics of epitaxial graphene on silicon carbide

    NASA Astrophysics Data System (ADS)

    de Heer, Walt A.

    2012-01-01

    Graphene electronics was officially invented at the Georgia Institute of Technology in 2003 after experimental and theoretical research on graphene properties starting from 2001. This paper focuses on the motivation and events leading to the invention of graphene electronics, as well as on recent developments. Graphene electronics was originally conceived as a new electronics paradigm to incorporate the room-temperature ballistic and coherent properties of carbon nanotubes in a patternable electronic material. Graphene on silicon carbide was chosen as the most suitable material. Other electronics schemes, involving transferred (exfoliated and chemical vapor deposition-produced) graphitic materials, that operate in the diffusive regime may not be competitive with standard methods and may therefore not significantly impact electronics. In recent years, epitaxial graphene has improved to the point where graphene electronics according to the original concept appears to be within reach. Beyond electronics, epitaxial graphene research has led to important developments in graphene physics in general and has become a leading platform for graphene science as well.

  7. Edge promoted ultrasensitive electrochemical detection of organic bio-molecules on epitaxial graphene nanowalls.

    PubMed

    Kumar Roy, Pradip; Ganguly, Abhijit; Yang, Wei-Hsun; Wu, Chien-Ting; Hwang, Jih-Shang; Tai, Yian; Chen, Kuei-Hsien; Chen, Li-Chyong; Chattopadhyay, Surojit

    2015-08-15

    We report the simultaneous electrochemical detection of dopamine (DA), uric acid (UA) and ascorbic acid (AA) on three dimensional (3D) unmodified 'as-grown' epitaxial graphene nanowall arrays (EGNWs). The 3D few layer EGNWs, unlike the 2D planar graphene, offers an abundance of vertically oriented nano-graphitic-edges that exhibit fast electron-transfer kinetics and high electroactive surface area to geometrical area (EAA/GA≈134%), as evident from the Fe(CN)6(3-/4-) redox kinetic study. The hexagonal sp(2)-C domains, on the basal plane of the EGNWs, facilitate efficient adsorption via spontaneous π-π interaction with the aromatic rings in DA and UA. Such affinity together with the fast electron kinetics enables simultaneous and unambiguous identification of individual AA, DA and UA from their mixture. The unique edge dominant EGNWs result in an unprecedented low limit of detection (experimental) of 0.033 nM and highest sensitivity of 476.2 µA/µM/cm(2), for UA, which are orders of magnitude higher than comparable existing reports. A reaction kinetics based modeling of the edge-oriented 3D EGNW system is proposed to illustrate the superior electro-activity for bio-sensing applications. PMID:25801954

  8. Edge promoted ultrasensitive electrochemical detection of organic bio-molecules on epitaxial graphene nanowalls.

    PubMed

    Kumar Roy, Pradip; Ganguly, Abhijit; Yang, Wei-Hsun; Wu, Chien-Ting; Hwang, Jih-Shang; Tai, Yian; Chen, Kuei-Hsien; Chen, Li-Chyong; Chattopadhyay, Surojit

    2015-08-15

    We report the simultaneous electrochemical detection of dopamine (DA), uric acid (UA) and ascorbic acid (AA) on three dimensional (3D) unmodified 'as-grown' epitaxial graphene nanowall arrays (EGNWs). The 3D few layer EGNWs, unlike the 2D planar graphene, offers an abundance of vertically oriented nano-graphitic-edges that exhibit fast electron-transfer kinetics and high electroactive surface area to geometrical area (EAA/GA≈134%), as evident from the Fe(CN)6(3-/4-) redox kinetic study. The hexagonal sp(2)-C domains, on the basal plane of the EGNWs, facilitate efficient adsorption via spontaneous π-π interaction with the aromatic rings in DA and UA. Such affinity together with the fast electron kinetics enables simultaneous and unambiguous identification of individual AA, DA and UA from their mixture. The unique edge dominant EGNWs result in an unprecedented low limit of detection (experimental) of 0.033 nM and highest sensitivity of 476.2 µA/µM/cm(2), for UA, which are orders of magnitude higher than comparable existing reports. A reaction kinetics based modeling of the edge-oriented 3D EGNW system is proposed to illustrate the superior electro-activity for bio-sensing applications.

  9. Imaging of Electron Beam Induced Current in Epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Mou, Shin; Boeckl, John; Lu, Weijie; Park, J. H.; Mitchel, W. C.; Tetlak, Stephen

    2012-02-01

    It has been observed that there forms a Schottky junction between graphene and SiC in epitaxial graphene due to the work function difference. As a result, it is viable to apply the electron beam induced current (EBIC) technique on epitaxial graphene due to the fact that it needs a built-in field and ample electron generation volume to generate EBIC. EBIC is an important characterization technique, which identifies electrically active impurities/defects, detects local built-in field, and measures minority carrier diffusion length. In this paper, we use a FEI SEM equipped with a current amplifier to investigate the spatial mapping of EBIC. The incident electron beam generates excited electron-hole pairs in SiC and the minority carriers are collected through the Schottky junction before flowing into graphene. EBIC imaging reveals mesoscopic domains of bright and dark contrast areas due to local EBIC polarity and magnitude, which is believed to be the result of spatial fluctuation in the carrier density in graphene. We also investigate the electron energy dependence, which modulates the EBIC magnitude. With an analytical drift-diffusion current model, we are able to extract the minority carrier diffusion length in the SiC, which is on the order of micro meter.

  10. Low contact resistance in epitaxial graphene devices for quantum metrology

    SciTech Connect

    Yager, Tom E-mail: ywpark@snu.ac.kr; Lartsev, Arseniy; Lara-Avila, Samuel; Kubatkin, Sergey; Cedergren, Karin; Yakimova, Rositsa; Panchal, Vishal; Kazakova, Olga; Tzalenchuk, Alexander; Kim, Kyung Ho; Park, Yung Woo E-mail: ywpark@snu.ac.kr

    2015-08-15

    We investigate Ti/Au contacts to monolayer epitaxial graphene on SiC (0001) for applications in quantum resistance metrology. Using three-terminal measurements in the quantum Hall regime we observed variations in contact resistances ranging from a minimal value of 0.6 Ω up to 11 kΩ. We identify a major source of high-resistance contacts to be due bilayer graphene interruptions to the quantum Hall current, whilst discarding the effects of interface cleanliness and contact geometry for our fabricated devices. Moreover, we experimentally demonstrate methods to improve the reproducibility of low resistance contacts (<10 Ω) suitable for high precision quantum resistance metrology.

  11. Highly p-doped epitaxial graphene obtained by fluorine intercalation

    NASA Astrophysics Data System (ADS)

    Walter, Andrew L.; Jeon, Ki-Joon; Bostwick, Aaron; Speck, Florian; Ostler, Markus; Seyller, Thomas; Moreschini, Luca; Kim, Yong Su; Chang, Young Jun; Horn, Karsten; Rotenberg, Eli

    2011-05-01

    We present a method for decoupling epitaxial graphene grown on SiC(0001) by intercalation of a layer of fluorine at the interface. The fluorine atoms do not enter into a covalent bond with graphene but rather saturate the substrate Si bonds. This configuration of the fluorine atoms induces a remarkably large hole density of p ≈4.5×1013 cm-2, equivalent to the location of the Fermi level at 0.79 eV above the Dirac point ED.

  12. Few-layer black phosphorus nanoparticles.

    PubMed

    Sofer, Zdenek; Bouša, Daniel; Luxa, Jan; Mazanek, Vlastimil; Pumera, Martin

    2016-01-28

    Herein, black phosphorus quantum dots and nanoparticles of a few layer thickness were prepared and characterized using STEM, AFM, dynamic light scattering, X-ray photoelectron spectroscopy, X-ray diffraction, Raman spectroscopy and photoluminescence. Impact electrochemistry of the induvidual black phosphorus nanoparticles allows their size determination. The centrifugation of colloidal black phosphorus nanoparticles allowed separation of quantum dots with sizes up to 15 nm. These black phosphorus nanoparticles exhibit a large band gap and are expected to find a wide range of applications from semiconductors to biomolecule tags. The use of black phosphorus nanoparticles for vapour sensing was successfully demonstrated.

  13. Multilayer epitaxial graphene grown on the SiC (000- 1) surface; structure and electronic properties

    SciTech Connect

    Sprinkle, M.; Hicks, J.; Tejeda, A.; Taleb-Ibrahimi, A.; Le Fevre, P.; Bertran, F.; Tinkey, H.; Clark, M.C.; Soukiassian, P.; Martinotti, D.; Hass, J.; Conrad, E.H.

    2010-10-22

    We review the progress towards developing epitaxial graphene as a material for carbon electronics. In particular, we discuss improvements in epitaxial graphene growth, interface control and the understanding of multilayer epitaxial graphene's (MEG's) electronic properties. Although graphene grown on both polar faces of SiC will be discussed, our discussions will focus on graphene grown on the (000{bar 1}) C-face of SiC. The unique properties of C-face MEG have become apparent. These films behave electronically like a stack of nearly independent graphene sheets rather than a thin Bernal stacked graphite sample. The origins of multilayer graphene's electronic behaviour are its unique highly ordered stacking of non-Bernal rotated graphene planes. While these rotations do not significantly affect the inter-layer interactions, they do break the stacking symmetry of graphite. It is this broken symmetry that leads to each sheet behaving like isolated graphene planes.

  14. Plasmarons in Quasi-freestanding Epitaxial Graphene

    NASA Astrophysics Data System (ADS)

    Bostwick, Aaron

    2011-03-01

    Graphene is a remarkable new electronic material with many unique properties. To realize its promise, it is essential to understand how its charge carriers interact. By measuring the spectral function of charge carriers in quasi-free-standing graphene, we show that at finite doping, the well-known linear Dirac spectrum does not provide a full description of the charge-carrying excitations. We find that there also exist composite ``plasmaron'' particles, consisting of holes coupled to density oscillatons of the graphene electron gas. The Dirac crossing point is resolved into three crossings: the first between pure charge bands, the second between pure plasmaron bands, and the third a ring-shaped crossing between charge and plasmaron bands.

  15. Epitaxial growth mechanisms of graphene and effects of substrates

    NASA Astrophysics Data System (ADS)

    Özçelik, V. Ongun; Cahangirov, S.; Ciraci, S.

    2012-06-01

    The growth process of single layer graphene with and without substrate is investigated using ab initio, finite temperature molecular dynamic calculations within density functional theory. An understanding of the epitaxial graphene growth mechanisms in the atomic level is provided by exploring the transient stages which occur at the growing edges of graphene. These stages are formation and collapse of large carbon rings together with the formation and healing of Stone-Wales like pentagon-heptagon defects. The activation barriers for the healing of these growth induced defects on various substrates are calculated using the climbing image nudge elastic band method and compared with that of the Stone-Wales defect. It is found that the healing of pentagon-heptagon defects occurring near the edge in the course of growth is much easier than that of Stone-Wales defect. The role of the substrate in the epitaxial growth and in the healing of defects are also investigated in detail, along with the effects of using carbon dimers as the building blocks of graphene growth.

  16. High mobility epitaxial graphene devices via aqueous-ozone processing

    NASA Astrophysics Data System (ADS)

    Yager, Tom; Webb, Matthew J.; Grennberg, Helena; Yakimova, Rositsa; Lara-Avila, Samuel; Kubatkin, Sergey

    2015-02-01

    We find that monolayer epitaxial graphene devices exposed to aggressive aqueous-ozone processing and annealing became cleaner from post-fabrication organic resist residuals and, significantly, maintain their high carrier mobility. Additionally, we observe a decrease in carrier density from inherent strong n-type doping to extremely low p-type doping after processing. This transition is explained to be a consequence of the cleaning effect of aqueous-ozone processing and annealing, since the observed removal of resist residuals from SiC/G enables the exposure of the bare graphene to dopants present in ambient conditions. The resulting combination of charge neutrality, high mobility, large area clean surfaces, and susceptibility to environmental species suggest this processed graphene system as an ideal candidate for gas sensing applications.

  17. Single-molecule junctions with epitaxial graphene nanoelectrodes.

    PubMed

    Ullmann, Konrad; Coto, Pedro B; Leitherer, Susanne; Molina-Ontoria, Agustín; Martín, Nazario; Thoss, Michael; Weber, Heiko B

    2015-05-13

    On the way to ultraflat single-molecule junctions with transparent electrodes, we present a fabrication scheme based on epitaxial graphene nanoelectrodes. As a suitable molecule, we identified a molecular wire with fullerene anchor groups. With these two components, stable electrical characteristics could be recorded. Electrical measurements show that single-molecule junctions with graphene and with gold electrodes display a striking agreement. This motivated a hypothesis that the differential conductance spectra are rather insensitive to the electrode material. It is further corroborated by the assignment of asymmetries and spectral features to internal molecular degrees of freedom. The demonstrated open-access graphene electrodes and the electrode-insensitive molecules provide a model system that will allow for a thorough investigation of an individual single-molecule contact with additional probes.

  18. Single-molecule junctions with epitaxial graphene nanoelectrodes.

    PubMed

    Ullmann, Konrad; Coto, Pedro B; Leitherer, Susanne; Molina-Ontoria, Agustín; Martín, Nazario; Thoss, Michael; Weber, Heiko B

    2015-05-13

    On the way to ultraflat single-molecule junctions with transparent electrodes, we present a fabrication scheme based on epitaxial graphene nanoelectrodes. As a suitable molecule, we identified a molecular wire with fullerene anchor groups. With these two components, stable electrical characteristics could be recorded. Electrical measurements show that single-molecule junctions with graphene and with gold electrodes display a striking agreement. This motivated a hypothesis that the differential conductance spectra are rather insensitive to the electrode material. It is further corroborated by the assignment of asymmetries and spectral features to internal molecular degrees of freedom. The demonstrated open-access graphene electrodes and the electrode-insensitive molecules provide a model system that will allow for a thorough investigation of an individual single-molecule contact with additional probes. PMID:25923590

  19. Controlled epitaxial graphene growth within removable amorphous carbon corrals

    SciTech Connect

    Palmer, James; Hu, Yike; Hankinson, John; Guo, Zelei; Heer, Walt A. de; Kunc, Jan; Berger, Claire

    2014-07-14

    We address the question of control of the silicon carbide (SiC) steps and terraces under epitaxial graphene on SiC and demonstrate amorphous carbon (aC) corrals as an ideal method to pin SiC surface steps. aC is compatible with graphene growth, structurally stable at high temperatures, and can be removed after graphene growth. For this, aC is first evaporated and patterned on SiC, then annealed in the graphene growth furnace. There at temperatures above 1200 °C, mobile SiC steps accumulate at the aC corral that provide effective step flow barriers. Aligned step free regions are thereby formed for subsequent graphene growth at temperatures above 1330 °C. Atomic force microscopy imaging supports the formation of step-free terraces on SiC with the step morphology aligned to the aC corrals. Raman spectroscopy indicates the presence of good graphene sheets on the step-free terraces.

  20. Extraordinary photoluminescence and strong temperature/angle-dependent Raman responses in few-layer phosphorene.

    PubMed

    Zhang, Shuang; Yang, Jiong; Xu, Renjing; Wang, Fan; Li, Weifeng; Ghufran, Muhammad; Zhang, Yong-Wei; Yu, Zongfu; Zhang, Gang; Qin, Qinghua; Lu, Yuerui

    2014-09-23

    Phosphorene is a new family member of two-dimensional materials. We observed strong and highly layer-dependent photoluminescence in few-layer phosphorene (two to five layers). The results confirmed the theoretical prediction that few-layer phosphorene has a direct and layer-sensitive band gap. We also demonstrated that few-layer phosphorene is more sensitive to temperature modulation than graphene and MoS2 in Raman scattering. The anisotropic Raman response in few-layer phosphorene has enabled us to use an optical method to quickly determine the crystalline orientation without tunneling electron microscopy or scanning tunneling microscopy. Our results provide much needed experimental information about the band structures and exciton nature in few-layer phosphorene.

  1. In-situ epitaxial growth of graphene/h-BN van der Waals heterostructures by molecular beam epitaxy.

    PubMed

    Zuo, Zheng; Xu, Zhongguang; Zheng, Renjing; Khanaki, Alireza; Zheng, Jian-Guo; Liu, Jianlin

    2015-01-01

    Van der Waals materials have received a great deal of attention for their exceptional layered structures and exotic properties, which can open up various device applications in nanoelectronics. However, in situ epitaxial growth of dissimilar van der Waals materials remains challenging. Here we demonstrate a solution for fabricating van der Waals heterostructures. Graphene/hexagonal boron nitride (h-BN) heterostructures were synthesized on cobalt substrates by using molecular beam epitaxy. Various characterizations were carried out to evaluate the heterostructures. Wafer-scale heterostructures consisting of single-layer/bilayer graphene and multilayer h-BN were achieved. The mismatch angle between graphene and h-BN is below 1°.

  2. Structure and transport of topological insulators on epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Kally, James; Reifsnyder Hickey, Danielle; Lin, Yu-Chuan; Richardella, Anthony; Lee, Joon Sue; Robinson, Joshua; Mkhoyan, K. Andre; Samarth, Nitin

    Recent advancements in spintronics have shown that a class of materials, topological insulators (TI), can be used as a spin-current generator or detector. Topological insulators have protected surface states with the electron's spin locked to its momentum. To access these surface states, (Bi, Sb)2Te3 can be grown by molecular beam epitaxy to have the Fermi energy near the Dirac point so that transport occurs only through the spin-dependent surface states. Graphene is another 2D material of great interest for spintronics because of its very long spin diffusion length. This is an ideal material to act as a spin channel in devices. The van der Waals nature of the growth exhibited by 2D materials such as (Bi, Sb)2Te3 and graphene allows heterostructures to be formed despite the large lattice mismatch. We explore the structure and transport of (Bi, Sb)2Te3 grown on epitaxial graphene on 6H-SiC substrates for spintronic applications. This work was supported in part by C-SPIN and LEAST, two of the six centers of STARnet, a Semiconductor Research Corporation program, sponsored by MARCO and DARPA.

  3. Principle of direct van der Waals epitaxy of single-crystalline films on epitaxial graphene.

    PubMed

    Kim, Jeehwan; Bayram, Can; Park, Hongsik; Cheng, Cheng-Wei; Dimitrakopoulos, Christos; Ott, John A; Reuter, Kathleen B; Bedell, Stephen W; Sadana, Devendra K

    2014-09-11

    There are numerous studies on the growth of planar films on sp(2)-bonded two-dimensional (2D) layered materials. However, it has been challenging to grow single-crystalline films on 2D materials due to the extremely low surface energy. Recently, buffer-assisted growth of crystalline films on 2D layered materials has been introduced, but the crystalline quality is not comparable with the films grown on sp(3)-bonded three-dimensional materials. Here we demonstrate direct van der Waals epitaxy of high-quality single-crystalline GaN films on epitaxial graphene with low defectivity and surface roughness comparable with that grown on conventional SiC or sapphire substrates. The GaN film is released and transferred onto arbitrary substrates. The post-released graphene/SiC substrate is reused for multiple growth and transfer cycles of GaN films. We demonstrate fully functional blue light-emitting diodes (LEDs) by growing LED stacks on reused graphene/SiC substrates followed by transfer onto plastic tapes.

  4. Principle of direct van der Waals epitaxy of single-crystalline films on epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Kim, Jeehwan; Bayram, Can; Park, Hongsik; Cheng, Cheng-Wei; Dimitrakopoulos, Christos; Ott, John A.; Reuter, Kathleen B.; Bedell, Stephen W.; Sadana, Devendra K.

    2014-09-01

    There are numerous studies on the growth of planar films on sp2-bonded two-dimensional (2D) layered materials. However, it has been challenging to grow single-crystalline films on 2D materials due to the extremely low surface energy. Recently, buffer-assisted growth of crystalline films on 2D layered materials has been introduced, but the crystalline quality is not comparable with the films grown on sp3-bonded three-dimensional materials. Here we demonstrate direct van der Waals epitaxy of high-quality single-crystalline GaN films on epitaxial graphene with low defectivity and surface roughness comparable with that grown on conventional SiC or sapphire substrates. The GaN film is released and transferred onto arbitrary substrates. The post-released graphene/SiC substrate is reused for multiple growth and transfer cycles of GaN films. We demonstrate fully functional blue light-emitting diodes (LEDs) by growing LED stacks on reused graphene/SiC substrates followed by transfer onto plastic tapes.

  5. Interlayer electronic hybridization leads to exceptional thickness-dependent vibrational properties in few-layer black phosphorus.

    PubMed

    Hu, Zhi-Xin; Kong, Xianghua; Qiao, Jingsi; Normand, Bruce; Ji, Wei

    2016-02-01

    Stacking two-dimensional (2D) materials into multi-layers or heterostructures, known as van der Waals (vdW) epitaxy, is an essential degree of freedom for tuning their properties on demand. Few-layer black phosphorus (FLBP), a material with high potential for nano- and optoelectronics applications, appears to have interlayer couplings much stronger than graphene and other 2D systems. Indeed, these couplings call into question whether the stacking of FLBP can be governed only by vdW interactions, which is of crucial importance for epitaxy and property refinement. Here, we perform a theoretical investigation of the vibrational properties of FLBP, which reflect directly its interlayer coupling, by discussing six Raman-observable phonons, including three optical, one breathing and two shear modes. With increasing sample thickness, we find anomalous redshifts of the frequencies for each optical mode but a blueshift for the armchair shear mode. Our calculations also show splitting of the phonon branches, due to anomalous surface phenomena, and strong phonon-phonon coupling. By computing uniaxial stress effects, inter-atomic force constants and electron densities, we provide a compelling demonstration that these properties are the consequence of strong and highly directional interlayer interactions arising from the electronic hybridization of the lone electron-pairs of FLBP, rather than from vdW interactions. This exceptional interlayer coupling mechanism controls the stacking stability of BP layers and thus opens a new avenue beyond vdW epitaxy for understanding the design of 2D heterostructures.

  6. Decoupling of epitaxial graphene via gold intercalation probed by dispersive Raman spectroscopy

    SciTech Connect

    Pillai, P. B. E-mail: m.desouza@sheffield.ac.uk; DeSouza, M. E-mail: m.desouza@sheffield.ac.uk; Narula, R.; Reich, S.; Wong, L. Y.; Batten, T.; Pokorny, J.

    2015-05-14

    Signatures of a superlattice structure composed of a quasi periodic arrangement of atomic gold clusters below an epitaxied graphene (EG) layer are examined using dispersive Raman spectroscopy. The gold-graphene system exhibits a laser excitation energy dependant red shift of the 2D mode as compared to pristine epitaxial graphene. The phonon dispersions in both the systems are mapped using the experimentally observed Raman signatures and a third-nearest neighbour tight binding electronic band structure model. Our results reveal that the observed excitation dependent Raman red shift in gold EG primarily arise from the modifications of the phonon dispersion in gold-graphene and shows that the extent of decoupling of graphene from the underlying SiC substrate can be monitored from the dispersive nature of the Raman 2D modes. The intercalated gold atoms restore the phonon band structure of epitaxial graphene towards free standing graphene.

  7. Thermoelectric imaging of structural disorder in epitaxial graphene.

    PubMed

    Cho, Sanghee; Kang, Stephen Dongmin; Kim, Wondong; Lee, Eui-Sup; Woo, Sung-Jae; Kong, Ki-Jeong; Kim, Ilyou; Kim, Hyeong-Do; Zhang, Tong; Stroscio, Joseph A; Kim, Yong-Hyun; Lyeo, Ho-Ki

    2013-10-01

    Heat is a familiar form of energy transported from a hot side to a colder side of an object, but not a notion associated with microscopic measurements of electronic properties. A temperature difference within a material causes charge carriers, electrons or holes to diffuse along the temperature gradient inducing a thermoelectric voltage. Here we show that local thermoelectric measurements can yield high-sensitivity imaging of structural disorder on the atomic and nanometre scales. The thermopower measurement acts to amplify the variations in the local density of states at the Fermi level, giving high differential contrast in thermoelectric signals. Using this imaging technique, we uncovered point defects in the first layer of epitaxial graphene, which generate soliton-like domain-wall line patterns separating regions of the different interlayer stacking of the second graphene layer.

  8. Epitaxial graphene quantum dots for high-performance terahertz bolometers

    NASA Astrophysics Data System (ADS)

    El Fatimy, Abdel; Myers-Ward, Rachael L.; Boyd, Anthony K.; Daniels, Kevin M.; Gaskill, D. Kurt; Barbara, Paola

    2016-04-01

    Light absorption in graphene causes a large change in electron temperature due to the low electronic heat capacity and weak electron-phonon coupling. This property makes graphene a very attractive material for hot-electron bolometers in the terahertz frequency range. Unfortunately, the weak variation of electrical resistance with temperature results in limited responsivity for absorbed power. Here, we show that, due to quantum confinement, quantum dots of epitaxial graphene on SiC exhibit an extraordinarily high variation of resistance with temperature (higher than 430 MΩ K-1 below 6 K), leading to responsivities of 1 × 1010 V W-1, a figure that is five orders of magnitude higher than other types of graphene hot-electron bolometer. The high responsivity, combined with an extremely low electrical noise-equivalent power (˜2 × 10-16 W Hz-1/2 at 2.5 K), already places our bolometers well above commercial cooled bolometers. Additionally, we show that these quantum dot bolometers demonstrate good performance at temperature as high as 77 K.

  9. Understanding controls on interfacial wetting at epitaxial graphene: Experiment and Theory

    SciTech Connect

    Zhou, Hua; Ganesh, Panchapakesan; Presser, Volker; Wander, Matthew C; Fenter, Paul; Kent, Paul R; Jiang, Deen; Chialvo, Ariel A; Mcdonough, John; Shuford, Kevin L; Gogotsi, Yury G.

    2012-01-01

    The interaction of interfacial water with graphitic carbon at the atomic scale is studied as a function of the hydrophobicity of epitaxial graphene. High resolution x-ray reflectivity shows that the graphene-water contact angle is controlled by the average graphene thickness, due to the fraction of the film surface expressed as the epitaxial buffer layer whose contact angle (contact angle c = 73 ) is substantially smaller than that of multilayer graphene ( c = 93 ). Classical and ab initio molecular dynamics simulations show that the reduced contact angle of the buffer layer is due to both its epitaxy with the SiC substrate and the presence of interfacial defects. This insight clarifies the relationship between interfacial water structure and hydrophobicity, in general, and suggests new routes to control interface properties of epitaxial graphene.

  10. Radio-Frequency Performance of Epitaxial Graphene Field-Effect Transistors on Sapphire Substrates

    NASA Astrophysics Data System (ADS)

    Liu, Qing-Bin; Yu, Cui; Li, Jia; Song, Xu-Bo; He, Ze-Zhao; Lu, Wei-Li; Gu, Guo-Dong; Wang, Yuan-Gang; Feng, Zhi-Hong

    2014-07-01

    We report dc and the first-ever measured small signal rf performance of epitaxial graphene field-effect transistors (GFETs), where the epitaxial graphene is grown by chemical vapor deposition (CVD) on a 2-inch c-plane sapphire substrate. Our epitaxial graphene material has a good flatness and uniformity due to the low carbon concentration during the graphene growth. With a gate length Lg = 100 nm, the maximum drain source current Ids and peak transconductance gm reach 0.92 A/mm and 0.143 S/mm, respectively, which are the highest results reported for GFETs directly grown on sapphire. The extrinsic cutoff frequency (fT) and maximum oscillation frequency (fmax) of the device are 12 GHz and 9.5 GHz, and up to 32 GHz and 21.5 GHz after de-embedding, respectively. Our work proves that epitaxial graphene on sapphire substrates is a promising candidate for rf electronics.

  11. Understanding controls on interfacial wetting at epitaxial graphene: Experiment and theory

    NASA Astrophysics Data System (ADS)

    Zhou, Hua; Ganesh, P.; Presser, Volker; Wander, Matthew C. F.; Fenter, Paul; Kent, Paul R. C.; Jiang, De-En; Chialvo, Ariel A.; McDonough, John; Shuford, Kevin L.; Gogotsi, Yury

    2012-01-01

    The interaction of interfacial water with graphitic carbon at the atomic scale is studied as a function of the hydrophobicity of epitaxial graphene. High resolution x-ray reflectivity shows that the graphene-water contact angle is controlled by the average graphene thickness, due to the fraction of the film surface expressed as the epitaxial buffer layer whose contact angle (contact angle θc = 73°) is substantially smaller than that of multilayer graphene (θc = 93°). Classical and ab initio molecular dynamics simulations show that the reduced contact angle of the buffer layer is due to both its epitaxy with the SiC substrate and the presence of interfacial defects. This insight clarifies the relationship between interfacial water structure and hydrophobicity, in general, and suggests new routes to control interface properties of epitaxial graphene.

  12. Understanding controls on interfacial wetting at epitaxial graphene: Experiment and Theory

    SciTech Connect

    Kent, Paul R

    2011-01-01

    The interaction of interfacial water with graphitic carbon at the atomic scale is studied as a function of the hydrophobicity of epitaxial graphene. High resolution x-ray reflectivity shows that the graphene-water contact angle is controlled by the average graphene thickness, due to the fraction of the film surface expressed as the epitaxial buffer layer whose contact angle (contact angle {Theta}{sub c} = 73{sup o}) is substantially smaller than that of multilayer graphene ({Theta}{sub c} = 93{sup o}). Classical and ab initio molecular dynamics simulations show that the reduced contact angle of the buffer layer is due to both its epitaxy with the SiC substrate and the presence of interfacial defects. This insight clarifies the relationship between interfacial water structure and hydrophobicity, in general, and suggests new routes to control interface properties of epitaxial graphene.

  13. Density functional theory modeling of multilayer "epitaxial" graphene oxide.

    PubMed

    Zhou, Si; Bongiorno, Angelo

    2014-11-18

    CONSPECTUS: Graphene oxide (GO) is a complex material of both fundamental and applied interest. Elucidating the structure of GO is crucial to achieve control over its properties and technological applications. GO is a nonstoichiometric and hygroscopic material with a lamellar structure, and its physical chemical properties depend critically on synthesis procedures and postsynthesis treatments. Numerous efforts are in place to both understand and exploit this versatile layered carbon material. This Account reports on recent density functional theory (DFT) studies of "epitaxial" graphene oxide (hereafter EGO), a type of GO obtained by oxidation of graphene films grown epitaxially on silicon carbide. Here, we rely on selected X-ray photoelectron spectroscopy (XPS), infrared spectroscopy (IR), and X-ray diffraction (XRD) measurements of EGO, and we discuss in great detail how we utilized DFT-based techniques to project out from the experimental data basic atomistic information about the chemistry and structure of these films. This Account provides an example as to how DFT modeling can be used to elucidate complex materials such as GO from a limited set of experimental information. EGO exhibits a uniform layered structure, consisting of a stack of graphene planes hosting predominantly epoxide and hydroxyl groups, and water molecules intercalated between the oxidized carbon layers. Here, we first focus on XPS measurements of EGO, and we use DFT to generate realistic model structures, calculate core-level chemical shifts, and through the comparison with experiment, gain insight on the chemical composition and metastability characteristics of EGO. DFT calculations are then used to devise a simplistic but accurate simulation scheme to study thermodynamic and kinetic stability and to predict the intralayer structure of EGO films aged at room temperature. Our simulations show that aged EGO encompasses layers with nanosized oxidized domains presenting a high concentration of

  14. Real-time observation of epitaxial graphene domain reorientation

    SciTech Connect

    Thuermer, Konrad; Foster, Michael E.; Bartelt, Norman Charles; Rogge, Paul C.; McCarty, Kevin F.; Dubon, Oscar D.; Bartelt, Norman C.

    2015-04-20

    Graphene films grown by vapour deposition tend to be polycrystalline due to the nucleation and growth of islands with different in-plane orientations. Here, using low-energy electron microscopy, we find that micron-sized graphene islands on Ir(111) rotate to a preferred orientation during thermal annealing. We observe three alignment mechanisms: the simultaneous growth of aligned domains and dissolution of rotated domains, that is, ‘ripening’; domain boundary motion within islands; and continuous lattice rotation of entire domains. By measuring the relative growth velocity of domains during ripening, we estimate that the driving force for alignment is on the order of 0.1 meV per C atom and increases with rotation angle. A simple model of the orientation-dependent energy associated with the moiré corrugation of the graphene sheet due to local variations in the graphene–substrate interaction reproduces the results. This study suggests new strategies for improving the van der Waals epitaxy of 2D materials.

  15. Real-time observation of epitaxial graphene domain reorientation

    DOE PAGESBeta

    Thuermer, Konrad; Foster, Michael E.; Bartelt, Norman Charles; Rogge, Paul C.; Lawrence Berkeley National Lab.; McCarty, Kevin F.; Dubon, Oscar D.; Lawrence Berkeley National Lab.; Bartelt, Norman C.

    2015-04-20

    Graphene films grown by vapour deposition tend to be polycrystalline due to the nucleation and growth of islands with different in-plane orientations. Here, using low-energy electron microscopy, we find that micron-sized graphene islands on Ir(111) rotate to a preferred orientation during thermal annealing. We observe three alignment mechanisms: the simultaneous growth of aligned domains and dissolution of rotated domains, that is, ‘ripening’; domain boundary motion within islands; and continuous lattice rotation of entire domains. By measuring the relative growth velocity of domains during ripening, we estimate that the driving force for alignment is on the order of 0.1 meV permore » C atom and increases with rotation angle. A simple model of the orientation-dependent energy associated with the moiré corrugation of the graphene sheet due to local variations in the graphene–substrate interaction reproduces the results. This study suggests new strategies for improving the van der Waals epitaxy of 2D materials.« less

  16. Understanding controls on interfacial wetting at epitaxial graphene: Experiment and Theory

    SciTech Connect

    Zhou, Hua; Ganesh, Panchapakesan; Presser, Volker; Wander, Matthew C; Fenter, Paul; Kent, Paul R; Jiang, Deen; Chialvo, Ariel A; Mcdonough, John; Shuford, Kevin L; Gogotsi, Yury G.

    2012-01-01

    The interaction of water with graphitic carbon at the atomic scale is studied as a function of the hydrophobicity of epitaxial graphene. High resolution X-ray reflectivity combined with both classical and ab initio molecular dynamics simulations allows us to understand how the graphene-water interface changes as the hydrophobicity of intrinsic multilayer graphene (contact angle c = 93 ) is reduced by the presence of substrate and surface defect sites, leading to increased hydrophilicity ( c = 73 ) for zero-layer graphene (i.e., the epitaxial buffer layer). The relationship between water depletion and hydrophobicity (i.e., the hydrophobic gap) is also clarified by the current findings.

  17. Suppression of inhomogeneous segregation in graphene growth on epitaxial metal films.

    PubMed

    Yoshii, Shigeo; Nozawa, Katsuya; Toyoda, Kenji; Matsukawa, Nozomu; Odagawa, Akihiro; Tsujimura, Ayumu

    2011-07-13

    Large-scale uniform graphene growth was achieved by suppressing inhomogeneous carbon segregation using a single domain Ru film epitaxially grown on a sapphire substrate. An investigation of how the metal thickness affected growth and a comparative study on metals with different crystal structures have revealed that locally enhanced carbon segregation at stacking domain boundaries of metal is the origin of inhomogeneous graphene growth. Single domain Ru film has no stacking domain boundary, and the graphene growth on it is mainly caused not by segregation but by a surface catalytic reaction. Suppression of local segregation is essential for uniform graphene growth on epitaxial metal films. PMID:21648391

  18. Epitaxial graphene on silicon carbide: Low-vacuum growth, characterization, and device fabrication

    NASA Astrophysics Data System (ADS)

    Sprinkle, Michael W.

    In the past several years, epitaxial graphene on silicon carbide has been transformed from an academic curiosity of social scientists to a leading candidate material to replace silicon in post-CMOS electronics. This has come with rapid development of growth technologies, improved understanding of epitaxial graphene on the polar faces of silicon carbide, and new device fabrication techniques. The contributions of this thesis include refinement and improved understanding of graphene growth on the silicon- and carbon-faces in the context of managed local silicon partial pressure, high-throughput epitaxial graphene thickness measurement and uniformity characterization by ellipsometry, observations of nearly ideal graphene band structures on rotationally stacked carbon-face multilayer epitaxial graphene, presentation of initial experiments on localized in situ chemical modification of epitaxial graphene for an alternate path to semiconducting behavior, and novel device fabrication methods to exploit the crystal structure of the silicon carbide substrate. The latter is a particularly exciting foray into three dimensional patterning of the substrate that may eliminate the critical problem of edge roughness in graphene nanoribbons.

  19. Direct growth of graphene on in situ epitaxial hexagonal boron nitride flakes by plasma-assisted molecular beam epitaxy

    SciTech Connect

    Xu, Zhongguang; Zheng, Renjing; Khanaki, Alireza; Zuo, Zheng; Liu, Jianlin

    2015-11-23

    Hexagonal boron nitride (h-BN) single-crystal domains were grown on cobalt (Co) substrates at a substrate temperature of 850–900 °C using plasma-assisted molecular beam epitaxy. Three-point star shape h-BN domains were observed by scanning electron microscopy, and confirmed by Raman and X-ray photoelectron spectroscopy. The h-BN on Co template was used for in situ growth of multilayer graphene, leading to an h-BN/graphene heterostructure. Carbon atoms preferentially nucleate on Co substrate and edges of h-BN and then grow laterally to form continuous graphene. Further introduction of carbon atoms results in layer-by-layer growth of graphene on graphene and lateral growth of graphene on h-BN until it may cover entire h-BN flakes.

  20. Van der Waals epitaxial double heterostructure: InAs/single-layer graphene/InAs.

    PubMed

    Hong, Young Joon; Yang, Jae Won; Lee, Wi Hyoung; Ruoff, Rodney S; Kim, Kwang S; Fukui, Takashi

    2013-12-17

    Van der Waals (vdW) epitaxial double heterostructures have been fabricated by vdW epitaxy of InAs nanostructures on both sides of graphene. InAs nanostructures diametrically form on/underneath graphene exclusively along As-polar direction, indicating polarity inversion of the double heterostructures. First-principles and density functional calculations demonstrate how and why InAs easily form to be double heterostructures with polarity inversion.

  1. Thermal Conductance of Epitaxial and Transferred CVD-Grown Graphene

    NASA Astrophysics Data System (ADS)

    Bin, Huang; Yee Kan, Koh

    2015-03-01

    The knowledge of how heat is carried across graphene-copper interface is crucial for the development of graphene devices with hybrid graphene-copper interconnects. Time-domain thermoreflectance (TDTR) is used to measure the interfacial thermal conductance of epitaxial grown single layer graphene (SLG) on copper foil and after it is transferred to a deposited copper substrate. It is found out that the thermal conductance of un-annealed transferred SLG on deposited copper is around 20 MW/m2K, much lower than that of SLG grown on copper foil which is approximately 30 MW/m2K. Annealing in forming gas/vacuum causes the thermal conductance of transferred SLG to increase to 31 MW/m2K. X-ray spectroscopy (XPS) and Atomic force microscopy (AFM) are then employed to investigate the various factors, (i.e., copper oxide, polycarbonate (PC) residue, roughness and conformity) that may cause a difference in thermal conductance after the transfer. XPS measurement results show an absence of PC residue, even before annealing. The results also reveal that annealing in forming gas reduces the copper oxide thickness by about 2.5nm, and such a small reduction in oxide thickness is not sufficient to cause a drastic increase of approximately 10MW/m2K in thermal conductance. AFM results show that before annealing, the SLG has elongated ridges-like morphology. This morphology is different from that of copper which has circular-like features. After annealing, the SLG morphology becomes very similar to that of copper - both exhibiting circular-like features. This shows that the SLG can conform better to the copper surface after annealing.

  2. Electronic cooling via interlayer Coulomb coupling in multilayer epitaxial graphene

    PubMed Central

    Mihnev, Momchil T.; Tolsma, John R.; Divin, Charles J.; Sun, Dong; Asgari, Reza; Polini, Marco; Berger, Claire; de Heer, Walt A.; MacDonald, Allan H.; Norris, Theodore B.

    2015-01-01

    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. We demonstrate here, however, that Coulomb interactions between electrons in different layers of multilayer epitaxial graphene provide an important mechanism for interlayer thermal transport, even though all electronic states are strongly confined within individual 2D layers. This effect is manifested in the relaxation dynamics of hot carriers in ultrafast time-resolved terahertz spectroscopy. We develop a theory of interlayer Coulomb coupling containing no free parameters that accounts for the experimentally observed trends in hot-carrier dynamics as temperature and the number of layers is varied. PMID:26399955

  3. Mini array of quantum Hall devices based on epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Novikov, S.; Lebedeva, N.; Hämäläinen, J.; Iisakka, I.; Immonen, P.; Manninen, A. J.; Satrapinski, A.

    2016-05-01

    Series connection of four quantum Hall effect (QHE) devices based on epitaxial graphene films was studied for realization of a quantum resistance standard with an up-scaled value. The tested devices showed quantum Hall plateaux RH,2 at a filling factor v = 2 starting from a relatively low magnetic field (between 4 T and 5 T) when the temperature was 1.5 K. The precision measurements of quantized Hall resistance of four QHE devices connected by triple series connections and external bonding wires were done at B = 7 T and T = 1.5 K using a commercial precision resistance bridge with 50 μA current through the QHE device. The results showed that the deviation of the quantized Hall resistance of the series connection of four graphene-based QHE devices from the expected value of 4×RH,2 = 2 h/e2 was smaller than the relative standard uncertainty of the measurement (<1 × 10-7) limited by the used resistance bridge.

  4. Polarized micro Raman scattering spectroscopy for curved edges of epitaxial graphene

    SciTech Connect

    Islam, Md. Sherajul Makino, T.; Hashimoto, A.; Bhuiyan, A. G.; Tanaka, S.

    2014-12-15

    This letter performed polarized microscopic laser Raman scattering spectroscopy on the curved edges of transferred epitaxial graphene on SiO{sub 2}/Si. The intensity ratio between the parallel and perpendicular polarized D band is evolved, providing a spectroscopy-based technique to probe the atomic-scale edge structures in graphene. A detailed analysis procedure for non-ideal disordered curved edges of graphene is developed combining the atomic-scale zigzag and armchair edge structures along with some point defects. These results could provide valuable information of the realistic edges of graphene at the atomic-scale that can strongly influence the performance of graphene-based nanodevices.

  5. Transfer-free electrical insulation of epitaxial graphene from its metal substrate.

    PubMed

    Lizzit, Silvano; Larciprete, Rosanna; Lacovig, Paolo; Dalmiglio, Matteo; Orlando, Fabrizio; Baraldi, Alessandro; Gammelgaard, Lauge; Barreto, Lucas; Bianchi, Marco; Perkins, Edward; Hofmann, Philip

    2012-09-12

    High-quality, large-area epitaxial graphene can be grown on metal surfaces, but its transport properties cannot be exploited because the electrical conduction is dominated by the substrate. Here we insulate epitaxial graphene on Ru(0001) by a stepwise intercalation of silicon and oxygen, and the eventual formation of a SiO(2) layer between the graphene and the metal. We follow the reaction steps by X-ray photoemission spectroscopy and demonstrate the electrical insulation using a nanoscale multipoint probe technique.

  6. Transfer-Free Electrical Insulation of Epitaxial Graphene from its Metal Substrate

    NASA Astrophysics Data System (ADS)

    Lizzit, Silvano; Larciprete, Rosanna; Lacovig, Paolo; Dalmiglio, Matteo; Orlando, Fabrizio; Baraldi, Alessandro; Gammelgaard, Lauge; Barreto, Lucas; Bianchi, Marco; Perkins, Edward; Hofmann, Philip

    2012-09-01

    High-quality, large-area epitaxial graphene can be grown on metal surfaces but its transport properties cannot be exploited because the electrical conduction is dominated by the substrate. Here we insulate epitaxial graphene on Ru(0001) by a step-wise intercalation of silicon and oxygen, and the eventual formation of a SiO$_2$ layer between the graphene and the metal. We follow the reaction steps by x-ray photoemission spectroscopy and demonstrate the electrical insulation using a nano-scale multipoint probe technique.

  7. Giant quantum Hall plateaus generated by charge transfer in epitaxial graphene.

    PubMed

    Alexander-Webber, J A; Huang, J; Maude, D K; Janssen, T J B M; Tzalenchuk, A; Antonov, V; Yager, T; Lara-Avila, S; Kubatkin, S; Yakimova, R; Nicholas, R J

    2016-01-01

    Epitaxial graphene has proven itself to be the best candidate for quantum electrical resistance standards due to its wide quantum Hall plateaus with exceptionally high breakdown currents. However one key underlying mechanism, a magnetic field dependent charge transfer process, is yet to be fully understood. Here we report measurements of the quantum Hall effect in epitaxial graphene showing the widest quantum Hall plateau observed to date extending over 50 T, attributed to an almost linear increase in carrier density with magnetic field. This behaviour is strong evidence for field dependent charge transfer from charge reservoirs with exceptionally high densities of states in close proximity to the graphene. Using a realistic framework of broadened Landau levels we model the densities of donor states and predict the field dependence of charge transfer in excellent agreement with experimental results, thus providing a guide towards engineering epitaxial graphene for applications such as quantum metrology.

  8. Giant quantum Hall plateaus generated by charge transfer in epitaxial graphene.

    PubMed

    Alexander-Webber, J A; Huang, J; Maude, D K; Janssen, T J B M; Tzalenchuk, A; Antonov, V; Yager, T; Lara-Avila, S; Kubatkin, S; Yakimova, R; Nicholas, R J

    2016-01-01

    Epitaxial graphene has proven itself to be the best candidate for quantum electrical resistance standards due to its wide quantum Hall plateaus with exceptionally high breakdown currents. However one key underlying mechanism, a magnetic field dependent charge transfer process, is yet to be fully understood. Here we report measurements of the quantum Hall effect in epitaxial graphene showing the widest quantum Hall plateau observed to date extending over 50 T, attributed to an almost linear increase in carrier density with magnetic field. This behaviour is strong evidence for field dependent charge transfer from charge reservoirs with exceptionally high densities of states in close proximity to the graphene. Using a realistic framework of broadened Landau levels we model the densities of donor states and predict the field dependence of charge transfer in excellent agreement with experimental results, thus providing a guide towards engineering epitaxial graphene for applications such as quantum metrology. PMID:27456765

  9. Giant quantum Hall plateaus generated by charge transfer in epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Alexander-Webber, J. A.; Huang, J.; Maude, D. K.; Janssen, T. J. B. M.; Tzalenchuk, A.; Antonov, V.; Yager, T.; Lara-Avila, S.; Kubatkin, S.; Yakimova, R.; Nicholas, R. J.

    2016-07-01

    Epitaxial graphene has proven itself to be the best candidate for quantum electrical resistance standards due to its wide quantum Hall plateaus with exceptionally high breakdown currents. However one key underlying mechanism, a magnetic field dependent charge transfer process, is yet to be fully understood. Here we report measurements of the quantum Hall effect in epitaxial graphene showing the widest quantum Hall plateau observed to date extending over 50 T, attributed to an almost linear increase in carrier density with magnetic field. This behaviour is strong evidence for field dependent charge transfer from charge reservoirs with exceptionally high densities of states in close proximity to the graphene. Using a realistic framework of broadened Landau levels we model the densities of donor states and predict the field dependence of charge transfer in excellent agreement with experimental results, thus providing a guide towards engineering epitaxial graphene for applications such as quantum metrology.

  10. Interlayer electronic hybridization leads to exceptional thickness-dependent vibrational properties in few-layer black phosphorus

    NASA Astrophysics Data System (ADS)

    Hu, Zhi-Xin; Kong, Xianghua; Qiao, Jingsi; Normand, Bruce; Ji, Wei

    2016-01-01

    Stacking two-dimensional (2D) materials into multi-layers or heterostructures, known as van der Waals (vdW) epitaxy, is an essential degree of freedom for tuning their properties on demand. Few-layer black phosphorus (FLBP), a material with high potential for nano- and optoelectronics applications, appears to have interlayer couplings much stronger than graphene and other 2D systems. Indeed, these couplings call into question whether the stacking of FLBP can be governed only by vdW interactions, which is of crucial importance for epitaxy and property refinement. Here, we perform a theoretical investigation of the vibrational properties of FLBP, which reflect directly its interlayer coupling, by discussing six Raman-observable phonons, including three optical, one breathing and two shear modes. With increasing sample thickness, we find anomalous redshifts of the frequencies for each optical mode but a blueshift for the armchair shear mode. Our calculations also show splitting of the phonon branches, due to anomalous surface phenomena, and strong phonon-phonon coupling. By computing uniaxial stress effects, inter-atomic force constants and electron densities, we provide a compelling demonstration that these properties are the consequence of strong and highly directional interlayer interactions arising from the electronic hybridization of the lone electron-pairs of FLBP, rather than from vdW interactions. This exceptional interlayer coupling mechanism controls the stacking stability of BP layers and thus opens a new avenue beyond vdW epitaxy for understanding the design of 2D heterostructures.Stacking two-dimensional (2D) materials into multi-layers or heterostructures, known as van der Waals (vdW) epitaxy, is an essential degree of freedom for tuning their properties on demand. Few-layer black phosphorus (FLBP), a material with high potential for nano- and optoelectronics applications, appears to have interlayer couplings much stronger than graphene and other 2D

  11. Selective Epitaxial Graphene Growth on SiC via AlN Capping

    NASA Astrophysics Data System (ADS)

    Zaman, Farhana; Rubio-Roy, Miguel; Moseley, Michael; Lowder, Jonathan; Doolittle, William; Berger, Claire; Dong, Rui; Meindl, James; de Heer, Walt; Georgia Institute of Technology Team

    2011-03-01

    Electronic-quality graphene is epitaxially grown by graphitization of carbon-face silicon carbide (SiC) by the sublimation of silicon atoms from selected regions uncapped by aluminum nitride (AlN). AlN (deposited by molecular beam epitaxy) withstands high graphitization temperatures of 1420o C, hence acting as an effective capping layer preventing the growth of graphene under it. The AlN is patterned and etched to open up windows onto the SiC surface for subsequent graphitization. Such selective epitaxial growth leads to the formation of high-quality graphene in desired patterns without the need for etching and lithographic patterning of graphene itself. No detrimental contact of the graphene with external chemicals occurs throughout the fabrication-process. The impact of process-conditions on the mobility of graphene is investigated. Graphene hall-bars were fabricated and characterized by scanning Raman spectroscopy, ellipsometry, and transport measurements. This controlled growth of graphene in selected regions represents a viable approach to fabrication of high-mobility graphene as the channel material for fast-switching field-effect transistors.

  12. Microfiber-based few-layer black phosphorus saturable absorber for ultra-fast fiber laser.

    PubMed

    Luo, Zhi-Chao; Liu, Meng; Guo, Zhi-Nan; Jiang, Xiao-Fang; Luo, Ai-Ping; Zhao, Chu-Jun; Yu, Xue-Feng; Xu, Wen-Cheng; Zhang, Han

    2015-07-27

    Few-layer black phosphorus (BP), as the most alluring graphene analogue owing to its similar structure as graphene and thickness dependent direct band-gap, has now triggered a new wave of research on two-dimensional (2D) materials based photonics and optoelectronics. However, a major obstacle of practical applications for few-layer BPs comes from their instabilities of laser-induced optical damage. Herein, we demonstrate that, few-layer BPs, which was fabricated through the liquid exfoliation approach, can be developed as a new and practical saturable absorber (SA) by depositing few-layer BPs with microfiber. The saturable absorption property of few-layer BPs had been verified through an open-aperture z-scan measurement at the telecommunication band. The microfiber-based BP device had been found to show a saturable average power of ~4.5 mW and a modulation depth of 10.9%, which is further confirmed through a balanced twin detection measurement. By integrating this optical SA device into an erbium-doped fiber laser, it was found that it can deliver the mode-locked pulse with duration down to 940 fs with central wavelength tunable from 1532 nm to 1570 nm. The prevention of BP from oxidation through the "lateral interaction scheme" owing to this microfiber-based few-layer BP SA device might partially mitigate the optical damage problem of BP. Our results not only demonstrate that black phosphorus might be another promising SA material for ultrafast photonics, but also provide a practical solution to solve the optical damage problem of black phosphorus by assembling with waveguide structures such as microfiber.

  13. Microfiber-based few-layer black phosphorus saturable absorber for ultra-fast fiber laser

    NASA Astrophysics Data System (ADS)

    Luo, Zhi-Chao; Liu, Meng; Guo, Zhi-Nan; Jiang, Xiao-Fang; Luo, Ai-Ping; Zhao, Chu-Jun; Yu, Xue-Feng; Xu, Wen-Cheng; Zhang, Han

    2015-07-01

    Few-layer black phosphorus (BP), as the most alluring graphene analogue owing to its similar structure as graphene and thickness dependent direct band-gap, has now triggered a new wave of research on two-dimensional (2D) materials based photonics and optoelectronics. However, a major obstacle of practical applications for few-layer BPs comes from their instabilities of laser-induced optical damage. Herein, we demonstrate that, few-layer BPs, fabricated through the liquid exfoliation approach, can be developed as a new and practical saturable absorber (SA) by depositing few-layer BPs with microfiber. The saturable absorption property of few-layer BPs had been verified through an open-aperture z-scan measurement at the telecommunication band and the microfiber-based BP device had been found to show a saturable average power of ~4.5 mW and a modulation depth of 10.9%, which is further confirmed through a balanced twin detection measurement. By further integrating this optical SA device into an erbium-doped fiber laser, it was found that it can deliver the mode-locked pulse with duration down to 940 fs with central wavelength tunable from 1532 nm to 1570 nm. The prevention of BP from oxidation through the 'lateral interaction scheme' owing to this microfiber-based few-layer BP SA device might partially mitigate the optical damage problem of BP. Our results not only demonstrate that black phosphorus might be another promising SA material for ultrafast photonics, but also provide a practical solution to solve the optical damage problem of black phosphorus by assembling with waveguide structures such as microfiber.

  14. Characterization of selective epitaxial graphene growth on silicon carbide: Limitations and opportunities

    NASA Astrophysics Data System (ADS)

    Zaman, Farhana

    The need for post-CMOS nanoelectronics has led to the investigation of innovative device structures and materials. Graphene, a zero bandgap semiconductor with ballistic transport properties, has great potential to extend diversification and miniaturization beyond the limits of CMOS. The goal of this work is to study the growth of graphene on SiC using the novel method of selective graphitization. The major contributions of this research are as follows — First, epitaxial graphene is successfully grown on selected regions of SiC not capped by AlN deposited by molecular beam epitaxy. This contribution enables the formation of electronic-grade graphene in desired patterns without having to etch the graphene or expose it to any detrimental contact with external chemicals. Etching of AlN opens up windows to the SiC in desirable patterns for subsequent graphitization without leaving etch-residues (determined by XPS). Second, the impact of process parameters on the growth of graphene is investigated. Temperature, time, and argon pressure are the primary growth-conditions altered. A temperature of 1400°C in 1 mbar argon for 20 min produced the most optimal graphene growth without significant damage to the AlN capping-layer. Third, first-ever electronic transport measurements are achieved on the selective epitaxial graphene. Hall mobility of about 1550 cm2/Vs has been obtained to date. Finally, the critical limitations of the selective epitaxial graphene growth are enumerated. The advent of enhanced processing techniques that will overcome these limitations will create a multitude of opportunities for applications for graphene grown in this manner. It is envisaged to be a viable approach to fabrication of radio-frequency field-effect transistors.

  15. Large area molybdenum disulphide- epitaxial graphene vertical Van der Waals heterostructures

    PubMed Central

    Pierucci, Debora; Henck, Hugo; Naylor, Carl H.; Sediri, Haikel; Lhuillier, Emmanuel; Balan, Adrian; Rault, Julien E.; Dappe, Yannick J.; Bertran, François; Fèvre, Patrick Le; Johnson, A. T. Charlie; Ouerghi, Abdelkarim

    2016-01-01

    Two-dimensional layered transition metal dichalcogenides (TMDCs) show great potential for optoelectronic devices due to their electronic and optical properties. A metal-semiconductor interface, as epitaxial graphene - molybdenum disulfide (MoS2), is of great interest from the standpoint of fundamental science, as it constitutes an outstanding platform to investigate the interlayer interaction in van der Waals heterostructures. Here, we study large area MoS2-graphene-heterostructures formed by direct transfer of chemical-vapor deposited MoS2 layer onto epitaxial graphene/SiC. We show that via a direct transfer, which minimizes interface contamination, we can obtain high quality and homogeneous van der Waals heterostructures. Angle-resolved photoemission spectroscopy (ARPES) measurements combined with Density Functional Theory (DFT) calculations show that the transition from indirect to direct bandgap in monolayer MoS2 is maintained in these heterostructures due to the weak van der Waals interaction with epitaxial graphene. A downshift of the Raman 2D band of the graphene, an up shift of the A1g peak of MoS2 and a significant photoluminescence quenching are observed for both monolayer and bilayer MoS2 as a result of charge transfer from MoS2 to epitaxial graphene under illumination. Our work provides a possible route to modify the thin film TDMCs photoluminescence properties via substrate engineering for future device design. PMID:27246929

  16. Large area molybdenum disulphide- epitaxial graphene vertical Van der Waals heterostructures

    NASA Astrophysics Data System (ADS)

    Pierucci, Debora; Henck, Hugo; Naylor, Carl H.; Sediri, Haikel; Lhuillier, Emmanuel; Balan, Adrian; Rault, Julien E.; Dappe, Yannick J.; Bertran, François; Fèvre, Patrick Le; Johnson, A. T. Charlie; Ouerghi, Abdelkarim

    2016-06-01

    Two-dimensional layered transition metal dichalcogenides (TMDCs) show great potential for optoelectronic devices due to their electronic and optical properties. A metal-semiconductor interface, as epitaxial graphene - molybdenum disulfide (MoS2), is of great interest from the standpoint of fundamental science, as it constitutes an outstanding platform to investigate the interlayer interaction in van der Waals heterostructures. Here, we study large area MoS2-graphene-heterostructures formed by direct transfer of chemical-vapor deposited MoS2 layer onto epitaxial graphene/SiC. We show that via a direct transfer, which minimizes interface contamination, we can obtain high quality and homogeneous van der Waals heterostructures. Angle-resolved photoemission spectroscopy (ARPES) measurements combined with Density Functional Theory (DFT) calculations show that the transition from indirect to direct bandgap in monolayer MoS2 is maintained in these heterostructures due to the weak van der Waals interaction with epitaxial graphene. A downshift of the Raman 2D band of the graphene, an up shift of the A1g peak of MoS2 and a significant photoluminescence quenching are observed for both monolayer and bilayer MoS2 as a result of charge transfer from MoS2 to epitaxial graphene under illumination. Our work provides a possible route to modify the thin film TDMCs photoluminescence properties via substrate engineering for future device design.

  17. Large area molybdenum disulphide- epitaxial graphene vertical Van der Waals heterostructures.

    PubMed

    Pierucci, Debora; Henck, Hugo; Naylor, Carl H; Sediri, Haikel; Lhuillier, Emmanuel; Balan, Adrian; Rault, Julien E; Dappe, Yannick J; Bertran, François; Fèvre, Patrick Le; Johnson, A T Charlie; Ouerghi, Abdelkarim

    2016-01-01

    Two-dimensional layered transition metal dichalcogenides (TMDCs) show great potential for optoelectronic devices due to their electronic and optical properties. A metal-semiconductor interface, as epitaxial graphene - molybdenum disulfide (MoS2), is of great interest from the standpoint of fundamental science, as it constitutes an outstanding platform to investigate the interlayer interaction in van der Waals heterostructures. Here, we study large area MoS2-graphene-heterostructures formed by direct transfer of chemical-vapor deposited MoS2 layer onto epitaxial graphene/SiC. We show that via a direct transfer, which minimizes interface contamination, we can obtain high quality and homogeneous van der Waals heterostructures. Angle-resolved photoemission spectroscopy (ARPES) measurements combined with Density Functional Theory (DFT) calculations show that the transition from indirect to direct bandgap in monolayer MoS2 is maintained in these heterostructures due to the weak van der Waals interaction with epitaxial graphene. A downshift of the Raman 2D band of the graphene, an up shift of the A1g peak of MoS2 and a significant photoluminescence quenching are observed for both monolayer and bilayer MoS2 as a result of charge transfer from MoS2 to epitaxial graphene under illumination. Our work provides a possible route to modify the thin film TDMCs photoluminescence properties via substrate engineering for future device design. PMID:27246929

  18. Energy Bandgap and Edge States in an Epitaxially Grown Graphene/h-BN Heterostructure.

    PubMed

    Hwang, Beomyong; Hwang, Jeongwoon; Yoon, Jong Keon; Lim, Sungjun; Kim, Sungmin; Lee, Minjun; Kwon, Jeong Hoon; Baek, Hongwoo; Sung, Dongchul; Kim, Gunn; Hong, Suklyun; Ihm, Jisoon; Stroscio, Joseph A; Kuk, Young

    2016-01-01

    Securing a semiconducting bandgap is essential for applying graphene layers in switching devices. Theoretical studies have suggested a created bulk bandgap in a graphene layer by introducing an asymmetry between the A and B sub-lattice sites. A recent transport measurement demonstrated the presence of a bandgap in a graphene layer where the asymmetry was introduced by placing a graphene layer on a hexagonal boron nitride (h-BN) substrate. Similar bandgap has been observed in graphene layers on metal substrates by local probe measurements; however, this phenomenon has not been observed in graphene layers on a near-insulating substrate. Here, we present bulk bandgap-like features in a graphene layer epitaxially grown on an h-BN substrate using scanning tunneling spectroscopy. We observed edge states at zigzag edges, edge resonances at armchair edges, and bandgap-like features in the bulk. PMID:27503427

  19. Energy Bandgap and Edge States in an Epitaxially Grown Graphene/h-BN Heterostructure

    NASA Astrophysics Data System (ADS)

    Hwang, Beomyong; Hwang, Jeongwoon; Yoon, Jong Keon; Lim, Sungjun; Kim, Sungmin; Lee, Minjun; Kwon, Jeong Hoon; Baek, Hongwoo; Sung, Dongchul; Kim, Gunn; Hong, Suklyun; Ihm, Jisoon; Stroscio, Joseph A.; Kuk, Young

    2016-08-01

    Securing a semiconducting bandgap is essential for applying graphene layers in switching devices. Theoretical studies have suggested a created bulk bandgap in a graphene layer by introducing an asymmetry between the A and B sub-lattice sites. A recent transport measurement demonstrated the presence of a bandgap in a graphene layer where the asymmetry was introduced by placing a graphene layer on a hexagonal boron nitride (h-BN) substrate. Similar bandgap has been observed in graphene layers on metal substrates by local probe measurements; however, this phenomenon has not been observed in graphene layers on a near-insulating substrate. Here, we present bulk bandgap-like features in a graphene layer epitaxially grown on an h-BN substrate using scanning tunneling spectroscopy. We observed edge states at zigzag edges, edge resonances at armchair edges, and bandgap-like features in the bulk.

  20. Energy Bandgap and Edge States in an Epitaxially Grown Graphene/h-BN Heterostructure

    PubMed Central

    Hwang, Beomyong; Hwang, Jeongwoon; Yoon, Jong Keon; Lim, Sungjun; Kim, Sungmin; Lee, Minjun; Kwon, Jeong Hoon; Baek, Hongwoo; Sung, Dongchul; Kim, Gunn; Hong, Suklyun; Ihm, Jisoon; Stroscio, Joseph A.; Kuk, Young

    2016-01-01

    Securing a semiconducting bandgap is essential for applying graphene layers in switching devices. Theoretical studies have suggested a created bulk bandgap in a graphene layer by introducing an asymmetry between the A and B sub-lattice sites. A recent transport measurement demonstrated the presence of a bandgap in a graphene layer where the asymmetry was introduced by placing a graphene layer on a hexagonal boron nitride (h-BN) substrate. Similar bandgap has been observed in graphene layers on metal substrates by local probe measurements; however, this phenomenon has not been observed in graphene layers on a near-insulating substrate. Here, we present bulk bandgap-like features in a graphene layer epitaxially grown on an h-BN substrate using scanning tunneling spectroscopy. We observed edge states at zigzag edges, edge resonances at armchair edges, and bandgap-like features in the bulk. PMID:27503427

  1. Energy Bandgap and Edge States in an Epitaxially Grown Graphene/h-BN Heterostructure.

    PubMed

    Hwang, Beomyong; Hwang, Jeongwoon; Yoon, Jong Keon; Lim, Sungjun; Kim, Sungmin; Lee, Minjun; Kwon, Jeong Hoon; Baek, Hongwoo; Sung, Dongchul; Kim, Gunn; Hong, Suklyun; Ihm, Jisoon; Stroscio, Joseph A; Kuk, Young

    2016-08-09

    Securing a semiconducting bandgap is essential for applying graphene layers in switching devices. Theoretical studies have suggested a created bulk bandgap in a graphene layer by introducing an asymmetry between the A and B sub-lattice sites. A recent transport measurement demonstrated the presence of a bandgap in a graphene layer where the asymmetry was introduced by placing a graphene layer on a hexagonal boron nitride (h-BN) substrate. Similar bandgap has been observed in graphene layers on metal substrates by local probe measurements; however, this phenomenon has not been observed in graphene layers on a near-insulating substrate. Here, we present bulk bandgap-like features in a graphene layer epitaxially grown on an h-BN substrate using scanning tunneling spectroscopy. We observed edge states at zigzag edges, edge resonances at armchair edges, and bandgap-like features in the bulk.

  2. The correlation of epitaxial graphene properties and morphology of SiC (0001)

    SciTech Connect

    Guo, Y.; Guo, L. W. E-mail: xlchen@iphy.ac.cn; Huang, J.; Jia, Y. P.; Lin, J. J.; Lu, W.; Li, Z. L.; Yang, R.; Chen, X. L. E-mail: xlchen@iphy.ac.cn

    2014-01-28

    The electronic properties of epitaxial graphene (EG) on SiC (0001) depend sensitively on the surface morphology of SiC substrate. Here, 2–3 layers of graphene were grown on on-axis 6H-SiC with different step densities realized through controlling growth temperature and ambient pressure. We show that epitaxial graphene on SiC (0001) with low step density and straight step edge possesses fewer point defects laying mostly on step edges and higher carrier mobility. A relationship between step density and EG mobility is established. The linear scan of Raman spectra combined with the atomic force microscopy morphology images revealed that the Raman fingerprint peaks are nearly the same on terraces, but shift significantly while cross step edges, suggesting the graphene is not homogeneous in strain and carrier concentration over terraces and step edges of substrates. Thus, control morphology of epitaxial graphene on SiC (0001) is a simple and effective method to pursue optimal route for high quality graphene and will be helpful to prepare wafer sized graphene for device applications.

  3. Adsorption of metal nanoparticles on carbon substrates and epitaxial graphene: Assessing models for dispersion forces

    NASA Astrophysics Data System (ADS)

    Förster, G. D.; Rabilloud, F.; Calvo, F.

    2015-06-01

    Carbon substrates such as graphite or epitaxial graphene can be employed to support metal nanoparticles for applications in diverse areas of surface science. In this paper, we address the computational modeling of such systems by means of semiempirical potentials, and in particular the possible role of long-range London dispersion forces. Following the Grimme (D2) strategy often used in combination with density-functional theory calculations, we propose some analytical extensions taking into account the crystalline and semi-infinite natures of the substrate and, in the case of epitaxial graphene, the possible screening of the van der Waals interaction by the bulk underlying metal. These ideas are tested in the specific case of platinum nanoparticles deposited on graphene, graphite, and graphene epitaxially grown on Pt(111) modeled using a many-body Brenner-type potential, and validated against available electronic-structure calculations. Systematic optimizations carried out at zero temperature indicate the relative stability of various nanoparticle shapes on their support, for adsorbates containing several thousand atoms. Using molecular dynamics simulations, we shed light on the thermal behavior and emphasize the key role of dispersion forces on the stabilization of the adsorbates at finite temperature. The vibrational properties of graphene layers in contact with a Pt nanoparticle or epitaxially grown on Pt(111) also reveal some clear sensitivity on temperature and strain.

  4. Tuning electronic transport in epitaxial graphene-based van der Waals heterostructures

    NASA Astrophysics Data System (ADS)

    Lin, Yu-Chuan; Li, Jun; de La Barrera, Sergio C.; Eichfeld, Sarah M.; Nie, Yifan; Addou, Rafik; Mende, Patrick C.; Wallace, Robert M.; Cho, Kyeongjae; Feenstra, Randall M.; Robinson, Joshua A.

    2016-04-01

    Two-dimensional tungsten diselenide (WSe2) has been used as a component in atomically thin photovoltaic devices, field effect transistors, and tunneling diodes in tandem with graphene. In some applications it is necessary to achieve efficient charge transport across the interface of layered WSe2-graphene, a semiconductor to semimetal junction with a van der Waals (vdW) gap. In such cases, band alignment engineering is required to ensure a low-resistance, ohmic contact. In this work, we investigate the impact of graphene electronic properties on the transport at the WSe2-graphene interface. Electrical transport measurements reveal a lower resistance between WSe2 and fully hydrogenated epitaxial graphene (EGFH) compared to WSe2 grown on partially hydrogenated epitaxial graphene (EGPH). Using low-energy electron microscopy and reflectivity on these samples, we extract the work function difference between the WSe2 and graphene and employ a charge transfer model to determine the WSe2 carrier density in both cases. The results indicate that WSe2-EGFH displays ohmic behavior at small biases due to a large hole density in the WSe2, whereas WSe2-EGPH forms a Schottky barrier junction.Two-dimensional tungsten diselenide (WSe2) has been used as a component in atomically thin photovoltaic devices, field effect transistors, and tunneling diodes in tandem with graphene. In some applications it is necessary to achieve efficient charge transport across the interface of layered WSe2-graphene, a semiconductor to semimetal junction with a van der Waals (vdW) gap. In such cases, band alignment engineering is required to ensure a low-resistance, ohmic contact. In this work, we investigate the impact of graphene electronic properties on the transport at the WSe2-graphene interface. Electrical transport measurements reveal a lower resistance between WSe2 and fully hydrogenated epitaxial graphene (EGFH) compared to WSe2 grown on partially hydrogenated epitaxial graphene (EGPH). Using low

  5. Small scale rotational disorder observed in epitaxial graphene on SiC(0001)

    NASA Astrophysics Data System (ADS)

    Walter, Andrew L.; Bostwick, Aaron; Speck, Florian; Ostler, Markus; Kim, Keun Su; Chang, Young Jun; Moreschini, Luca; Innocenti, Davide; Seyller, Thomas; Horn, Karsten; Rotenberg, Eli

    2013-02-01

    Interest in the use of graphene in electronic devices has motivated an explosion in the study of this remarkable material. The simple, linear, Dirac cone band structure offers a unique possibility to investigate its finer details by angle-resolved photoelectron spectroscopy (ARPES). Indeed, ARPES has been performed on graphene grown on metal substrates but electronic applications require an insulating substrate. Epitaxial graphene grown by the thermal decomposition of silicon carbide (SiC) is an ideal candidate for this due to the large scale, uniform, graphene layers produced. The experimental spectral function of epitaxial graphene on SiC has been extensively studied. However, until now the cause of an anisotropy in the spectral width of the Fermi surface has not been determined. In the current work we show, by comparison of the spectral function to a semi-empirical model, that the anisotropy is due to small scale rotational disorder (˜± 0.15°) of graphene domains in graphene grown on SiC(0001) samples. The complicated shape described by the line-width is accurately reproduced by the semi-empirical model only when rotational disorder is included. While spectra from rare regions of the sample containing only one or two rotational domains is also presented. In addition to the direct benefit in the understanding of graphene's electronic structure this work suggests a mechanism to explain similar variations in related ARPES data.

  6. Single orientation graphene synthesized on iridium thin films grown by molecular beam epitaxy

    NASA Astrophysics Data System (ADS)

    Dangwal Pandey, A.; Krausert, K.; Franz, D.; Grânäs, E.; Shayduk, R.; Müller, P.; Keller, T. F.; Noei, H.; Vonk, V.; Stierle, A.

    2016-08-01

    Heteroepitaxial iridium thin films were deposited on (0001) sapphire substrates by means of molecular beam epitaxy, and subsequently, one monolayer of graphene was synthesized by chemical vapor deposition. The influence of the growth parameters on the quality of the Ir films, as well as of graphene, was investigated systematically by means of low energy electron diffraction, x-ray reflectivity, x-ray diffraction, Auger electron spectroscopy, scanning electron microscopy, and atomic force microscopy. Our study reveals (111) oriented iridium films with high crystalline quality and extremely low surface roughness, on which the formation of large-area epitaxial graphene is achieved. The presence of defects, like dislocations, twins, and 30° rotated domains in the iridium films is also discussed. The coverage of graphene was found to be influenced by the presence of 30° rotated domains in the Ir films. Low iridium deposition rates suppress these rotated domains and an almost complete coverage of graphene was obtained. This synthesis route yields inexpensive, air-stable, and large-area graphene with a well-defined orientation, making it accessible to a wider community of researchers for numerous experiments or applications, including those which use destructive analysis techniques or irreversible processes. Moreover, this approach can be used to tune the structural quality of graphene, allowing a systematic study of the influence of defects in various processes like intercalation below graphene.

  7. Electrostatic transfer of patterned epitaxial graphene from SiC(0001) to glass

    NASA Astrophysics Data System (ADS)

    Biedermann, Laura B.; Beechem, Thomas E.; Ross, Anthony J.; Ohta, Taisuke; Howell, Stephen W.

    2010-12-01

    We report on a scalable electrostatic process to transfer epitaxial graphene onto alkali-containing glass substrates. Multilayer epitaxial graphene (MEG) was grown by heating silicon carbide (000\\bar{1} ) to high temperatures (1650-1700 °C) in an argon-mediated environment. Optical lithography was used to define patterned graphene regions, typically 20×20 μm2, which were then transferred to Pyrex substrates. For the electrostatic transfer, a large electric potential (1.2 kV) was applied between the donor MEG sample (anode) and the heated acceptor glass substrate (cathode). Atomic force microscopy scans of the transferred graphene showed that the morphology of the transferred multilayer graphene resembles that of the donor MEG. Raman spectroscopy analysis confirmed that the graphene can be transferred without inducing defects. The sheet resistance of the transferred graphene was as low as 150 Ω/squ. The transfer of small (1-2 μm wide) and large (~70×70 μm2) graphene patterns to Zerodur demonstrates the versatility of this transfer technique.

  8. Large area and structured epitaxial graphene produced by confinement controlled sublimation of silicon carbide.

    PubMed

    de Heer, Walt A; Berger, Claire; Ruan, Ming; Sprinkle, Mike; Li, Xuebin; Hu, Yike; Zhang, Baiqian; Hankinson, John; Conrad, Edward

    2011-10-11

    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. At these temperatures, silicon sublimes from the surface and the carbon rich surface layer transforms to graphene. However the quality of the graphene produced in ultrahigh vacuum is poor due to the high sublimation rates at relatively low temperatures. The Georgia Tech team developed growth methods involving encapsulating the SiC crystals in graphite enclosures, thereby sequestering the evaporated silicon and bringing growth process closer to equilibrium. In this confinement controlled sublimation (CCS) process, very high-quality graphene is grown on both polar faces of the SiC crystals. Since 2003, over 50 publications used CCS grown graphene, where it is known as the "furnace grown" graphene. Graphene multilayers grown on the carbon-terminated face of SiC, using the CCS method, were shown to consist of decoupled high mobility graphene layers. The CCS method is now applied on structured silicon carbide surfaces to produce high mobility nano-patterned graphene structures thereby demonstrating that EG is a viable contender for next-generation electronics. Here we present for the first time the CCS method that outperforms other epitaxial graphene production methods.

  9. Weak localization in few-layer black phosphorus

    NASA Astrophysics Data System (ADS)

    Du, Yuchen; Neal, Adam T.; Zhou, Hong; Ye, Peide D.

    2016-06-01

    We have conducted a comprehensive investigation into the magneto-transport properties of few-layer black phosphorus in terms of phase coherence length, phase coherence time, and mobility via weak localization measurement and Hall-effect measurement. We present magnetoresistance data showing the weak localization effect in bare p-type few-layer black phosphorus and reveal its strong dependence on temperature and carrier concentration. The measured weak localization agrees well with the Hikami-Larkin-Nagaoka model and the extracted phase coherence length of 104 nm at 350 mK, decreasing as ˜T-0.513+-0.053 with increased temperature. Weak localization measurement allows us to qualitatively probe the temperature-dependent phase coherence time τ ϕ , which is in agreement with the theory of carrier interaction in the diffusive regime. We also observe the universal conductance fluctuation phenomenon in few-layer black phosphorus within moderate magnetic field and low temperature regime.

  10. Express optical analysis of epitaxial graphene on SiC: impact of morphology on quantum transport.

    PubMed

    Yager, Tom; Lartsev, Arseniy; Mahashabde, Sumedh; Charpentier, Sophie; Davidovikj, Dejan; Danilov, Andrey; Yakimova, Rositza; Panchal, Vishal; Kazakova, Olga; Tzalenchuk, Alexander; Lara-Avila, Samuel; Kubatkin, Sergey

    2013-09-11

    We show that inspection with an optical microscope allows surprisingly simple and accurate identification of single and multilayer graphene domains in epitaxial graphene on silicon carbide (SiC/G) and is informative about nanoscopic details of the SiC topography, making it ideal for rapid and noninvasive quality control of as-grown SiC/G. As an illustration of the power of the method, we apply it to demonstrate the correlations between graphene morphology and its electronic properties by quantum magneto-transport.

  11. Resonant optical third-harmonic generation in few-layer black phosphorus

    NASA Astrophysics Data System (ADS)

    de Matos, Christiano J. S.; Rodrigues, Manuel J. L. F.; de Oliveira, Rafael E. P.; Peixoto, Hélder X. P.; Wu, Hsin-Yu; Wei, Ho Y.; Castro Neto, Antonio H.; Viana-Gomes, José C.

    Black phosphorus (BP), a layered monoatomic anisotropic crystal, has recently re-emerged due to demonstrations of its exfoliation down to few-layer thicknesses. It has been shown that BP remains a direct bandgap semiconductor from the bulk to the monolayer, which has triggered interest in its optoelectronic applications. However, optical characterization has been largely restricted to the linear regime, with nonlinear characterization limited to z-scan and saturable absorption measurements. In this work, we show optical third-harmonic generation measurements in bulk and few-layer BP. Results indicate a resonant increase in the generation efficiency of the latter, with signal intensities reaching values three orders of magnitude higher then those of graphene. The mechanisms leading to the resonant increase will be discussed. This work is supported by Fapesp (2012/50259-8 and 2015/11779-4), MackPesquisa, NRF-CRP (R-144-000-295-281), and NRF - Medium Sized Centre Programme.

  12. van der Waals Epitaxy of MoS2 Layers Using Graphene As Growth Templates

    SciTech Connect

    Shi, Yumeng; Zhou, Wu; Lu, Ang-Yu; Fang, Wenjing; Lee, Yi-Hsien; Hsu, Allen Long; Kim, Soo Min; Kim, Ki Kang; Yang, Hui Ying; Liang, Lain-Jong; Idrobo Tapia, Juan C; Kong, Jing

    2012-01-01

    We present a method for synthesizing MoS{sub 2}/Graphene hybrid heterostructures with a growth template of graphene-covered Cu foil. Compared to other recent reports, a much lower growth temperature of 400 C is required for this procedure. The chemical vapor deposition of MoS{sub 2} on the graphene surface gives rise to single crystalline hexagonal flakes with a typical lateral size ranging from several hundred nanometers to several micrometers. The precursor (ammonium thiomolybdate) together with solvent was transported to graphene surface by a carrier gas at room temperature, which was then followed by post annealing. At an elevated temperature, the precursor self-assembles to form MoS{sub 2} flakes epitaxially on the graphene surface via thermal decomposition. With higher amount of precursor delivered onto the graphene surface, a continuous MoS{sub 2} film on graphene can be obtained. This simple chemical vapor deposition method provides a unique approach for the synthesis of graphene heterostructures and surface functionalization of graphene. The synthesized two-dimensional MoS{sub 2}/Graphene hybrids possess great potential toward the development of new optical and electronic devices as well as a wide variety of newly synthesizable compounds for catalysts.

  13. Nanoselective area growth of GaN by metalorganic vapor phase epitaxy on 4H-SiC using epitaxial graphene as a mask

    NASA Astrophysics Data System (ADS)

    Puybaret, Renaud; Patriarche, Gilles; Jordan, Matthew B.; Sundaram, Suresh; El Gmili, Youssef; Salvestrini, Jean-Paul; Voss, Paul L.; de Heer, Walt A.; Berger, Claire; Ougazzaden, Abdallah

    2016-03-01

    We report the growth of high-quality triangular GaN nanomesas, 30-nm thick, on the C-face of 4H-SiC using nanoselective area growth (NSAG) with patterned epitaxial graphene grown on SiC as an embedded mask. NSAG alleviates the problems of defects in heteroepitaxy, and the high mobility graphene film could readily provide the back low-dissipative electrode in GaN-based optoelectronic devices. A 5-8 graphene-layer film is first grown on the C-face of 4H-SiC by confinement-controlled sublimation of silicon carbide. Graphene is then patterned and arrays of 75-nm-wide openings are etched in graphene revealing the SiC substrate. A 30-nm-thick GaN is subsequently grown by metal organic vapor phase epitaxy. GaN nanomesas grow epitaxially with perfect selectivity on SiC, in the openings patterned through graphene. The up-or-down orientation of the mesas on SiC, their triangular faceting, and cross-sectional scanning transmission electron microscopy show that they are biphasic. The core is a zinc blende monocrystal surrounded with single-crystal wurtzite. The GaN crystalline nanomesas have no threading dislocations or V-pits. This NSAG process potentially leads to integration of high-quality III-nitrides on the wafer scalable epitaxial graphene/silicon carbide platform.

  14. Hofstadter Butterfly and Many-Body Effects in Epitaxial Graphene Superlattice.

    PubMed

    Yang, Wei; Lu, Xiaobo; Chen, Guorui; Wu, Shuang; Xie, Guibai; Cheng, Meng; Wang, Duoming; Yang, Rong; Shi, Dongxia; Watanabe, Kenji; Taniguchi, Takashi; Voisin, Christophe; Plaçais, Bernard; Zhang, Yuanbo; Zhang, Guangyu

    2016-04-13

    Graphene placed on hexagonal boron nitride (h-BN) has received a wide range of interest due to the improved electrical performance and rich physics from the interface, especially the emergence of superlattice Dirac points as well as Hofstadter butterfly in high magnetic field. Instead of transferring graphene onto h-BN, epitaxial growth of graphene directly on a single-crystal h-BN provides an alternative and promising way to study these interesting superlattice effects due to their precise lattice alignment. Here we report an electrical transport study on epitaxial graphene superlattice on h-BN with a period of ∼15.6 nm. The epitaxial graphene superlattice is clean, intrinsic, and of high quality with a carrier mobility of ∼27 000 cm(2) V(-1) s(-1), which enables the observation of Hofstadter butterfly features originated from the superlattice at a magnetic field as low as 6.4 T. A metal-insulator transition and magnetic field dependent Fermi velocity were also observed, suggesting prominent electron-electron interaction-induced many-body effects. PMID:26950258

  15. Flower-shaped domains and wrinkles in trilayer epitaxial graphene on silicon carbide.

    PubMed

    Lalmi, B; Girard, J C; Pallecchi, E; Silly, M; David, C; Latil, S; Sirotti, F; Ouerghi, A

    2014-01-01

    Trilayer graphene is of particular interest to the 2D materials community because of its unique tunable electronic structure. However, to date, there is a lack of fundamental understanding of the properties of epitaxial trilayer graphene on silicon carbide. Here, following successful synthesis of large-area uniform trilayer graphene, atomic force microscopy (AFM) showed that the trilayer graphene on 6H-SiC(0001) was uniform over a large scale. Additionally, distinct defects, identified as flower-shaped domains and isolated wrinkle structures, were observed randomly on the surface using scanning tunneling microscopy and spectroscopy (STM/STS). These carbon nanostructures formed during growth, has different structural and electronic properties when compared with the adjacent flat regions of the graphene. Finally, using low temperature STM/STS at 4K, we found that the isolated wrinkles showed an irreversible rotational motion between two 60° configurations at different densities of states. PMID:24513669

  16. Tunneling Spectroscopy Studies of Epitaxial Graphene on Silicon Carbide(0001) and Its Interfaces

    NASA Astrophysics Data System (ADS)

    Sandin, Andreas Axel Tomas

    A two dimensional network of sp2 bonded carbon atoms is defined as graphene. This novel material possesses remarkable electronic properties due to its unique band structure at the vicinity of the Fermi energy. The toughest challenge to bring use of graphene electronic properties in device geometries is that graphene is exceptionally sensitive to its electrical environment for integration into macroscopic system of electrical contacts and substrates. One of the most promising substrates for graphene is the polar surfaces of SiC for the reason it can be grown epitaxially by sublimating Si from the top-most SiC atomic layers. In this work, the interfaces of graphene grown on the Si-terminated polar surface SiC(0001) is studied in UHV using scanning tunneling microscopy (STM), scanning tunneling spectroscopy (STS), low energy electron diffraction (LEED) and auger electron Spectroscopy (AES). STM is used image the graphene surface and interfaces with the capability of atomic resolution. LEED is used to study surface atomic reciprocal ordering and AES is used to determine surface atomic composition during the graphene formation. Interfacial layer (Buffer layer), Single layer graphene and bilayer graphene are identified electronically by means of probing the first member of the image potential derived state. This state is found by dZ/dV spectroscopy in the high energy unoccupied states and is exceptionally sensitive to electrostatic changes to the surface which is detected by energy shifts of image potential states (IPS). This sensitivity is utilized to probe the graphene screening of external electric fields by varying the electric field in the tunneling junction and addresses the fact that charged impurity scattering is likely to be crucial for epitaxial graphene on SiC(0001) when it comes to transport parameters. Shifts of IPS energy position has also been used verify work function changes for identification of several Sodium Intercalation structures of epitaxial

  17. Epitaxial graphene on SiC formed by the surface structure control technique

    NASA Astrophysics Data System (ADS)

    Aritsuki, Takuya; Nakashima, Takeshi; Kobayashi, Keisuke; Ohno, Yasuhide; Nagase, Masao

    2016-06-01

    The thermal decomposition of silicon carbide (SiC) is a promising method for producing wafer-scale single-crystal graphene. The optimal growth condition for high-mobility epitaxial graphene fabricated by infrared rapid thermal annealing is discussed in this paper. The surface structures, such as step–terrace and graphene coverage structures, on a non-off-axis SiC(0001) substrate were well controlled by varying the annealing time in a range below 10 min. The mobility of graphene grown at 1620 °C for 5 min in 100 Torr Ar ambient had a maximum value of 2089 cm2 V‑1 s‑1. We found that the causes of the mobility reduction were low graphene coverage, high sheet carrier density, and nonuniformity of the step structure.

  18. Epitaxial assembly of graphene on face (0001) of silicon carbide: Modeling by semiempirical methods

    NASA Astrophysics Data System (ADS)

    Alekseev, N. I.; Kal'nin, A. A.; Karmanov, D. D.; Luchinin, V. V.; Tarasov, S. A.; Charykov, N. A.

    2013-10-01

    The epitaxial growth of graphene on silicon face (0001) of silicon carbide is simulated using the semiempirical methods of quantum chemistry. The experimental conditions for the epitaxial growth of graphene on SiC, at which the probability of seams and similar defects appearing is reduced to a minimum, are formulated. Possible ways of the emergence of reconstructions of the singular carbon and silicon SiC faces during the synthesis of graphenes are investigated as a test of the approach's efficiency. It is noted that simulation reproduces the reconstruction periods experimentally determined for both faces, and yields the most likely atomic arrangements in cases where the experimental formula of the superstructure allows different versions of such arrangements.

  19. Liquid-Gated Epitaxial Graphene: How Leakage Currents Affect Ionic Strength Sensing

    NASA Astrophysics Data System (ADS)

    Bedoya, Mauricio D.; Metaxas, Peter J.; Scrimgeour, Jan; Hu, Yike; Dong, Rui; Berger, Claire; de Heer, Walt A.; Curtis, Jennifer E.

    2013-03-01

    Graphene is a promising material for the fabrication of miniaturized biological and chemical sensors. Epitaxial graphene is an exciting candidate due to its compatibility with standard processing techniques and its intrinsic robustness. We have fabricated liquid-gated FET-like devices based upon sub-millimeter wide epitaxial graphene strips defined using optical lithography methods. The devices exhibit a bipolar conductance versus gate voltage behavior with the minimum conductance point being dependent upon the ionic strength of a KCl solution. Measurements of the graphene conductance and gate-leakage currents during the stepping of the gate voltage demonstrate the presence of time dependent nA-scale leakage currents which limit signal stability at short times. Notably, these currents depend upon the gate voltage and the composition of the gate electrode. These and other electrode dependent effects have ramifications for graphene sensor design and implementation such as the need to limit gate voltage operating windows as and carefully design electrodes. With high transconductance and controlled doping, such devices should be able to function at low gate voltages if a full understanding of charge and charge transport at the graphene interface is obtained. NSF Grant No. DMR-0820382. PJM thanks the ANN and DIISR.

  20. Transport measurements on monolayer and few-layer WSe2

    NASA Astrophysics Data System (ADS)

    Palomaki, Tauno; Zhao, Wenjin; Finney, Joe; Fei, Zaiyao; Nguyen, Paul; McKay, Frank; Cobden, David

    The behavior of the electrical contacts often dominates transport measurements in mono and few-layer transition metal dichalcogenide (TMD) devices. Creating good contacts for some TMDs is particularly challenging since the fabrication procedure should prevent the TMD from oxidizing or chemically interacting with the contacts. In this talk, we discuss our progress on creating mono and few-layer WSe2 devices with both good electrical contacts and minimal effects from the substrate, polymer contamination, oxidation and other chemistry. For example, we have developed a technique for encapsulating metallic contacts and WSe2 flakes together in hexagonal boron nitride with multiple gates to separate and control the contributions from the channel and the Schottky barriers at the contacts. Research supported in part by Samsung GRO grant US 040814

  1. Electron-Transport Properties of Few-Layer Black Phosphorus.

    PubMed

    Xu, Yuehua; Dai, Jun; Zeng, Xiao Cheng

    2015-06-01

    We perform the first-principles computational study of the effect of number of stacking layers and stacking style of the few-layer black phosphorus (BPs) on the electronic properties, including transport gap, current-voltage (i-v) relation, and differential conductance. Our computation is based on the nonequilibrium Green's function approach combined with density functional theory calculations. Specifically, we compute electron-transport properties of monolayer BP, bilayer BP, and trilayer BP as well as bilayer BPs with AB-, AA-, or AC-stacking. We find that the stacking number has greater influence on the transport gap than the stacking type. Conversely, the stacking type has greater influence on i-v curve and differential conductance than on the transport gap. This study offers useful guidance for determining the number of stacking layers and the stacking style of few-layer BP sheets in future experimental measurements and for potential applications in nanoelectronic devices.

  2. van der Waals epitaxy of CdTe thin film on graphene

    NASA Astrophysics Data System (ADS)

    Mohanty, Dibyajyoti; Xie, Weiyu; Wang, Yiping; Lu, Zonghuan; Shi, Jian; Zhang, Shengbai; Wang, Gwo-Ching; Lu, Toh-Ming; Bhat, Ishwara B.

    2016-10-01

    van der Waals epitaxy (vdWE) facilitates the epitaxial growth of materials having a large lattice mismatch with the substrate. Although vdWE of two-dimensional (2D) materials on 2D materials have been extensively studied, the vdWE for three-dimensional (3D) materials on 2D substrates remains a challenge. It is perceived that a 2D substrate passes little information to dictate the 3D growth. In this article, we demonstrated the vdWE growth of the CdTe(111) thin film on a graphene buffered SiO2/Si substrate using metalorganic chemical vapor deposition technique, despite a 46% large lattice mismatch between CdTe and graphene and a symmetry change from cubic to hexagonal. Our CdTe films produce a very narrow X-ray rocking curve, and the X-ray pole figure analysis showed 12 CdTe (111) peaks at a chi angle of 70°. This was attributed to two sets of parallel epitaxy of CdTe on graphene with a 30° relative orientation giving rise to a 12-fold symmetry in the pole figure. First-principles calculations reveal that, despite the relatively small energy differences, the graphene buffer layer does pass epitaxial information to CdTe as the parallel epitaxy, obtained in the experiment, is energetically favored. The work paves a way for the growth of high quality CdTe film on a large area as well as on the amorphous substrates.

  3. Temperature dependent phonon shifts in few-layer black phosphorus.

    PubMed

    Late, Dattatray J

    2015-03-18

    Atomically thin two-dimensional (2D) sheets of black phosphorus have attracted much attention due to their potential for future nanoelectronic and photonics device applications. Present investigations deal with the temperature dependent phonon shifts in a few-layer black phosphorus nanosheet sample prepared using micromechanical exfoliation on a 300 nm SiO2/Si substrate. The temperature dependent Raman spectroscopy experiments were carried out on a few-layer black phosphorus sample, which depicts softening of Ag(1), B2g, and Ag(2) modes as temperature increases from 77 to 673 K. The calculated temperature coefficients for Ag(1), B2g, and Ag(2) modes of the few-layer black phosphorus nanosheet sample were observed to be -0.01, -0.013, and -0.014 cm(-1) K(-1), respectively. The temperature dependent softening modes of black phosphorus results were explained on the basis of a double resonance process which is more active in an atomically thin sample. This process can also be fundamentally pertinent in other promising and emerging 2D ultrathin layer and heterostructured materials.

  4. Quasi-free-standing bilayer epitaxial graphene field-effect transistors on 4H-SiC (0001) substrates

    NASA Astrophysics Data System (ADS)

    Yu, C.; He, Z. Z.; Li, J.; Song, X. B.; Liu, Q. B.; Cai, S. J.; Feng, Z. H.

    2016-01-01

    Quasi-free-standing epitaxial graphene grown on wide band gap semiconductor SiC demonstrates high carrier mobility and good material uniformity, which make it promising for graphene-based electronic devices. In this work, quasi-free-standing bilayer epitaxial graphene is prepared and its transistors with gate lengths of 100 nm and 200 nm are fabricated and characterized. The 100 nm gate length graphene transistor shows improved DC and RF performances including a maximum current density Ids of 4.2 A/mm, and a peak transconductance gm of 2880 mS/mm. Intrinsic current-gain cutoff frequency fT of 407 GHz is obtained. The exciting DC and RF performances obtained in the quasi-free-standing bilayer epitaxial graphene transistor show the great application potential of this material system.

  5. Epitaxial growth and electrochemical transfer of graphene on Ir(111)/α-Al2O3(0001) substrates

    NASA Astrophysics Data System (ADS)

    Koh, Shinji; Saito, Yuta; Kodama, Hideyuki; Sawabe, Atsuhito

    2016-07-01

    Low-pressure chemical vapor deposition growth of graphene on Iridium (Ir) layers epitaxially deposited on α-Al2O3 (0001) substrates was investigated. The X-ray diffraction, Raman and reflection high energy electron diffraction characterizations revealed that graphene films were epitaxially grown on Ir(111) layers, and the in-plane epitaxial relationship between graphene, Ir(111), and α-Al2O3(0001) was graphene ⟨ 1 1 ¯ 00 ⟩//Ir⟨ 11 2 ¯ ⟩//α-Al2O3⟨ 11 2 ¯ 0 ⟩. The graphene on Ir(111) was electrochemically transferred onto SiO2/Si substrates. We also demonstrated the reuse of the Ir(111)/α-Al2O3(0001) substrates in multiple growth and transfer cycles.

  6. High Electron Mobility in Epitaxial Trilayer Graphene on Off-axis SiC(0001).

    PubMed

    Hajlaoui, Mahdi; Sediri, Haikel; Pierucci, Debora; Henck, Hugo; Phuphachong, Thanyanan; Silly, Mathieu G; de Vaulchier, Louis-Anne; Sirotti, Fausto; Guldner, Yves; Belkhou, Rachid; Ouerghi, Abdelkarim

    2016-01-01

    The van de Waals heterostructure formed by an epitaxial trilayer graphene is of particular interest due to its unique tunable electronic band structure and stacking sequence. However, to date, there has been a lack in the fundamental understanding of the electronic properties of epitaxial trilayer graphene. Here, we investigate the electronic properties of large-area epitaxial trilayer graphene on a 4° off-axis SiC(0001) substrate. Micro-Raman mappings and atomic force microscopy (AFM) confirmed predominantly trilayer on the sample obtained under optimized conditions. We used angle-resolved photoemission spectroscopy (ARPES) and Density Functional Theory (DFT) calculations to study in detail the structure of valence electronic states, in particular the dispersion of π bands in reciprocal space and the exact determination of the number of graphene layers. Using far-infrared magneto-transmission (FIR-MT), we demonstrate, that the electron cyclotron resonance (CR) occurs between Landau levels with a (B)(1/2) dependence. The CR line-width is consistent with a high Dirac fermions mobility of ~3000 cm(2)·V(-1)·s(-1) at 4 K. PMID:26739366

  7. High Electron Mobility in Epitaxial Trilayer Graphene on Off-axis SiC(0001)

    PubMed Central

    Hajlaoui, Mahdi; Sediri, Haikel; Pierucci, Debora; Henck, Hugo; Phuphachong, Thanyanan; Silly, Mathieu G.; de Vaulchier, Louis-Anne; Sirotti, Fausto; Guldner, Yves; Belkhou, Rachid; Ouerghi, Abdelkarim

    2016-01-01

    The van de Waals heterostructure formed by an epitaxial trilayer graphene is of particular interest due to its unique tunable electronic band structure and stacking sequence. However, to date, there has been a lack in the fundamental understanding of the electronic properties of epitaxial trilayer graphene. Here, we investigate the electronic properties of large-area epitaxial trilayer graphene on a 4° off-axis SiC(0001) substrate. Micro-Raman mappings and atomic force microscopy (AFM) confirmed predominantly trilayer on the sample obtained under optimized conditions. We used angle-resolved photoemission spectroscopy (ARPES) and Density Functional Theory (DFT) calculations to study in detail the structure of valence electronic states, in particular the dispersion of π bands in reciprocal space and the exact determination of the number of graphene layers. Using far-infrared magneto-transmission (FIR-MT), we demonstrate, that the electron cyclotron resonance (CR) occurs between Landau levels with a (B)1/2 dependence. The CR line-width is consistent with a high Dirac fermions mobility of ~3000 cm2·V−1·s−1 at 4 K. PMID:26739366

  8. Controlling the growth of epitaxial graphene on metalized diamond (111) surface

    SciTech Connect

    Cooil, S. P.; Wells, J. W.; Hu, D.; Evans, D. A.; Niu, Y. R.; Zakharov, A. A.; Bianchi, M.

    2015-11-02

    The 2-dimensional transformation of the diamond (111) surface to graphene has been demonstrated using ultrathin Fe films that catalytically reduce the reaction temperature needed for the conversion of sp{sup 3} to sp{sup 2} carbon. An epitaxial system is formed, which involves the re-crystallization of carbon at the Fe/vacuum interface and that enables the controlled growth of monolayer and multilayer graphene films. In order to study the initial stages of single and multilayer graphene growth, real time monitoring of the system was preformed within a photoemission and low energy electron microscope. It was found that the initial graphene growth occurred at temperatures as low as 500 °C, whilst increasing the temperature to 560 °C was required to produce multi-layer graphene of high structural quality. Angle resolved photoelectron spectroscopy was used to study the electronic properties of the grown material, where a graphene-like energy momentum dispersion was observed. The Dirac point for the first layer is located at 2.5 eV below the Fermi level, indicating an n-type doping of the graphene due to substrate interactions, while that of the second graphene layer lies close to the Fermi level.

  9. In silico carbon molecular beam epitaxial growth of graphene on the h-BN substrate: carbon source effect on van der Waals epitaxy.

    PubMed

    Lee, Jonghoon; Varshney, Vikas; Park, Jeongho; Farmer, Barry L; Roy, Ajit K

    2016-05-01

    Against the presumption that hexagonal boron-nitride (h-BN) should provide an ideal substrate for van der Waals (vdW) epitaxy to grow high quality graphene films, carbon molecular beam epitaxy (CMBE) techniques using solid carbon sublimation have reported relatively poor quality of the graphene. In this article, the CMBE growth of graphene on the h-BN substrate is numerically studied in order to identify the effect of the carbon source on the quality of the graphene film. The carbon molecular beam generated by the sublimation of solid carbon source materials such as graphite and glassy carbon is mostly composed of atomic carbon, carbon dimers and carbon trimers. Therefore, the graphene film growth becomes a complex process involving various deposition characteristics of a multitude of carbon entities. Based on the study of surface adsorption and film growth characteristics of these three major carbon entities comprising graphite vapour, we report that carbon trimers convey strong traits of vdW epitaxy prone to high quality graphene growth, while atomic carbon deposition is a surface-reaction limited process accompanied by strong chemisorption. The vdW epitaxial behaviour of carbon trimers is found to be substantial enough to nucleate and develop into graphene like planar films within a nanosecond of high flux growth simulation, while reactive atomic carbons tend to impair the structural integrity of the crystalline h-BN substrate upon deposition to form an amorphous interface between the substrate and the growing carbon film. The content of reactive atomic carbons in the molecular beam is suspected to be the primary cause of low quality graphene reported in the literature. A possible optimization of the molecular beam composition towards the synthesis of better quality graphene films is suggested.

  10. In silico carbon molecular beam epitaxial growth of graphene on the h-BN substrate: carbon source effect on van der Waals epitaxy.

    PubMed

    Lee, Jonghoon; Varshney, Vikas; Park, Jeongho; Farmer, Barry L; Roy, Ajit K

    2016-05-01

    Against the presumption that hexagonal boron-nitride (h-BN) should provide an ideal substrate for van der Waals (vdW) epitaxy to grow high quality graphene films, carbon molecular beam epitaxy (CMBE) techniques using solid carbon sublimation have reported relatively poor quality of the graphene. In this article, the CMBE growth of graphene on the h-BN substrate is numerically studied in order to identify the effect of the carbon source on the quality of the graphene film. The carbon molecular beam generated by the sublimation of solid carbon source materials such as graphite and glassy carbon is mostly composed of atomic carbon, carbon dimers and carbon trimers. Therefore, the graphene film growth becomes a complex process involving various deposition characteristics of a multitude of carbon entities. Based on the study of surface adsorption and film growth characteristics of these three major carbon entities comprising graphite vapour, we report that carbon trimers convey strong traits of vdW epitaxy prone to high quality graphene growth, while atomic carbon deposition is a surface-reaction limited process accompanied by strong chemisorption. The vdW epitaxial behaviour of carbon trimers is found to be substantial enough to nucleate and develop into graphene like planar films within a nanosecond of high flux growth simulation, while reactive atomic carbons tend to impair the structural integrity of the crystalline h-BN substrate upon deposition to form an amorphous interface between the substrate and the growing carbon film. The content of reactive atomic carbons in the molecular beam is suspected to be the primary cause of low quality graphene reported in the literature. A possible optimization of the molecular beam composition towards the synthesis of better quality graphene films is suggested. PMID:27108606

  11. Achieving clean epitaxial graphene surfaces suitable for device applications by improved lithographic process

    SciTech Connect

    Nath, A. Rao, M. V.; Koehler, A. D.; Jernigan, G. G.; Wheeler, V. D.; Hite, J. K.; Hernández, S. C.; Robinson, Z. R.; Myers-Ward, R. L.; Eddy, C. R.; Gaskill, D. K.; Garces, N. Y.

    2014-06-02

    It is well-known that the performance of graphene electronic devices is often limited by extrinsic scattering related to resist residue from transfer, lithography, and other processes. Here, we report a polymer-assisted fabrication procedure that produces a clean graphene surface following device fabrication by a standard lithography process. The effectiveness of this improved lithography process is demonstrated by examining the temperature dependence of epitaxial graphene-metal contact resistance using the transfer length method for Ti/Au (10 nm/50 nm) metallization. The Landauer-Buttiker model was used to explain carrier transport at the graphene-metal interface as a function of temperature. At room temperature, a contact resistance of 140 Ω-μm was obtained after a thermal anneal at 523 K for 2 hr under vacuum, which is comparable to state-of-the-art values.

  12. Quantitative atomic resolution force imaging on epitaxial graphene with reactive and nonreactive AFM probes.

    PubMed

    Boneschanscher, Mark P; van der Lit, Joost; Sun, Zhixiang; Swart, Ingmar; Liljeroth, Peter; Vanmaekelbergh, Daniël

    2012-11-27

    Atomic force microscopy (AFM) images of graphene and graphite show contrast with atomic periodicity. However, the contrast patterns vary depending on the atomic termination of the AFM tip apex and the tip-sample distance, hampering the identification of the atomic positions. Here, we report quantitative AFM imaging of epitaxial graphene using inert (carbon-monoxide-terminated) and reactive (iridium-terminated) tips. The atomic image contrast is markedly different with these tip terminations. With a reactive tip, we observe an inversion from attractive to repulsive atomic contrast with decreasing tip-sample distance, while a nonreactive tip only yields repulsive atomic contrast. We are able to identify the atoms with both tips at any tip-sample distance. This is a prerequisite for future structural and chemical analysis of adatoms, defects, and the edges of graphene nanostructures, crucial for understanding nanoscale graphene devices.

  13. Structural investigations of hydrogenated epitaxial graphene grown on 4H-SiC (0001)

    SciTech Connect

    Tokarczyk, M.; Kowalski, G. Stępniewski, R.; Możdżonek, M.; Strupiński, W.; Ciepielewski, P.; Borysiuk, J.

    2013-12-09

    Structural investigations of hydrogenated epitaxial graphene grown on SiC(0001) are presented. It is shown that hydrogen plays a dual role. In addition to contributing to the well-known removal of the buffer layer, it goes between the graphene planes, resulting in an increase of the interlayer spacing to 3.6 Å–3.8 Å. It is explained by the intercalation of molecular hydrogen between carbon planes, which is followed by H{sub 2} dissociation, resulting in negatively charged hydrogen atoms trapped between the graphene layers, with some addition of covalent bonding to carbon atoms. Negatively charged hydrogen may be responsible for p-doping observed in hydrogenated multilayer graphene.

  14. Mini-Dirac cones in the band structure of a copper intercalated epitaxial graphene superlattice

    NASA Astrophysics Data System (ADS)

    Forti, S.; Stöhr, A.; Zakharov, A. A.; Coletti, C.; Emtsev, K. V.; Starke, U.

    2016-09-01

    The electronic band structure of an epitaxial graphene superlattice, generated by intercalating a monolayer of Cu atoms, is directly imaged by angle-resolved photoelectron spectroscopy. The 3.2 nm lateral period of the superlattice is induced by a varying registry between the graphene honeycomb and the Cu atoms as imposed by the heteroepitaxial interface Cu/SiC. The carbon atoms experience a lateral potential across the supercell of an estimated value of about 65 meV. The potential leads to strong energy renormalization in the band structure of the graphene layer and the emergence of mini-Dirac cones. The mini-cones’ band velocity is reduced to about half of graphene's Fermi velocity. Notably, the ordering of the interfacial Cu atoms can be reversibly blocked by mild annealing. The superlattice indeed disappears at ∼220 °C.

  15. Few-layer III-VI and IV-VI 2D semiconductor transistors

    NASA Astrophysics Data System (ADS)

    Sucharitakul, Sukrit; Liu, Mei; Kumar, Rajesh; Sankar, Raman; Chou, Fang C.; Chen, Yit-Tsong; Gao, Xuan

    Since the discovery of atomically thin graphene, a large variety of exfoliable 2D materials have been thoroughly explored for their exotic transport behavior and promises in technological breakthroughs. While most attention on 2D materials beyond graphene is focused on transition metal-dichalcogenides, relatively less attention is paid to layered III-VI and IV-VI semiconductors such as InSe, SnSe etc which bear stronger potential as 2D materials with high electron mobility or thermoelectric figure of merit. We will discuss our recent work on few-layer InSe 2D field effect transistors which exhibit carrier mobility approaching 1000 cm2/Vs and ON-OFF ratio exceeding 107 at room temperature. In addition, the fabrication and device performance of transistors made of mechanically exfoliated multilayer IV-VI semiconductor SnSe and SnSe2 will be discussed.

  16. Strain-Engineered Graphene Grown on Hexagonal Boron Nitride by Molecular Beam Epitaxy.

    PubMed

    Summerfield, Alex; Davies, Andrew; Cheng, Tin S; Korolkov, Vladimir V; Cho, YongJin; Mellor, Christopher J; Foxon, C Thomas; Khlobystov, Andrei N; Watanabe, Kenji; Taniguchi, Takashi; Eaves, Laurence; Novikov, Sergei V; Beton, Peter H

    2016-01-01

    Graphene grown by high temperature molecular beam epitaxy on hexagonal boron nitride (hBN) forms continuous domains with dimensions of order 20 μm, and exhibits moiré patterns with large periodicities, up to ~30 nm, indicating that the layers are highly strained. Topological defects in the moiré patterns are observed and attributed to the relaxation of graphene islands which nucleate at different sites and subsequently coalesce. In addition, cracks are formed leading to strain relaxation, highly anisotropic strain fields, and abrupt boundaries between regions with different moiré periods. These cracks can also be formed by modification of the layers with a local probe resulting in the contraction and physical displacement of graphene layers. The Raman spectra of regions with a large moiré period reveal split and shifted G and 2D peaks confirming the presence of strain. Our work demonstrates a new approach to the growth of epitaxial graphene and a means of generating and modifying strain in graphene.

  17. Strain-Engineered Graphene Grown on Hexagonal Boron Nitride by Molecular Beam Epitaxy

    PubMed Central

    Summerfield, Alex; Davies, Andrew; Cheng, Tin S.; Korolkov, Vladimir V.; Cho, YongJin; Mellor, Christopher J.; Foxon, C. Thomas; Khlobystov, Andrei N.; Watanabe, Kenji; Taniguchi, Takashi; Eaves, Laurence; Novikov, Sergei V.; Beton, Peter H.

    2016-01-01

    Graphene grown by high temperature molecular beam epitaxy on hexagonal boron nitride (hBN) forms continuous domains with dimensions of order 20 μm, and exhibits moiré patterns with large periodicities, up to ~30 nm, indicating that the layers are highly strained. Topological defects in the moiré patterns are observed and attributed to the relaxation of graphene islands which nucleate at different sites and subsequently coalesce. In addition, cracks are formed leading to strain relaxation, highly anisotropic strain fields, and abrupt boundaries between regions with different moiré periods. These cracks can also be formed by modification of the layers with a local probe resulting in the contraction and physical displacement of graphene layers. The Raman spectra of regions with a large moiré period reveal split and shifted G and 2D peaks confirming the presence of strain. Our work demonstrates a new approach to the growth of epitaxial graphene and a means of generating and modifying strain in graphene. PMID:26928710

  18. Graphene nanoribbon field-effect transistors on wafer-scale epitaxial graphene on SiC substrates

    SciTech Connect

    Hwang, Wan Sik E-mail: djena@nd.edu; Zhao, Pei; Tahy, Kristof; Xing, Huili; Seabaugh, Alan; Jena, Debdeep E-mail: djena@nd.edu; Nyakiti, Luke O.; Wheeler, Virginia D.; Myers-Ward, Rachael L.; Eddy, Charles R.; Gaskill, D. Kurt; Robinson, Joshua A.; Haensch, Wilfried

    2015-01-01

    We report the realization of top-gated graphene nanoribbon field effect transistors (GNRFETs) of ∼10 nm width on large-area epitaxial graphene exhibiting the opening of a band gap of ∼0.14 eV. Contrary to prior observations of disordered transport and severe edge-roughness effects of graphene nanoribbons (GNRs), the experimental results presented here clearly show that the transport mechanism in carefully fabricated GNRFETs is conventional band-transport at room temperature and inter-band tunneling at low temperature. The entire space of temperature, size, and geometry dependent transport properties and electrostatics of the GNRFETs are explained by a conventional thermionic emission and tunneling current model. Our combined experimental and modeling work proves that carefully fabricated narrow GNRs behave as conventional semiconductors and remain potential candidates for electronic switching devices.

  19. Phase coherence and energy relaxation in epitaxial graphene under microwave radiation

    NASA Astrophysics Data System (ADS)

    Eless, V.; Yager, T.; Spasov, S.; Lara-Avila, S.; Yakimova, R.; Kubatkin, S.; Janssen, T. J. B. M.; Tzalenchuk, A.; Antonov, V.

    2013-08-01

    We have performed low-temperature magnetotransport measurements on monolayer epitaxial graphene under microwave radiation and extracted the radiation-induced effective temperatures, energy relaxation, and the dephasing times. We established that the response of the graphene sample is entirely bolometric at least up to 170 GHz. Dynamic dephasing, i.e., the time-reversal symmetry breaking effect of the ac electromagnetic field rather than mediated by heating, may become significant in the terahertz frequency range and in samples with longer phase coherence time.

  20. Voltage-controlled inversion of tunnel magnetoresistance in epitaxial nickel/graphene/MgO/cobalt junctions

    NASA Astrophysics Data System (ADS)

    Godel, F.; Venkata Kamalakar, M.; Doudin, B.; Henry, Y.; Halley, D.; Dayen, J.-F.

    2014-10-01

    We report on the fabrication and characterization of vertical spin-valve structures using a thick epitaxial MgO barrier as spacer layer and a graphene-passivated Ni film as bottom ferromagnetic electrode. The devices show robust and scalable tunnel magnetoresistance, with several changes of sign upon varying the applied bias voltage. These findings are explained by a model of phonon-assisted transport mechanisms that relies on the peculiarity of the band structure and spin density of states at the hybrid graphene|Ni interface.

  1. Voltage-controlled inversion of tunnel magnetoresistance in epitaxial nickel/graphene/MgO/cobalt junctions

    SciTech Connect

    Godel, F.; Doudin, B.; Henry, Y.; Halley, D. E-mail: dayen@ipcms.unistra.fr; Dayen, J.-F. E-mail: dayen@ipcms.unistra.fr; Venkata Kamalakar, M.

    2014-10-13

    We report on the fabrication and characterization of vertical spin-valve structures using a thick epitaxial MgO barrier as spacer layer and a graphene-passivated Ni film as bottom ferromagnetic electrode. The devices show robust and scalable tunnel magnetoresistance, with several changes of sign upon varying the applied bias voltage. These findings are explained by a model of phonon-assisted transport mechanisms that relies on the peculiarity of the band structure and spin density of states at the hybrid graphene|Ni interface.

  2. Atomic oxidation of large area epitaxial graphene on 4H-SiC(0001)

    SciTech Connect

    Velez-Fort, E.; Ouerghi, A.; Silly, M. G.; Sirtti, F.; Eddrief, M.; Marangolo, M.; Shukla, A.

    2014-03-03

    Structural and electronic properties of epitaxial graphene on 4H-SiC were studied before and after an atomic oxidation process. X-ray photoemission spectroscopy indicates that oxygen penetrates into the substrate and decouples a part of the interface layer. Raman spectroscopy demonstrates the increase of defects due to the presence of oxygen. Interestingly, we observed on the near edge x-ray absorption fine structure spectra a splitting of the π* peak into two distinct resonances centered at 284.7 and 285.2 eV. This double structure smears out after the oxidation process and permits to probe the interface architecture between graphene and the substrate.

  3. Tuning carrier density across Dirac point in epitaxial graphene on SiC by corona discharge

    SciTech Connect

    Lartsev, Arseniy; Yager, Tom; Lara-Avila, Samuel Kubatkin, Sergey; Bergsten, Tobias; Tzalenchuk, Alexander; Janssen, T. J. B. M; Yakimova, Rositza

    2014-08-11

    We demonstrate reversible carrier density control across the Dirac point (Δn ∼ 10{sup 13 }cm{sup −2}) in epitaxial graphene on SiC (SiC/G) via high electrostatic potential gating with ions produced by corona discharge. The method is attractive for applications where graphene with a fixed carrier density is needed, such as quantum metrology, and more generally as a simple method of gating 2DEGs formed at semiconductor interfaces and in topological insulators.

  4. Influence of Impurity Spin Dynamics on Quantum Transport in Epitaxial Graphene

    NASA Astrophysics Data System (ADS)

    Lara-Avila, Samuel; Kubatkin, Sergey; Kashuba, Oleksiy; Folk, Joshua A.; Lüscher, Silvia; Yakimova, Rositza; Janssen, T. J. B. M.; Tzalenchuk, Alexander; Fal'ko, Vladimir

    2015-09-01

    Experimental evidence from both spin-valve and quantum transport measurements points towards unexpectedly fast spin relaxation in graphene. We report magnetotransport studies of epitaxial graphene on SiC in a vector magnetic field showing that spin relaxation, detected using weak-localization analysis, is suppressed by an in-plane magnetic field B∥, and thereby proving that it is caused at least in part by spinful scatterers. A nonmonotonic dependence of the effective decoherence rate on B∥ reveals the intricate role of the scatterers' spin dynamics in forming the interference correction to the conductivity, an effect that has gone unnoticed in earlier weak localization studies.

  5. High temperature characteristics of bilayer epitaxial graphene field-effect transistors on SiC Substrate

    NASA Astrophysics Data System (ADS)

    Ze-Zhao, He; Ke-Wu, Yang; Cui, Yu; Qing-Bin, Liu; Jing-Jing, Wang; Jia, Li; Wei-Li, Lu; Zhi-Hong, Feng; Shu-Jun, Cai

    2016-06-01

    In this paper, high temperature direct current (DC) performance of bilayer epitaxial graphene device on SiC substrate is studied in a temperature range from 25 °C to 200 °C. At a gate voltage of -8 V (far from Dirac point), the drain-source current decreases obviously with increasing temperature, but it has little change at a gate bias of +8 V (near Dirac point). The competing interactions between scattering and thermal activation are responsible for the different reduction tendencies. Four different kinds of scatterings are taken into account to qualitatively analyze the carrier mobility under different temperatures. The devices exhibit almost unchanged DC performances after high temperature measurements at 200 °C for 5 hours in air ambience, demonstrating the high thermal stabilities of the bilayer epitaxial graphene devices. Project supported by the National Natural Science Foundation of China (Grant No. 61306006).

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

    NASA Astrophysics Data System (ADS)

    Pan, Zhou; Da-Wei, He

    2016-01-01

    On the basis of first principles calculations, we report that the type and density of charge carriers of epitaxial graphene on SiC(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. Project supported by the National Natural Science Foundation of China (Grant Nos. 61335006, 61378073, and 61527817), the Beijing Municipal Science and Technology Committee, China (Grant No. Z151100003315006), and Fundamental Research Funds for the Central Universities of Beijing Jiaotong University, China (Grant No. 2012YJS123).

  7. Vertical Single-Crystalline Organic Nanowires on Graphene: Solution-Phase Epitaxy and Optical Microcavities.

    PubMed

    Zheng, Jian-Yao; Xu, Hongjun; Wang, Jing Jing; Winters, Sinéad; Motta, Carlo; Karademir, Ertuğrul; Zhu, Weigang; Varrla, Eswaraiah; Duesberg, Georg S; Sanvito, Stefano; Hu, Wenping; Donegan, John F

    2016-08-10

    Vertically aligned nanowires (NWs) of single crystal semiconductors have attracted a great deal of interest in the past few years. They have strong potential to be used in device structures with high density and with intriguing optoelectronic properties. However, fabricating such nanowire structures using organic semiconducting materials remains technically challenging. Here we report a simple procedure for the synthesis of crystalline 9,10-bis(phenylethynyl) anthracene (BPEA) NWs on a graphene surface utilizing a solution-phase van der Waals (vdW) epitaxial strategy. The wires are found to grow preferentially in a vertical direction on the surface of graphene. Structural characterization and first-principles ab initio simulations were performed to investigate the epitaxial growth and the molecular orientation of the BPEA molecules on graphene was studied, revealing the role of interactions at the graphene-BPEA interface in determining the molecular orientation. These free-standing NWs showed not only efficient optical waveguiding with low loss along the NW but also confinement of light between the two end facets of the NW forming a microcavity Fabry-Pérot resonator. From an analysis of the optical dispersion within such NW microcavities, we observed strong slowing of the waveguided light with a group velocity reduced to one-tenth the speed of light. Applications of the vertical single-crystalline organic NWs grown on graphene will benefit from a combination of the unique electronic properties and flexibility of graphene and the tunable optical and electronic properties of organic NWs. Therefore, these vertical organic NW arrays on graphene offer the potential for realizing future on-chip light sources. PMID:27438189

  8. Mechanical and Electrical Anisotropy of Few-Layer Black Phosphorus.

    PubMed

    Tao, Jin; Shen, Wanfu; Wu, Sen; Liu, Lu; Feng, Zhihong; Wang, Chao; Hu, Chunguang; Yao, Pei; Zhang, Hao; Pang, Wei; Duan, Xuexin; Liu, Jing; Zhou, Chongwu; Zhang, Daihua

    2015-11-24

    We combined reflection difference microscopy, electron transport measurements, and atomic force microscopy to characterize the mechanical and electrical anisotropy of few-layer black phosphorus. We were able to identify the lattice orientations of the two-dimensional material and construct suspended structures aligned with specific crystal axes. The approach allowed us to probe the anisotropic mechanical and electrical properties along each lattice axis in separate measurements. We measured the Young's modulus of few-layer black phosphorus to be 58.6 ± 11.7 and 27.2 ± 4.1 GPa in zigzag and armchair directions. The breaking stress scaled almost linearly with the Young's modulus and was measured to be 4.79 ± 1.43 and 2.31 ± 0.71 GPa in the two directions. We have also observed highly anisotropic transport behavior in black phosphorus and derived the conductance anisotropy to be 63.7%. The test results agreed well with theoretical predictions. Our work provided very valuable experimental data and suggested an effective characterization means for future studies on black phosphorus and anisotropic two-dimensional nanomaterials in general.

  9. Large Ultraviolet Photoresponsivity of Few-layer Black Phosphorus

    NASA Astrophysics Data System (ADS)

    Wu, Jing; Kok Wai Koon, Gavin; Xiang, Du; Castro Neto, Antonio H.; Özyilmaz, Barbaros; Centre of Advanced 2D Materials Team

    Black phosphorus has recently gained much attention in the scientific community. Black phosphorus can be seen as a crystal generated by periodic repetition of tetraphosphorus (P4) molecules. It is known that tetraphosphorus P4 can be transformed temporarily to diphosphorus P2 upon ultraviolet (UV) irradiation. Thus, it is expected that the P4 structured black phosphorus also has strong interaction with light especially in the UV range. Here we report on the optoelectronic characteristics of few-layer black phosphorus field effect transistors (FETs) ranging from the UV to the near infrared (NIR). We demonstrate that black phosphorus is an excellent ultraviolet (UV) photodetector with a specific detectivity ~3x1013 Jones. We report also an exceptional photo responsivity of 107 times higher than previously reported values for black phosphorus visible light photodetectors. We attribute such a colossal UV photo responsivity to the resonant-interband transition between two specially nested valence and conduction bands. These nested bands provide an unusually high density of states for high-efficient UV absorption due to their singularity nature. Large Ultraviolet Photoresponsivity of Few-layer Black Phosphorus.

  10. Hydrogen assisted growth of high quality epitaxial graphene on the C-face of 4H-SiC

    SciTech Connect

    Cai, Tuocheng; Jia, Zhenzhao; Yan, Baoming; Yu, Dapeng; Wu, Xiaosong

    2015-01-05

    We demonstrate hydrogen assisted growth of high quality epitaxial graphene on the C-face of 4H-SiC. Compared with the conventional thermal decomposition technique, the size of the growth domain by this method is substantially increased and the thickness variation is reduced. Based on the morphology of epitaxial graphene, the role of hydrogen is revealed. It is found that hydrogen acts as a carbon etchant. It suppresses the defect formation and nucleation of graphene. It also improves the kinetics of carbon atoms via hydrocarbon species. These effects lead to increase of the domain size and the structure quality. The consequent capping effect results in smooth surface morphology and suppression of multilayer growth. Our method provides a viable route to fine tune the growth kinetics of epitaxial graphene on SiC.

  11. Aqueous dispersions of few-layer-thick chemically modified magnesium diboride nanosheets by ultrasonication assisted exfoliation.

    PubMed

    Das, Saroj Kumar; Bedar, Amita; Kannan, Aadithya; Jasuja, Kabeer

    2015-01-01

    The discovery of graphene has led to a rising interest in seeking quasi two-dimensional allotropes of several elements and inorganic compounds. Boron, carbon's neighbour in the periodic table, presents a curious case in its ability to be structured as graphene. Although it cannot independently constitute a honeycomb planar structure, it forms a graphenic arrangement in association with electron-donor elements. This is exemplified in magnesium diboride (MgB2): an inorganic layered compound comprising boron honeycomb planes alternated by Mg atoms. Till date, MgB2 has been primarily researched for its superconducting properties; it hasn't been explored for the possibility of its exfoliation. Here we show that ultrasonication of MgB2 in water results in its exfoliation to yield few-layer-thick Mg-deficient hydroxyl-functionalized nanosheets. The hydroxyl groups enable an electrostatically stabilized aqueous dispersion and create a heterogeneity leading to an excitation wavelength dependent photoluminescence. These chemically modified MgB2 nanosheets exhibit an extremely small absorption coefficient of 2.9 ml mg(-1) cm(-1) compared to graphene and its analogs. This ability to exfoliate MgB2 to yield nanosheets with a chemically modified lattice and properties distinct from the parent material presents a fundamentally new perspective to the science of MgB2 and forms a first foundational step towards exfoliating metal borides. PMID:26041686

  12. Aqueous dispersions of few-layer-thick chemically modified magnesium diboride nanosheets by ultrasonication assisted exfoliation.

    PubMed

    Das, Saroj Kumar; Bedar, Amita; Kannan, Aadithya; Jasuja, Kabeer

    2015-06-04

    The discovery of graphene has led to a rising interest in seeking quasi two-dimensional allotropes of several elements and inorganic compounds. Boron, carbon's neighbour in the periodic table, presents a curious case in its ability to be structured as graphene. Although it cannot independently constitute a honeycomb planar structure, it forms a graphenic arrangement in association with electron-donor elements. This is exemplified in magnesium diboride (MgB2): an inorganic layered compound comprising boron honeycomb planes alternated by Mg atoms. Till date, MgB2 has been primarily researched for its superconducting properties; it hasn't been explored for the possibility of its exfoliation. Here we show that ultrasonication of MgB2 in water results in its exfoliation to yield few-layer-thick Mg-deficient hydroxyl-functionalized nanosheets. The hydroxyl groups enable an electrostatically stabilized aqueous dispersion and create a heterogeneity leading to an excitation wavelength dependent photoluminescence. These chemically modified MgB2 nanosheets exhibit an extremely small absorption coefficient of 2.9 ml mg(-1) cm(-1) compared to graphene and its analogs. This ability to exfoliate MgB2 to yield nanosheets with a chemically modified lattice and properties distinct from the parent material presents a fundamentally new perspective to the science of MgB2 and forms a first foundational step towards exfoliating metal borides.

  13. Aqueous dispersions of few-layer-thick chemically modified magnesium diboride nanosheets by ultrasonication assisted exfoliation

    PubMed Central

    Das, Saroj Kumar; Bedar, Amita; Kannan, Aadithya; Jasuja, Kabeer

    2015-01-01

    The discovery of graphene has led to a rising interest in seeking quasi two-dimensional allotropes of several elements and inorganic compounds. Boron, carbon’s neighbour in the periodic table, presents a curious case in its ability to be structured as graphene. Although it cannot independently constitute a honeycomb planar structure, it forms a graphenic arrangement in association with electron-donor elements. This is exemplified in magnesium diboride (MgB2): an inorganic layered compound comprising boron honeycomb planes alternated by Mg atoms. Till date, MgB2 has been primarily researched for its superconducting properties; it hasn’t been explored for the possibility of its exfoliation. Here we show that ultrasonication of MgB2 in water results in its exfoliation to yield few-layer-thick Mg-deficient hydroxyl-functionalized nanosheets. The hydroxyl groups enable an electrostatically stabilized aqueous dispersion and create a heterogeneity leading to an excitation wavelength dependent photoluminescence. These chemically modified MgB2 nanosheets exhibit an extremely small absorption coefficient of 2.9 ml mg−1 cm−1 compared to graphene and its analogs. This ability to exfoliate MgB2 to yield nanosheets with a chemically modified lattice and properties distinct from the parent material presents a fundamentally new perspective to the science of MgB2 and forms a first foundational step towards exfoliating metal borides. PMID:26041686

  14. Tailoring low-dimensional structures of bismuth on monolayer epitaxial graphene

    PubMed Central

    Chen, H.-H.; Su, S. H.; Chang, S.-L.; Cheng, B.-Y.; Chen, S. W.; Chen, H.-Y.; Lin, M.-F.; Huang, J. C. A.

    2015-01-01

    To improve graphene-based multifunctional devices at nanoscale, a stepwise and controllable fabrication procedure must be elucidated. Here, a series of structural transition of bismuth (Bi) adatoms, adsorbed on monolayer epitaxial graphene (MEG), is explored at room temperature. Bi adatoms undergo a structural transition from one-dimensional (1D) linear structures to two-dimensional (2D) triangular islands and such 2D growth mode is affected by the corrugated substrate. Upon Bi deposition, a little charge transfer occurs and a characteristic peak can be observed in the tunneling spectrum, reflecting the distinctive electronic structure of the Bi adatoms. When annealed to ~500 K, 2D triangular Bi islands aggregate into Bi nanoclusters (NCs) of uniform size. A well-controlled fabrication method is thus demonstrated. The approaches adopted herein provide perspectives for fabricating and characterizing periodic networks on MEG and related systems, which are useful in realizing graphene-based electronic, energy, sensor and spintronic devices. PMID:26100604

  15. Theory of the Growth of Epitaxial Graphene on Close-Packed Metals

    NASA Astrophysics Data System (ADS)

    Zangwill, Andrew; Vvedensky, Dimitri

    2011-03-01

    We present a simple rate theory of epitaxial graphene growth on close-packed metals. Motivated by recent low-energy electron microscopy experiments [E. Loginova, N.C.Bartelt, P.J. Feibelman, and K.F. McCarty, New Journal of Physics, 10, 093026 (2008)], our theory supposes that graphene islands grow predominantly by the addition of five-atom clusters, rather than solely by the capture of diffusing carbon atoms. With suitably chosen kinetic parameters, we find quantitative agreement with (i) the measured time-evolution of the adatom density and (ii) the measured temperature-dependence of the adatom density at the onset of nucleation by assuming that the smallest stable precursor to graphene growth is an immobile island composed of six five-atom clusters.

  16. Tailoring low-dimensional structures of bismuth on monolayer epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Chen, H.-H.; Su, S. H.; Chang, S.-L.; Cheng, B.-Y.; Chen, S. W.; Chen, H.-Y.; Lin, M.-F.; Huang, J. C. A.

    2015-06-01

    To improve graphene-based multifunctional devices at nanoscale, a stepwise and controllable fabrication procedure must be elucidated. Here, a series of structural transition of bismuth (Bi) adatoms, adsorbed on monolayer epitaxial graphene (MEG), is explored at room temperature. Bi adatoms undergo a structural transition from one-dimensional (1D) linear structures to two-dimensional (2D) triangular islands and such 2D growth mode is affected by the corrugated substrate. Upon Bi deposition, a little charge transfer occurs and a characteristic peak can be observed in the tunneling spectrum, reflecting the distinctive electronic structure of the Bi adatoms. When annealed to ~500 K, 2D triangular Bi islands aggregate into Bi nanoclusters (NCs) of uniform size. A well-controlled fabrication method is thus demonstrated. The approaches adopted herein provide perspectives for fabricating and characterizing periodic networks on MEG and related systems, which are useful in realizing graphene-based electronic, energy, sensor and spintronic devices.

  17. Atomically Sharp Interface in an h-BN-epitaxial graphene van der Waals Heterostructure

    PubMed Central

    Sediri, Haikel; Pierucci, Debora; Hajlaoui, Mahdi; Henck, Hugo; Patriarche, Gilles; Dappe, Yannick J.; Yuan, Sheng; Toury, Bérangère; Belkhou, Rachid; Silly, Mathieu G.; Sirotti, Fausto; Boutchich, Mohamed; Ouerghi, Abdelkarim

    2015-01-01

    Stacking various two-dimensional atomic crystals is a feasible approach to creating unique multilayered van der Waals heterostructures with tailored properties. Herein for the first time, we present a controlled preparation of large-area h-BN/graphene heterostructures via a simple chemical deposition of h-BN layers on epitaxial graphene/SiC(0001). Van der Waals forces, which are responsible for the cohesion of the multilayer system, give rise to an abrupt interface without interdiffusion between graphene and h-BN, as shown by X-ray Photoemission Spectroscopy (XPS) and direct observation using scanning and High-Resolution Transmission Electron Microscopy (STEM/HRTEM). The electronic properties of graphene, such as the Dirac cone, remain intact and no significant charge transfer i.e. doping, is observed. These results are supported by Density Functional Theory (DFT) calculations. We demonstrate that the h-BN capped graphene allows the fabrication of vdW heterostructures without altering the electronic properties of graphene. PMID:26585245

  18. Atomically Sharp Interface in an h-BN-epitaxial graphene van der Waals Heterostructure.

    PubMed

    Sediri, Haikel; Pierucci, Debora; Hajlaoui, Mahdi; Henck, Hugo; Patriarche, Gilles; Dappe, Yannick J; Yuan, Sheng; Toury, Bérangère; Belkhou, Rachid; Silly, Mathieu G; Sirotti, Fausto; Boutchich, Mohamed; Ouerghi, Abdelkarim

    2015-01-01

    Stacking various two-dimensional atomic crystals is a feasible approach to creating unique multilayered van der Waals heterostructures with tailored properties. Herein for the first time, we present a controlled preparation of large-area h-BN/graphene heterostructures via a simple chemical deposition of h-BN layers on epitaxial graphene/SiC(0001). Van der Waals forces, which are responsible for the cohesion of the multilayer system, give rise to an abrupt interface without interdiffusion between graphene and h-BN, as shown by X-ray Photoemission Spectroscopy (XPS) and direct observation using scanning and High-Resolution Transmission Electron Microscopy (STEM/HRTEM). The electronic properties of graphene, such as the Dirac cone, remain intact and no significant charge transfer i.e. doping, is observed. These results are supported by Density Functional Theory (DFT) calculations. We demonstrate that the h-BN capped graphene allows the fabrication of vdW heterostructures without altering the electronic properties of graphene. PMID:26585245

  19. Approach to multifunctional device platform with epitaxial graphene on transition metal oxide

    PubMed Central

    Park, Jeongho; Back, Tyson; Mitchel, William C.; Kim, Steve S.; Elhamri, Said; Boeckl, John; Fairchild, Steven B.; Naik, Rajesh; Voevodin, Andrey A.

    2015-01-01

    Heterostructures consisting of two-dimensional materials have shown new physical phenomena, novel electronic and optical properties, and new device concepts not observed in bulk material systems or purely three dimensional heterostructures. These new effects originated mostly from the van der Waals interaction between the different layers. Here we report that a new optical and electronic device platform can be provided by heterostructures of 2D graphene with a metal oxide (TiO2). Our novel direct synthesis of graphene/TiO2 heterostructure is achieved by C60 deposition on transition Ti metal surface using a molecular beam epitaxy approach and O2 intercalation method, which is compatible with wafer scale growth of heterostructures. As-grown heterostructures exhibit inherent photosensitivity in the visible light spectrum with high photo responsivity. The photo sensitivity is 25 times higher than that of reported graphene photo detectors. The improved responsivity is attributed to optical transitions between O 2p orbitals in the valence band of TiO2 and C 2p orbitals in the conduction band of graphene enabled by Coulomb interactions at the interface. In addition, this heterostructure provides a platform for realization of bottom gated graphene field effect devices with graphene and TiO2 playing the roles of channel and gate dielectric layers, respectively. PMID:26395160

  20. Wafer-scale epitaxial graphene on SiC for sensing applications

    NASA Astrophysics Data System (ADS)

    Karlsson, Mikael; Wang, Qin; Zhao, Yichen; Zhao, Wei; Toprak, Muhammet S.; Iakimov, Tihomir; Ali, Amer; Yakimova, Rositza; Syväjärvi, Mikael; Ivanov, Ivan G.

    2015-12-01

    The epitaxial graphene-on-silicon carbide (SiC-G) has advantages of high quality and large area coverage owing to a natural interface between graphene and SiC substrate with dimension up to 100 mm. It enables cost effective and reliable solutions for bridging the graphene-based sensors/devices from lab to industrial applications and commercialization. In this work, the structural, optical and electrical properties of wafer-scale graphene grown on 2'' 4H semi-insulating (SI) SiC utilizing sublimation process were systemically investigated with focus on evaluation of the graphene's uniformity across the wafer. As proof of concept, two types of glucose sensors based on SiC-G/Nafion/Glucose-oxidase (GOx) and SiC-G/Nafion/Chitosan/GOx were fabricated and their electrochemical properties were characterized by cyclic voltammetry (CV) measurements. In addition, a few similar glucose sensors based on graphene by chemical synthesis using modified Hummer's method were also fabricated for comparison.

  1. Plasma-Modified, Epitaxial Fabricated Graphene on SiC for the Electrochemical Detection of TNT

    PubMed Central

    Trammell, Scott A.; Hernández, Sandra C.; Myers-Ward, Rachael L.; Zabetakis, Daniel; Stenger, David A.; Gaskill, D. Kurt; Walton, Scott G.

    2016-01-01

    Using square wave voltammetry, we show an increase in the electrochemical detection of trinitrotoluene (TNT) with a working electrode constructed from plasma modified graphene on a SiC surface vs. unmodified graphene. The graphene surface was chemically modified using electron beam generated plasmas produced in oxygen or nitrogen containing backgrounds to introduce oxygen or nitrogen moieties. The use of this chemical modification route enabled enhancement of the electrochemical signal for TNT, with the oxygen treatment showing a more pronounced detection than the nitrogen treatment. For graphene modified with oxygen, the electrochemical response to TNT can be fit to a two-site Langmuir isotherm suggesting different sites on the graphene surface with different affinities for TNT. We estimate a limit of detection for TNT equal to 20 ppb based on the analytical standard S/N ratio of 3. In addition, this approach to sensor fabrication is inherently a high-throughput, high-volume process amenable to industrial applications. High quality epitaxial graphene is easily grown over large area SiC substrates, while plasma processing is a rapid approach to large area substrate processing. This combination facilitates low cost, mass production of sensors. PMID:27529251

  2. Plasma-Modified, Epitaxial Fabricated Graphene on SiC for the Electrochemical Detection of TNT.

    PubMed

    Trammell, Scott A; Hernández, Sandra C; Myers-Ward, Rachael L; Zabetakis, Daniel; Stenger, David A; Gaskill, D Kurt; Walton, Scott G

    2016-01-01

    Using square wave voltammetry, we show an increase in the electrochemical detection of trinitrotoluene (TNT) with a working electrode constructed from plasma modified graphene on a SiC surface vs. unmodified graphene. The graphene surface was chemically modified using electron beam generated plasmas produced in oxygen or nitrogen containing backgrounds to introduce oxygen or nitrogen moieties. The use of this chemical modification route enabled enhancement of the electrochemical signal for TNT, with the oxygen treatment showing a more pronounced detection than the nitrogen treatment. For graphene modified with oxygen, the electrochemical response to TNT can be fit to a two-site Langmuir isotherm suggesting different sites on the graphene surface with different affinities for TNT. We estimate a limit of detection for TNT equal to 20 ppb based on the analytical standard S/N ratio of 3. In addition, this approach to sensor fabrication is inherently a high-throughput, high-volume process amenable to industrial applications. High quality epitaxial graphene is easily grown over large area SiC substrates, while plasma processing is a rapid approach to large area substrate processing. This combination facilitates low cost, mass production of sensors. PMID:27529251

  3. Performance change of few layer black phosphorus transistors in ambient

    NASA Astrophysics Data System (ADS)

    Ma, Xiaomeng; Lu, Wanglin; Chen, Bingyan; Zhong, Donglai; Huang, Le; Dong, Lijun; Jin, Chuanhong; Zhang, Zhiyong

    2015-10-01

    Transistors were fabricated based on mechanical exfoliated few layer black phosphorus (BP) flakes, and performance change of these devices exposed to air was explored systematically. BP devices were found to suffer severe performance degradation in ambient conditions, and the field effect mobility drops to less than 1/10 of the original in no more than 120 hours after fabrication. However the current on/off ratio shows completely different time dependent behavior to the published result, i.e. increases with exposure time in air, since the minimum current decreases with exposure time to air, which is probably originated from the decrease of layer number in BP. A model is developed to estimate the bandgap change of BP according to the time dependent minimum current of the BP device.

  4. Few-layer HfS2 transistors

    PubMed Central

    Kanazawa, Toru; Amemiya, Tomohiro; Ishikawa, Atsushi; Upadhyaya, Vikrant; Tsuruta, Kenji; Tanaka, Takuo; Miyamoto, Yasuyuki

    2016-01-01

    HfS2 is the novel transition metal dichalcogenide, which has not been experimentally investigated as the material for electron devices. As per the theoretical calculations, HfS2 has the potential for well-balanced mobility (1,800 cm2/V·s) and bandgap (1.2 eV) and hence it can be a good candidate for realizing low-power devices. In this paper, the fundamental properties of few-layer HfS2 flakes were experimentally evaluated. Micromechanical exfoliation using scotch tape extracted atomically thin HfS2 flakes with varying colour contrasts associated with the number of layers and resonant Raman peaks. We demonstrated the I-V characteristics of the back-gated few-layer (3.8 nm) HfS2 transistor with the robust current saturation. The on/off ratio was more than 104 and the maximum drain current of 0.2 μA/μm was observed. Moreover, using the electric double-layer gate structure with LiClO4:PEO electrolyte, the drain current of the HfS2 transistor significantly increased to 0.75 mA/μm and the mobility was estimated to be 45 cm2/V·s at least. This improved current seemed to indicate superior intrinsic properties of HfS2. These results provides the basic information for the experimental researches of electron devices based on HfS2. PMID:26926098

  5. Few-layer HfS2 transistors

    NASA Astrophysics Data System (ADS)

    Kanazawa, Toru; Amemiya, Tomohiro; Ishikawa, Atsushi; Upadhyaya, Vikrant; Tsuruta, Kenji; Tanaka, Takuo; Miyamoto, Yasuyuki

    2016-03-01

    HfS2 is the novel transition metal dichalcogenide, which has not been experimentally investigated as the material for electron devices. As per the theoretical calculations, HfS2 has the potential for well-balanced mobility (1,800 cm2/V·s) and bandgap (1.2 eV) and hence it can be a good candidate for realizing low-power devices. In this paper, the fundamental properties of few-layer HfS2 flakes were experimentally evaluated. Micromechanical exfoliation using scotch tape extracted atomically thin HfS2 flakes with varying colour contrasts associated with the number of layers and resonant Raman peaks. We demonstrated the I-V characteristics of the back-gated few-layer (3.8 nm) HfS2 transistor with the robust current saturation. The on/off ratio was more than 104 and the maximum drain current of 0.2 μA/μm was observed. Moreover, using the electric double-layer gate structure with LiClO4:PEO electrolyte, the drain current of the HfS2 transistor significantly increased to 0.75 mA/μm and the mobility was estimated to be 45 cm2/V·s at least. This improved current seemed to indicate superior intrinsic properties of HfS2. These results provides the basic information for the experimental researches of electron devices based on HfS2.

  6. Environmental Effects on the Terahertz Surface Plasmons in Epitaxial Graphene

    NASA Astrophysics Data System (ADS)

    Fekete, Paula; Gumbs, Godfrey; Iurov, Andrii; Wu, Jhao-Ying; Lin, Ming-Fa

    We predict the existence of low-frequency nonlocal plasmons at the vacuum-surface interface of a superlattice of N graphene layers interacting with conducting substrate. We derive a dispersion function that incorporates the polarization function of both the graphene monolayers and the semi-infinite electron liquid at whose surface the electrons scatter specularly. We find a surface plasmon-polariton that is not damped by particle-hole excitations or the bulk modes and which separates below the continuum mini-band of bulk plasmon modes. The surface plasmon frequency of the hybrid structure always lies below a limiting value of the surface plasmon frequency of the conducting substrate. The intensity of this mode depends on the distance of the graphene layers from the conductor's surface, the energy band gap between valence and conduction bands of graphene monolayer and, most importantly, on the number of two-dimensional layers. For a sufficiently large number of layers (N >7) the hybrid structure has no surface plasmon. The existence of two plasmons with different dispersion relations indicates that quasiparticles with different group velocity may coexist for various ranges of wavelengths determined by the number of layers in the superlattice.

  7. Spin transport in epitaxial graphene on the C-terminated ( 000 1 ¯ )-face of silicon carbide

    NASA Astrophysics Data System (ADS)

    van den Berg, J. J.; Yakimova, R.; van Wees, B. J.

    2016-07-01

    We performed a temperature dependent study of the charge and spin transport properties of epitaxial graphene on the C-terminated ( 000 1 ¯ ) face of silicon carbide (SiC), a system without a carbon buffer layer between the graphene and the SiC. Using spin Hanle precession in the nonlocal geometry, we measured a spin relaxation length of λS = 0.7 μm at room temperature, lower than in exfoliated graphene. We show that the charge and spin diffusion coefficient, DC and DS, respectively, increasingly deviate from each other during electrical measurements up to a difference of a factor 4. Thus, we show that a model of localized states that was previously used to explain DC ≠ DS, can also be applied to epitaxial graphene systems without a carbon buffer layer. We attribute the effect to charge trap states in the interface between the graphene and the SiC.

  8. Scalable Clean Exfoliation of High-Quality Few-Layer Black Phosphorus for a Flexible Lithium Ion Battery.

    PubMed

    Chen, Long; Zhou, Guangmin; Liu, Zhibo; Ma, Xiaomeng; Chen, Jing; Zhang, Zhiyong; Ma, Xiuliang; Li, Feng; Cheng, Hui-Ming; Ren, Wencai

    2016-01-20

    Few-layer black phosphorus (BP) nanosheets that are clean and of high quality, are efficiently produced by exfoliating bulk BP crystals, which are prepared by a scalable gas-phase catalytic transformation method in water. They are stable enough in water for further processing and applications. As an example, these BP nanosheets are combined with graphene to give high-performance flexible lithium-ion batteries.

  9. Anisotropic diffusion of oxygen on a few layers of black phosphorous

    NASA Astrophysics Data System (ADS)

    Fernández-Escamilla, Hector Noe; González-Chávez, Víctor Hugo; Martínez-Guerra, Eduardo; Garay-Tapia, Andrés; Martínez-Guerra, Edgar

    Recently, phosporene has also been scored well as a functional material for two-dimensional electronic and optoelectronic devices. That is, because in contrast to graphene, black phosphorous has an inherent, direct and appreciable band gap that can be modulated with the numbers of layes. However, the presence of exposed lone pairs at the surface makes phosphorous very reactive to air and humidity and consequently, degradation of its properties. No such fundamental explanation have been made, thus corresponding first principle predictions to evaluate diffusion of O over and along a mono- and a few layers are indispensable. Energy barriers and the mechanisms of oxygen diffusion on mono- and a few layer of black phosphorous were calculated using the NEB(Nudge Elastic band) method as implemented in Quantum Espresso. The electronic states are expanded in plane waves with kinetic-energy cutoffs of 25 and 200 Ry for the wave function and charge density, respectively. Also, as the H2O and O2 are polar molecules, spin-polarized calculations have been carried out. We evaluated the diffusion barriers for O2 and H2O on phosphorene along zigzag, armchair and intermediated directions. Our calculations show that diffusion of O is preferred on zigzag directions and dissociation of O2 is favored as a result of energy gains of about 2 eV. Also, apparently diffusion pathways are blocked along layers.

  10. High-mobility transport anisotropy and linear dichroism in few-layer black phosphorus.

    PubMed

    Qiao, Jingsi; Kong, Xianghua; Hu, Zhi-Xin; Yang, Feng; Ji, Wei

    2014-07-21

    Two-dimensional crystals are emerging materials for nanoelectronics. Development of the field requires candidate systems with both a high carrier mobility and, in contrast to graphene, a sufficiently large electronic bandgap. Here we present a detailed theoretical investigation of the atomic and electronic structure of few-layer black phosphorus (BP) to predict its electrical and optical properties. This system has a direct bandgap, tunable from 1.51 eV for a monolayer to 0.59 eV for a five-layer sample. We predict that the mobilities are hole-dominated, rather high and highly anisotropic. The monolayer is exceptional in having an extremely high hole mobility (of order 10,000 cm(2) V(-1) s(-1)) and anomalous elastic properties which reverse the anisotropy. Light absorption spectra indicate linear dichroism between perpendicular in-plane directions, which allows optical determination of the crystalline orientation and optical activation of the anisotropic transport properties. These results make few-layer BP a promising candidate for future electronics.

  11. Quasiparticle scattering off phase boundaries in epitaxial graphene.

    PubMed

    Mahmood, A; Mallet, P; Veuillen, J-Y

    2012-02-10

    We investigate the electronic structure of terraces of single layer graphene (SLG) by scanning tunnelling microscopy (STM) on samples grown by thermal decomposition of 6H-SiC(0001) crystals in ultra-high vacuum. We focus on the perturbations of the local density of states (LDOS) in the vicinity of edges of SLG terraces. Armchair edges are found to favour intervalley quasiparticle scattering, leading to the (√3 x √3)R30° LDOS superstructure already reported for graphite edges and more recently for SLG on SiC(0001). Using the Fourier transform of LDOS images, we demonstrate that the intrinsic doping of SLG is responsible for a LDOS pattern at the Fermi energy which is more complex than for neutral graphene or graphite, since it combines local (√3 x √3)R30° superstructure and long range beating modulation. Although these features have already been reported by Yang et al (2010 Nano Lett. 10 943-7) we propose here an alternative interpretation based on simple arguments classically used to describe standing wave patterns in standard two-dimensional systems. Finally, we discuss the absence of intervalley scattering off other typical boundaries: zig-zag edges and SLG/bilayer graphene junctions.

  12. Rapid epitaxy-free graphene synthesis on silicidated polycrystalline platinum

    PubMed Central

    Babenko, Vitaliy; Murdock, Adrian T.; Koós, Antal A.; Britton, Jude; Crossley, Alison; Holdway, Philip; Moffat, Jonathan; Huang, Jian; Alexander-Webber, Jack A.; Nicholas, Robin J.; Grobert, Nicole

    2015-01-01

    Large-area synthesis of high-quality graphene by chemical vapour deposition on metallic substrates requires polishing or substrate grain enlargement followed by a lengthy growth period. Here we demonstrate a novel substrate processing method for facile synthesis of mm-sized, single-crystal graphene by coating polycrystalline platinum foils with a silicon-containing film. The film reacts with platinum on heating, resulting in the formation of a liquid platinum silicide layer that screens the platinum lattice and fills topographic defects. This reduces the dependence on the surface properties of the catalytic substrate, improving the crystallinity, uniformity and size of graphene domains. At elevated temperatures growth rates of more than an order of magnitude higher (120 μm min−1) than typically reported are achieved, allowing savings in costs for consumable materials, energy and time. This generic technique paves the way for using a whole new range of eutectic substrates for the large-area synthesis of 2D materials. PMID:26175062

  13. Incorporating isolated molybdenum (Mo) atoms into Bilayer Epitaxial Graphene on 4H-SiC(0001)

    NASA Astrophysics Data System (ADS)

    Huang, Han; Wan, Wen; Li, Hui; Wong, Swee Liang; Lv, Lu; Gao, Yongli; Wee, Andrew T. S.

    2014-03-01

    The atomic structures and electronic properties of isolated Mo atoms in bilayer epitaxial graphene (BLEG) on 4H-SiC(0001) are investigated by low temperature scanning tunneling microscopy (LT-STM). LT-STM results reveal that isolated Mo dopants prefer to substitute C atoms at α-sites, and preferentially locate between the graphene bilayers. First-principles calculations confirm that the embedding of single Mo dopants within BLEG is energetically favorable as compared to monolayer graphene. The calculated bandstructures show that Mo-doped BLEG is n-doped, and each Mo atom introduces a local magnetic moment of 1.81 μB. Our findings demonstrate a simple and stable method to incorporate single transition metal dopants into the graphene lattice to tune its electronic and magnetic properties for possible use in graphene spin devices. NRF-CRP (Singapore) grants R-143-000-360-281and R-144-000-295-281. ``Shenghua Professorship'' startup funding from CSU and the support from the NSF of China (Grant No.11304398).

  14. Epitaxial growth of graphene on 6H-silicon carbide substrate by simulated annealing method.

    PubMed

    Yoon, T L; Lim, T L; Min, T K; Hung, S H; Jakse, N; Lai, S K

    2013-11-28

    We grew graphene epitaxially on 6H-SiC(0001) substrate by the simulated annealing method. The mechanisms that govern the growth process were investigated by testing two empirical potentials, namely, the widely used Tersoff potential [J. Tersoff, Phys. Rev. B 39, 5566 (1989)] and its more refined version published years later by Erhart and Albe [Phys. Rev. B 71, 035211 (2005)]. Upon contrasting the results obtained by these two potentials, we found that the potential proposed by Erhart and Albe is generally more physical and realistic, since the annealing temperature at which the graphene structure just coming into view at approximately 1200 K is unambiguously predicted and close to the experimentally observed pit formation at 1298 K within which the graphene nucleates. We evaluated the reasonableness of our layers of graphene by calculating carbon-carbon (i) average bond-length, (ii) binding energy, and (iii) pair correlation function. Also, we compared with related experiments the various distance of separation parameters between the overlaid layers of graphene and substrate surface. PMID:24289364

  15. Simulating structural transitions with kinetic Monte Carlo: The case of epitaxial graphene on SiC

    NASA Astrophysics Data System (ADS)

    Deretzis, I.; La Magna, A.

    2016-03-01

    We have developed a kinetic Monte Carlo numerical scheme, specifically suited to simulate structural transitions in crystalline materials, and implemented it for the case of epitaxial graphene on SiC. In this process, surface Si atoms selectively sublimate, while the residual C atoms rearrange from a position occupied in the SiC hexagonal lattice to the graphene honeycomb structure, modifying their hybridization (from s p3 to s p2 ) and bond partners (from Si-C to C-C). The model is based on the assumption that the Monte Carlo particles follow the evolution of their reference crystal until they experience a thermally activated reversible transition to another crystal structure. We demonstrate that, in a formulation based on three parallel lattices, the method is able to recover the complex evolution steps of epitaxial graphene on SiC. Moreover, the simulation results are in noteworthy agreement with the overall experimental scenario, both when varying the structural properties of the material (e.g., the initial surface configuration or polarity) as well as the process conditions (e.g., the temperature and pressure).

  16. Rotationally Commensurate Growth of MoS2 on Epitaxial Graphene.

    PubMed

    Liu, Xiaolong; Balla, Itamar; Bergeron, Hadallia; Campbell, Gavin P; Bedzyk, Michael J; Hersam, Mark C

    2016-01-26

    Atomically thin MoS2/graphene heterostructures are promising candidates for nanoelectronic and optoelectronic technologies. Among different graphene substrates, epitaxial graphene (EG) on SiC provides several potential advantages for such heterostructures, including high electronic quality, tunable substrate coupling, wafer-scale processability, and crystalline ordering that can template commensurate growth. Exploiting these attributes, we demonstrate here the thickness-controlled van der Waals epitaxial growth of MoS2 on EG via chemical vapor deposition, giving rise to transfer-free synthesis of a two-dimensional heterostructure with registry between its constituent materials. The rotational commensurability observed between the MoS2 and EG is driven by the energetically favorable alignment of their respective lattices and results in nearly strain-free MoS2, as evidenced by synchrotron X-ray scattering and atomic-resolution scanning tunneling microscopy (STM). The electronic nature of the MoS2/EG heterostructure is elucidated with STM and scanning tunneling spectroscopy, which reveals bias-dependent apparent thickness, band bending, and a reduced band gap of ∼0.4 eV at the monolayer MoS2 edges. PMID:26565112

  17. Raman scattering of few-layers MoTe2

    NASA Astrophysics Data System (ADS)

    Grzeszczyk, M.; Gołasa, K.; Zinkiewicz, M.; Nogajewski, K.; Molas, M. R.; Potemski, M.; Wysmołek, A.; Babiński, A.

    2016-06-01

    We report on room-temperature Raman scattering measurements in few-layer crystals of exfoliated molybdenum ditelluride (MoTe2) performed with the use of 632.8 nm (1.96 eV) laser light excitation. In agreement with a recent study reported by Froehlicher et al (2015 Nano Lett. 15 6481) we observe a complex structure of the out-of-plane vibrational modes ({{{A}}}1{{g}}{/{{A}}}1\\prime ), which can be explained in terms of interlayer interactions between single atomic planes of MoTe2. In the case of low-energy shear and breathing modes of rigid interlayer vibrations, it is shown that their energy evolution with the number of layers can be well reproduced within a linear chain model with only the nearest neighbor interaction taken into account. Based on this model the corresponding in-plane and out-of-plane force constants are determined. We also show that the Raman scattering in MoTe2 measured using 514.5 nm (2.41 eV) laser light excitation results in much simpler spectra. We argue that the rich structure of the out-of-plane vibrational modes observed in Raman scattering spectra excited with the use of 632.8 nm laser light results from its resonance with the electronic transition at the M point of the MoTe2 first Brillouin zone.

  18. Colossal Ultraviolet Photoresponsivity of Few-Layer Black Phosphorus.

    PubMed

    Wu, Jing; Koon, Gavin Kok Wai; Xiang, Du; Han, Cheng; Toh, Chee Tat; Kulkarni, Eeshan S; Verzhbitskiy, Ivan; Carvalho, Alexandra; Rodin, Aleksandr S; Koenig, Steven P; Eda, Goki; Chen, Wei; Neto, A H Castro; Özyilmaz, Barbaros

    2015-08-25

    Black phosphorus has an orthorhombic layered structure with a layer-dependent direct band gap from monolayer to bulk, making this material an emerging material for photodetection. Inspired by this and the recent excitement over this material, we studied the optoelectronics characteristics of high-quality, few-layer black phosphorus-based photodetectors over a wide spectrum ranging from near-ultraviolet (UV) to near-infrared (NIR). It is demonstrated for the first time that black phosphorus can be configured as an excellent UV photodetector with a specific detectivity ∼3 × 10(13) Jones. More critically, we found that the UV photoresponsivity can be significantly enhanced to ∼9 × 10(4) A W(-1) by applying a source-drain bias (VSD) of 3 V, which is the highest ever measured in any 2D material and 10(7) times higher than the previously reported value for black phosphorus. We attribute such a colossal UV photoresponsivity to the resonant-interband transition between two specially nested valence and conduction bands. These nested bands provide an unusually high density of states for highly efficient UV absorption due to the singularity of their nature.

  19. Charge trap memory based on few-layer black phosphorus.

    PubMed

    Feng, Qi; Yan, Faguang; Luo, Wengang; Wang, Kaiyou

    2016-02-01

    Atomically thin layered two-dimensional materials, including transition-metal dichalcogenide (TMDC) and black phosphorus (BP), have been receiving much attention, because of their promising physical properties and potential applications in flexible and transparent electronic devices. Here, for the first time we show nonvolatile charge-trap memory devices, based on field-effect transistors with large hysteresis, consisting of a few-layer black phosphorus channel and a three dimensional (3D) Al2O3/HfO2/Al2O3 charge-trap gate stack. An unprecedented memory window exceeding 12 V is observed, due to the extraordinary trapping ability of the high-k HfO2. The device shows a high endurance of over 120 cycles and a stable retention of ∼30% charge loss after 10 years, even lower than the reported MoS2 flash memory. The high program/erase current ratio, large memory window, stable retention and high on/off current ratio, provide a promising route towards flexible and transparent memory devices utilising atomically thin two-dimensional materials. The combination of 2D materials with traditional high-k charge-trap gate stacks opens up an exciting field of nonvolatile memory devices.

  20. Charge trap memory based on few-layer black phosphorus

    NASA Astrophysics Data System (ADS)

    Feng, Qi; Yan, Faguang; Luo, Wengang; Wang, Kaiyou

    2016-01-01

    Atomically thin layered two-dimensional materials, including transition-metal dichalcogenide (TMDC) and black phosphorus (BP), have been receiving much attention, because of their promising physical properties and potential applications in flexible and transparent electronic devices. Here, for the first time we show nonvolatile charge-trap memory devices, based on field-effect transistors with large hysteresis, consisting of a few-layer black phosphorus channel and a three dimensional (3D) Al2O3/HfO2/Al2O3 charge-trap gate stack. An unprecedented memory window exceeding 12 V is observed, due to the extraordinary trapping ability of the high-k HfO2. The device shows a high endurance of over 120 cycles and a stable retention of ~30% charge loss after 10 years, even lower than the reported MoS2 flash memory. The high program/erase current ratio, large memory window, stable retention and high on/off current ratio, provide a promising route towards flexible and transparent memory devices utilising atomically thin two-dimensional materials. The combination of 2D materials with traditional high-k charge-trap gate stacks opens up an exciting field of nonvolatile memory devices.

  1. Environmental instability of few-layer black phosphorus

    NASA Astrophysics Data System (ADS)

    Island, Joshua O.; Steele, Gary A.; van der Zant, Herre S. J.; Castellanos-Gomez, Andres

    2015-03-01

    We study the environmental instability of mechanically exfoliated few-layer black phosphorus (BP). From continuous measurements of flake topography over several days, we observe an increase of over 200% in volume due to the condensation of moisture from air. We find that long term exposure to ambient conditions results in a layer-by-layer etching process of BP flakes. Interestingly, flakes can be etched down to single layer (phosphorene) thicknesses. BP's strong affinity for water greatly modifies the performance of fabricated field-effect transistors (FETs) measured in ambient conditions. Upon exposure to air, we differentiate between two timescales for changes in BP FET transfer characteristics: a short timescale (minutes) in which a shift in the threshold voltage occurs due to physisorbed oxygen and nitrogen, and a long timescale (hours) in which strong p-type doping occurs from water absorption. Continuous measurements of BP FETs in air reveal eventual degradation and break-down of the channel material after several days due to the layer-by-layer etching process.

  2. Role of silicon dangling bonds in the electronic properties of epitaxial graphene on silicon carbide.

    PubMed

    Ridene, Mohamed; Kha, Calvin S; Flipse, Cees F J

    2016-03-29

    In this paper, we study the electronic properties of epitaxial graphene (EG) on silicon carbide by means of ab initio calculations based on the local spin density approximation + U method taking into account the Coulomb interaction between Si localized electrons. We show that this interaction is not completely suppressed but is screened by carbon layers grown on-top of silicon carbide. This finding leads to a good qualitative understanding of the experimental results reported on EG on silicon carbide. Our results highlight the presence of the Si localized states and might explain the anomalous Hanle curve and the high values of spin relaxation time in EG.

  3. SU(4) symmetry breaking revealed by magneto-optical spectroscopy in epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Tan, Liang Z.; Orlita, Milan; Potemski, Marek; Palmer, James; Berger, Claire; de Heer, Walter A.; Louie, Steven G.; Martinez, Gérard

    2015-06-01

    Refined infrared magnetotransmission experiments have been performed in magnetic fields B up to 35 T on a series of multilayer epitaxial graphene samples. Following the main optical transition involving the n =0 Landau level (LL), we observe a new absorption transition increasing in intensity with magnetic fields B ≥26 T. Our analysis shows that this is a signature of the breaking of the SU(4) symmetry of the n =0 LL. Using a quantitative model, we show that the only symmetry-breaking scheme consistent with our experiments is a charge density wave (CDW).

  4. Role of silicon dangling bonds in the electronic properties of epitaxial graphene on silicon carbide.

    PubMed

    Ridene, Mohamed; Kha, Calvin S; Flipse, Cees F J

    2016-03-29

    In this paper, we study the electronic properties of epitaxial graphene (EG) on silicon carbide by means of ab initio calculations based on the local spin density approximation + U method taking into account the Coulomb interaction between Si localized electrons. We show that this interaction is not completely suppressed but is screened by carbon layers grown on-top of silicon carbide. This finding leads to a good qualitative understanding of the experimental results reported on EG on silicon carbide. Our results highlight the presence of the Si localized states and might explain the anomalous Hanle curve and the high values of spin relaxation time in EG. PMID:26891244

  5. Variable range hopping and nonlinear transport in monolayer epitaxial graphene grown on SiC

    NASA Astrophysics Data System (ADS)

    Liu, Chieh-I.; Wu, Bi-Yi; Chuang, Chiashain; Lee, Ya-Chi; Ho, Yi-Ju; Yang, Yanfei; Elmquist, Randolph E.; Lo, Shun-Tsung; Liang, Chi-Te

    2016-10-01

    We report experimental results on variable range hopping (VRH) and nonlinear transport in monolayer epitaxial graphene. In the linear regime in which the conductance is independent of voltage, the resistance curve derivative analysis method can be used to unequivocally determine whether Mott VRH or Efros-Shklovskii VRH is the dominant transport mechanism in our devices. In the nonlinear regime in which the conductance shows a strong dependence on voltage, we find that our experimental results can be successfully described by existing theoretical models. We suggest that the observed vastly different exponents in the threshold voltage-temperature dependence require further experimental and theoretical studies.

  6. High island densities and long range repulsive interactions: Fe on epitaxial graphene.

    PubMed

    Binz, S M; Hupalo, M; Liu, Xiaojie; Wang, C Z; Lu, Wen-Cai; Thiel, P A; Ho, K M; Conrad, E H; Tringides, M C

    2012-07-13

    The understanding of metal nucleation on graphene is essential for promising future applications, especially of magnetic metals which can be used in spintronics or computer storage media. A common method to study the grown morphology is to measure the nucleated island density n as a function of growth parameters. Surprisingly, the growth of Fe on graphene is found to be unusual because it does not follow classical nucleation: n is unexpectedtly high, it increases continuously with the deposited amount θ and shows no temperature dependence. These unusual results indicate the presence of long range repulsive interactions. Kinetic Monte Carlo simulations and density functional theory calculations support this conclusion. In addition to answering an outstanding question in epitaxial growth, i.e., to find systems where long range interactions are present, the high density of magnetic islands, tunable with θ, is of interest for nanomagnetism applications.

  7. Nickel enhanced graphene growth directly on dielectric substrates by molecular beam epitaxy

    NASA Astrophysics Data System (ADS)

    Wofford, Joseph M.; Speck, Florian; Seyller, Thomas; Lopes, Joao Marcelo J.; Riechert, Henning

    2016-07-01

    The efficacy of Ni as a surfactant to improve the crystalline quality of graphene grown directly on dielectric Al2O3(0001) substrates by molecular beam epitaxy is examined. Simultaneously exposing the substrate to a Ni flux throughout C deposition at 950 °C led to improved charge carrier mobility and a Raman spectrum indicating less structural disorder in the resulting nanocrystalline graphene film. X-ray photoelectron spectroscopy confirmed that no residual Ni could be detected in the film and showed a decrease in the intensity of the defect-related component of the C1s level. Similar improvements were not observed when a lower substrate temperature (850 °C) was used. A close examination of the Raman spectra suggests that Ni reduces the concentration of lattice vacancies in the film, possibly by catalytically assisting adatom incorporation.

  8. Large-scale epitaxial growth kinetics of graphene: A kinetic Monte Carlo study

    SciTech Connect

    Jiang, Huijun; Hou, Zhonghuai

    2015-08-28

    Epitaxial growth via chemical vapor deposition is considered to be the most promising way towards synthesizing large area graphene with high quality. However, it remains a big theoretical challenge to reveal growth kinetics with atomically energetic and large-scale spatial information included. Here, we propose a minimal kinetic Monte Carlo model to address such an issue on an active catalyst surface with graphene/substrate lattice mismatch, which facilitates us to perform large scale simulations of the growth kinetics over two dimensional surface with growth fronts of complex shapes. A geometry-determined large-scale growth mechanism is revealed, where the rate-dominating event is found to be C{sub 1}-attachment for concave growth-front segments and C{sub 5}-attachment for others. This growth mechanism leads to an interesting time-resolved growth behavior which is well consistent with that observed in a recent scanning tunneling microscopy experiment.

  9. Influence of defects in SiC (0001) on epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Guo, Yu; Guo, Li-Wei; Lu, Wei; Huang, Jiao; Jia, Yu-Ping; Sun, Wei; Li, Zhi-Lin; Wang, Yi-Fei

    2014-08-01

    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.

  10. Moiré induced organization of size-selected Pt clusters soft landed on epitaxial graphene

    PubMed Central

    Linas, Sébastien; Jean, Fabien; Zhou, Tao; Albin, Clément; Renaud, Gilles; Bardotti, Laurent; Tournus, Florent

    2015-01-01

    Two-dimensional hexagonal arrays of Pt nanoparticles (1.5 nm diameter) have been obtained by deposition of preformed and size selected Pt nanoparticles on graphene. This original self-organization is induced, at room temperature, by the 2D periodic undulation (the moiré pattern) of graphene epitaxially grown on the Ir(111) surface. By means of complementary techniques (scanning tunneling microscopy, grazing incidence X ray scattering), the Pt clusters shapes and organization are characterized and the structural evolution during annealing is investigated. The soft-landed clusters remain quasi-spherical and a large proportion appears to be pinned on specific moiré sites. The quantitative determination of the proportion of organized clusters reveals that the obtained hexagonal array of the almost spherical nanoparticles is stable up to 650 K, which is an indication of a strong cluster-surface interaction. PMID:26278787

  11. Flexible GaN Light-Emitting Diodes Using GaN Microdisks Epitaxial Laterally Overgrown on Graphene Dots.

    PubMed

    Chung, Kunook; Yoo, Hyobin; Hyun, Jerome K; Oh, Hongseok; Tchoe, Youngbin; Lee, Keundong; Baek, Hyeonjun; Kim, Miyoung; Yi, Gyu-Chul

    2016-09-01

    The epitaxial lateral overgrowth (ELOG) of GaN microdisks on graphene microdots and the fabrication of flexible light-emitting diodes (LEDs) using these microdisks is reported. An ELOG technique with only patterned graphene microdots is used, without any growth mask. The discrete micro-LED arrays are transferred onto Cu foil by a simple lift-off technique, which works reliably under various bending conditions. PMID:27346527

  12. Direct experimental evidence for the reversal of carrier type upon hydrogen intercalation in epitaxial graphene/SiC(0001)

    SciTech Connect

    Rajput, S. Li, Y. Y.; Li, L.

    2014-01-27

    Raman spectroscopy and scanning tunneling microscopy/spectroscopy measurements are performed to determine the atomic structure and electronic properties of H-intercalated graphene/SiC(0001) obtained by annealing the as-grown epitaxial graphene in hydrogen atmosphere. While the as-grown graphene is found to be n-type with the Dirac point (E{sub D}) at 450 and 350 meV below Fermi level for the 1st and 2nd layer, the H-intercalated graphene is p-type with E{sub D} at 320 and 200 meV above. In addition, ripples are observed in the now quasi-free standing graphene decoupled from the SiC substrate. This causes fluctuations in the Dirac point that directly follow the undulations of the ripples, resulting in electron and hole puddles in the H-intercalated graphene/SiC(0001)

  13. Anomalous thermomagnetic effects in an epitaxial and irradiated graphene monolayer

    NASA Astrophysics Data System (ADS)

    Zhou, Xingfei; Xu, Yafang; Jin, Guojun

    2015-12-01

    We study valley-dependent anomalous thermomagnetic effects, including the Nernst and Ettingshausen effects, in a graphene monolayer that is subjected to a staggered sublattice potential and off-resonant circularly polarized light. It is found that a topological phase transition in this system can significantly affect the signs of the Nernst conductivity as well as the Ettingshausen thermal conductivity, which provides an alternative method to characterize the phase transition between band and topological insulators. At the topological phase-transition point, pure valley-polarized electric and heat currents are generated. In contrast to traditional thermomagnetism, an anomalous thermomagnetic figure of merit is formulated and used to characterize conversion efficiency. The theoretical approach, including numerical calculations and analytical treatment, can also be used to study the same properties of other graphenelike materials.

  14. Investigation of structural and electronic properties of epitaxial graphene on 3C-SiC(100)/Si(100) substrates.

    PubMed

    Gogneau, Noelle; Ben Gouider Trabelsi, Amira; Silly, Mathieu G; Ridene, Mohamed; Portail, Marc; Michon, Adrien; Oueslati, Mehrezi; Belkhou, Rachid; Sirotti, Fausto; Ouerghi, Abdelkarim

    2014-01-01

    Graphene has been intensively studied in recent years in order to take advantage of its unique properties. Its synthesis on SiC substrates by solid-state graphitization appears a suitable option for graphene-based electronics. However, before developing devices based on epitaxial graphene, it is desirable to understand and finely control the synthesis of material with the most promising properties. To achieve these prerequisites, many studies are being conducted on various SiC substrates. Here, we review 3C-SiC(100) epilayers grown by chemical vapor deposition on Si(100) substrates for producing graphene by solid state graphitization under ultrahigh-vacuum conditions. Based on various characterization techniques, the structural and electrical properties of epitaxial graphene layer grown on 3C-SiC(100)/Si(100) are discussed. We establish that epitaxial graphene presents properties similar to those obtained using hexagonal SiC substrates, with the advantage of being compatible with current Si-processing technology. PMID:25339846

  15. Investigation of structural and electronic properties of epitaxial graphene on 3C–SiC(100)/Si(100) substrates

    PubMed Central

    Gogneau, Noelle; Ben Gouider Trabelsi, Amira; Silly, Mathieu G; Ridene, Mohamed; Portail, Marc; Michon, Adrien; Oueslati, Mehrezi; Belkhou, Rachid; Sirotti, Fausto; Ouerghi, Abdelkarim

    2014-01-01

    Graphene has been intensively studied in recent years in order to take advantage of its unique properties. Its synthesis on SiC substrates by solid-state graphitization appears a suitable option for graphene-based electronics. However, before developing devices based on epitaxial graphene, it is desirable to understand and finely control the synthesis of material with the most promising properties. To achieve these prerequisites, many studies are being conducted on various SiC substrates. Here, we review 3C–SiC(100) epilayers grown by chemical vapor deposition on Si(100) substrates for producing graphene by solid state graphitization under ultrahigh-vacuum conditions. Based on various characterization techniques, the structural and electrical properties of epitaxial graphene layer grown on 3C–SiC(100)/Si(100) are discussed. We establish that epitaxial graphene presents properties similar to those obtained using hexagonal SiC substrates, with the advantage of being compatible with current Si-processing technology. PMID:25339846

  16. Atomic structure of epitaxial graphene sidewall nanoribbons: flat graphene, miniribbons, and the confinement gap.

    PubMed

    Palacio, Irene; Celis, Arlensiú; Nair, Maya N; Gloter, Alexandre; Zobelli, Alberto; Sicot, Muriel; Malterre, Daniel; Nevius, Meredith S; de Heer, Walt A; Berger, Claire; Conrad, Edward H; Taleb-Ibrahimi, Amina; Tejeda, Antonio

    2015-01-14

    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. We show that the nanoribbons consist of a single graphene layer essentially decoupled from the facet surface. The nanoribbons are bordered by 1-2 nm wide bent miniribbons at both the top and bottom edges of the nanoribbons. We establish that nanoscale confinement in the graphene miniribbons is the origin of the local large band gap observed in ARPES. The structural results presented here show how this gap is formed and provide a framework to help understand ballistic transport in sidewall graphene.

  17. In silico carbon molecular beam epitaxial growth of graphene on the h-BN substrate: carbon source effect on van der Waals epitaxy

    NASA Astrophysics Data System (ADS)

    Lee, Jonghoon; Varshney, Vikas; Park, Jeongho; Farmer, Barry L.; Roy, Ajit K.

    2016-05-01

    Against the presumption that hexagonal boron-nitride (h-BN) should provide an ideal substrate for van der Waals (vdW) epitaxy to grow high quality graphene films, carbon molecular beam epitaxy (CMBE) techniques using solid carbon sublimation have reported relatively poor quality of the graphene. In this article, the CMBE growth of graphene on the h-BN substrate is numerically studied in order to identify the effect of the carbon source on the quality of the graphene film. The carbon molecular beam generated by the sublimation of solid carbon source materials such as graphite and glassy carbon is mostly composed of atomic carbon, carbon dimers and carbon trimers. Therefore, the graphene film growth becomes a complex process involving various deposition characteristics of a multitude of carbon entities. Based on the study of surface adsorption and film growth characteristics of these three major carbon entities comprising graphite vapour, we report that carbon trimers convey strong traits of vdW epitaxy prone to high quality graphene growth, while atomic carbon deposition is a surface-reaction limited process accompanied by strong chemisorption. The vdW epitaxial behaviour of carbon trimers is found to be substantial enough to nucleate and develop into graphene like planar films within a nanosecond of high flux growth simulation, while reactive atomic carbons tend to impair the structural integrity of the crystalline h-BN substrate upon deposition to form an amorphous interface between the substrate and the growing carbon film. The content of reactive atomic carbons in the molecular beam is suspected to be the primary cause of low quality graphene reported in the literature. A possible optimization of the molecular beam composition towards the synthesis of better quality graphene films is suggested.Against the presumption that hexagonal boron-nitride (h-BN) should provide an ideal substrate for van der Waals (vdW) epitaxy to grow high quality graphene films, carbon

  18. In silico carbon molecular beam epitaxial growth of graphene on the h-BN substrate: carbon source effect on van der Waals epitaxy

    NASA Astrophysics Data System (ADS)

    Lee, Jonghoon; Varshney, Vikas; Park, Jeongho; Farmer, Barry L.; Roy, Ajit K.

    2016-05-01

    Against the presumption that hexagonal boron-nitride (h-BN) should provide an ideal substrate for van der Waals (vdW) epitaxy to grow high quality graphene films, carbon molecular beam epitaxy (CMBE) techniques using solid carbon sublimation have reported relatively poor quality of the graphene. In this article, the CMBE growth of graphene on the h-BN substrate is numerically studied in order to identify the effect of the carbon source on the quality of the graphene film. The carbon molecular beam generated by the sublimation of solid carbon source materials such as graphite and glassy carbon is mostly composed of atomic carbon, carbon dimers and carbon trimers. Therefore, the graphene film growth becomes a complex process involving various deposition characteristics of a multitude of carbon entities. Based on the study of surface adsorption and film growth characteristics of these three major carbon entities comprising graphite vapour, we report that carbon trimers convey strong traits of vdW epitaxy prone to high quality graphene growth, while atomic carbon deposition is a surface-reaction limited process accompanied by strong chemisorption. The vdW epitaxial behaviour of carbon trimers is found to be substantial enough to nucleate and develop into graphene like planar films within a nanosecond of high flux growth simulation, while reactive atomic carbons tend to impair the structural integrity of the crystalline h-BN substrate upon deposition to form an amorphous interface between the substrate and the growing carbon film. The content of reactive atomic carbons in the molecular beam is suspected to be the primary cause of low quality graphene reported in the literature. A possible optimization of the molecular beam composition towards the synthesis of better quality graphene films is suggested.Against the presumption that hexagonal boron-nitride (h-BN) should provide an ideal substrate for van der Waals (vdW) epitaxy to grow high quality graphene films, carbon

  19. Infrared cyclotron resonances of Dirac electrons in SiC epitaxial graphene in ultra-high magnetic fields

    SciTech Connect

    Saito, H.; Nakamura, D.; Takeyama, S.; Hibino, H.

    2013-12-04

    To investigate the high magnetic field properties of the Dirac fermion system, we performed magneto-absorption measurements of epitaxially grown graphene at high magnetic field using the single-turn coil (STC) method. We observed the cyclotron resonance absorption corresponding to n = 0 to 1 intraband transitions.

  20. van der Waals epitaxial growth of graphene on sapphire by chemical vapor deposition without a metal catalyst.

    PubMed

    Hwang, Jeonghyun; Kim, Moonkyung; Campbell, Dorr; Alsalman, Hussain A; Kwak, Joon Young; Shivaraman, Shriram; Woll, Arthur R; Singh, Arunima K; Hennig, Richard G; Gorantla, Sandeep; Rümmeli, Mark H; Spencer, Michael G

    2013-01-22

    van der Waals epitaxial growth of graphene on c-plane (0001) sapphire by CVD without a metal catalyst is presented. The effects of CH(4) partial pressure, growth temperature, and H(2)/CH(4) ratio were investigated and growth conditions optimized. The formation of monolayer graphene was shown by Raman spectroscopy, optical transmission, grazing incidence X-ray diffraction (GIXRD), and low voltage transmission electron microscopy (LVTEM). Electrical analysis revealed that a room temperature Hall mobility above 2000 cm(2)/V·s was achieved, and the mobility and carrier type were correlated to growth conditions. Both GIXRD and LVTEM studies confirm a dominant crystal orientation (principally graphene [10-10] || sapphire [11-20]) for about 80-90% of the material concomitant with epitaxial growth. The initial phase of the nucleation and the lateral growth from the nucleation seeds were observed using atomic force microscopy. The initial nuclei density was ~24 μm(-2), and a lateral growth rate of ~82 nm/min was determined. Density functional theory calculations reveal that the binding between graphene and sapphire is dominated by weak dispersion interactions and indicate that the epitaxial relation as observed by GIXRD is due to preferential binding of small molecules on sapphire during early stages of graphene formation. PMID:23244231

  1. Blinking suppression of CdTe quantum dots on epitaxial graphene and the analysis with Marcus electron transfer

    SciTech Connect

    Hirose, Takuya; Tamai, Naoto; Kutsuma, Yasunori; Kurita, Atsusi; Kaneko, Tadaaki

    2014-08-25

    We have prepared epitaxial graphene by a Si sublimation method from 4H-SiC. Single-particle spectroscopy of CdTe quantum dots (QDs) on epitaxial graphene covered with polyvinylpyrrolidone (PVP) or polyethylene glycol (PEG) showed the suppression of luminescence blinking and ∼10 times decreased luminescence intensity as compared with those on a glass. The electronic coupling constant, H{sub 01}, between CdTe QDs and graphene was calculated to be (3.3 ± 0.4) × 10{sup 2 }cm{sup −1} in PVP and (3.7 ± 0.8) × 10{sup 2 }cm{sup −1} in PEG based on Marcus theory of electron transfer and Tang-Marcus model of blinking with statistical distribution.

  2. Blinking suppression of CdTe quantum dots on epitaxial graphene and the analysis with Marcus electron transfer

    NASA Astrophysics Data System (ADS)

    Hirose, Takuya; Kutsuma, Yasunori; Kurita, Atsusi; Kaneko, Tadaaki; Tamai, Naoto

    2014-08-01

    We have prepared epitaxial graphene by a Si sublimation method from 4H-SiC. Single-particle spectroscopy of CdTe quantum dots (QDs) on epitaxial graphene covered with polyvinylpyrrolidone (PVP) or polyethylene glycol (PEG) showed the suppression of luminescence blinking and ˜10 times decreased luminescence intensity as compared with those on a glass. The electronic coupling constant, H01, between CdTe QDs and graphene was calculated to be (3.3 ± 0.4) × 102 cm-1 in PVP and (3.7 ± 0.8) × 102 cm-1 in PEG based on Marcus theory of electron transfer and Tang-Marcus model of blinking with statistical distribution.

  3. CROSS-DISCIPLINARY PHYSICS AND RELATED AREAS OF SCIENCE AND TECHNOLOGY: Epitaxial Growth of Graphene on 6H-SiC (0001) by Thermal Annealing

    NASA Astrophysics Data System (ADS)

    Tang, Jun; Liu, Zhong-Liang; Kang, Chao-Yang; Pan, Hai-Bin; Wei, Shi-Qiang; Xu, Peng-Shou; Gao, Yu-Qiang; Xu, Xian-Gang

    2009-08-01

    An epitaxial graphene (EG) layer is successfully grown on a Si-terminated 6H-SiC (0001) substrate by the method of thermal annealing in an ultrahigh vacuum molecular beam epitaxy chamber. The structure and morphology of the EG sample are characterized by reflection high energy diffraction (RHEED), Raman spectroscopy and atomic force microscopy (AFM). Graphene diffraction streaks can be seen in RHEED. The G and 2D peaks of graphene are clearly observed in the Raman spectrum. The AFM results show that the graphene nominal thickness is about 4-10 layers.

  4. Topological phase transition and quantum spin Hall edge states of antimony few layers

    PubMed Central

    Kim, Sung Hwan; Jin, Kyung-Hwan; Park, Joonbum; Kim, Jun Sung; Jhi, Seung-Hoon; Yeom, Han Woong

    2016-01-01

    While two-dimensional (2D) topological insulators (TI’s) initiated the field of topological materials, only very few materials were discovered to date and the direct access to their quantum spin Hall edge states has been challenging due to material issues. Here, we introduce a new 2D TI material, Sb few layer films. Electronic structures of ultrathin Sb islands grown on Bi2Te2Se are investigated by scanning tunneling microscopy. The maps of local density of states clearly identify robust edge electronic states over the thickness of three bilayers in clear contrast to thinner islands. This indicates that topological edge states emerge through a 2D topological phase transition predicted between three and four bilayer films in recent theory. The non-trivial phase transition and edge states are confirmed for epitaxial films by extensive density-functional-theory calculations. This work provides an important material platform to exploit microscopic aspects of the quantum spin Hall phase and its quantum phase transition. PMID:27624972

  5. One-step Synthesis of Few-layer WS2 by Pulsed Laser Deposition

    NASA Astrophysics Data System (ADS)

    Loh, Tamie A. J.; Chua, Daniel H. C.; Wee, Andrew T. S.

    2015-12-01

    Atomically thin tungsten disulfide (WS2) has attracted much attention in recent years due its indirect-to-direct band gap transition, band gap tunability, and giant spin splitting. However, the fabrication of atomically thin WS2 remains largely underdeveloped in comparison to its structural analogue MoS2. Here we report the direct fabrication of highly crystalline few-layer WS2 on silver substrates by pulse laser deposition at the relatively low temperature of 450 °C. The growth takes places by conventional epitaxy, through the in-situ formation of nearly lattice-matching Ag2S on the silver surface. Intriguingly, it was observed that the resulting film was composed of not only the usual semiconducting 2H-WS2 structure but also the less common metallic 1T-WS2. Modifications of the synthesis parameters allow for control over the crystalline quality, film thickness and crystal phase composition of the resulting WS2 film.

  6. Topological phase transition and quantum spin Hall edge states of antimony few layers

    NASA Astrophysics Data System (ADS)

    Kim, Sung Hwan; Jin, Kyung-Hwan; Park, Joonbum; Kim, Jun Sung; Jhi, Seung-Hoon; Yeom, Han Woong

    2016-09-01

    While two-dimensional (2D) topological insulators (TI’s) initiated the field of topological materials, only very few materials were discovered to date and the direct access to their quantum spin Hall edge states has been challenging due to material issues. Here, we introduce a new 2D TI material, Sb few layer films. Electronic structures of ultrathin Sb islands grown on Bi2Te2Se are investigated by scanning tunneling microscopy. The maps of local density of states clearly identify robust edge electronic states over the thickness of three bilayers in clear contrast to thinner islands. This indicates that topological edge states emerge through a 2D topological phase transition predicted between three and four bilayer films in recent theory. The non-trivial phase transition and edge states are confirmed for epitaxial films by extensive density-functional-theory calculations. This work provides an important material platform to exploit microscopic aspects of the quantum spin Hall phase and its quantum phase transition.

  7. Thickness-Dependent Dielectric Constant of Few-Layer In₂Se₃ Nanoflakes.

    PubMed

    Wu, Di; Pak, Alexander J; Liu, Yingnan; Zhou, Yu; Wu, Xiaoyu; Zhu, Yihan; Lin, Min; Han, Yu; Ren, Yuan; Peng, Hailin; Tsai, Yu-Hao; Hwang, Gyeong S; Lai, Keji

    2015-12-01

    The dielectric constant or relative permittivity (ε(r)) of a dielectric material, which describes how the net electric field in the medium is reduced with respect to the external field, is a parameter of critical importance for charging and screening in electronic devices. Such a fundamental material property is intimately related to not only the polarizability of individual atoms but also the specific atomic arrangement in the crystal lattice. In this Letter, we present both experimental and theoretical investigations on the dielectric constant of few-layer In2Se3 nanoflakes grown on mica substrates by van der Waals epitaxy. A nondestructive microwave impedance microscope is employed to simultaneously quantify the number of layers and local electrical properties. The measured ε(r) increases monotonically as a function of the thickness and saturates to the bulk value at around 6-8 quintuple layers. The same trend of layer-dependent dielectric constant is also revealed by first-principles calculations. Our results of the dielectric response, being ubiquitously applicable to layered 2D semiconductors, are expected to be significant for this vibrant research field.

  8. Vertically oriented few-layered HfS2 nanosheets: growth mechanism and optical properties

    NASA Astrophysics Data System (ADS)

    Zheng, Binjie; Chen, Yuanfu; Wang, Zegao; Qi, Fei; Huang, Zhishuo; Hao, Xin; Li, Pingjian; Zhang, Wanli; Li, Yanrong

    2016-09-01

    For the first time, large-area, vertically oriented few-layered hafnium disulfide (V-{{{HfS}}}2) nanosheets have been grown by chemical vapor deposition. The individual {{{HfS}}}2 nanosheets are well [001] oriented, with highly crystalline quality. Far different from conventional van der Waals epitaxial growth mechanism for two-dimensional transition metal dichalcogenides, a novel dangling-bond-assisted self-seeding growth mechanism is proposed to describe the growth of V-{{{HfS}}}2 nanosheets: difficult migration of {{{HfS}}}2 adatoms on substrate surface results in {{{HfS}}}2 seeds growing perpendicularly to the substrate; V-{{{HfS}}}2 nanosheets inherit the growth direction of {{{HfS}}}2 seeds; V-{{{HfS}}}2 nanosheets further expand in the in-plane direction with time evolution. Moreover, the V-{{{HfS}}}2 nanosheets show strong and broadened photons absorption from near infrared to ultraviolet; the V-{{{HfS}}}2-based photodetector exhibits an ultrafast photoresponse time of 24 ms, and a high photosensitivity ca. 103 for 405 nm laser.

  9. Topological phase transition and quantum spin Hall edge states of antimony few layers.

    PubMed

    Kim, Sung Hwan; Jin, Kyung-Hwan; Park, Joonbum; Kim, Jun Sung; Jhi, Seung-Hoon; Yeom, Han Woong

    2016-01-01

    While two-dimensional (2D) topological insulators (TI's) initiated the field of topological materials, only very few materials were discovered to date and the direct access to their quantum spin Hall edge states has been challenging due to material issues. Here, we introduce a new 2D TI material, Sb few layer films. Electronic structures of ultrathin Sb islands grown on Bi2Te2Se are investigated by scanning tunneling microscopy. The maps of local density of states clearly identify robust edge electronic states over the thickness of three bilayers in clear contrast to thinner islands. This indicates that topological edge states emerge through a 2D topological phase transition predicted between three and four bilayer films in recent theory. The non-trivial phase transition and edge states are confirmed for epitaxial films by extensive density-functional-theory calculations. This work provides an important material platform to exploit microscopic aspects of the quantum spin Hall phase and its quantum phase transition. PMID:27624972

  10. One-step Synthesis of Few-layer WS2 by Pulsed Laser Deposition

    PubMed Central

    Loh, Tamie A. J.; Chua, Daniel H. C.; Wee, Andrew T. S.

    2015-01-01

    Atomically thin tungsten disulfide (WS2) has attracted much attention in recent years due its indirect-to-direct band gap transition, band gap tunability, and giant spin splitting. However, the fabrication of atomically thin WS2 remains largely underdeveloped in comparison to its structural analogue MoS2. Here we report the direct fabrication of highly crystalline few-layer WS2 on silver substrates by pulse laser deposition at the relatively low temperature of 450 °C. The growth takes places by conventional epitaxy, through the in-situ formation of nearly lattice-matching Ag2S on the silver surface. Intriguingly, it was observed that the resulting film was composed of not only the usual semiconducting 2H-WS2 structure but also the less common metallic 1T-WS2. Modifications of the synthesis parameters allow for control over the crystalline quality, film thickness and crystal phase composition of the resulting WS2 film. PMID:26657172

  11. Vibrational spectra of nanowires measured using laser doppler vibrometry and STM studies of epitaxial graphene : an LDRD fellowship report.

    SciTech Connect

    Biedermann, Laura Butler

    2009-09-01

    , their vibration spectra was more extensively studied. The thermal vibration spectra of Ag{sub 2}Ga nanoneedles was measured under both ambient and low-vacuum conditions. The operational deflection shapes of the vibrating Ag{sub 2}Ga nanoneedles was also measured, allowing confirmation of the eigenmodes of vibration. The modulus of the crystalline nanoneedles was 84.3 {+-} 1.0 GPa. Gas damping is the dominate mechanism of energy loss for nanowires oscillating under ambient conditions. The measured quality factors, Q, of oscillation are in line with theoretical predictions of air damping in the free molecular gas damping regime. In the free molecular regime, Q{sub gas} is linearly proportional to the density and diameter of the nanowire and inversely proportional to the air pressure. Since the density of the Ag{sub 2}Ga nanoneedles is three times that of the MWNTs, the Ag{sub 2}Ga nanoneedles have greater Q at atmospheric pressures. Our initial measurements of Q for Ag{sub 2}Ga nanoneedles in low-vacuum (10 Torr) suggest that the intrinsic Q of these nanoneedles may be on the order of 1000. The epitaxial carbon that grows after heating (000{bar 1}) silicon carbide (SiC) to high temperatures (1450-1600) in vacuum was also studied. At these high temperatures, the surface Si atoms sublime and the remaining C atoms reconstruct to form graphene. X-ray photoelectron spectroscopy (XPS) and scanning tunneling microscopy (STM) were used to characterize the quality of the few-layer graphene (FLG) surface. The XPS studies were useful in confirming the graphitic composition and measuring the thickness of the FLG samples. STM studies revealed a wide variety of nanometer-scale features that include sharp carbon-rich ridges, moire superlattices, one-dimensional line defects, and grain boundaries. By imaging these features with atomic scale resolution, considerable insight into the growth mechanisms of FLG on the carbon-face of SiC is obtained.

  12. Direct growth of single- and few-layer MoS2 on h-BN by CVD method

    NASA Astrophysics Data System (ADS)

    Yan, Aiming; Velasco, Jairo, Jr.; Kahn, Salman; Watanabe, Kenji; Taniguchi, Takashi; Wang, Feng; Crommie, Michael; Zettl, Alex

    As a promising candidate for the next-generation electronics, large-scale single- and few-layer molybdenum disulfide (MoS2) grown by CVD method is an important advancement towards technological implementation of this material. However, the choice of substrate can significantly affect the performance of MoS2 based devices. An attractive insulating substrate or mate for MoS2 (and related materials such as graphene) is hexagonal boron nitride (h-BN). Stacked heterostructures of MoS2 and h-BN have been produced by manual transfer methods, but a more efficient and scalable assembly method is needed. Here we demonstrate the direct growth of single- and few-layer MoS2 on h-BN by chemical vapor deposition (CVD) method. The growth mechanisms for single- and few-layer samples are found to be distinct, and for single-layer samples low relative rotation angles (<5°) between the MoS2 and h-BN lattices prevail. In addition, MoS2 directly grown on h-BN maintains its intrinsic 1.89 eV bandgap. Our CVD synthesis method presents a viable path towards high-quality MoS2 based field effect transistors in a controllable and scalable fashion. Acknowledgement: the U.S. Department of Energy under Contract DE-AC02-05CH11231; NSF Grant DMR-1206512.

  13. Large Frequency Change with Thickness in Interlayer Breathing Mode--Significant Interlayer Interactions in Few Layer Black Phosphorus.

    PubMed

    Luo, Xin; Lu, Xin; Koon, Gavin Kok Wai; Castro Neto, Antonio H; Özyilmaz, Barbaros; Xiong, Qihua; Quek, Su Ying

    2015-06-10

    Bulk black phosphorus (BP) consists of puckered layers of phosphorus atoms. Few-layer BP, obtained from bulk BP by exfoliation, is an emerging candidate as a channel material in post-silicon electronics. A deep understanding of its physical properties and its full range of applications are still being uncovered. In this paper, we present a theoretical and experimental investigation of phonon properties in few-layer BP, focusing on the low-frequency regime corresponding to interlayer vibrational modes. We show that the interlayer breathing mode A(3)g shows a large redshift with increasing thickness; the experimental and theoretical results agree well. This thickness dependence is two times larger than that in the chalcogenide materials, such as few-layer MoS2 and WSe2, because of the significantly larger interlayer force constant and smaller atomic mass in BP. The derived interlayer out-of-plane force constant is about 50% larger than that of graphene and MoS2. We show that this large interlayer force constant arises from the sizable covalent interaction between phosphorus atoms in adjacent layers and that interlayer interactions are not merely of the weak van der Waals type. These significant interlayer interactions are consistent with the known surface reactivity of BP and have been shown to be important for electric-field induced formation of Dirac cones in thin film BP.

  14. Large Frequency Change with Thickness in Interlayer Breathing Mode—Significant Interlayer Interactions in Few Layer Black Phosphorus

    NASA Astrophysics Data System (ADS)

    Luo, Xin; Lu, Xin; Koon, Gavin Kok Wai; Castro Neto, Antonio H.; Özyilmaz, Barbaros; Xiong, Qihua; Quek, Su Ying

    2015-06-01

    Bulk black phosphorus (BP) consists of puckered layers of phosphorus atoms. Few-layer BP, obtained from bulk BP by exfoliation, is an emerging candidate as a channel material in post-silicon electronics. A deep understanding of its physical properties and its full range of applications are still being uncovered. In this paper, we present a theoretical and experimental investigation of phonon properties in few-layer BP, focusing on the low-frequency regime corresponding to interlayer vibrational modes. We show that the interlayer breathing mode A3g shows a large redshift with increasing thickness; the experimental and theoretical results agreeing well. This thickness dependence is two times larger than that in the chalcogenide materials such as few-layer MoS2 and WSe2, because of the significantly larger interlayer force constant and smaller atomic mass in BP. The derived interlayer out-of-plane force constant is about 50% larger than that in graphene and MoS2. We show that this large interlayer force constant arises from the sizable covalent interaction between phosphorus atoms in adjacent layers, and that interlayer interactions are not merely of the weak van der Waals type. These significant interlayer interactions are consistent with the known surface reactivity of BP, and have been shown to be important for electric-field induced formation of Dirac cones in thin film BP.

  15. Direct growth of hexagonal boron nitride/graphene heterostructures on cobalt foil substrates by plasma-assisted molecular beam epitaxy

    NASA Astrophysics Data System (ADS)

    Xu, Zhongguang; Khanaki, Alireza; Tian, Hao; Zheng, Renjing; Suja, Mohammad; Zheng, Jian-Guo; Liu, Jianlin

    2016-07-01

    Graphene/hexagonal boron nitride (G/h-BN) heterostructures have attracted a great deal of attention because of their exceptional properties and wide variety of potential applications in nanoelectronics. However, direct growth of large-area, high-quality, and stacked structures in a controllable and scalable way remains challenging. In this work, we demonstrate the synthesis of h-BN/graphene (h-BN/G) heterostructures on cobalt (Co) foil by sequential deposition of graphene and h-BN layers using plasma-assisted molecular beam epitaxy. It is found that the coverage of h-BN layers can be readily controlled on the epitaxial graphene by growth time. Large-area, uniform-quality, and multi-layer h-BN films on thin graphite layers were achieved. Based on an h-BN (5-6 nm)/G (26-27 nm) heterostructure, capacitor devices with Co(foil)/G/h-BN/Co(contact) configuration were fabricated to evaluate the dielectric properties of h-BN. The measured breakdown electric field showed a high value of ˜2.5-3.2 MV/cm. Both I-V and C-V characteristics indicate that the epitaxial h-BN film has good insulating characteristics.

  16. Evidence for Flat Bands near the Fermi Level in Epitaxial Rhombohedral Multilayer Graphene.

    PubMed

    Pierucci, Debora; Sediri, Haikel; Hajlaoui, Mahdi; Girard, Jean-Christophe; Brumme, Thomas; Calandra, Matteo; Velez-Fort, Emilio; Patriarche, Gilles; Silly, Mathieu G; Ferro, Gabriel; Soulière, Véronique; Marangolo, Massimiliano; Sirotti, Fausto; Mauri, Francesco; Ouerghi, Abdelkarim

    2015-05-26

    The stacking order of multilayer graphene has a profound influence on its electronic properties. In particular, it has been predicted that a rhombohedral stacking sequence displays a very flat conducting surface state: the longer the sequence, the flatter the band. In such a flat band, the role of electron-electron correlation is enhanced, possibly resulting in high Tc superconductivity, magnetic order, or charge density wave order. Here we demonstrate that rhombohedral multilayers are easily obtained by epitaxial growth on 3C-SiC(111) on a 2° off-axis 6H-SiC(0001). The resulting samples contain rhombohedral sequences of five layers on 70% of the surface. We confirm the presence of the flat band at the Fermi level by scanning tunneling spectroscopy and angle-resolved photoemission spectroscopy, in close agreement with the predictions of density functional theory calculations. PMID:25893537

  17. Evidence for Flat Bands near the Fermi Level in Epitaxial Rhombohedral Multilayer Graphene.

    PubMed

    Pierucci, Debora; Sediri, Haikel; Hajlaoui, Mahdi; Girard, Jean-Christophe; Brumme, Thomas; Calandra, Matteo; Velez-Fort, Emilio; Patriarche, Gilles; Silly, Mathieu G; Ferro, Gabriel; Soulière, Véronique; Marangolo, Massimiliano; Sirotti, Fausto; Mauri, Francesco; Ouerghi, Abdelkarim

    2015-05-26

    The stacking order of multilayer graphene has a profound influence on its electronic properties. In particular, it has been predicted that a rhombohedral stacking sequence displays a very flat conducting surface state: the longer the sequence, the flatter the band. In such a flat band, the role of electron-electron correlation is enhanced, possibly resulting in high Tc superconductivity, magnetic order, or charge density wave order. Here we demonstrate that rhombohedral multilayers are easily obtained by epitaxial growth on 3C-SiC(111) on a 2° off-axis 6H-SiC(0001). The resulting samples contain rhombohedral sequences of five layers on 70% of the surface. We confirm the presence of the flat band at the Fermi level by scanning tunneling spectroscopy and angle-resolved photoemission spectroscopy, in close agreement with the predictions of density functional theory calculations.

  18. Phase Space for the Breakdown of the Quantum Hall Effect in Epitaxial Graphene

    NASA Astrophysics Data System (ADS)

    Alexander-Webber, J. A.; Baker, A. M. R.; Janssen, T. J. B. M.; Tzalenchuk, A.; Lara-Avila, S.; Kubatkin, S.; Yakimova, R.; Piot, B. A.; Maude, D. K.; Nicholas, R. J.

    2013-08-01

    We report the phase space defined by the quantum Hall effect breakdown in polymer gated epitaxial graphene on SiC (SiC/G) as a function of temperature, current, carrier density, and magnetic fields up to 30 T. At 2 K, breakdown currents (Ic) almost 2 orders of magnitude greater than in GaAs devices are observed. The phase boundary of the dissipationless state (ρxx=0) shows a [1-(T/Tc)2] dependence and persists up to Tc>45K at 29 T. With magnetic field Ic was found to increase ∝B3/2 and Tc∝B2. As the Fermi energy approaches the Dirac point, the ν=2 quantized Hall plateau appears continuously from fields as low as 1 T up to at least 19 T due to a strong magnetic field dependence of the carrier density.

  19. Capture Zone Distributions and Island Morphologies in Organic Epitaxy and Graphene Formation

    NASA Astrophysics Data System (ADS)

    Pimpinelli, Alberto; Einstein, T. L.

    2013-03-01

    Stating that island nucleation is an essential step in the formation of an epitaxial or supported layer may appear trivially obvious. However, less trivial is the observation that the size of the critical nucleus plays a crucial role in that it determines both the island density (and therefore the size of domains) and the evolution of the island morphology. In this talk we will describe recent developments in the analysis of capture zone distributions (CZD) specifically tailored for application to organic materials. We will also describe specific features of organic and graphene island morphologies, and discuss how they are related to the nucleation process and to the size of the critical nucleus. Work at UMD supported by NSF-MRSEC, Grant DMR 05-20471 and NSF CHE 07-49949

  20. High performance and bendable few-layered InSe photodetectors with broad spectral response.

    PubMed

    Tamalampudi, Srinivasa Reddy; Lu, Yi-Ying; Kumar U, Rajesh; Sankar, Raman; Liao, Chun-Da; Moorthy B, Karukanara; Cheng, Che-Hsuan; Chou, Fang Cheng; Chen, Yit-Tsong

    2014-05-14

    Two-dimensional crystals with a wealth of exotic dimensional-dependent properties are promising candidates for next-generation ultrathin and flexible optoelectronic devices. For the first time, we demonstrate that few-layered InSe photodetectors, fabricated on both a rigid SiO2/Si substrate and a flexible polyethylene terephthalate (PET) film, are capable of conducting broadband photodetection from the visible to near-infrared region (450-785 nm) with high photoresponsivities of up to 12.3 AW(-1) at 450 nm (on SiO2/Si) and 3.9 AW(-1) at 633 nm (on PET). These photoresponsivities are superior to those of other recently reported two-dimensional (2D) crystal-based (graphene, MoS2, GaS, and GaSe) photodetectors. The InSe devices fabricated on rigid SiO2/Si substrates possess a response time of ∼50 ms and exhibit long-term stability in photoswitching. These InSe devices can also operate on a flexible substrate with or without bending and reveal comparable performance to those devices on SiO2/Si. With these excellent optoelectronic merits, we envision that the nanoscale InSe layers will not only find applications in flexible optoelectronics but also act as an active component to configure versatile 2D heterostructure devices.

  1. Tunable charge-trap memory based on few-layer MoS2.

    PubMed

    Zhang, Enze; Wang, Weiyi; Zhang, Cheng; Jin, Yibo; Zhu, Guodong; Sun, Qingqing; Zhang, David Wei; Zhou, Peng; Xiu, Faxian

    2015-01-27

    Charge-trap memory with high-κ dielectric materials is considered to be a promising candidate for next-generation memory devices. Ultrathin layered two-dimensional (2D) materials like graphene and MoS2 have been receiving much attention because of their fantastic physical properties and potential applications in electronic devices. Here, we report on a dual-gate charge-trap memory device composed of a few-layer MoS2 channel and a three-dimensional (3D) Al2O3/HfO2/Al2O3 charge-trap gate stack. Because of the extraordinary trapping ability of both electrons and holes in HfO2, the MoS2 memory device exhibits an unprecedented memory window exceeding 20 V. Importantly, with a back gate the window size can be effectively tuned from 15.6 to 21 V; the program/erase current ratio can reach up to 10(4), allowing for multibit information storage. Moreover, the device shows a high endurance of hundreds of cycles and a stable retention of ∼ 28% charge loss after 10 years, which is drastically lower than ever reported MoS2 flash memory. The combination of 2D materials with traditional high-κ charge-trap gate stacks opens up an exciting field of nonvolatile memory devices.

  2. Superior mechanical flexibility of phosphorene and few-layer black phosphorus

    SciTech Connect

    Wei, Qun; Peng, Xihong

    2014-06-23

    Recently, fabricated two dimensional (2D) phosphorene crystal structures have demonstrated great potential in applications of electronics. Mechanical strain was demonstrated to be able to significantly modify the electronic properties of phosphorene and few-layer black phosphorus. In this work, we employed first principles density functional theory calculations to explore the mechanical properties of phosphorene, including ideal tensile strength and critical strain. It was found that a monolayer phosphorene can sustain tensile strain up to 27% and 30% in the zigzag and armchair directions, respectively. This enormous strain limit of phosphorene results from its unique puckered crystal structure. We found that the tensile strain applied in the armchair direction stretches the pucker of phosphorene, rather than significantly extending the P-P bond lengths. The compromised dihedral angles dramatically reduce the required strain energy. Compared to other 2D materials, such as graphene, phosphorene demonstrates superior flexibility with an order of magnitude smaller Young's modulus. This is especially useful in practical large-magnitude-strain engineering. Furthermore, the anisotropic nature of phosphorene was also explored. We derived a general model to calculate the Young's modulus along different directions for a 2D system.

  3. Spiral growth of few-layer MoS2 by chemical vapor deposition

    NASA Astrophysics Data System (ADS)

    Dong, X.; Yan, C.; Tomer, D.; Li, C. H.; Li, L.

    2016-08-01

    Growth spirals exhibit appealing properties due to a preferred layer stacking and lack of inversion symmetry. Here, we report spiral growth of MoS2 during chemical vapor deposition on SiO2/Si and epitaxial graphene/SiC substrates, and their physical and electronic properties. We determine the layer-dependence of the MoS2 bandgap, ranging from 2.4 eV for the monolayer to a constant of 1.3 eV beyond the fifth layer. We further observe that spirals predominantly initiate at the step edges of the SiC substrate, based on which we propose a growth mechanism driven by screw dislocation created by the coalescence of two growth fronts at steps.

  4. SU(4) symmetry breaking revealed by magneto-optical spectroscopy in epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Tan, Liang Z.; Orlita, Milan; Potemski, Marek; Sprinkle, Mike; Berger, Claire; de Heer, Walter; Louie, Steven; Martinez, Gerard

    2015-03-01

    Electron-electron and electron-phonon interactions break the spin and valley degeneracies of the lowest Landau level (LL) in graphene. Multiple theoretical models have been proposed for the broken symmetry ground state. Previous tilted magnetic field transport experiments have obtained partial information on the ground state by probing the spin degree of freedom. In this work, we show that, via the valley-dependent electron-phonon interaction, symmetry breaking of the valley degree of freedom can be detected in infra-red transmission signatures close to magneto-phonon resonances. We have performed infra-red magneto-transmission experiments on multi-layer epitaxial graphene samples in magnetic fields up to 35 T. Following the main optical transition involving the lowest LL, we observe a new absorption transition increasing in intensity with magnetic fields greater than 26 T. Our theoretical calculations quantitatively explain these features, and unambiguously identify the charge density wave as the ground state in our samples. This work was supported by National Science Foundation Grant No. DMR10-1006184, the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Computational resources have been provided by the NSF through XSEDE resources at NICS.

  5. Sequential oxygen and alkali intercalation of epitaxial graphene on Ir(111): enhanced many-body effects and formation of pn-interfaces

    NASA Astrophysics Data System (ADS)

    Ulstrup, Søren; Andersen, Mie; Bianchi, Marco; Barreto, Lucas; Hammer, Bjørk; Hornekær, Liv; Hofmann, Philip

    2014-09-01

    High quality epitaxial graphene films can be applied as templates for tailoring graphene-substrate interfaces that allow for precise control of the charge carrier behavior in graphene through doping and many-body effects. By combining scanning tunneling microscopy, angle-resolved photoemission spectroscopy and density functional theory we demonstrate that oxygen intercalated epitaxial graphene on Ir(111) has high structural quality, is quasi free-standing, and shows signatures of many-body interactions. Using this system as a template, we show that pn-interfaces can be patterned by adsorption and intercalation of rubidium, and that the n-doped graphene regions exhibit a reduced Coulomb screening via enhanced electron-plasmon coupling. These findings are central for understanding and tailoring the properties of graphene-metal contacts e.g. for realizing quantum tunneling devices.

  6. SiC Homoepitaxy, Etching and Graphene Epitaxial Growth on SiC Substrates Using a Novel Fluorinated Si Precursor Gas (SiF4)

    NASA Astrophysics Data System (ADS)

    Rana, Tawhid; Chandrashekhar, M. V. S.; Daniels, Kevin; Sudarshan, Tangali

    2016-04-01

    Tetrafluorosilane (SiF4 or TFS), a novel precursor gas, has been demonstrated to perform three primary operations of silicon carbide-related processing: SiC etching, SiC epitaxial growth and graphene epitaxial growth. TFS etches SiC substrate vigorously in a H2 ambient by efficient Si removal from the surface, where SiC etch rate is a function of TFS gas concentration. In this SiC etching process, Si is removed by TFS and C is removed by H2. When propane is added to a H2 and TFS gas mixture, etching is halted and high-quality SiC epitaxy takes place in a Si droplet-free condition. TFS's ability to remove Si can also be exploited to grow epitaxial graphene in a controllable manner in an inert (Ar) ambient. Here, TFS enhances graphene growth by selective etching of Si from the SiC surface.

  7. Observing hot carrier distribution in an n-type epitaxial graphene on a SiC substrate

    SciTech Connect

    Someya, T.; Ishida, Y.; Yoshida, R.; Iimori, T.; Yukawa, R.; Akikubo, K.; Yamamoto, Sh.; Yamamoto, S.; Kanai, T.; Itatani, J.; Komori, F.; Shin, S.; Matsuda, I.; Fukidome, H.; Funakubo, K.; Suemitsu, M.; Yamamoto, T.

    2014-04-21

    Hot carrier dynamics in the Dirac band of n-type epitaxial graphene on a SiC substrate were traced in real time using femtosecond-time-resolved photoemission spectroscopy. The spectral evolution directly reflects the energetically linear density of states superimposed with a Fermi–Dirac distribution. The relaxation time is governed by the internal energy dissipation of electron–electron scattering, and the observed electronic temperature indicates cascade carrier multiplication.

  8. Van der Waals Epitaxy of Two-Dimensional MoS2-Graphene Heterostructures in Ultrahigh Vacuum.

    PubMed

    Miwa, Jill A; Dendzik, Maciej; Grønborg, Signe S; Bianchi, Marco; Lauritsen, Jeppe V; Hofmann, Philip; Ulstrup, Søren

    2015-06-23

    In this work, we demonstrate direct van der Waals epitaxy of MoS2-graphene heterostructures on a semiconducting silicon carbide (SiC) substrate under ultrahigh vacuum conditions. Angle-resolved photoemission spectroscopy (ARPES) measurements show that the electronic structure of free-standing single-layer (SL) MoS2 is retained in these heterostructures due to the weak van der Waals interaction between adjacent materials. The MoS2 synthesis is based on a reactive physical vapor deposition technique involving Mo evaporation and sulfurization in a H2S atmosphere on a template consisting of epitaxially grown graphene on SiC. Using scanning tunneling microscopy, we study the seeding of Mo on this substrate and the evolution from nanoscale MoS2 islands to SL and bilayer (BL) MoS2 sheets during H2S exposure. Our ARPES measurements of SL and BL MoS2 on graphene reveal the coexistence of the Dirac states of graphene and the expected valence band of MoS2 with the band maximum shifted to the corner of the Brillouin zone at K̅ in the SL limit. We confirm the 2D character of these electronic states via a lack of dispersion with photon energy. The growth of epitaxial MoS2-graphene heterostructures on SiC opens new opportunities for further in situ studies of the fundamental properties of these complex materials, as well as perspectives for implementing them in various device schemes to exploit their many promising electronic and optical properties.

  9. Role of the Pinning Points in epitaxial Graphene Moiré Superstructures on the Pt(111) Surface.

    PubMed

    Martínez, José I; Merino, Pablo; Pinardi, Anna L; Gonzalo, Otero-Irurueta; López, María F; Méndez, Javier; Martín-Gago, José A

    2016-01-01

    The intrinsic atomic mechanisms responsible for electronic doping of epitaxial graphene Moirés on transition metal surfaces is still an open issue. To better understand this process we have carried out a first-principles full characterization of the most representative Moiré superstructures observed on the Gr/Pt(111) system and confronted the results with atomically resolved scanning tunneling microscopy experiments. We find that for all reported Moirés the system relaxes inducing a non-negligible atomic corrugation both, at the graphene and at the outermost platinum layer. Interestingly, a mirror "anti-Moiré" reconstruction appears at the substrate, giving rise to the appearance of pinning-points. We show that these points are responsible for the development of the superstructure, while charge from the Pt substrate is injected into the graphene, inducing a local n-doping, mostly localized at these specific pinning-point positions.

  10. Role of the Pinning Points in epitaxial Graphene Moiré Superstructures on the Pt(111) Surface

    PubMed Central

    Martínez, José I.; Merino, Pablo; Pinardi, Anna L.; Gonzalo, Otero-Irurueta; López, María F.; Méndez, Javier; Martín-Gago, José A.

    2016-01-01

    The intrinsic atomic mechanisms responsible for electronic doping of epitaxial graphene Moirés on transition metal surfaces is still an open issue. To better understand this process we have carried out a first-principles full characterization of the most representative Moiré superstructures observed on the Gr/Pt(111) system and confronted the results with atomically resolved scanning tunneling microscopy experiments. We find that for all reported Moirés the system relaxes inducing a non-negligible atomic corrugation both, at the graphene and at the outermost platinum layer. Interestingly, a mirror “anti-Moiré” reconstruction appears at the substrate, giving rise to the appearance of pinning-points. We show that these points are responsible for the development of the superstructure, while charge from the Pt substrate is injected into the graphene, inducing a local n-doping, mostly localized at these specific pinning-point positions. PMID:26852920

  11. Role of the Pinning Points in epitaxial Graphene Moiré Superstructures on the Pt(111) Surface.

    PubMed

    Martínez, José I; Merino, Pablo; Pinardi, Anna L; Gonzalo, Otero-Irurueta; López, María F; Méndez, Javier; Martín-Gago, José A

    2016-01-01

    The intrinsic atomic mechanisms responsible for electronic doping of epitaxial graphene Moirés on transition metal surfaces is still an open issue. To better understand this process we have carried out a first-principles full characterization of the most representative Moiré superstructures observed on the Gr/Pt(111) system and confronted the results with atomically resolved scanning tunneling microscopy experiments. We find that for all reported Moirés the system relaxes inducing a non-negligible atomic corrugation both, at the graphene and at the outermost platinum layer. Interestingly, a mirror "anti-Moiré" reconstruction appears at the substrate, giving rise to the appearance of pinning-points. We show that these points are responsible for the development of the superstructure, while charge from the Pt substrate is injected into the graphene, inducing a local n-doping, mostly localized at these specific pinning-point positions. PMID:26852920

  12. Van der Waals epitaxial growth of two-dimensional single-crystalline GaSe domains on graphene

    DOE PAGESBeta

    Li, Xufan; Basile, Leonardo; Huang, Bing; Ma, Cheng; Lee, Jaekwang; Vlassiouk, Ivan V.; Puretzky, Alexander A.; Lin, Ming -Wei; Chi, Miaofang; Idrobo Tapia, Juan Carlos; et al

    2015-07-22

    Two-dimensional (2D) van der Waals (vdW) heterostructures are a family of artificially-structured materials that promise tunable optoelectronic properties for devices with enhanced functionalities. Compared to stamping, direct epitaxy of vdW heterostructures is ideal for clean interlayer interfaces and scalable device fabrication. Here, we explore the synthesis and preferred orientations of 2D GaSe atomic layers on graphene (Gr) by vdW epitaxy. Guided by the wrinkles on graphene, GaSe nuclei form that share a predominant lattice orientation. Due to vdW epitaxial growth many nuclei grow as perfectly aligned crystals and coalesce to form large (tens of microns), single-crystal flakes. Through theoretical investigationsmore » of interlayer energetics, and measurements of preferred orientations by atomic-resolution STEM and electron diffraction, a 10.9 interlayer rotation of the GaSe lattice with respect to the underlying graphene is found to be the most energetically preferred vdW heterostructure with the largest binding energy and the longest-range ordering. These GaSe/Gr vdW heterostructures exhibit an enhanced Raman E21g band of monolayer GaSe along with highly-quenched photoluminescence due to strong charge transfer. Despite the very large lattice mismatch of GaSe/Gr through vdW epitaxy, the predominant orientation control and convergent formation of large single-crystal flakes demonstrated here is promising for the scalable synthesis of large-area vdW heterostructures for the development of new optical and optoelectronic devices.« less

  13. Van der Waals epitaxial growth of two-dimensional single-crystalline GaSe domains on graphene

    SciTech Connect

    Li, Xufan; Basile, Leonardo; Huang, Bing; Ma, Cheng; Lee, Jaekwang; Vlassiouk, Ivan V.; Puretzky, Alexander A.; Lin, Ming -Wei; Chi, Miaofang; Idrobo Tapia, Juan Carlos; Rouleau, Christopher M.; Sumpter, Bobby G.; Yoon, Mina; Geohegan, David B.; Xiao, Kai

    2015-07-22

    Two-dimensional (2D) van der Waals (vdW) heterostructures are a family of artificially-structured materials that promise tunable optoelectronic properties for devices with enhanced functionalities. Compared to stamping, direct epitaxy of vdW heterostructures is ideal for clean interlayer interfaces and scalable device fabrication. Here, we explore the synthesis and preferred orientations of 2D GaSe atomic layers on graphene (Gr) by vdW epitaxy. Guided by the wrinkles on graphene, GaSe nuclei form that share a predominant lattice orientation. Due to vdW epitaxial growth many nuclei grow as perfectly aligned crystals and coalesce to form large (tens of microns), single-crystal flakes. Through theoretical investigations of interlayer energetics, and measurements of preferred orientations by atomic-resolution STEM and electron diffraction, a 10.9 interlayer rotation of the GaSe lattice with respect to the underlying graphene is found to be the most energetically preferred vdW heterostructure with the largest binding energy and the longest-range ordering. These GaSe/Gr vdW heterostructures exhibit an enhanced Raman E21g band of monolayer GaSe along with highly-quenched photoluminescence due to strong charge transfer. Despite the very large lattice mismatch of GaSe/Gr through vdW epitaxy, the predominant orientation control and convergent formation of large single-crystal flakes demonstrated here is promising for the scalable synthesis of large-area vdW heterostructures for the development of new optical and optoelectronic devices.

  14. Atomic Layer Epitaxy of h-BN(0001) Multilayers on Co(0001) and Molecular Beam Epitaxy Growth of Graphene on h-BN(0001)/Co(0001).

    PubMed

    Driver, M Sky; Beatty, John D; Olanipekun, Opeyemi; Reid, Kimberly; Rath, Ashutosh; Voyles, Paul M; Kelber, Jeffry A

    2016-03-22

    The direct growth of hexagonal boron nitride (h-BN) by industrially scalable methods is of broad interest for spintronic and nanoelectronic device applications. Such applications often require atomically precise control of film thickness and azimuthal registry between layers and substrate. We report the formation, by atomic layer epitaxy (ALE), of multilayer h-BN(0001) films (up to 7 monolayers) on Co(0001). The ALE process employs BCl3/NH3 cycles at 600 K substrate temperature. X-ray photoelectron spectroscopy (XPS) and low energy electron diffraction (LEED) data show that this process yields an increase in h-BN average film thickness linearly proportional to the number of BCl3/NH3 cycles, with BN layers in azimuthal registry with each other and with the Co(0001) substrate. LEED diffraction spot profile data indicate an average BN domain size of at least 1900 Å. Optical microscopy data indicate the presence of some domains as large as ∼20 μm. Transmission electron microscopy (TEM) and ambient exposure studies demonstrate macroscopic and microscopic continuity of the h-BN film, with the h-BN film highly conformal to the Co substrate. Photoemission data show that the h-BN(0001) film is p-type, with band bending near the Co/h-BN interface. Growth of graphene by molecular beam epitaxy (MBE) is observed on the surface of multilayer h-BN(0001) at temperatures of 800 K. LEED data indicate azimuthal graphene alignment with the h-BN and Co(0001) lattices, with domain size similar to BN. The evidence of multilayer BN and graphene azimuthal alignment with the lattice of the Co(0001) substrate demonstrates that this procedure is suitable for scalable production of heterojunctions for spintronic applications.

  15. Electronic energy loss spectra from mono-layer to few layers of phosphorene

    NASA Astrophysics Data System (ADS)

    Mohan, Brij; Thakur, Rajesh; Ahluwalia, P. K.

    2016-05-01

    Using first principles calculations, electronic and optical properties of few-layers phosphorene has been investigated. Electronic band structure show a moderate band gap of 0.9 eV in monolayer phosphorene which decreases with increasing number of layers. Optical properties of few-layers of phosphorene in infrared and visible region shows tunability with number of layers. Electron energy loss function has been plotted and huge red shift in plasmonic behaviours is found. These tunable electronic and optical properties of few-layers of phosphorene can be useful for the applications of optoelectronic devices.

  16. Van der Waals Epitaxial Growth of Two-Dimensional Single-Crystalline GaSe Domains on Graphene.

    PubMed

    Li, Xufan; Basile, Leonardo; Huang, Bing; Ma, Cheng; Lee, Jaekwang; Vlassiouk, Ivan V; Puretzky, Alexander A; Lin, Ming-Wei; Yoon, Mina; Chi, Miaofang; Idrobo, Juan C; Rouleau, Christopher M; Sumpter, Bobby G; Geohegan, David B; Xiao, Kai

    2015-08-25

    Two-dimensional (2D) van der Waals (vdW) heterostructures are a family of artificially structured materials that promise tunable optoelectronic properties for devices with enhanced functionalities. Compared to transferring, direct epitaxy of vdW heterostructures is ideal for clean interlayer interfaces and scalable device fabrication. Here we report the synthesis and preferred orientations of 2D GaSe atomic layers on graphene (Gr) by vdW epitaxy. GaSe crystals are found to nucleate predominantly on random wrinkles or grain boundaries of graphene, share a preferred lattice orientation with underlying graphene, and grow into large (tens of micrometers) irregularly shaped, single-crystalline domains. The domains are found to propagate with triangular edges that merge into the large single crystals during growth. Electron diffraction reveals that approximately 50% of the GaSe domains are oriented with a 10.5 ± 0.3° interlayer rotation with respect to the underlying graphene. Theoretical investigations of interlayer energetics reveal that a 10.9° interlayer rotation is the most energetically preferred vdW heterostructure. In addition, strong charge transfer in these GaSe/Gr vdW heterostructures is predicted, which agrees with the observed enhancement in the Raman E(2)1g band of monolayer GaSe and highly quenched photoluminescence compared to GaSe/SiO2. Despite the very large lattice mismatch of GaSe/Gr through vdW epitaxy, the predominant orientation control and convergent formation of large single-crystal flakes demonstrated here is promising for the scalable synthesis of large-area vdW heterostructures for the development of new optical and optoelectronic devices.

  17. Van der Waals Epitaxial Growth of Two-Dimensional Single-Crystalline GaSe Domains on Graphene.

    PubMed

    Li, Xufan; Basile, Leonardo; Huang, Bing; Ma, Cheng; Lee, Jaekwang; Vlassiouk, Ivan V; Puretzky, Alexander A; Lin, Ming-Wei; Yoon, Mina; Chi, Miaofang; Idrobo, Juan C; Rouleau, Christopher M; Sumpter, Bobby G; Geohegan, David B; Xiao, Kai

    2015-08-25

    Two-dimensional (2D) van der Waals (vdW) heterostructures are a family of artificially structured materials that promise tunable optoelectronic properties for devices with enhanced functionalities. Compared to transferring, direct epitaxy of vdW heterostructures is ideal for clean interlayer interfaces and scalable device fabrication. Here we report the synthesis and preferred orientations of 2D GaSe atomic layers on graphene (Gr) by vdW epitaxy. GaSe crystals are found to nucleate predominantly on random wrinkles or grain boundaries of graphene, share a preferred lattice orientation with underlying graphene, and grow into large (tens of micrometers) irregularly shaped, single-crystalline domains. The domains are found to propagate with triangular edges that merge into the large single crystals during growth. Electron diffraction reveals that approximately 50% of the GaSe domains are oriented with a 10.5 ± 0.3° interlayer rotation with respect to the underlying graphene. Theoretical investigations of interlayer energetics reveal that a 10.9° interlayer rotation is the most energetically preferred vdW heterostructure. In addition, strong charge transfer in these GaSe/Gr vdW heterostructures is predicted, which agrees with the observed enhancement in the Raman E(2)1g band of monolayer GaSe and highly quenched photoluminescence compared to GaSe/SiO2. Despite the very large lattice mismatch of GaSe/Gr through vdW epitaxy, the predominant orientation control and convergent formation of large single-crystal flakes demonstrated here is promising for the scalable synthesis of large-area vdW heterostructures for the development of new optical and optoelectronic devices. PMID:26202730

  18. Toward epitaxially grown two-dimensional crystal hetero-structures: Single and double MoS2/graphene hetero-structures by chemical vapor depositions

    NASA Astrophysics Data System (ADS)

    Lin, Meng-Yu; Chang, Chung-En; Wang, Cheng-Hung; Su, Chen-Fung; Chen, Chi; Lee, Si-Chen; Lin, Shih-Yen

    2014-08-01

    Uniform large-size MoS2/graphene hetero-structures fabricated directly on sapphire substrates are demonstrated with layer-number controllability by chemical vapor deposition (CVD). The cross-sectional high-resolution transmission electron microscopy (HRTEM) images provide the direct evidences of layer numbers of MoS2/graphene hetero-structures. Photo-excited electron induced Fermi level shift of the graphene channel are observed on the single MoS2/graphene hetero-structure transistors. Furthermore, double hetero-structures of graphene/MoS2/graphene are achieved by CVD fabrication of graphene layers on top of the MoS2, as confirmed by the cross-sectional HRTEM. These results have paved the possibility of epitaxially grown multi-hetero-structures for practical applications.

  19. Toward epitaxially grown two-dimensional crystal hetero-structures: Single and double MoS{sub 2}/graphene hetero-structures by chemical vapor depositions

    SciTech Connect

    Lin, Meng-Yu; Chang, Chung-En; Wang, Cheng-Hung; Su, Chen-Fung; Chen, Chi; Lee, Si-Chen; Lin, Shih-Yen

    2014-08-18

    Uniform large-size MoS{sub 2}/graphene hetero-structures fabricated directly on sapphire substrates are demonstrated with layer-number controllability by chemical vapor deposition (CVD). The cross-sectional high-resolution transmission electron microscopy (HRTEM) images provide the direct evidences of layer numbers of MoS{sub 2}/graphene hetero-structures. Photo-excited electron induced Fermi level shift of the graphene channel are observed on the single MoS{sub 2}/graphene hetero-structure transistors. Furthermore, double hetero-structures of graphene/MoS{sub 2}/graphene are achieved by CVD fabrication of graphene layers on top of the MoS{sub 2}, as confirmed by the cross-sectional HRTEM. These results have paved the possibility of epitaxially grown multi-hetero-structures for practical applications.

  20. Probing the extended-state width of disorder-broadened Landau levels in epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Takase, K.; Hibino, H.; Muraki, K.

    2015-09-01

    We experimentally investigate the width of extended states in disorder-broadened Landau levels (LLs) in top-gated epitaxial graphene on silicon carbide using two different methods: gated transport spectroscopy and activation gap measurements on integer quantum Hall states. The transport spectroscopy reveals that the widths of the extended states in the zero-energy (N =0 ) and first excited (N =1 ) LLs are of similar magnitude over the ranges of magnetic field (4-16 T) and temperature studied (1.6-150 K). Under certain assumptions we find that the extended-state width follows a power-law temperature dependence with the exponent η ˜0.3 in the N =0 (N =1 ) LL, with almost no (very weak) magnetic-field dependence. Activation gap measurements at the filling factors of ν =2 and 6 give results consistent with transport spectroscopy for the N =1 LL, but indicate a larger broadening for the N =0 LL than deduced from the spectroscopy.

  1. Magnetotransport of Epitaxial Graphene on Hexagonal SiC Surface Grown with Metal Plate Capping

    NASA Astrophysics Data System (ADS)

    Park, Kibog; Jin, Han Byul; Jung, Sungchul; Kim, Junhyoung; Chae, Dong-Hun; Kim, Wan-Seop; Park, Jaesung

    High quality epitaxial graphene (EG) was grown on a Si-face hexagonal SiC substrate by capping the surface with a metal plate (Molybdenum, Tungsten) during UHV annealing. The growth temperature was ~ 950 degree C, significantly lower than the conventional UHV annealing. The crystallinity of EG film was examined with Raman spectrum measurements. Almost no D-peak and a large narrow 2D-peak ensure that a thin (mono- or bi-layer) EG film was grown with a negligible number of defects. The electrical properties of EG film were also characterized by performing magnetotransport measurements with Hall-bar structures. The carrier type was found to be n-type, the sheet carrier density be (3.6-9.2)x1012 /cm2, and the Hall mobility be ~2100 cm2/Vs. Due to the relatively high carrier density, the Quantum Hall Effect was observed only for high filling factors up to 14 T. However, clear Shubnikov-de-Hass oscillations were observed, indicating that the random carrier scattering due to impurities or defects is minimal in the EG film grown with metal plate capping. Supported by NRF in South Korea (2014M2B2A9031944).

  2. Probing the role of interlayer coupling and coulomb interactions on electronic structure in few-layer MoSe₂ nanostructures.

    PubMed

    Bradley, Aaron J; Ugeda, Miguel M; da Jornada, Felipe H; Qiu, Diana Y; Ruan, Wei; Zhang, Yi; Wickenburg, Sebastian; Riss, Alexander; Lu, Jiong; Mo, Sung-Kwan; Hussain, Zahid; Shen, Zhi-Xun; Louie, Steven G; Crommie, Michael F

    2015-04-01

    Despite the weak nature of interlayer forces in transition metal dichalcogenide (TMD) materials, their properties are highly dependent on the number of layers in the few-layer two-dimensional (2D) limit. Here, we present a combined scanning tunneling microscopy/spectroscopy and GW theoretical study of the electronic structure of high quality single- and few-layer MoSe2 grown on bilayer graphene. We find that the electronic (quasiparticle) bandgap, a fundamental parameter for transport and optical phenomena, decreases by nearly one electronvolt when going from one layer to three due to interlayer coupling and screening effects. Our results paint a clear picture of the evolution of the electronic wave function hybridization in the valleys of both the valence and conduction bands as the number of layers is changed. This demonstrates the importance of layer number and electron-electron interactions on van der Waals heterostructures and helps to clarify how their electronic properties might be tuned in future 2D nanodevices.

  3. Controllable synthesis of few-layered and hierarchically porous boron nitride nanosheets.

    PubMed

    Xiao, Feng; Chen, Zhixin; Casillas, Gilberto; Richardson, Christopher; Li, Huijun; Huang, Zhenguo

    2016-03-11

    Few-layered porous boron nitride nanosheets (BNNS) have been prepared using a dynamic magnesium diboride (MgB2) template and ammonium chloride (NH4Cl) etchant. Magnesium-based intermediates serve as layer separators in the synthesis and prevent extensive aggregation, resulting in few-layered BNNS. The resultant BNNS are hierarchically porous and show good CO2/N2 adsorption selectivity. PMID:26871737

  4. Transport properties of pristine few-layer black phosphorus by van der Waals passivation in an inert atmosphere.

    PubMed

    Doganov, Rostislav A; O'Farrell, Eoin C T; Koenig, Steven P; Yeo, Yuting; Ziletti, Angelo; Carvalho, Alexandra; Campbell, David K; Coker, David F; Watanabe, Kenji; Taniguchi, Takashi; Castro Neto, Antonio H; Özyilmaz, Barbaros

    2015-04-10

    Ultrathin black phosphorus is a two-dimensional semiconductor with a sizeable band gap. Its excellent electronic properties make it attractive for applications in transistor, logic and optoelectronic devices. However, it is also the first widely investigated two-dimensional material to undergo degradation upon exposure to ambient air. Therefore a passivation method is required to study the intrinsic material properties, understand how oxidation affects the physical properties and enable applications of phosphorene. Here we demonstrate that atomically thin graphene and hexagonal boron nitride can be used for passivation of ultrathin black phosphorus. We report that few-layer pristine black phosphorus channels passivated in an inert gas environment, without any prior exposure to air, exhibit greatly improved n-type charge transport resulting in symmetric electron and hole transconductance characteristics.

  5. Transport properties of pristine few-layer black phosphorus by van der Waals passivation in an inert atmosphere

    NASA Astrophysics Data System (ADS)

    Doganov, Rostislav A.; O'Farrell, Eoin C. T.; Koenig, Steven P.; Yeo, Yuting; Ziletti, Angelo; Carvalho, Alexandra; Campbell, David K.; Coker, David F.; Watanabe, Kenji; Taniguchi, Takashi; Neto, Antonio H. Castro; Özyilmaz, Barbaros

    2015-04-01

    Ultrathin black phosphorus is a two-dimensional semiconductor with a sizeable band gap. Its excellent electronic properties make it attractive for applications in transistor, logic and optoelectronic devices. However, it is also the first widely investigated two-dimensional material to undergo degradation upon exposure to ambient air. Therefore a passivation method is required to study the intrinsic material properties, understand how oxidation affects the physical properties and enable applications of phosphorene. Here we demonstrate that atomically thin graphene and hexagonal boron nitride can be used for passivation of ultrathin black phosphorus. We report that few-layer pristine black phosphorus channels passivated in an inert gas environment, without any prior exposure to air, exhibit greatly improved n-type charge transport resulting in symmetric electron and hole transconductance characteristics.

  6. Layer-dependent Band Alignment and Work Function of Few-Layer Phosphorene

    PubMed Central

    Cai, Yongqing; Zhang, Gang; Zhang, Yong-Wei

    2014-01-01

    Using first-principles calculations, we study the electronic properties of few-layer phosphorene focusing on layer-dependent behavior of band gap, work function band alignment and carrier effective mass. It is found that few-layer phosphorene shows a robust direct band gap character, and its band gap decreases with the number of layers following a power law. The work function decreases rapidly from monolayer (5.16 eV) to trilayer (4.56 eV), and then slowly upon further increasing the layer number. Compared to monolayer phosphorene, there is a drastic decrease of hole effective mass along the ridge (zigzag) direction for bilayer phosphorene, indicating a strong interlayer coupling and screening effect. Our study suggests that 1). Few-layer phosphorene with a layer-dependent band gap and a robust direct band gap character is promising for efficient solar energy harvest. 2). Few-layer phosphorene outperforms monolayer counterpart in terms of a lighter carrier effective mass, a higher carrier density and a weaker scattering due to enhanced screening. 3). The layer-dependent band edges and work functions of few-layer phosphorene allow for modification of Schottky barrier with enhanced carrier injection efficiency. It is expected that few-layer phosphorene will present abundant opportunities for a plethora of new electronic applications. PMID:25327586

  7. Layer-dependent band alignment and work function of few-layer phosphorene.

    PubMed

    Cai, Yongqing; Zhang, Gang; Zhang, Yong-Wei

    2014-10-20

    Using first-principles calculations, we study the electronic properties of few-layer phosphorene focusing on layer-dependent behavior of band gap, work function band alignment and carrier effective mass. It is found that few-layer phosphorene shows a robust direct band gap character, and its band gap decreases with the number of layers following a power law. The work function decreases rapidly from monolayer (5.16 eV) to trilayer (4.56 eV), and then slowly upon further increasing the layer number. Compared to monolayer phosphorene, there is a drastic decrease of hole effective mass along the ridge (zigzag) direction for bilayer phosphorene, indicating a strong interlayer coupling and screening effect. Our study suggests that 1). Few-layer phosphorene with a layer-dependent band gap and a robust direct band gap character is promising for efficient solar energy harvest. 2). Few-layer phosphorene outperforms monolayer counterpart in terms of a lighter carrier effective mass, a higher carrier density and a weaker scattering due to enhanced screening. 3). The layer-dependent band edges and work functions of few-layer phosphorene allow for modification of Schottky barrier with enhanced carrier injection efficiency. It is expected that few-layer phosphorene will present abundant opportunities for a plethora of new electronic applications.

  8. Epitaxial Growth of Thin Ferroelectric Polymer Films on Graphene Layer for Fully Transparent and Flexible Nonvolatile Memory.

    PubMed

    Kim, Kang Lib; Lee, Wonho; Hwang, Sun Kak; Joo, Se Hun; Cho, Suk Man; Song, Giyoung; Cho, Sung Hwan; Jeong, Beomjin; Hwang, Ihn; Ahn, Jong-Hyun; Yu, Young-Jun; Shin, Tae Joo; Kwak, Sang Kyu; Kang, Seok Ju; Park, Cheolmin

    2016-01-13

    Enhancing the device performance of organic memory devices while providing high optical transparency and mechanical flexibility requires an optimized combination of functional materials and smart device architecture design. However, it remains a great challenge to realize fully functional transparent and mechanically durable nonvolatile memory because of the limitations of conventional rigid, opaque metal electrodes. Here, we demonstrate ferroelectric nonvolatile memory devices that use graphene electrodes as the epitaxial growth substrate for crystalline poly(vinylidene fluoride-trifluoroethylene) (PVDF-TrFE) polymer. The strong crystallographic interaction between PVDF-TrFE and graphene results in the orientation of the crystals with distinct symmetry, which is favorable for polarization switching upon the electric field. The epitaxial growth of PVDF-TrFE on a graphene layer thus provides excellent ferroelectric performance with high remnant polarization in metal/ferroelectric polymer/metal devices. Furthermore, a fully transparent and flexible array of ferroelectric field effect transistors was successfully realized by adopting transparent poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] semiconducting polymer.

  9. Effects of Pb Intercalation on the Structural and Electronic Properties of Epitaxial Graphene on SiC.

    PubMed

    Yurtsever, Ayhan; Onoda, Jo; Iimori, Takushi; Niki, Kohei; Miyamachi, Toshio; Abe, Masayuki; Mizuno, Seigi; Tanaka, Satoru; Komori, Fumio; Sugimoto, Yoshiaki

    2016-08-01

    The effects of Pb intercalation on the structural and electronic properties of epitaxial single-layer graphene grown on SiC(0001) substrate are investigated using scanning tunneling microscopy (STM), noncontact atomic force microscopy, Kelvin probe force microscopy (KPFM), X-ray photoelectron spectroscopy, and angle-resolved photoemission spectroscopy (ARPES) methods. The STM results show the formation of an ordered moiré superstructure pattern induced by Pb atom intercalation underneath the graphene layer. ARPES measurements reveal the presence of two additional linearly dispersing π-bands, providing evidence for the decoupling of the buffer layer from the underlying SiC substrate. Upon Pb intercalation, the Si 2p core level spectra show a signature for the existence of PbSi chemical bonds at the interface region, as manifested in a shift of 1.2 eV of the bulk SiC component toward lower binding energies. The Pb intercalation gives rise to hole-doping of graphene and results in a shift of the Dirac point energy by about 0.1 eV above the Fermi level, as revealed by the ARPES measurements. The KPFM experiments have shown that decoupling of the graphene layer by Pb intercalation is accompanied by a work function increase. The observed increase in the work function is attributed to the suppression of the electron transfer from the SiC substrate to the graphene layer. The Pb intercalated structure is found to be stable in ambient conditions and at high temperatures up to 1250 °C. These results demonstrate that the construction of a graphene-capped Pb/SiC system offers a possibility of tuning the graphene electronic properties and exploring intriguing physical properties such as superconductivity and spintronics. PMID:27295020

  10. Seeding Atomic Layer Deposition of High-k Dielectrics on Epitaxial Graphene with Organic Self-assembled Monolayers

    SciTech Connect

    Alaboson, Justice M. P.; Wang, Qing Hua; Emery, Jonathan D.; Lipson, Albert L.; Bedzyk, Michael J.; Elam, Jeffrey W.; Pellin, Michael J.; Hersam, Mark C.

    2011-06-28

    The development of high-performance graphene-based nanoelectronics requires the integration of ultrathin and pinhole-free high-k dielectric films with graphene at the wafer scale. Here, we demonstrate that self-assembled monolayers of perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) act as effective organic seeding layers for atomic layer deposition (ALD) of HfO₂ and Al₂O₃ on epitaxial graphene on SiC(0001). The PTCDA is deposited via sublimation in ultrahigh vacuum and shown to be highly ordered with low defect density by molecular-resolution scanning tunneling microscopy. Whereas identical ALD conditions lead to incomplete and rough dielectric deposition on bare graphene, the chemical functionality provided by the PTCDA seeding layer yields highly uniform and conformal films. The morphology and chemistry of the dielectric films are characterized by atomic force microscopy, ellipsometry, cross-sectional scanning electron microscopy, and X-ray photoelectron spectroscopy, while high-resolution X-ray reflectivity measurements indicate that the underlying graphene remains intact following ALD. Using the PTCDA seeding layer, metal-oxide-graphene capacitors fabricated with a 3 nm Al₂O₃ and 10 nm HfO₂ dielectric stack show high capacitance values of ~700 nF/cm² and low leakage currents of ~5 × 10{sup –9} A/cm² at 1 V applied bias. These results demonstrate the viability of sublimated organic self-assembled monolayers as seeding layers for high-k dielectric films in graphene-based nanoelectronics.

  11. Molecular beam epitaxy growth of SrO buffer layers on graphite and graphene for the integration of complex oxides

    NASA Astrophysics Data System (ADS)

    Ahmed, Adam S.; Wen, Hua; Ohta, Taisuke; Pinchuk, Igor V.; Zhu, Tiancong; Beechem, Thomas; Kawakami, Roland K.

    2016-08-01

    We report the successful growth of high-quality SrO films on highly-ordered pyrolytic graphite (HOPG) and single-layer graphene by molecular beam epitaxy. The SrO layers have (001) orientation as confirmed by X-ray diffraction (XRD) while atomic force microscopy measurements show continuous pinhole-free films having rms surface roughness of <1.5 Å. Transport measurements of exfoliated graphene after SrO deposition show a strong dependence between the Dirac point and Sr oxidation. Subsequently, the SrO is leveraged as a buffer layer for more complex oxide integration via the demonstration of (001) oriented SrTiO3 grown atop a SrO/HOPG stack.

  12. Detecting the local transport properties and the dimensionality of transport of epitaxial graphene by a multi-point probe approach

    NASA Astrophysics Data System (ADS)

    Barreto, Lucas; Perkins, Edward; Johannsen, Jens; Ulstrup, Søren; Fromm, Felix; Raidel, Christian; Seyller, Thomas; Hofmann, Philip

    2013-01-01

    The electronic transport properties of epitaxial monolayer graphene (MLG) and hydrogen-intercalated quasi free-standing bilayer graphene (QFBLG) on SiC(0001) are investigated by micro multi-point probes. Using a probe with 12 contacts, we perform four-point probe measurements with the possibility to effectively vary the contact spacing over more than one order of magnitude, allowing us to establish that the transport is purely two-dimensional. Combined with the carrier density obtained by angle-resolved photoemission spectroscopy, we find the room temperature mobility of MLG to be (870±120) cm2/V s. The transport in QFBLG is also found to be two-dimensional with a mobility of (1600±160) cm2/V s.

  13. Molecular beam epitaxy growth of SrO buffer layers on graphite and graphene for the integration of complex oxides

    DOE PAGESBeta

    Ahmed, Adam S.; Wen, Hua; Ohta, Taisuke; Pinchuk, Igor V.; Zhu, Tiancong; Beechem, Thomas; Kawakami, Roland K.

    2016-04-27

    Here, we report the successful growth of high-quality SrO films on highly-ordered pyrolytic graphite (HOPG) and single-layer graphene by molecular beam epitaxy. The SrO layers have (001) orientation as confirmed by X-ray diffraction (XRD) while atomic force microscopy measurements show continuous pinhole-free films having rms surface roughness of <1.5 Å. Moreover, transport measurements of exfoliated graphene, after SrO deposition, show a strong dependence between the Dirac point and Sr oxidation. As a result, the SrO is leveraged as a buffer layer for more complex oxide integration via the demonstration of (001) oriented SrTiO3 grown atop a SrO/HOPG stack.

  14. Observation of the integer quantum Hall effect in high quality, uniform wafer-scale epitaxial graphene films

    NASA Astrophysics Data System (ADS)

    Pan, Wei; Howell, Stephen W.; Ross, Anthony Joseph; Ohta, Taisuke; Friedmann, Thomas A.

    2010-12-01

    We report the observation of the integer quantum Hall states at Landau level fillings of ν =2, 6, and 10 in a Hall bar device made of a single-layer epitaxial graphene film on the silicon-face of silicon-carbide prepared via argon-assisted graphitization. The two-dimensional electron gas exhibits a low-temperature (at 4 K) carrier mobility of ˜14 000 cm2/V s at the electron density of 6.1×1011 cm-2. Furthermore, the sheet resistance obtained from four-probe measurements across the whole area (12×6 mm2) of another specimen grown under similar condition displays roughly uniform values (˜1600 Ω/square), suggesting that the macroscopic steps and accompanying multilayer graphene domains play a minor role in the low-temperature electronic transport.

  15. Exciton dynamics in suspended monolayer and few-layer MoS₂ 2D crystals.

    PubMed

    Shi, Hongyan; Yan, Rusen; Bertolazzi, Simone; Brivio, Jacopo; Gao, Bo; Kis, Andras; Jena, Debdeep; Xing, Huili Grace; Huang, Libai

    2013-02-26

    Femtosecond transient absorption spectroscopy and microscopy were employed to study exciton dynamics in suspended and Si₃N₄ substrate-supported monolayer and few-layer MoS₂ 2D crystals. Exciton dynamics for the monolayer and few-layer structures were found to be remarkably different from those of thick crystals when probed at energies near that of the lowest energy direct exciton (A exciton). The intraband relaxation rate was enhanced by more than 40 fold in the monolayer in comparison to that observed in the thick crystals, which we attributed to defect assisted scattering. Faster electron-hole recombination was found in monolayer and few-layer structures due to quantum confinement effects that lead to an indirect-direct band gap crossover. Nonradiative rather than radiative relaxation pathways dominate the dynamics in the monolayer and few-layer MoS₂. Fast trapping of excitons by surface trap states was observed in monolayer and few-layer structures, pointing to the importance of controlling surface properties in atomically thin crystals such as MoS₂ along with controlling their dimensions.

  16. Weak Localization in Bulk Black Phosphorus and Few-Layer Phosphorene

    NASA Astrophysics Data System (ADS)

    Du, Yuchen; Neal, Adam; Zhou, Hong; Ye, Peide

    2015-03-01

    Most of the recent experimental research on black phosphorus (BP) or phosphorene has been focused on device applications with few systematic studies on electrical transport properties of single-layer or few-layer phosphorene. Here, we report on the magnetotransport experiments on thick BP films and few-layer phosphorene at low temperatures. The observed weak localization is well fitted by the Hikami-Larkin-Nagaoka model where the temperature dependence of the phase coherence length has demonstrated to be a power-law behavior of T- 0 . 5. In addition, the temperature dependence of Hall mobility as a function of the film thickness is also examined to uncover the limitation of mobility in few-layer phosphorene with different mechanisms.

  17. Fabrication of suspended few-layer black phosphorus nanopores and nanoribbons via electron beam nanosculpting

    NASA Astrophysics Data System (ADS)

    Masih Das, Paul; Danda, Gopinath; Parkin, William; Cupo, Andrew; Kharche, Neerav; Ling, Xi; Huang, Shengxi; Dresselhaus, Mildred; Meunier, Vincent; Drndic, Marija

    We present nanopores, nanoribbons, and nanogaps in suspended few-layer black phosphorus (BP) flakes that have been realized using in situ transmission electron microscope nanosculpting. Few-layer BP flakes were first produced through a liquid exfoliation procedure and suspended on holey SiNx membranes. We investigate the structural characteristics of few-layer BP and further show the time-dependent properties of various nanostructures under exposure to an electron beam. It is shown that high-resolution structural modification of nanopores and nanoribbons can be achieved with nanometer-scale precision on timescales of a few minutes. We also used density functional theory to provide a model for the observed anisotropy in edge formation by computing energy barriers for various edge geometries.

  18. Two-dimensional massless Dirac fermions, chiral pseudo-spins, and Berry's phase in few-layer black phosphorus

    NASA Astrophysics Data System (ADS)

    Baik, Seung Su; Choi, Hyoung Joon

    Black phosphorus (BP) and its two-dimensional (2D) derivative phosphorene are rapidly emerging nanoelectronic materials with potential applicability to field effect transistors and optoelectronic devices. Unlike the gapless semiconductor graphene, multilayer BP has a substantial band gap of 0.2 eV, and this band-gap size is predicted being sensitive to the external perturbations such as pressure, strain, and electric field. Very recently, a semiconductor-semimetal transition in BP was realized by the surface potassium (K) doping, producing a Dirac semimetal state with a linear dispersion in the armchair direction and a quadratic one in the zigzag direction. Here, based on first-principles density functional calculations, we present that beyond the critical K density, 2D massless Dirac fermions emerge in K-doped few-layer BP, and the electronic states around Dirac points have chiral pseudo-spins and Berry's phase. These features are robust with respect to the spin-orbit interaction. The switchable massless Dirac fermions discussed here may open a new way for the development of high performance devices in 2D materials beyond graphene. This work was supported by NRF of Korea (Grant No. 2011-0018306) and KISTI supercomputing center (Project No. KSC-2015-C3-039).

  19. Three-fold diffraction symmetry in epitaxial graphene and the SiC substrate

    SciTech Connect

    Siegel, D A; Zhou, S Y; El Gabaly, F; Schmid, A K; McCarty, K F; Lanzara, A

    2009-12-10

    The crystallographic symmetries and spatial distribution of stacking domains in graphene films on 6H-SiC(0001) have been studied by low energy electron diffraction (LEED) and dark field imaging in a low energy electron microscope (LEEM). We find that the graphene diffraction spots from 2 and 3 atomic layers of graphene have 3-fold symmetry consistent with AB (Bernal or rhombohedral) stacking of the layers. On the contrary, graphene diffraction spots from the buffer layer and monolayer graphene have apparent 6-fold symmetry, although the 3-fold nature of the satellite spots indicates a more complex periodicity in the graphene sheets.

  20. Few-layer SnSe2 transistors with high on/off ratios

    NASA Astrophysics Data System (ADS)

    Pei, Tengfei; Bao, Lihong; Wang, Guocai; Ma, Ruisong; Yang, Haifang; Li, Junjie; Gu, Changzhi; Pantelides, Sokrates; Du, Shixuan; Gao, Hong-jun

    2016-02-01

    We report few-layer SnSe2 field effect transistors (FETs) with high current on/off ratios. By trying different gate configurations, 300 nm SiO2 and 70 nm HfO2 as back gate only and 70 nm HfO2 as back gate combined with a top capping layer of polymer electrolyte, few-layer SnSe2 FET with a current on/off ratio of 104 can be obtained. This provides a reliable solution for electrically modulating quasi-two-dimensional materials with high electron density (over 1013 cm-2) for field-effect transistor applications.

  1. The Nature of the Interlayer Interaction in Bulk and Few-Layer Phosphorus.

    PubMed

    Shulenburger, L; Baczewski, A D; Zhu, Z; Guan, J; Tománek, D

    2015-12-01

    Sensitive dependence of the electronic structure on the number of layers in few-layer phosphorene raises a question about the true nature of the interlayer interaction in so-called "van der Waals (vdW) solids". We performed quantum Monte Carlo calculations and found that the interlayer interaction in bulk black phosphorus and related few-layer phosphorene is associated with a significant charge redistribution that is incompatible with purely dispersive forces and not captured by density functional theory calculations with different vdW corrected functionals. These findings confirm the necessity of more sophisticated treatment of nonlocal electron correlation in total energy calculations.

  2. Strain-induced semiconductor to metal transition in few-layer black phosphorus from first principles

    NASA Astrophysics Data System (ADS)

    Ju, Weiwei; Li, Tongwei; Wang, Hui; Yong, Yongliang; Sun, Jinfeng

    2015-02-01

    Electronic structures of few-layer black phosphorus (BP) with biaxial strain are investigated by using methods based on density functional theory. The compressive strain can result in a semiconductor-metal transition (SMT) for few-layer BP, whereas the tensile strain only affects the band gaps. The critical compressive strain for the SMT is larger in the thinner 2D BP. The band structures and charge densities are calculated in order to provide imperative understanding on SMT. With the compressive strain, the energy of conduction bands moves down, which is induced by the structural change and is essential reason of SMT.

  3. The nature of the interlayer interaction in bulk and few-layer phosphorus

    DOE PAGESBeta

    Shulenburger, Luke; Baczewski, A. D.; Zhu, Z.; Guan, J.; Tomanek, David

    2015-11-02

    Sensitive dependence of the electronic structure on the number of layers in few-layer phosphorene raises a question about the true nature of the interlayer interaction in so-called van der Waals (vdW) solids . We performed quantum Monte Carlo calculations and found that the interlayer interaction in bulk black phosphorus and related few-layer phosphorene is associated with a significant charge redistribution that is incompatible with purely dispersive forces and not captured by density functional theory calculations with different vdW corrected functionals. Lastly, these findings confirm the necessity of more sophisticated treatment of nonlocal electron correlation in total energy calculations.

  4. Quantum transport measurement of few-layer WTe2 field effect devices

    NASA Astrophysics Data System (ADS)

    Chen, Jianhao; Liu, Xin; Tian, Shibing; Zhang, Chenglong; Jia, Shuang

    2015-03-01

    We have performed systematic quantum transport measurement on field effect devices fabricated from few-layer WTe2 single crystals. We found that the magnetoresistance of few-layer WTe2 could be very different from that of bulk samples, which may arise from the imbalance of electron and hole carriers in the samples. We shall discuss our findings in more details in light of recent progress in our experiment. This work is supported by National Natural Science Foundation of China (11374021 and 11327406); by China Ministry of Science and Technology under Contract # 2014CB920900 and 2013CB921900; and by the Young 1000-Talent Program of China.

  5. Visualization of Grain Structure and Boundaries of Polycrystalline Graphene and Two-Dimensional Materials by Epitaxial Growth of Transition Metal Dichalcogenides.

    PubMed

    Ago, Hiroki; Fukamachi, Satoru; Endo, Hiroko; Solís-Fernández, Pablo; Yunus, Rozan Mohamad; Uchida, Yuki; Panchal, Vishal; Kazakova, Olga; Tsuji, Masaharu

    2016-03-22

    The presence of grain boundaries in two-dimensional (2D) materials is known to greatly affect their physical, electrical, and chemical properties. Given the difficulty in growing perfect large single-crystals of 2D materials, revealing the presence and characteristics of grain boundaries becomes an important issue for practical applications. Here, we present a method to visualize the grain structure and boundaries of 2D materials by epitaxially growing transition metal dichalcogenides (TMDCs) over them. Triangular single-crystals of molybdenum disulfide (MoS2) epitaxially grown on the surface of graphene allowed us to determine the orientation and size of the graphene grains. Grain boundaries in the polycrystalline graphene were also visualized reflecting their higher chemical reactivity than the basal plane. The method was successfully applied to graphene field-effect transistors, revealing the actual grain structures of the graphene channels. Moreover, we demonstrate that this method can be extended to determine the grain structure of other 2D materials, such as tungsten disulfide (WS2). Our visualization method based on van der Waals epitaxy can offer a facile and large-scale labeling technique to investigate the grain structures of various 2D materials, and it will also contribute to understand the relationship between their grain structure and physical properties. PMID:26943750

  6. Visualization of Grain Structure and Boundaries of Polycrystalline Graphene and Two-Dimensional Materials by Epitaxial Growth of Transition Metal Dichalcogenides.

    PubMed

    Ago, Hiroki; Fukamachi, Satoru; Endo, Hiroko; Solís-Fernández, Pablo; Yunus, Rozan Mohamad; Uchida, Yuki; Panchal, Vishal; Kazakova, Olga; Tsuji, Masaharu

    2016-03-22

    The presence of grain boundaries in two-dimensional (2D) materials is known to greatly affect their physical, electrical, and chemical properties. Given the difficulty in growing perfect large single-crystals of 2D materials, revealing the presence and characteristics of grain boundaries becomes an important issue for practical applications. Here, we present a method to visualize the grain structure and boundaries of 2D materials by epitaxially growing transition metal dichalcogenides (TMDCs) over them. Triangular single-crystals of molybdenum disulfide (MoS2) epitaxially grown on the surface of graphene allowed us to determine the orientation and size of the graphene grains. Grain boundaries in the polycrystalline graphene were also visualized reflecting their higher chemical reactivity than the basal plane. The method was successfully applied to graphene field-effect transistors, revealing the actual grain structures of the graphene channels. Moreover, we demonstrate that this method can be extended to determine the grain structure of other 2D materials, such as tungsten disulfide (WS2). Our visualization method based on van der Waals epitaxy can offer a facile and large-scale labeling technique to investigate the grain structures of various 2D materials, and it will also contribute to understand the relationship between their grain structure and physical properties.

  7. Isolation and characterization of nanosheets containing few layers of the Aurivillius family of oxides and metal-organic compounds

    SciTech Connect

    Sreedhara, M.B.; Prasad, B.E.; Moirangthem, Monali; Murugavel, R.; Rao, C.N.R.

    2015-04-15

    Nanosheets containing few-layers of ferroelectric Aurivillius family of oxides, Bi{sub 2}A{sub n−1}B{sub n}O{sub 3n+3} (where A=Bi{sup 3+}, Ba{sup 2+} etc. and B=Ti{sup 4+}, Fe{sup 3+} etc.) with n=3, 4, 5, 6 and 7 have been prepared by reaction with n-butyllithium, followed by exfoliation in water. The few-layer samples have been characterized by Tyndall cones, atomic force microscopy, optical spectroscopy and other techniques. The few-layer species have a thickness corresponding to a fraction of the c-parameter along which axis the perovskite layers are stacked. Magnetization measurements have been carried out on the few-layer samples containing iron. Few-layer species of a few layered metal-organic compounds have been obtained by ultrasonication and characterized by Tyndall cones, atomic force microscopy, optical spectroscopy and magnetic measurements. Significant changes in the optical spectra and magnetic properties are found in the few-layer species compared to the bulk samples. Few-layer species of the Aurivillius family of oxides may find uses as thin layer dielectrics in photovoltaics and other applications. - Graphical abstract: Exfoliation of the layered Aurivillius oxides into few-layer nanosheets by chemical Li intercalation using n-BuLi followed by reaction in water. Exfoliation of the layered metal-organic compounds into few-layer nanosheets by ultrasonication. - Highlights: • Few-layer nanosheets of Aurivillius family of oxides with perovskite layers have been generated by lithium intercalation. • Few-layer nanosheets of few layered metal-organic compounds have been generated by ultrasonication. • Few-layer nanosheets of the Aurivillius oxides have been characterized by AFM, TEM and optical spectroscopy. • Aurivillius oxides containing Fe show layer dependent magnetic properties. • Exfoliated few-layer metal-organic compounds show changes in spectroscopic and magnetic properties compared with bulk materials.

  8. Integration of hexagonal boron nitride with quasi-freestanding epitaxial graphene: toward wafer-scale, high-performance devices.

    PubMed

    Bresnehan, Michael S; Hollander, Matthew J; Wetherington, Maxwell; LaBella, Michael; Trumbull, Kathleen A; Cavalero, Randal; Snyder, David W; Robinson, Joshua A

    2012-06-26

    Hexagonal boron nitride (h-BN) is a promising dielectric material for graphene-based electronic devices. Here we investigate the potential of h-BN gate dielectrics, grown by chemical vapor deposition (CVD), for integration with quasi-freestanding epitaxial graphene (QFEG). We discuss the large scale growth of h-BN on copper foil via a catalytic thermal CVD process and the subsequent transfer of h-BN to a 75 mm QFEG wafer. X-ray photoelectron spectroscopy (XPS) measurements confirm the absence of h-BN/graphitic domains and indicate that the film is chemically stable throughout the transfer process, while Raman spectroscopy indicates a 42% relaxation of compressive stress following removal of the copper substrate and subsequent transfer of h-BN to QFEG. Despite stress-induced wrinkling observed in the films, Hall effect measurements show little degradation (<10%) in carrier mobility for h-BN coated QFEG. Temperature dependent Hall measurements indicate little contribution from remote surface optical phonon scattering and suggest that, compared to HfO(2) based dielectrics, h-BN can be an excellent material for preserving electrical transport properties. Graphene transistors utilizing h-BN gates exhibit peak intrinsic cutoff frequencies >30 GHz (2.4× that of HfO(2)-based devices). PMID:22545808

  9. Femtosecond solid-state laser based on a few-layered black phosphorus saturable absorber.

    PubMed

    Su, Xiancui; Wang, Yiran; Zhang, Baitao; Zhao, Ruwei; Yang, Kejian; He, Jingliang; Hu, Qiangqiang; Jia, Zhitai; Tao, Xutang

    2016-05-01

    In this Letter, a high-quality, few-layered black phosphorus (BP) saturable absorber (SA) was fabricated successfully, and a femtosecond solid-state laser modulated by BP-SA was experimentally demonstrated for the first time, to the best of our knowledge. Pulses as short as 272 fs were achieved with an average output power of 0.82 W, corresponding to the pulse energy of 6.48 nJ and peak power of 23.8 MW. So far, these represent the shortest pulse duration and highest output power ever obtained with a BP-based mode-locked solid-state laser. The results indicate the promising potential of few-layered BP-SA for applications in solid-state femtosecond mode-locked lasers. PMID:27128045

  10. Liquid exfoliation of solvent-stabilized few-layer black phosphorus for applications beyond electronics

    PubMed Central

    Hanlon, Damien; Backes, Claudia; Doherty, Evie; Cucinotta, Clotilde S.; Berner, Nina C.; Boland, Conor; Lee, Kangho; Harvey, Andrew; Lynch, Peter; Gholamvand, Zahra; Zhang, Saifeng; Wang, Kangpeng; Moynihan, Glenn; Pokle, Anuj; Ramasse, Quentin M.; McEvoy, Niall; Blau, Werner J.; Wang, Jun; Abellan, Gonzalo; Hauke, Frank; Hirsch, Andreas; Sanvito, Stefano; O'Regan, David D.; Duesberg, Georg S.; Nicolosi, Valeria; Coleman, Jonathan N.

    2015-01-01

    Few-layer black phosphorus (BP) is a new two-dimensional material which is of great interest for applications, mainly in electronics. However, its lack of environmental stability severely limits its synthesis and processing. Here we demonstrate that high-quality, few-layer BP nanosheets, with controllable size and observable photoluminescence, can be produced in large quantities by liquid phase exfoliation under ambient conditions in solvents such as N-cyclohexyl-2-pyrrolidone (CHP). Nanosheets are surprisingly stable in CHP, probably due to the solvation shell protecting the nanosheets from reacting with water or oxygen. Experiments, supported by simulations, show reactions to occur only at the nanosheet edge, with the rate and extent of the reaction dependent on the water/oxygen content. We demonstrate that liquid-exfoliated BP nanosheets are potentially useful in a range of applications from ultrafast saturable absorbers to gas sensors to fillers for composite reinforcement. PMID:26469634

  11. Large-Area Synthesis of High-Quality Uniform Few-Layer MoTe2.

    PubMed

    Zhou, Lin; Xu, Kai; Zubair, Ahmad; Liao, Albert D; Fang, Wenjing; Ouyang, Fangping; Lee, Yi-Hsien; Ueno, Keiji; Saito, Riichiro; Palacios, Tomás; Kong, Jing; Dresselhaus, Mildred S

    2015-09-23

    The controlled synthesis of large-area, atomically thin molybdenum ditelluride (MoTe2) crystals is crucial for its various applications based on the attractive properties of this emerging material. In this work, we developed a chemical vapor deposition synthesis to produce large-area, uniform, and highly crystalline few-layer 2H and 1T' MoTe2 films. It was found that these two different phases of MoTe2 can be grown depending on the choice of Mo precursor. Because of the highly crystalline structure, the as-grown few-layer 2H MoTe2 films display electronic properties that are comparable to those of mechanically exfoliated MoTe2 flakes. Our growth method paves the way for the large-scale application of MoTe2 in high-performance nanoelectronics and optoelectronics. PMID:26305492

  12. Low-Frequency Interlayer Breathing Modes in Few-Layer Black Phosphorus

    DOE PAGESBeta

    Ling, Xi; Liang, Liangbo; Huang, Shengxi; Puretzky, Alexander A.; Geohegan, David B.; Sumpter, Bobby G.; Kong, Jing; Meunier, Vincent; Dresselhaus, Mildred S.

    2015-05-08

    As a new two-dimensional layered material, black phosphorus (BP) is a very promising material for nanoelectronics and nano-optoelectronics. We use Raman spectroscopy and first-principles theory to characterize and understand low-frequency (LF) interlayer breathing modes (<100 cm-1) in few-layer BP for the first time. Using laser polarization dependence study and group theory analysis the breathing modes are assigned to Ag symmetry. Compared to the high-frequency (HF) Raman modes, the LF breathing modes are considerably more sensitive to interlayer coupling and thus their frequencies show stronger dependence on the number of layers. Hence, they constitute an effective means to probe both themore » crystalline orientation and thickness of few-layer BP. Furthermore, the temperature dependence shows that the breathing modes have a harmonic behavior, in contrast to HF Raman modes which exhibit anharmonicity.« less

  13. Strain- and twist-engineered optical absorption of few-layer black phosphorus

    NASA Astrophysics Data System (ADS)

    Jia, Qian; Kong, XiangHua; Qiao, JingSi; Ji, Wei

    2016-09-01

    Density functional and many-body perturbation theories calculations were carried out to investigate fundamental and optical bandgap, exciton binding energy and optical absorption property of normal and strain- and twist-engineered few-layer black phosphorus (BP). We found that the fundamental bandgaps of few layer BP can be engineered by layer stacking and in-plane strain, with linear relationships to their associated exciton binding energies. The strain-dependent optical absorption behaviors are also anisotropic that the position of the first absorption peak monotonically blue-shifts as the strain applies to either direction for incident light polarized along the armchair direction, but this is not the case for that along the zigzag direction. Given those striking properties, we proposed two prototype devices for building potentially more balanced light absorbers and light filter passes, which promotes further applications and investigations of BP in nanoelectronics and optoelectronics.

  14. Low-Frequency Interlayer Breathing Modes in Few-Layer Black Phosphorus

    SciTech Connect

    Ling, Xi; Liang, Liangbo; Huang, Shengxi; Puretzky, Alexander A.; Geohegan, David B.; Sumpter, Bobby G.; Kong, Jing; Meunier, Vincent; Dresselhaus, Mildred S.

    2015-05-08

    As a new two-dimensional layered material, black phosphorus (BP) is a very promising material for nanoelectronics and nano-optoelectronics. We use Raman spectroscopy and first-principles theory to characterize and understand low-frequency (LF) interlayer breathing modes (<100 cm-1) in few-layer BP for the first time. Using laser polarization dependence study and group theory analysis the breathing modes are assigned to Ag symmetry. Compared to the high-frequency (HF) Raman modes, the LF breathing modes are considerably more sensitive to interlayer coupling and thus their frequencies show stronger dependence on the number of layers. Hence, they constitute an effective means to probe both the crystalline orientation and thickness of few-layer BP. Furthermore, the temperature dependence shows that the breathing modes have a harmonic behavior, in contrast to HF Raman modes which exhibit anharmonicity.

  15. Low-Frequency Interlayer Breathing Modes in Few-Layer Black Phosphorus

    NASA Astrophysics Data System (ADS)

    Ling, Xi; Liang, Liangbo; Huang, Shengxi; Puretzky, Alexander A.; Geohegan, David B.; Sumpter, Bobby G.; Kong, Jing; Meunier, Vincent; Dresselhaus, Mildred S.

    2015-06-01

    As a new two-dimensional layered material, black phosphorus (BP) is a promising material for nanoelectronics and nano-optoelectronics. We use Raman spectroscopy and first-principles theory to report our findings related to low-frequency (LF) interlayer breathing modes (<100 cm-1) in few-layer BP for the first time. The breathing modes are assigned to Ag symmetry by the laser polarization dependence study and group theory analysis. Compared to the high-frequency (HF) Raman modes, the LF breathing modes are much more sensitive to interlayer coupling and thus their frequencies show much stronger dependence on the number of layers. Hence, they could be used as effective means to probe both the crystalline orientation and thickness for few-layer BP. Furthermore, the temperature dependence study shows that the breathing modes have a harmonic behavior, in contrast to HF Raman modes which are known to exhibit anharmonicity.

  16. Liquid exfoliation of solvent-stabilized few-layer black phosphorus for applications beyond electronics.

    PubMed

    Hanlon, Damien; Backes, Claudia; Doherty, Evie; Cucinotta, Clotilde S; Berner, Nina C; Boland, Conor; Lee, Kangho; Harvey, Andrew; Lynch, Peter; Gholamvand, Zahra; Zhang, Saifeng; Wang, Kangpeng; Moynihan, Glenn; Pokle, Anuj; Ramasse, Quentin M; McEvoy, Niall; Blau, Werner J; Wang, Jun; Abellan, Gonzalo; Hauke, Frank; Hirsch, Andreas; Sanvito, Stefano; O'Regan, David D; Duesberg, Georg S; Nicolosi, Valeria; Coleman, Jonathan N

    2015-10-15

    Few-layer black phosphorus (BP) is a new two-dimensional material which is of great interest for applications, mainly in electronics. However, its lack of environmental stability severely limits its synthesis and processing. Here we demonstrate that high-quality, few-layer BP nanosheets, with controllable size and observable photoluminescence, can be produced in large quantities by liquid phase exfoliation under ambient conditions in solvents such as N-cyclohexyl-2-pyrrolidone (CHP). Nanosheets are surprisingly stable in CHP, probably due to the solvation shell protecting the nanosheets from reacting with water or oxygen. Experiments, supported by simulations, show reactions to occur only at the nanosheet edge, with the rate and extent of the reaction dependent on the water/oxygen content. We demonstrate that liquid-exfoliated BP nanosheets are potentially useful in a range of applications from ultrafast saturable absorbers to gas sensors to fillers for composite reinforcement.

  17. Low-Frequency Interlayer Breathing Modes in Few-Layer Black Phosphorus.

    PubMed

    Ling, Xi; Liang, Liangbo; Huang, Shengxi; Puretzky, Alexander A; Geohegan, David B; Sumpter, Bobby G; Kong, Jing; Meunier, Vincent; Dresselhaus, Mildred S

    2015-06-10

    As a new two-dimensional layered material, black phosphorus (BP) is a very promising material for nanoelectronics and optoelectronics. We use Raman spectroscopy and first-principles theory to characterize and understand the low-frequency (LF) interlayer breathing modes (<100 cm(-1)) in few-layer BP for the first time. Using a laser polarization dependence study and group theory analysis, the breathing modes are assigned to Ag symmetry. Compared to the high-frequency (HF) Raman modes, the LF breathing modes are considerably more sensitive to interlayer coupling and, thus, their frequencies show a stronger dependence on the number of layers. Hence, they constitute an effective means to probe both the crystalline orientation and thickness of few-layer BP. Furthermore, the temperature dependence shows that in the temperature range -150 to 30 °C, the breathing modes have a weak anharmonic behavior, in contrast to the HF Raman modes that exhibit strong anharmonicity.

  18. Near-field optical microscopy and spectroscopy of few-layer black phosphorous

    NASA Astrophysics Data System (ADS)

    Frenzel, A. J.; Tran, S.; Hinton, J. P.; Sternbach, A. J.; Yang, J.; Gillgren, N.; Lau, C. N.; Basov, D. N.

    Few-layer black phosphorous is a recent addition to the family of two-dimensional (2D) materials which exhibits strongly anisotropic transport and optical properties due to its puckered honeycomb structure. It was recently predicted that this intrinsic anisotropy should manifest in the plasmon dispersion. Additionally, tuning layer number and carrier density can control the dispersion of these collective modes. Scanning near-field optical microscopy (SNOM) has been demonstrated as a powerful method to probe electronic properties, including propagating collective modes, in layered 2D materials. We used SNOM to investigate anisotropic carrier response in few-layer black phosphorous encapsulated by hexagonal boron nitride. In addition to exploring gate-voltage tunability of the electronic response, we demonstrate effective modulation of the near-field signal by ultrafast photoexcitation.

  19. Liquid exfoliation of solvent-stabilized few-layer black phosphorus for applications beyond electronics

    NASA Astrophysics Data System (ADS)

    Hanlon, Damien; Backes, Claudia; Doherty, Evie; Cucinotta, Clotilde S.; Berner, Nina C.; Boland, Conor; Lee, Kangho; Harvey, Andrew; Lynch, Peter; Gholamvand, Zahra; Zhang, Saifeng; Wang, Kangpeng; Moynihan, Glenn; Pokle, Anuj; Ramasse, Quentin M.; McEvoy, Niall; Blau, Werner J.; Wang, Jun; Abellan, Gonzalo; Hauke, Frank; Hirsch, Andreas; Sanvito, Stefano; O'Regan, David D.; Duesberg, Georg S.; Nicolosi, Valeria; Coleman, Jonathan N.

    2015-10-01

    Few-layer black phosphorus (BP) is a new two-dimensional material which is of great interest for applications, mainly in electronics. However, its lack of environmental stability severely limits its synthesis and processing. Here we demonstrate that high-quality, few-layer BP nanosheets, with controllable size and observable photoluminescence, can be produced in large quantities by liquid phase exfoliation under ambient conditions in solvents such as N-cyclohexyl-2-pyrrolidone (CHP). Nanosheets are surprisingly stable in CHP, probably due to the solvation shell protecting the nanosheets from reacting with water or oxygen. Experiments, supported by simulations, show reactions to occur only at the nanosheet edge, with the rate and extent of the reaction dependent on the water/oxygen content. We demonstrate that liquid-exfoliated BP nanosheets are potentially useful in a range of applications from ultrafast saturable absorbers to gas sensors to fillers for composite reinforcement.

  20. Interlayer breathing and shear modes in few-layer black phosphorus.

    PubMed

    Jiang, Jin-Wu; Wang, Bing-Shen; Park, Harold S

    2016-04-27

    The interlayer breathing and shear modes in few-layer black phosphorus are investigated for their symmetry and lattice dynamical properties. The symmetry groups for the even-layer and odd-layer few-layer black phosphorus are utilized to determine the irreducible representation and the infrared and Raman activity for the interlayer modes. The valence force field model is applied to calculate the eigenvectors and frequencies for the interlayer breathing and shear modes, which are explained using the atomic chain model. The anisotropic puckered configuration for black phosphorus leads to a highly anisotropic frequency for the two interlayer shear modes. More specifically, the frequency for the shear mode in the direction perpendicular to the pucker is less than half of the shear mode in the direction parallel with the pucker. We also report a set of specular interlayer modes having the same frequency for all few-layer black phosphorus with layer numbers N being a multiple of 3, because these modes manifest themselves as collective vibrations of atoms in specific layers. The optical activity of the collective modes enables possible experimental identification for these modes. PMID:26988113

  1. Metalorganic chemical vapor deposition of few-layer sp2 bonded boron nitride films

    NASA Astrophysics Data System (ADS)

    Paduano, Qing; Snure, Michael; Weyburne, David; Kiefer, Arnold; Siegel, Gene; Hu, Jianjun

    2016-09-01

    A systematic study of the growth of atomically smooth few-layer sp2 bonded BN on 50 mm sapphire substrates by metalorganic chemical vapor deposition (MOCVD) using Triethylboron (TEB) and NH3 as precursors is described. Based on the experimental results obtained using Raman spectroscopy, atomic force microscopy (AFM), X-ray reflectance measurements and transmission electron microscopy, we explored the growth parameter space and identified three different growth modes: random three-dimensional (3D) growth, a self-terminating few-layer growth mode, and a very slow layer-by-layer mode. The growth mode depends on the temperature, pressure, V/III ratio, and surface nitridation conditions, as follows: 3D island growth is dominant in the low V/III range and is characterized by a decreasing growth rate with increasing deposition temperature. When the V/III ratio is increased this 3D island growth mode transitions to a self-terminating few-layer growth mode. An additional transition from self-terminating growth to 3D growth occurs when the growth pressure is increased. Very slow layer by layer growth is found at high temperature and low pressure. Finally, substrate surface nitridation promotes self-terminating growth that results in atomically smooth films.

  2. Anisotropic optical properties of few-layer transition metal dichalcogenide ReS2

    NASA Astrophysics Data System (ADS)

    Li, Zhenglu; Cao, Ting; da Jornada, Felipe H.; Wu, Meng; Louie, Steven G.

    We present first-principles (DFT, GW and GW-BSE) calculations of the electronic and optical properties of few-layer rhenium disulfide (ReS2). Monolayer ReS2 shows strong many-electron effects with a fundamental quasiparticle band gap of 2.38 eV based on G0W0 calculation and a large exciton binding energy of 690 meV based on solving the Bethe-Salpeter equation. Highly anisotropic linear-polarized optical absorptions are revealed for few-layer and bulk ReS2. The band gap shows a decreasing trend with the optical polarization direction near the absorption edge gradually rotating from around 67 degree in the monolayer to 85 degree in the bulk, referencing to the Re-chain. Our calculations are consistent with recent experimental data and theoretical studies, and provide a systematic understanding of the electronic and optical properties in few-layer ReS2. This work was supported by National Science Foundation Grant No. DMR15-1508412 and the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Computational resources have been provided by DOE at Lawrence Berkeley National Laboratory's NERSC facility.

  3. Fast and broadband photoresponse of few-layer black phosphorus field-effect transistors.

    PubMed

    Buscema, Michele; Groenendijk, Dirk J; Blanter, Sofya I; Steele, Gary A; van der Zant, Herre S J; Castellanos-Gomez, Andres

    2014-06-11

    Few-layer black phosphorus, a new elemental two-dimensional (2D) material recently isolated by mechanical exfoliation, is a high-mobility layered semiconductor with a direct bandgap that is predicted to strongly depend on the number of layers, from 0.35 eV (bulk) to 2.0 eV (single layer). Therefore, black phosphorus is an appealing candidate for tunable photodetection from the visible to the infrared part of the spectrum. We study the photoresponse of field-effect transistors (FETs) made of few-layer black phosphorus (3-8 nm thick), as a function of excitation wavelength, power, and frequency. In the dark state, the black phosphorus FETs can be tuned both in hole and electron doping regimes allowing for ambipolar operation. We measure mobilities in the order of 100 cm(2)/V s and a current ON/OFF ratio larger than 10(3). Upon illumination, the black phosphorus transistors show a response to excitation wavelengths from the visible region up to 940 nm and a rise time of about 1 ms, demonstrating broadband and fast detection. The responsivity reaches 4.8 mA/W, and it could be drastically enhanced by engineering a detector based on a PN junction. The ambipolar behavior coupled to the fast and broadband photodetection make few-layer black phosphorus a promising 2D material for photodetection across the visible and near-infrared part of the electromagnetic spectrum. PMID:24821381

  4. Fast and broadband photoresponse of few-layer black phosphorus field-effect transistors.

    PubMed

    Buscema, Michele; Groenendijk, Dirk J; Blanter, Sofya I; Steele, Gary A; van der Zant, Herre S J; Castellanos-Gomez, Andres

    2014-06-11

    Few-layer black phosphorus, a new elemental two-dimensional (2D) material recently isolated by mechanical exfoliation, is a high-mobility layered semiconductor with a direct bandgap that is predicted to strongly depend on the number of layers, from 0.35 eV (bulk) to 2.0 eV (single layer). Therefore, black phosphorus is an appealing candidate for tunable photodetection from the visible to the infrared part of the spectrum. We study the photoresponse of field-effect transistors (FETs) made of few-layer black phosphorus (3-8 nm thick), as a function of excitation wavelength, power, and frequency. In the dark state, the black phosphorus FETs can be tuned both in hole and electron doping regimes allowing for ambipolar operation. We measure mobilities in the order of 100 cm(2)/V s and a current ON/OFF ratio larger than 10(3). Upon illumination, the black phosphorus transistors show a response to excitation wavelengths from the visible region up to 940 nm and a rise time of about 1 ms, demonstrating broadband and fast detection. The responsivity reaches 4.8 mA/W, and it could be drastically enhanced by engineering a detector based on a PN junction. The ambipolar behavior coupled to the fast and broadband photodetection make few-layer black phosphorus a promising 2D material for photodetection across the visible and near-infrared part of the electromagnetic spectrum.

  5. Interlayer breathing and shear modes in few-layer black phosphorus.

    PubMed

    Jiang, Jin-Wu; Wang, Bing-Shen; Park, Harold S

    2016-04-27

    The interlayer breathing and shear modes in few-layer black phosphorus are investigated for their symmetry and lattice dynamical properties. The symmetry groups for the even-layer and odd-layer few-layer black phosphorus are utilized to determine the irreducible representation and the infrared and Raman activity for the interlayer modes. The valence force field model is applied to calculate the eigenvectors and frequencies for the interlayer breathing and shear modes, which are explained using the atomic chain model. The anisotropic puckered configuration for black phosphorus leads to a highly anisotropic frequency for the two interlayer shear modes. More specifically, the frequency for the shear mode in the direction perpendicular to the pucker is less than half of the shear mode in the direction parallel with the pucker. We also report a set of specular interlayer modes having the same frequency for all few-layer black phosphorus with layer numbers N being a multiple of 3, because these modes manifest themselves as collective vibrations of atoms in specific layers. The optical activity of the collective modes enables possible experimental identification for these modes.

  6. Interlayer breathing and shear modes in few-layer black phosphorus

    NASA Astrophysics Data System (ADS)

    Jiang, Jin-Wu; Wang, Bing-Shen; Park, Harold S.

    2016-04-01

    The interlayer breathing and shear modes in few-layer black phosphorus are investigated for their symmetry and lattice dynamical properties. The symmetry groups for the even-layer and odd-layer few-layer black phosphorus are utilized to determine the irreducible representation and the infrared and Raman activity for the interlayer modes. The valence force field model is applied to calculate the eigenvectors and frequencies for the interlayer breathing and shear modes, which are explained using the atomic chain model. The anisotropic puckered configuration for black phosphorus leads to a highly anisotropic frequency for the two interlayer shear modes. More specifically, the frequency for the shear mode in the direction perpendicular to the pucker is less than half of the shear mode in the direction parallel with the pucker. We also report a set of specular interlayer modes having the same frequency for all few-layer black phosphorus with layer numbers N being a multiple of 3, because these modes manifest themselves as collective vibrations of atoms in specific layers. The optical activity of the collective modes enables possible experimental identification for these modes.

  7. Intrinsic transport of h-BN encapsulated few-layer black phosphorus

    NASA Astrophysics Data System (ADS)

    Arefe, Ghidewon; Kim, Young Duck; Chenet, Daniel; Cui, Xu; Chang, Damien; Hone, James

    2015-03-01

    Few-layer black phosphorus (BP) is an exciting two-dimensional material with ambipolar behavior, large on/off ratio, and high mobility with a direct bandgap. The anisotropic atomic nature of black phosphorus exhibits unique angle dependent electronic and optical features. One of the primary difficulties in fabricating few-layer BP devices to study transport is the reactive nature of the material in ambient conditions as it degrades in the presence of air and moisture. In order to characterize the intrinsic physical properties of BP, we fabricated few-layer BP flakes that are fully encapsulated by hexagonal boron nitride (h-BN) with a clean stacking technique. We also characterized the electrical transport of h-BN encapsulated BP devices that show greatly improved environmental stability and high mobility at low temperature due to the suppression of extrinsic scattering effects such as charge impurities, surface polar optical phonons, and absorbents from air. H-BN encapsulated BP devices will be an essential platform for the observation of new physics from BP and realization of BP based advanced opto-electronic application devices body.

  8. Few-layer black phosphorus field-effect transistors with reduced current fluctuation.

    PubMed

    Na, Junhong; Lee, Young Tack; Lim, Jung Ah; Hwang, Do Kyung; Kim, Gyu-Tae; Choi, Won Kook; Song, Yong-Won

    2014-11-25

    We investigated the reduction of current fluctuations in few-layer black phosphorus (BP) field-effect transistors resulting from Al2O3 passivation. In order to verify the effect of Al2O3 passivation on device characteristics, measurements and analyses were conducted on thermally annealed devices before and after the passivation. More specifically, static and low-frequency noise analyses were used in monitoring the charge transport characteristics in the devices. The carrier number fluctuation (CNF) model, which is related to the charge trapping/detrapping process near the interface between the channel and gate dielectric, was employed to describe the current fluctuation phenomena. Noise reduction due to the Al2O3 passivation was expressed in terms of the reduced interface trap density values D(it) and N(it), extracted from the subthreshold slope (SS) and the CNF model, respectively. The deviations between the interface trap density values extracted using the SS value and CNF model are elucidated in terms of the role of the Schottky barrier between the few-layer BP and metal contact. Furthermore, the preservation of the Al2O3-passivated few-layer BP flakes in ambient air for two months was confirmed by identical Raman spectra.

  9. Surface-Induced Orientation Control of CuPc Molecules for the Epitaxial Growth of Highly Ordered Organic Crystals on Graphene

    SciTech Connect

    Xiao, Kai; Deng, Wan; Keum, Jong Kahk; Yoon, Mina; Vlassiouk, Ivan V; Clark, Kendal W; Li, An-Ping; Kravchenko, Ivan I; Gu, Gong; Payzant, E Andrew; Sumpter, Bobby; Smith, Sean C; Browning, Jim; Geohegan, David B

    2013-01-01

    The epitaxial growth and preferred molecular orientation of copper phthalocyanine (CuPc) molecules on graphene has been systematically investigated and compared with growth on Si substrates, demonstrating the role of surface-mediated interactions in determining molecular orientation. X-ray scattering and diffraction, scanning tunneling microscopy, scanning electron microscopy, and first-principles theoretical calculations were used to show that the nucleation, orientation and packing of CuPc molecules on films of graphene are fundamentally different compared to those grown on Si substrates. Interfacial dipole interactions induced by charge transfer between CuPc molecules and graphene are shown to epitaxially align the CuPc mole-cules in a face-on orientation in a series of ordered superstructures. At high temperatures, CuPc molecules lie flat with respect to the graphene substrate to form strip-like CuPc crystals with micron sizes containing monocrystalline grains. Such large epitaxial crystals may potentially enable bulk-like properties to improve the device properties in organic electronics, which charge transport, exciton diffusion and dissociation are currently limited by grain size effects and molecular orientation.

  10. Comparison study of PE epitaxy on carbon nanotubes and graphene oxide and PE/graphene oxide as amphiphilic molecular structure for solvent separation

    NASA Astrophysics Data System (ADS)

    He, Linghao; Zheng, Xiaoli; Xu, Qun; Chen, Zhimin; Fu, Jianwei

    2012-03-01

    Carbon nanotubes (CNTs) and graphene nanosheets, as one-dimensional and two-dimensional carbon-based nanomaterials respectively, have different abilities to induce the polymer crystallization. In this study, hybrid materials, polyethylene (PE) decorating on CNTs and graphene oxide (GO), were prepared by a facile and efficient method using supercritical carbon dioxide (SC CO2) as anti-solvent. And the morphology and crystallization behavior of PE on CNTs and GO were investigated by transmission electron microscopy, Fourier transform infrared spectroscopy, Raman spectra, wide angle X-ray diffraction, and differential scanning calorimetry. Although both CNTs and GO could act as nucleating agents to induce PE epitaxial growth, CNTs were decorated by PE lamellar crystals forming nanohybrid "shish-kebab" (NHSK) structure, whereas GO sheets were only decorated with petal-like PE crystals. The varying morphologies of the nanohybrids depend on the PE epitaxy and the interactions between polymer chains and substrates. High surface curvature and the perfect ordered crystal structure of CNTs make PE crystals periodically grow on CNTs. While PE crystals grow and form multiple orientation-lamellae on GO due to the lattice matching and complex interactions between PE chains and GO. In addition, our experimental results show an interesting and evident stratification phenomenon for the PE/GO hybrid material, implying that GO decorated by PE have a screening function for the solvents. We anticipate that this work can widen the area of functionalization of carbon-based nanomaterials with a controlled means by an environmentally benign method, which are important for the functional design in nanodevice applications.

  11. Quantum-confinement and Structural Anisotropy result in Electrically-Tunable Dirac Cone in Few-layer Black Phosphorous

    PubMed Central

    Dolui, Kapildeb; Quek, Su Ying

    2015-01-01

    Two-dimensional (2D) materials are well-known to exhibit interesting phenomena due to quantum confinement. Here, we show that quantum confinement, together with structural anisotropy, result in an electric-field-tunable Dirac cone in 2D black phosphorus. Using density functional theory calculations, we find that an electric field, Eext, applied normal to a 2D black phosphorus thin film, can reduce the direct band gap of few-layer black phosphorus, resulting in an insulator-to-metal transition at a critical field, Ec. Increasing Eext beyond Ec can induce a Dirac cone in the system, provided the black phosphorus film is sufficiently thin. The electric field strength can tune the position of the Dirac cone and the Dirac-Fermi velocities, the latter being similar in magnitude to that in graphene. We show that the Dirac cone arises from an anisotropic interaction term between the frontier orbitals that are spatially separated due to the applied field, on different halves of the 2D slab. When this interaction term becomes vanishingly small for thicker films, the Dirac cone can no longer be induced. Spin-orbit coupling can gap out the Dirac cone at certain electric fields; however, a further increase in field strength reduces the spin-orbit-induced gap, eventually resulting in a topological-insulator-to-Dirac-semimetal transition. PMID:26129645

  12. Thermal expansion, anharmonicity and temperature-dependent Raman spectra of single- and few-layer MoSe₂ and WSe₂.

    PubMed

    Late, Dattatray J; Shirodkar, Sharmila N; Waghmare, Umesh V; Dravid, Vinayak P; Rao, C N R

    2014-06-01

    We report the temperature-dependent Raman spectra of single- and few-layer MoSe2 and WSe2 in the range 77-700 K. We observed linear variation in the peak positions and widths of the bands arising from contributions of anharmonicity and thermal expansion. After characterization using atomic force microscopy and high-resolution transmission electron microscopy, the temperature coefficients of the Raman modes were determined. Interestingly, the temperature coefficient of the A(2)(2u) mode is larger than that of the A(1g) mode, the latter being much smaller than the corresponding temperature coefficients of the same mode in single-layer MoS2 and of the G band of graphene. The temperature coefficients of the two modes in single-layer MoSe2 are larger than those of the same modes in single-layer WSe2. We have estimated thermal expansion coefficients and temperature dependence of the vibrational frequencies of MoS2 and MoSe2 within a quasi-harmonic approximation, with inputs from first-principles calculations based on density functional theory. We show that the contrasting temperature dependence of the Raman-active mode A(1g) in MoS2 and MoSe2 arises essentially from the difference in their strain-phonon coupling. PMID:24692405

  13. Quantum-confinement and Structural Anisotropy result in Electrically-Tunable Dirac Cone in Few-layer Black Phosphorous.

    PubMed

    Dolui, Kapildeb; Quek, Su Ying

    2015-07-01

    Two-dimensional (2D) materials are well-known to exhibit interesting phenomena due to quantum confinement. Here, we show that quantum confinement, together with structural anisotropy, result in an electric-field-tunable Dirac cone in 2D black phosphorus. Using density functional theory calculations, we find that an electric field, E ext, applied normal to a 2D black phosphorus thin film, can reduce the direct band gap of few-layer black phosphorus, resulting in an insulator-to-metal transition at a critical field, Ec. Increasing E ext beyond Ec can induce a Dirac cone in the system, provided the black phosphorus film is sufficiently thin. The electric field strength can tune the position of the Dirac cone and the Dirac-Fermi velocities, the latter being similar in magnitude to that in graphene. We show that the Dirac cone arises from an anisotropic interaction term between the frontier orbitals that are spatially separated due to the applied field, on different halves of the 2D slab. When this interaction term becomes vanishingly small for thicker films, the Dirac cone can no longer be induced. Spin-orbit coupling can gap out the Dirac cone at certain electric fields; however, a further increase in field strength reduces the spin-orbit-induced gap, eventually resulting in a topological-insulator-to-Dirac-semimetal transition.

  14. Quantum-confinement and Structural Anisotropy result in Electrically-Tunable Dirac Cone in Few-layer Black Phosphorous

    NASA Astrophysics Data System (ADS)

    Dolui, Kapildeb; Quek, Su Ying

    2015-07-01

    Two-dimensional (2D) materials are well-known to exhibit interesting phenomena due to quantum confinement. Here, we show that quantum confinement, together with structural anisotropy, result in an electric-field-tunable Dirac cone in 2D black phosphorus. Using density functional theory calculations, we find that an electric field, Eext, applied normal to a 2D black phosphorus thin film, can reduce the direct band gap of few-layer black phosphorus, resulting in an insulator-to-metal transition at a critical field, Ec. Increasing Eext beyond Ec can induce a Dirac cone in the system, provided the black phosphorus film is sufficiently thin. The electric field strength can tune the position of the Dirac cone and the Dirac-Fermi velocities, the latter being similar in magnitude to that in graphene. We show that the Dirac cone arises from an anisotropic interaction term between the frontier orbitals that are spatially separated due to the applied field, on different halves of the 2D slab. When this interaction term becomes vanishingly small for thicker films, the Dirac cone can no longer be induced. Spin-orbit coupling can gap out the Dirac cone at certain electric fields; however, a further increase in field strength reduces the spin-orbit-induced gap, eventually resulting in a topological-insulator-to-Dirac-semimetal transition.

  15. The role of carbon surface diffusion on the growth of epitaxial graphene on SiC.

    SciTech Connect

    Thurmer, Konrad; Ohta, Taisuke; Nie, Shu; Bartelt, Norman Charles; Kellogg, Gary Lee

    2010-03-01

    Growth of high quality graphene films on SiC is regarded as one of the more viable pathways toward graphene-based electronics. Graphitic films form on SiC at elevated temperature because of preferential sublimation of Si. Little is known, however, about the atomistic processes of interrelated SiC decomposition and graphene growth. We have observed the formation of graphene on SiC by Si sublimation in an Ar atmosphere using low energy electron microscopy, scanning tunneling microcopy and atomic force microscopy. This work reveals that the growth mechanism depends strongly on the initial surface morphology, and that carbon diffusion governs the spatial relationship between SiC decomposition and graphene growth. Isolated bilayer SiC steps generate narrow ribbons of graphene, whereas triple bilayer steps allow large graphene sheets to grow by step flow. We demonstrate how graphene quality can be improved by controlling the initial surface morphology specifically by avoiding the instabilities inherent in diffusion-limited growth.

  16. Epitaxial graphene on 4H-SiC(0001) grown under nitrogen flux: evidence of low nitrogen doping and high charge transfer.

    PubMed

    Velez-Fort, Emilio; Mathieu, Claire; Pallecchi, Emiliano; Pigneur, Marine; Silly, Mathieu G; Belkhou, Rachid; Marangolo, Massimiliano; Shukla, Abhay; Sirotti, Fausto; Ouerghi, Abdelkarim

    2012-12-21

    Nitrogen doping of graphene is of great interest for both fundamental research to explore the effect of dopants on a 2D electrical conductor and applications such as lithium storage, composites, and nanoelectronic devices. Here, we report on the modifications of the electronic properties of epitaxial graphene thanks to the introduction, during the growth, of nitrogen-atom substitution in the carbon honeycomb lattice. High-resolution transmission microscopy and low-energy electron microscopy investigations indicate that the nitrogen-doped graphene is uniform at large scale. The substitution of nitrogen atoms in the graphene planes was confirmed by high-resolution X-ray photoelectron spectroscopy, which reveals several atomic configurations for the nitrogen atoms: graphitic-like, pyridine-like, and pyrrolic-like. Angle-resolved photoemission measurements show that the N-doped graphene exhibits large n-type carrier concentrations of 2.6 × 10(13) cm(-2), about 4 times more than what is found for pristine graphene, grown under similar pressure conditions. Our experiments demonstrate that a small amount of dopants (<1%) can significantly tune the electronic properties of graphene by shifting the Dirac cone about 0.3 eV toward higher binding energies with respect to the π band of pristine graphene, which is a key feature for envisioning applications in nanoelectronics. PMID:23148722

  17. Characterizing silicon intercalated graphene grown epitaxially on Ir films by atomic force microscopy

    NASA Astrophysics Data System (ADS)

    Zhang, Yong; Wang, Ye-Liang; Que, Yan-De; Gao, Hong-Jun

    2015-07-01

    An efficient method based on atomic force microscopy (AFM) has been developed to characterize silicon intercalated graphene grown on single crystalline Ir(111) thin films. By combining analyses of the phase image, force curves, and friction-force mapping, acquired by AFM, the locations and coverages of graphene and silicon oxide can be well distinguished. We can also demonstrate that silicon atoms have been successfully intercalated between graphene and the substrate. Our method gives an efficient and simple way to characterize graphene samples with interacted atoms and is very helpful for future applications of graphene-based devices in the modern microelectronic industry, where AFM is already widely used. Project supported by the National Basic Research Program of China (Grant Nos. 2013CBA01600 and 2011CB932700), the National Natural Science Foundation of China (Grant Nos. 61222112, 61390501 and 51325204), and Chinese Academy of Sciences (Grant Nos. 1731300500015 and XDB07030100).

  18. Exposure of epitaxial graphene on SiC(0001) to atomic hydrogen.

    PubMed

    Guisinger, Nathan P; Rutter, Gregory M; Crain, Jason N; First, Phillip N; Stroscio, Joseph A

    2009-04-01

    Graphene films on SiC exhibit coherent transport properties that suggest the potential for novel carbon-based nanoelectronics applications. Recent studies suggest that the role of the interface between single layer graphene and silicon-terminated SiC can strongly influence the electronic properties of the graphene overlayer. In this study, we have exposed the graphitized SiC to atomic hydrogen in an effort to passivate dangling bonds at the interface, while investigating the results utilizing room temperature scanning tunneling microscopy.

  19. Stark Effect Spectroscopy of Mono- and Few-Layer MoS2.

    PubMed

    Klein, J; Wierzbowski, J; Regler, A; Becker, J; Heimbach, F; Müller, K; Kaniber, M; Finley, J J

    2016-03-01

    We demonstrate electrical control of the A-exciton interband transition in mono- and few-layer MoS2 crystals embedded into photocapacitor devices via the DC Stark effect. Electric field-dependent low-temperature photoluminescence spectroscopy reveals a significant tuneability of the A-exciton transition energy up to ∼ 16 meV from which we extract the mean DC exciton polarizability ⟨β̅N⟩ = (0.58 ± 0.25) × 10(-8) Dm V(-1). The exciton polarizability is shown to be layer-independent, indicating a strong localization of both electron and hole wave functions in each individual layer.

  20. Optical properties and band gap of single- and few-layer MoTe2 crystals.

    PubMed

    Ruppert, Claudia; Aslan, Ozgur Burak; Heinz, Tony F

    2014-11-12

    Single- and few-layer crystals of exfoliated MoTe2 have been characterized spectroscopically by photoluminescence, Raman scattering, and optical absorption measurements. We find that MoTe2 in the monolayer limit displays strong photoluminescence. On the basis of complementary optical absorption results, we conclude that monolayer MoTe2 is a direct-gap semiconductor with an optical band gap of 1.10 eV. This new monolayer material extends the spectral range of atomically thin direct-gap materials from the visible to the near-infrared.

  1. Optical properties and band gap of single- and few-layer MoTe2 crystals.

    PubMed

    Ruppert, Claudia; Aslan, Ozgur Burak; Heinz, Tony F

    2014-11-12

    Single- and few-layer crystals of exfoliated MoTe2 have been characterized spectroscopically by photoluminescence, Raman scattering, and optical absorption measurements. We find that MoTe2 in the monolayer limit displays strong photoluminescence. On the basis of complementary optical absorption results, we conclude that monolayer MoTe2 is a direct-gap semiconductor with an optical band gap of 1.10 eV. This new monolayer material extends the spectral range of atomically thin direct-gap materials from the visible to the near-infrared. PMID:25302768

  2. Third order nonlinear optical response exhibited by mono- and few-layers of WS2

    DOE PAGESBeta

    Torres-Torres, Carlos; Perea-López, Néstor; Elías, Ana Laura; Gutiérrez, Humberto R.; Cullen, David A.; Berkdemir, Ayse; López-Urías, Florentino; Terrones, Humberto; Terrones, Mauricio

    2016-04-13

    In this work, strong third order nonlinear optical properties exhibited by WS2 layers are presented. Optical Kerr effect was identified as the dominant physical mechanism responsible for these third order optical nonlinearities. An extraordinary nonlinear refractive index together with an important contribution of a saturated absorptive response was observed to depend on the atomic layer stacking. Comparative experiments performed in mono- and few-layer samples of WS2 revealed that this material is potentially capable of modulating nonlinear optical processes by selective near resonant induced birefringence. In conclusion, we envision applications for developing all-optical bidimensional nonlinear optical devices.

  3. Stark Effect Spectroscopy of Mono- and Few-Layer MoS2.

    PubMed

    Klein, J; Wierzbowski, J; Regler, A; Becker, J; Heimbach, F; Müller, K; Kaniber, M; Finley, J J

    2016-03-01

    We demonstrate electrical control of the A-exciton interband transition in mono- and few-layer MoS2 crystals embedded into photocapacitor devices via the DC Stark effect. Electric field-dependent low-temperature photoluminescence spectroscopy reveals a significant tuneability of the A-exciton transition energy up to ∼ 16 meV from which we extract the mean DC exciton polarizability ⟨β̅N⟩ = (0.58 ± 0.25) × 10(-8) Dm V(-1). The exciton polarizability is shown to be layer-independent, indicating a strong localization of both electron and hole wave functions in each individual layer. PMID:26845085

  4. Third order nonlinear optical response exhibited by mono- and few-layers of WS2

    NASA Astrophysics Data System (ADS)

    Torres-Torres, Carlos; Perea-López, Néstor; Elías, Ana Laura; Gutiérrez, Humberto R.; Cullen, David A.; Berkdemir, Ayse; López-Urías, Florentino; Terrones, Humberto; Terrones, Mauricio

    2016-06-01

    In this work, strong third order nonlinear optical properties exhibited by WS2 layers are presented. Optical Kerr effect was identified as the dominant physical mechanism responsible for these third order optical nonlinearities. An extraordinary nonlinear refractive index together with an important contribution of a saturated absorptive response was observed to depend on the atomic layer stacking. Comparative experiments performed in mono- and few-layer samples of WS2 revealed that this material is potentially capable of modulating nonlinear optical processes by selective near resonant induced birefringence. We envision applications for developing all-optical bidimensional nonlinear optical devices.

  5. Weak localization and electron-electron interactions in few layer black phosphorus devices

    NASA Astrophysics Data System (ADS)

    Shi, Yanmeng; Gillgren, Nathaniel; Espiritu, Timothy; Tran, Son; Yang, Jiawei; Watanabe, Kenji; Taniguchi, Takahashi; Lau, Chun Ning

    2016-09-01

    Few layer phosphorene (FLP) devices are extensively studied due to their unique electronic properties and potential applications on nano-electronics. Here we present magnetotransport studies which reveal electron-electron interactions as the dominant scattering mechanism in hexagonal boron nitride-encapsulated FLP devices. From weak localization measurements, we estimate the electron dephasing length to be 30 to 100 nm at low temperatures, which exhibits a strong dependence on carrier density n and a power-law dependence on temperature (˜T -0.4). These results establish that the dominant scattering mechanism in FLP is electron-electron interactions.

  6. Determination of the Schottky barrier height of ferromagnetic contacts to few-layer phosphorene

    SciTech Connect

    Anugrah, Yoska; Robbins, Matthew C.; Koester, Steven J.; Crowell, Paul A.

    2015-03-09

    Phosphorene, the 2D analogue of black phosphorus, is a promising material for studying spin transport due to its low spin-orbit coupling and its ½ nuclear spin, which could allow the study of hyperfine effects. In this work, the properties of permalloy (Py) and cobalt (Co) contacts to few-layer phosphorene are presented. The Schottky barrier height was extracted and determined as a function of gate bias. Flat-band barrier heights, relative to the valence band edge, of 110 meV and 200 meV were determined for Py and Co, respectively. These results are important for future studies of spin transport in phosphorene.

  7. Determination of the Schottky barrier height of ferromagnetic contacts to few-layer phosphorene

    NASA Astrophysics Data System (ADS)

    Anugrah, Yoska; Robbins, Matthew C.; Crowell, Paul A.; Koester, Steven J.

    2015-03-01

    Phosphorene, the 2D analogue of black phosphorus, is a promising material for studying spin transport due to its low spin-orbit coupling and its ½ nuclear spin, which could allow the study of hyperfine effects. In this work, the properties of permalloy (Py) and cobalt (Co) contacts to few-layer phosphorene are presented. The Schottky barrier height was extracted and determined as a function of gate bias. Flat-band barrier heights, relative to the valence band edge, of 110 meV and 200 meV were determined for Py and Co, respectively. These results are important for future studies of spin transport in phosphorene.

  8. Strain-engineering the anisotropic electrical conductance of few-layer black phosphorus.

    PubMed

    Fei, Ruixiang; Yang, Li

    2014-05-14

    Newly fabricated few-layer black phosphorus and its monolayer structure, phosphorene, are expected to be promising for electronic and optical applications because of their finite direct band gaps and sizable but anisotropic electronic mobility. By first-principles simulations, we show that this unique anisotropic free-carrier mobility can be controlled by using simple strain conditions. With the appropriate biaxial or uniaxial strain (4-6%), we can rotate the preferred conducting direction by 90°. This will be useful for exploring unusual quantum Hall effects and exotic electronic and mechanical applications based on phosphorene.

  9. Strain-Engineering the Anisotropic Electrical Conductance of Few-Layer Black Phosphorus

    NASA Astrophysics Data System (ADS)

    Fei, Ruixiang; Yang, Li

    2014-05-01

    Newly fabricated monolayer phosphorene and its few-layer structures are expected to be promising for electronic and optical applications because of their finite direct band gaps and sizable but anisotropic electronic mobility. By first-principles simulations, we show that this unique anisotropic conductance can be controlled by using simple strain conditions. With the appropriate biaxial or uniaxial strain, we can rotate the preferred conducting direction by 90 degrees. This will be of useful for exploring quantum Hall effects, and exotic electronic and mechanical applications based on phosphorene.

  10. Weak localization and electron–electron interactions in few layer black phosphorus devices

    NASA Astrophysics Data System (ADS)

    Shi, Yanmeng; Gillgren, Nathaniel; Espiritu, Timothy; Tran, Son; Yang, Jiawei; Watanabe, Kenji; Taniguchi, Takahashi; Lau, Chun Ning

    2016-09-01

    Few layer phosphorene (FLP) devices are extensively studied due to their unique electronic properties and potential applications on nano-electronics. Here we present magnetotransport studies which reveal electron–electron interactions as the dominant scattering mechanism in hexagonal boron nitride-encapsulated FLP devices. From weak localization measurements, we estimate the electron dephasing length to be 30 to 100 nm at low temperatures, which exhibits a strong dependence on carrier density n and a power-law dependence on temperature (∼T ‑0.4). These results establish that the dominant scattering mechanism in FLP is electron–electron interactions.

  11. Step edge influence on barrier height and contact area in vertical heterojunctions between epitaxial graphene and n-type 4H-SiC

    SciTech Connect

    Tadjer, M. J. Nyakiti, L. O.; Robinson, Z.; Anderson, T. J.; Myers-Ward, R. L.; Wheeler, V. D.; Eddy, C. R.; Gaskill, D. K.; Koehler, A. D.; Hobart, K. D.; Kub, F. J.

    2014-02-17

    Vertical rectifying contacts of epitaxial graphene grown by Si sublimation on the Si-face of 4H-SiC epilayers were investigated. Forward bias preferential conduction through the step edges was correlated by linear current density normalization. This phenomenon was observed on samples with 2.7–5.8 monolayers of epitaxial graphene as determined by X-ray photoelectron spectroscopy. A modified Richardson plot was implemented to extract the barrier height (0.81 eV at 290 K, 0.99 eV at 30 K) and the electrically dominant SiC step length of a Ti/Al contact overlapping a known region of approximately 0.52 μm wide SiC terraces.

  12. Growth and characterization of Al2O3 films on fluorine functionalized epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Robinson, Zachary R.; Jernigan, Glenn G.; Wheeler, Virginia D.; Hernández, Sandra C.; Eddy, Charles R.; Mowll, Tyler R.; Ong, Eng Wen; Ventrice, Carl A.; Geisler, Heike; Pletikosic, Ivo; Yang, Hongbo; Valla, Tonica

    2016-08-01

    Intelligent engineering of graphene-based electronic devices on SiC(0001) requires a better understanding of processes used to deposit gate-dielectric materials on graphene. Recently, Al2O3 dielectrics have been shown to form conformal, pinhole-free thin films by functionalizing the top surface of the graphene with fluorine prior to atomic layer deposition (ALD) of the Al2O3 using a trimethylaluminum (TMA) precursor. In this work, the functionalization and ALD-precursor adsorption processes have been studied with angle-resolved photoelectron spectroscopy, low energy electron diffraction, and X-ray photoelectron spectroscopy. It has been found that the functionalization process has a negligible effect on the electronic structure of the graphene, and that it results in a twofold increase in the adsorption of the ALD-precursor. In situ TMA-dosing and XPS studies were also performed on three different Si(100) substrates that were terminated with H, OH, or dangling Si-bonds. This dosing experiment revealed that OH is required for TMA adsorption. Based on those data along with supportive in situ measurements that showed F-functionalization increases the amount of oxygen (in the form of adsorbed H2O) on the surface of the graphene, a model for TMA-adsorption on graphene is proposed that is based on a reaction of a TMA molecule with OH.

  13. Bandgap opening in few-layered monoclinic MoTe2

    NASA Astrophysics Data System (ADS)

    Keum, Dong Hoon; Cho, Suyeon; Kim, Jung Ho; Choe, Duk-Hyun; Sung, Ha-Jun; Kan, Min; Kang, Haeyong; Hwang, Jae-Yeol; Kim, Sung Wng; Yang, Heejun; Chang, K. J.; Lee, Young Hee

    2015-06-01

    Layered transition metal dichalcogenides (TMDs) have attracted renewed interest owing to their potential use as two-dimensional components in next-generation devices. Although group 6 TMDs, such as MX2 with M = (Mo, W) and X = (S, Se, Te), can exist in several polymorphs, most studies have been conducted with the semiconducting hexagonal (2H) phase as other polymorphs often exhibit inhomogeneous formation. Here, we report a reversible structural phase transition between the hexagonal and stable monoclinic (distorted octahedral or 1T') phases in bulk single-crystalline MoTe2. Furthermore, an electronic phase transition from semimetallic to semiconducting is shown as 1T'-MoTe2 crystals go from bulk to few-layered. Bulk 1T'-MoTe2 crystals exhibit a maximum carrier mobility of 4,000 cm2 V-1 s-1 and a giant magnetoresistance of 16,000% in a magnetic field of 14 T at 1.8 K. In the few-layered form, 1T'-MoTe2 exhibits a bandgap opening of up to 60 meV, which our density functional theory calculations identify as arising from strong interband spin-orbit coupling. We further clarify that the Peierls distortion is a key mechanism to stabilize the monoclinic structure. This class of semiconducting MoTe2 unlocks the possibility of topological quantum devices based on non-trivial Z2-band-topology quantum spin Hall insulators in monoclinic TMDs (ref. ).

  14. Electronic and thermoelectric properties of few-layer transition metal dichalcogenides

    SciTech Connect

    Wickramaratne, Darshana; Lake, Roger K.; Zahid, Ferdows

    2014-03-28

    The electronic and thermoelectric properties of one to four monolayers of MoS{sub 2}, MoSe{sub 2}, WS{sub 2}, and WSe{sub 2} are calculated. For few layer thicknesses, the near degeneracies of the conduction band K and Σ valleys and the valence band Γ and K valleys enhance the n-type and p-type thermoelectric performance. The interlayer hybridization and energy level splitting determine how the number of modes within k{sub B}T of a valley minimum changes with layer thickness. In all cases, the maximum ZT coincides with the greatest near-degeneracy within k{sub B}T of the band edge that results in the sharpest turn-on of the density of modes. The thickness at which this maximum occurs is, in general, not a monolayer. The transition from few layers to bulk is discussed. Effective masses, energy gaps, power-factors, and ZT values are tabulated for all materials and layer thicknesses.

  15. Ionic-Liquid Gated Few-layer MoS2 Field-Effect Transistors

    NASA Astrophysics Data System (ADS)

    Perera, Meeghage; Lin, Ming-Wei; Chuang, Hsun-Jen; Chamlagain, Bhim; Wang, Chongyu; Tan, Xuebin; Cheng, Mark Ming-Cheng; Zhou, Zhixian

    2013-03-01

    We report the electrical characterization of ionic-liquid-gated bilayer and few-layer MoS2 field-effect transistors. The extrinsic mobility of our ionic-liquid-gated devices exceeds 70 cm2V-1S-1 at 250 K, which is 1-2 orders of magnitude higher than that measured in the Si back-gate configuration (without ionic liquid). These devices also show ambipolar behavior with a high ON-OFF current ratio of > 107 for electrons and > 106 for holes, and a near ideal subthreshold swing (SS) of ~ 50 mV/decade at 250 K for the electron channel. More significantly, we show that the mobility increases from ~ 100 cm2V-1S-1 at 180 K to ~ 220 cm2V-1S-1 at 77K as the temperature decreases following a μ ~ T-γ dependence with γ ~ 1, indicating that the intrinsic phonon-limited mobility can be achieved in few-layer MoS2 FETs. We attribute the enhanced device performance to the drastic reduction of the Schottky barrier width (thus higher tunneling efficiency) via highly efficient band bending at the MoS2/metal interface afforded by the extremely large electrical double layer capacitance of the ionic liquid. This work was supported by NSF (No. ECCS-1128297).

  16. Characterizing and tuning excitons in monolayer and few-layer MoS 2

    NASA Astrophysics Data System (ADS)

    Qiu, Diana Y.; da Jornada, Felipe H.; Louie, Steven G.

    2015-03-01

    We use the GW-BSE method to study excitons arising from transitions in different regions of momentum space in mono- and few-layer MoS2 and consider mechanisms to fundamentally change the features and character of the optical spectra. Our calculations show that sharp spatial variations in dielectric screening make 2D systems, such as MoS2 , computationally challenging, requiring very fine k-space sampling to resolve the structure of excitonic wave functions and converge binding energies. In highly converged calculations, we identify a series of excitons arising from transitions at the K/K' valleys in the Brillouin zone, a higher energy series arising from transitions in the valley of a Mexican hat potential centered at the Γ point, and transitions at the indirect gap from Γ to Λ in few-layer MoS2 . As layer number changes, these states, which have varying character, momentum-space structure and real-space locations, are affected differently by changes in confinement and hybridization. By tuning layer number and strain, we find that we not only can tune the excitation energies but can also change the relative energies of the various excitonic series, allowing for movement of the lowest energy exciton between different regions of the Brillouin zone This work was supported by NSF Grant No. DMR10-1006184 and U.S. DOE under Contract No. DE-AC02-05CH11231.

  17. Ripples near edge terminals in MoS2 few layers and pyramid nanostructures

    NASA Astrophysics Data System (ADS)

    Mills, Adam; Yu, Yifei; Chen, Chuanhui; Huang, Bevin; Cao, Linyou; Tao, Chenggang

    2016-02-01

    Atomically thin transition-metal dichalcogenides are of great interest due to their intriguing physical properties and potential applications. Here, we report our findings from scanning tunneling microscopy and spectroscopy investigations on molybdenum disulfide (MoS2) mono- to few-layers and pyramid nanostructures synthesized through chemical vapor deposition. On the few-layered MoS2 nanoplatelets grown on gallium nitride (GaN) and pyramid nanostructures on highly oriented pyrolytic graphite, we observed an intriguing curved region near the edge terminals. The measured band gap on these curved regions is 1.96 ± 0.10 eV, consistent with the value of the direct band gap in MoS2 monolayers. The curved features near the edge terminals and the associated electronic properties may contribute to the catalytic behaviors of MoS2 nanostructures and have potential applications in future electronic devices and energy-related products based on MoS2 nanostructures.

  18. Photovoltaic effect in few-layer black phosphorus PN junctions defined by local electrostatic gating.

    PubMed

    Buscema, Michele; Groenendijk, Dirk J; Steele, Gary A; van der Zant, Herre S J; Castellanos-Gomez, Andres

    2014-08-28

    In conventional photovoltaic solar cells, photogenerated carriers are extracted by the built-in electric field of a semiconductor PN junction, defined by ionic dopants. In atomically thin semiconductors, the doping level can be controlled by the field effect, enabling the implementation of electrically tunable PN junctions. However, most two-dimensional (2D) semiconductors do not show ambipolar transport, which is necessary to realize PN junctions. Few-layer black phosphorus (b-P) is a recently isolated 2D semiconductor with direct bandgap, high mobility, large current on/off ratios and ambipolar operation. Here we fabricate few-layer b-P field-effect transistors with split gates and hexagonal boron nitride dielectric. We demonstrate electrostatic control of the local charge carrier type and density in the device. Illuminating a gate-defined PN junction, we observe zero-bias photocurrents and significant open-circuit voltages due to the photovoltaic effect. The small bandgap of the material allows power generation for illumination wavelengths up to 940 nm, attractive for energy harvesting in the near-infrared.

  19. Low-frequency interlayer breathing mode in few-layer black phosphorus

    NASA Astrophysics Data System (ADS)

    Ling, Xi; Huang, Shengxi; Liang, Liangbo; Meunier, Vincent; Dresselhaus, Mildred

    2015-03-01

    Black phosphorus (BP), as a layered material, has attracted intense interest recently. Many interesting electronic and optoelectronic properties are being explored based on its unique anisotropic structure. In this work, we studied the Raman spectra in few-layer BP, including the intralayer and interlayer vibrational modes. Besides the three typical Raman modes Agfew-layer BP, as predicted by the first-principles density functional theory (DFT) calculation. The interlayer breathing mode at around 87 cm-1 was assigned as Ag0, since the DFT calculation result showed it has the symmetry of Ag0. In addition, the polarization dependence of the Raman modes in BP is studied systematically. Both the DFT calculation and the experimental results show that the polarization dependence profiles are sensitive to the crystal orientation of BP. In addition, the temperature dependence of the modes is studied in the range of -150 °C to room temperature. It is found that the Ag0 mode has almost no dependence on the temperature change, and the out-of-plane mode (Ag1) has weaker dependence than the in-plane modes (B2g and Ag2) .

  20. Gate tunable quantum oscillations in air-stable and high mobility few-layer phosphorene heterostructures

    NASA Astrophysics Data System (ADS)

    Gillgren, Nathaniel; Wickramaratne, Darshana; Shi, Yanmeng; Espiritu, Tim; Yang, Jiawei; Hu, Jin; Wei, Jiang; Liu, Xue; Mao, Zhiqiang; Watanabe, Kenji; Taniguchi, Takashi; Bockrath, Marc; Barlas, Yafis; Lake, Roger K.; Lau, Chun Ning

    2015-03-01

    As the only non-carbon elemental layered allotrope, few-layer black phosphorus or phosphorene has emerged as a novel two-dimensional (2D) semiconductor with both high bulk mobility and a band gap. Here we report fabrication and transport measurements of phosphorene-hexagonal BN (hBN) heterostructures with one-dimensional edge contacts. These transistors are stable in ambient conditions for >300 h, and display ambipolar behavior, a gate-dependent metal-insulator transition, and mobility up to 4000 cm2 V-1 s-1. At low temperatures, we observe gate-tunable Shubnikov de Haas magneto-oscillations and Zeeman splitting in magnetic field with an estimated g-factor ˜2. The cyclotron mass of few-layer phosphorene (FLP) holes is determined to increase from 0.25 to 0.31 me as the Fermi level moves towards the valence band edge. Our results underscore the potential of FLP as both a platform for novel 2D physics and an electronic material for semiconductor applications.

  1. Atomically resolved orientational ordering of C60 molecules on epitaxial graphene on Cu(111)

    NASA Astrophysics Data System (ADS)

    Jung, Minbok; Shin, Dongbin; Sohn, So-Dam; Kwon, Soon-Yong; Park, Noejung; Shin, Hyung-Joon

    2014-09-01

    A detailed understanding of interactions between molecules and graphene is one of the key issues for tailoring the properties of graphene-based molecular devices, because the electronic and structural properties of molecular layers on surfaces are determined by intermolecular and molecule-substrate interactions. Here, we present the atomically resolved experimental measurements of the self-assembled fullerene molecules on single-layer graphene on Cu(111). Fullerene molecules form a (4 × 4) superstructure on graphene/Cu(111), revealing only single molecular orientation. We can resolve the exact adsorption site and the configuration of fullerene by means of low-temperature scanning tunnelling microscopy (LT-STM) and density functional theory (DFT) calculations. The adsorption orientation can be explained in terms of the competition between intermolecular interactions and molecule-substrate interactions, where strong Coulomb interactions among the fullerenes determine the in-plane orientation of the fullerene. Our results provide important implications for developing carbon-based organic devices using a graphene template in the future.A detailed understanding of interactions between molecules and graphene is one of the key issues for tailoring the properties of graphene-based molecular devices, because the electronic and structural properties of molecular layers on surfaces are determined by intermolecular and molecule-substrate interactions. Here, we present the atomically resolved experimental measurements of the self-assembled fullerene molecules on single-layer graphene on Cu(111). Fullerene molecules form a (4 × 4) superstructure on graphene/Cu(111), revealing only single molecular orientation. We can resolve the exact adsorption site and the configuration of fullerene by means of low-temperature scanning tunnelling microscopy (LT-STM) and density functional theory (DFT) calculations. The adsorption orientation can be explained in terms of the competition

  2. Isolation and characterization of nanosheets containing few layers of the Aurivillius family of oxides and metal-organic compounds

    NASA Astrophysics Data System (ADS)

    Sreedhara, M. B.; Prasad, B. E.; Moirangthem, Monali; Murugavel, R.; Rao, C. N. R.

    2015-04-01

    Nanosheets containing few-layers of ferroelectric Aurivillius family of oxides, Bi2An-1BnO3n+3 (where A=Bi3+, Ba2+ etc. and B=Ti4+, Fe3+ etc.) with n=3, 4, 5, 6 and 7 have been prepared by reaction with n-butyllithium, followed by exfoliation in water. The few-layer samples have been characterized by Tyndall cones, atomic force microscopy, optical spectroscopy and other techniques. The few-layer species have a thickness corresponding to a fraction of the c-parameter along which axis the perovskite layers are stacked. Magnetization measurements have been carried out on the few-layer samples containing iron. Few-layer species of a few layered metal-organic compounds have been obtained by ultrasonication and characterized by Tyndall cones, atomic force microscopy, optical spectroscopy and magnetic measurements. Significant changes in the optical spectra and magnetic properties are found in the few-layer species compared to the bulk samples. Few-layer species of the Aurivillius family of oxides may find uses as thin layer dielectrics in photovoltaics and other applications.

  3. Observation of the retarded transportation of a photogenerated hole on epitaxial graphene.

    PubMed

    Wang, Shujie; Yuan, Xizhi; Bi, Xiaofeng; Wang, Xiaomei; Huang, Qingsong

    2015-10-01

    Graphene is usually adopted as an assistant additive for catalysts in photocatalytic processes, because of its ability to accelerate the separation of photogenerated charge carriers. To elucidate the mechanism, hydrogen peroxide is adopted to convert the O2(-)˙ active species into OH˙ for degradation of an organic dye. If the pH value is less than 7, the concentration of the OH˙ species can be reduced more quickly with the addition of graphene than without, because negatively charged electrons can be transported quickly on graphene. If the pH value is larger than 7, the concentration of OH˙ can be promoted by the catalyst SiC with photogenerated h(+) release and reaction with OH(-), however the concentration is reduced if the SiC catalyst is covered by a graphene sheet, as it retards h(+) release from the SiC substrate. Our findings have provided a certification for the role of graphene in photo-catalytic processes. PMID:26308861

  4. Few-layered MoS2 nanosheets wrapped ultrafine TiO2 nanobelts with enhanced photocatalytic property

    NASA Astrophysics Data System (ADS)

    Li, Haidong; Wang, Yana; Chen, Guohui; Sang, Yuanhua; Jiang, Huaidong; He, Jiating; Li, Xu; Liu, Hong

    2016-03-01

    Photocatalytic materials comprised of semiconductor nanostructures have attracted tremendous scientific and technological interest over the last 30 years. This is due to the fact that these photocatalytic materials have unique properties that allow for an effective direct energy transfer from light to highly reactive chemical species which are applicable in the remediation of environmental pollutants and photocatalytic hydrogen generation. Heterostructured photocatalysts are a promising type of photocatalyst which can combine the properties of different components to generate a synergic effect, resulting in a high photocatalytic activity. In this work, a heterostructured photocatalyst comprised of few-layered MoS2 nanosheets coated on a TiO2 nanobelts surface was synthesized through a simple hydrothermal treatment. The hybrid heterostructures with enhanced broad spectrum photocatalytic properties can harness UV and visible light energy to decompose organic contaminants in aqueous solutions as well as split water to hydrogen and oxygen. The mechanism of the enhancement is that the MoS2/TiO2 nanobelts heterostructure can enhance the separation of the photo-induced carriers, which results in a higher photocurrent due to the special electronic characteristics of the graphene-like layered MoS2 nanosheets. This methodology is potentially applicable to the synthesis of a range of hybrid nanostructures with promising applications in photocatalysis and other relevant areas.Photocatalytic materials comprised of semiconductor nanostructures have attracted tremendous scientific and technological interest over the last 30 years. This is due to the fact that these photocatalytic materials have unique properties that allow for an effective direct energy transfer from light to highly reactive chemical species which are applicable in the remediation of environmental pollutants and photocatalytic hydrogen generation. Heterostructured photocatalysts are a promising type of

  5. Epitaxial growth of π-stacked perfluoropentacene on graphene-coated quartz.

    PubMed

    Salzmann, Ingo; Moser, Armin; Oehzelt, Martin; Breuer, Tobias; Feng, Xinliang; Juang, Zhen-Yu; Nabok, Dmitrii; Della Valle, Raffaele G; Duhm, Steffen; Heimel, Georg; Brillante, Aldo; Venuti, Elisabetta; Bilotti, Ivano; Christodoulou, Christos; Frisch, Johannes; Puschnig, Peter; Draxl, Claudia; Witte, Gregor; Müllen, Klaus; Koch, Norbert

    2012-12-21

    Chemical-vapor-deposited large-area graphene is employed as the coating of transparent substrates for the growth of the prototypical organic n-type semiconductor perfluoropentacene (PFP). The graphene coating is found to cause face-on growth of PFP in a yet unknown substrate-mediated polymorph, which is solved by combining grazing-incidence X-ray diffraction with theoretical structure modeling. In contrast to the otherwise common herringbone arrangement of PFP in single crystals and "standing" films, we report a π-stacked arrangement of coplanar molecules in "flat-lying" films, which exhibit an exceedingly low π-stacking distance of only 3.07 Å, giving rise to significant electronic band dispersion along the π-stacking direction, as evidenced by ultraviolet photoelectron spectroscopy. Our study underlines the high potential of graphene for use as a transparent electrode in (opto-)electronic applications, where optimized vertical transport through flat-lying conjugated organic molecules is desired.

  6. Light-Induced Ambient Degradation of Few-Layer Black Phosphorus: Mechanism and Protection.

    PubMed

    Zhou, Qionghua; Chen, Qian; Tong, Yilong; Wang, Jinlan

    2016-09-12

    The environmental instability of single- or few-layer black phosphorus (BP) has become a major hurdle for BP-based devices. The degradation mechanism remains unclear and finding ways to protect BP from degradation is still highly challenging. Based on ab initio electronic structure calculations and molecular dynamics simulations, a three-step picture on the ambient degradation of BP is provided: generation of superoxide under light, dissociation of the superoxide, and eventual breakdown under the action of water. The well-matched band gap and band-edge positions for the redox potential accelerates the degradation of thinner BP. Furthermore, it was found that the formation of P-O-P bonds can greatly stabilize the BP framework. A possible protection strategy using a fully oxidized BP layer as the native capping is thus proposed. Such a fully oxidization layer can resist corrosion from water and leave the BP underneath intact with simultaneous high hole mobility. PMID:27529543

  7. Role of Interlayer Coupling on the Evolution of Band Edges in Few-Layer Phosphorene.

    PubMed

    Wang, V; Liu, Y C; Kawazoe, Y; Geng, W T

    2015-12-17

    Using first-principles calculations, we have investigated the evolution of band edges in few-layer phosphorene as a function of the number of P layers. Our results predict that monolayer phosphorene is an indirect band gap semiconductor and its valence band edge is extremely sensitive to strain. Its band gap could undergo an indirect-to-direct transition under a lattice expansion as small as 1% along the zigzag direction. A semiempirical interlayer coupling model is proposed, which can reproduce the evolution of valence band edges obtained by first-principles calculations well. We conclude that the interlayer coupling plays a dominant role in the evolution of the band edges via decreasing both band gap and carrier effective masses with the increase of phosphorene thickness. Scrutiny of the orbital-decomposed band structure provides a better understanding of the upward shift of the valence band maximum, surpassing that of the conduction band minimum.

  8. Optical Properties and Band Gap of Single- and Few-Layer MoTe2 Crystals

    NASA Astrophysics Data System (ADS)

    Aslan, Ozgur Burak; Ruppert, Claudia; Heinz, Tony

    2015-03-01

    Single- and few-layer crystals of exfoliated MoTe2 have been characterized spectroscopically by photoluminescence, Raman scattering, and optical absorption measurements. We find that MoTe2 in the monolayer limit displays strong photoluminescence. On the basis of complementary optical absorption results, we conclude that monolayer MoTe2 is a direct-gap semiconductor with an optical band gap of 1.10 eV. This new monolayer material extends the spectral range of atomically thin direct-gap materials from the visible to the near-infrared. Supported by the NSF through Grant DMR-1124894 for sample preparation and characterization by the O?ce of Naval Research for analysis. C.R. acknowledges support from the Alexander von Humboldt Foundation.

  9. Double resonance Raman modes in monolayer and few-layer MoTe2

    NASA Astrophysics Data System (ADS)

    Guo, Huaihong; Yang, Teng; Yamamoto, Mahito; Zhou, Lin; Ishikawa, Ryo; Ueno, Keiji; Tsukagoshi, Kazuhito; Zhang, Zhidong; Dresselhaus, Mildred S.; Saito, Riichiro

    2015-05-01

    We study the second-order Raman process of mono- and few-layer MoTe2, by combining ab initio density functional perturbation calculations with experimental Raman spectroscopy using 532, 633, and 785 nm excitation lasers. The calculated electronic band structure and the density of states show that the resonance Raman process occurs at the M point in the Brillouin zone, where a strong optical absorption occurs due to a logarithmic Van Hove singularity of the electronic density of states. The double resonance Raman process with intervalley electron-phonon coupling connects two of the three inequivalent M points in the Brillouin zone, giving rise to second-order Raman peaks due to the M -point phonons. The calculated vibrational frequencies of the second-order Raman spectra agree with the observed laser-energy-dependent Raman shifts in the experiment.

  10. Large-area few-layer MoS2 deposited by sputtering

    NASA Astrophysics Data System (ADS)

    Huang, Jyun-Hong; Chen, Hsing-Hung; Liu, Pang-Shiuan; Lu, Li-Syuan; Wu, Chien-Ting; Chou, Cheng-Tung; Lee, Yao-Jen; Li, Lain-Jong; Chang, Wen-Hao; Hou, Tuo-Hung

    2016-06-01

    Direct magnetron sputtering of transition metal dichalcogenide targets is proposed as a new approach for depositing large-area two-dimensional layered materials. Bilayer to few-layer MoS2 deposited by magnetron sputtering followed by post-deposition annealing shows superior area scalability over 20 cm2 and layer-by-layer controllability. High crystallinity of layered MoS2 was confirmed by Raman, photo-luminescence, and transmission electron microscopy analysis. The sputtering temperature and annealing ambience were found to play an important role in the film quality. The top-gate field-effect transistor by using the layered MoS2 channel shows typical n-type characteristics with a current on/off ratio of approximately 104. The relatively low mobility is attributed to the small grain size of 0.1-1 μm with a trap charge density in grain boundaries of the order of 1013 cm-2.

  11. Structure and Electronic Properties of Single- to Few Layers Molybdenum Disulfide Films

    NASA Astrophysics Data System (ADS)

    Trainer, D.; Putilov, A.; Wolak, M.; Chandrasena, R. U.; Kronast, F.; Gray, A. X.; Xi, X. X.; Iavarone, M.

    Using high resolution scanning tunneling microscopy and spectroscopy (STM/STS) we have investigated the electronic properties of mono- to few layers molybdenum disulfide films grown on HOPG using ambient pressure chemical vapor deposition (APCVD). Atomic force microscopy and STM show that this growth technique produces crystalline triangular and hexagonal islands with varying thicknesses in 1ML increments. The films exhibited a suppression of quasiparticle band-gap as a function of layer number as measured by local spectroscopy. Changes in the valence band edge were supported by photoemission electron microscopy (PEEM) measurements. We also report on a strain-induced contraction of the quasiparticle band-gap in proximity to grain boundaries and defects. This work was supported as part of the Center for the Computational Design of Functional Layered Materials, an Energy Frontier Research Center funded by the U.S. DOE, BES under Award DE-SC0012575.

  12. Frenkel-like Wannier-Mott excitons in few-layer Pb I2

    NASA Astrophysics Data System (ADS)

    Toulouse, Alexis S.; Isaacoff, Benjamin P.; Shi, Guangsha; Matuchová, Marie; Kioupakis, Emmanouil; Merlin, Roberto

    2015-04-01

    Optical measurements and first-principles calculations of the band structure and exciton states in direct-gap bulk and few-layer Pb I2 indicate that the n =1 exciton is Frenkel-like in nature in that its energy exhibits a weak dependence on thickness down to atomic-length scales. Results reveal large increases in the gap and exciton binding energy with a decreasing number of layers and a transition of the fundamental gap, which becomes indirect for one and two monolayers. Calculated values are in reasonable agreement with a particle-in-a-box model relying on the Wannier-Mott theory of exciton formation. General arguments and existing data suggest that the Frenkel-like character of the lowest exciton is a universal feature of wide-gap layered semiconductors whose effective masses and dielectric constants give bulk Bohr radii that are on the order of the layer spacing.

  13. Stacking Fault Enriching the Electronic and Transport Properties of Few-Layer Phosphorenes and Black Phosphorus.

    PubMed

    Lei, Shuangying; Wang, Han; Huang, Lan; Sun, Yi-Yang; Zhang, Shengbai

    2016-02-10

    Interface engineering is critical for enriching the electronic and transport properties of two-dimensional materials. Here, we identify a new stacking, named Aδ, in few-layer phosphorenes (FLPs) and black phosphorus (BP) based on first-principles calculation. With its low formation energy, the Aδ stacking could exist in FLPs and BP as a stacking fault. The presence of the Aδ stacking fault induces a direct to indirect transition of the band gap in FLPs. It also affects the carrier mobilities by significantly increasing the carrier effective masses. More importantly, the Aδ stacking enables the fabrication of a whole spectrum of lateral junctions with all the type-I, II, and III alignments simply through the manipulation of the van der Waals stacking without resorting to any chemical modification. This is achieved by the widely tunable electron affinity and ionization potential of FLPs and BP with the Aδ stacking. PMID:26799596

  14. Basal-plane thermal conductivity of few-layer molybdenum disulfide

    SciTech Connect

    Jo, Insun; Ou, Eric; Shi, Li; Pettes, Michael Thompson; Wu, Wei

    2014-05-19

    We report the in-plane thermal conductivity of suspended exfoliated few-layer molybdenum disulfide (MoS{sub 2}) samples that were measured by suspended micro-devices with integrated resistance thermometers. The obtained room-temperature thermal conductivity values are (44–50) and (48–52) W m{sup −1} K{sup −1} for two samples that are 4 and 7 layers thick, respectively. For both samples, the peak thermal conductivity occurs at a temperature close to 120 K, above which the thermal conductivity is dominated by intrinsic phonon-phonon scattering although phonon scattering by surface disorders can still play an important role in these samples especially at low temperatures.

  15. Environmental effects in mechanical properties of few-layer black phosphorus

    NASA Astrophysics Data System (ADS)

    Moreno-Moreno, Miriam; Lopez-Polin, Guillermo; Castellanos-Gomez, Andres; Gomez-Navarro, Cristina; Gomez-Herrero, Julio

    2016-09-01

    We report on the mechanical properties of few-layer black phosphorus (BP) nanosheets, in high vacuum and as a function of time of exposure to atmospheric conditions. BP flakes with thicknesses ranging from 4 to 30 nm suspended over circular holes are characterized by nanoindentations using an atomic force microscope tip. From measurements in high vacuum an elastic modulus of 46 ± 10 GPa and breaking strength of 2.4 ± 1 GPa are estimated. Both magnitudes are independent of the thickness of the flakes. Our results show that the exposure to air has substantial influence in the mechanical response of flakes thinner than 6 nm but small effects on thicker flakes.

  16. Quasiparticle energies, excitons, and optical spectra of few-layer black phosphorus

    NASA Astrophysics Data System (ADS)

    Tran, Vy; Fei, Ruixiang; Yang, Li

    2015-12-01

    We report first-principles GW-Bethe-Salpeter-equation (BSE) studies of excited-state properties of few-layer black phosphorus (BP) (phosphorene). With improved GW computational methods, we obtained converged quasiparticle band gaps and optical absorption spectra by the single-shot (G0W0) procedure. Moreover, we reveal fine structures of anisotropic excitons, including the series of one-dimensional like wave functions, spin singlet-triplet splitting, and electron-hole binding energy spectra by solving BSE. An effective-mass model is employed to describe these electron-hole pairs, shedding light on estimating the exciton binding energy of anisotropic two-dimensional semiconductors without expensive ab initio simulations. Finally, the anisotropic optical response of BP is explained by using optical selection rules based on the projected single-particle density of states at band edges.

  17. Nonlocal Response and Anamorphosis: The Case of Few-Layer Black Phosphorus.

    PubMed

    Mishchenko, A; Cao, Y; Yu, G L; Woods, C R; Gorbachev, R V; Novoselov, K S; Geim, A K; Levitov, L S

    2015-10-14

    Few-layer black phosphorus was recently rediscovered as a narrow-bandgap atomically thin semiconductor, attracting unprecedented attention due to its interesting properties. One feature of this material that sets it apart from other atomically thin crystals is its structural in-plane anisotropy which manifests in strongly anisotropic transport characteristics. However, traditional angle-resolved conductance measurements present a challenge for nanoscale systems, calling for new approaches in precision studies of transport anisotropy. Here, we show that the nonlocal response, being exponentially sensitive to the anisotropy value, provides a powerful tool for determining the anisotropy in black phosphorus. This is established by combining measurements of the orientation-dependent nonlocal resistance response with the analysis based on the anamorphosis relations. We demonstrate that the nonlocal response can differ by orders of magnitude for different crystallographic directions even when the anisotropy is at most order-one, allowing us to extract accurate anisotropy values.

  18. Light-Induced Ambient Degradation of Few-Layer Black Phosphorus: Mechanism and Protection.

    PubMed

    Zhou, Qionghua; Chen, Qian; Tong, Yilong; Wang, Jinlan

    2016-09-12

    The environmental instability of single- or few-layer black phosphorus (BP) has become a major hurdle for BP-based devices. The degradation mechanism remains unclear and finding ways to protect BP from degradation is still highly challenging. Based on ab initio electronic structure calculations and molecular dynamics simulations, a three-step picture on the ambient degradation of BP is provided: generation of superoxide under light, dissociation of the superoxide, and eventual breakdown under the action of water. The well-matched band gap and band-edge positions for the redox potential accelerates the degradation of thinner BP. Furthermore, it was found that the formation of P-O-P bonds can greatly stabilize the BP framework. A possible protection strategy using a fully oxidized BP layer as the native capping is thus proposed. Such a fully oxidization layer can resist corrosion from water and leave the BP underneath intact with simultaneous high hole mobility.

  19. Stacking Fault Enriching the Electronic and Transport Properties of Few-Layer Phosphorenes and Black Phosphorus.

    PubMed

    Lei, Shuangying; Wang, Han; Huang, Lan; Sun, Yi-Yang; Zhang, Shengbai

    2016-02-10

    Interface engineering is critical for enriching the electronic and transport properties of two-dimensional materials. Here, we identify a new stacking, named Aδ, in few-layer phosphorenes (FLPs) and black phosphorus (BP) based on first-principles calculation. With its low formation energy, the Aδ stacking could exist in FLPs and BP as a stacking fault. The presence of the Aδ stacking fault induces a direct to indirect transition of the band gap in FLPs. It also affects the carrier mobilities by significantly increasing the carrier effective masses. More importantly, the Aδ stacking enables the fabrication of a whole spectrum of lateral junctions with all the type-I, II, and III alignments simply through the manipulation of the van der Waals stacking without resorting to any chemical modification. This is achieved by the widely tunable electron affinity and ionization potential of FLPs and BP with the Aδ stacking.

  20. Few-layer black phosphorus based saturable absorber mirror for pulsed solid-state lasers.

    PubMed

    Ma, Jie; Lu, Shunbin; Guo, Zhinan; Xu, Xiaodong; Zhang, Han; Tang, Dingyuan; Fan, Dianyuan

    2015-08-24

    We experimentally demonstrated that few-layer black phosphorus (BP) could be used as an optical modulator for solid-state lasers to generate short laser pulses. The BP flakes were fabricated by the liquid phase exfoliation method and drop-casted on a high-reflection mirror to form a BP-based saturable absorber mirror (BP-SAM). Stable Q-switched pulses with a pulse width of 620 ns at the wavelength of 1046 nm were obtained in a Yb:CaYAlO(4) (Yb:CYA) laser with the BP-SAM. The generated pulse train has a repetition rate of 113.6 kHz and an average output power of 37 mW. Our results show that the BP-SAMs could have excellent prospective for ultrafast photonics applications.

  1. Nonlocal Response and Anamorphosis: The Case of Few-Layer Black Phosphorus

    NASA Astrophysics Data System (ADS)

    Mishchenko, A.; Cao, Y.; Yu, G. L.; Woods, C. R.; Gorbachev, R. V.; Novoselov, K. S.; Geim, A. K.; Levitov, L. S.

    2015-10-01

    Few-layer black phosphorus was recently rediscovered as a narrow-bandgap atomically thin semiconductor and has already attracted unprecedented attention due to its interesting properties. One feature of this material that sets it apart from other atomically thin crystals is its structural in-plane anisotropy which manifests in strongly anisotropic transport characteristics. However, traditional angle-resolved conductance measurements present a challenge for nanoscale systems such as black phosphorus, calling for new approaches in precision studies of transport anisotropy. Here we show that the nonlocal response, being exponentially sensitive to the anisotropy value, provides a powerful tool for determining the anisotropy. This is established by combining measurements of the orientation-dependent nonlocal resistance response with the analysis based on the anamorphosis relations. We demonstrate that the nonlocal response can differ by orders of magnitude for different crystallographic directions even when the anisotropy is at most order-one, allowing us to extract accurate anisotropy values.

  2. Coherent Lattice Vibrations in Mono- and Few-Layer WSe2.

    PubMed

    Jeong, Tae Young; Jin, Byung Moon; Rhim, Sonny H; Debbichi, Lamjed; Park, Jaesung; Jang, Yu Dong; Lee, Hyang Rok; Chae, Dong-Hun; Lee, Donghan; Kim, Yong-Hoon; Jung, Suyong; Yee, Ki Ju

    2016-05-24

    We report the observation of coherent lattice vibrations in mono- and few-layer WSe2 in the time domain, which were obtained by performing time-resolved transmission measurements. Upon the excitation of ultrashort pulses with the energy resonant to that of A excitons, coherent oscillations of the A1g optical phonon and longitudinal acoustic phonon at the M point of the Brillouin zone (LA(M)) were impulsively generated in monolayer WSe2. In multilayer WSe2 flakes, the interlayer breathing mode (B1) is found to be sensitive to the number of layers, demonstrating its usefulness in characterizing layered transition metal dichalcogenide materials. On the basis of temperature-dependent measurements, we find that the A1g optical phonon mode decays into two acoustic phonons through the anharmonic decay process. PMID:27102714

  3. Micro-Raman and micro-transmission imaging of epitaxial graphene grown on the Si and C faces of 6H-SiC

    PubMed Central

    2011-01-01

    Micro-Raman and micro-transmission imaging experiments have been done on epitaxial graphene grown on the C- and Si-faces of on-axis 6H-SiC substrates. On the C-face it is shown that the SiC sublimation process results in the growth of long and isolated graphene ribbons (up to 600 μm) that are strain-relaxed and lightly p-type doped. In this case, combining the results of micro-Raman spectroscopy with micro-transmission measurements, we were able to ascertain that uniform monolayer ribbons were grown and found also Bernal stacked and misoriented bilayer ribbons. On the Si-face, the situation is completely different. A full graphene coverage of the SiC surface is achieved but anisotropic growth still occurs, because of the step-bunched SiC surface reconstruction. While in the middle of reconstructed terraces thin graphene stacks (up to 5 layers) are grown, thicker graphene stripes appear at step edges. In both the cases, the strong interaction between the graphene layers and the underlying SiC substrate induces a high compressive thermal strain and n-type doping. PMID:21801347

  4. Controlled Gas Exfoliation of Boron Nitride into Few-Layered Nanosheets

    DOE PAGESBeta

    Zhu, Wenshuai; Gao, Xiang; Li, Qian; Li, Hongping; Chao, Yanhong; Li, Meijun; Mahurin, Shannon M.; Li, Huaming; Zhu, Huiyuan; Dai, Sheng

    2016-07-22

    The controlled exfoliation of hexagonal boron nitride (h-BN) into single- or few-layered nanosheets remains a grand challenge and becomes the bottleneck to essential studies and applications of h-BN. Here, we present an efficient strategy for the scalable synthesis of few-layered h-BN nanosheets (BNNS) via a novel gas exfoliation of bulk h-BN in liquid N2 (L-N2). The essence of this strategy lies in the combination of a high temperature triggered expansion of bulk h-BN and the cryogenic L-N2 gasification to exfoliate the h-BN. The produced BNNS after ten cycles (BNNS-10) consisted primarily of fewer than five atomic layers with high amore » mass yield of 16~20%. N2 sorption and desorption isotherms show that the BNNS-10 exhibited a much higher specific surface area of 278 m2/g–1 than that of bulk BN (10 m2/g–1). Through the investigation of the exfoliated intermediates combined with a theoretical calculation, we found that the huge temperature variation initiates the expansion and curling of the bulk h-BN. Subseqently, the L-N2 penetrates into the interlayers of h-BN along the curling edge, followed by an immediate drastic gasification of L-N2, further peeling off h-BN. In conclusion, this novel gas exfoliation of high surface area BNNS not only opens up potential opportunities for wide applications, but also can be extended to produce other layered materials with high yeilds.« less

  5. Controlled Gas Exfoliation of Boron Nitride into Few-Layered Nanosheets.

    PubMed

    Zhu, Wenshuai; Gao, Xiang; Li, Qian; Li, Hongping; Chao, Yanhong; Li, Meijun; Mahurin, Shannon M; Li, Huaming; Zhu, Huiyuan; Dai, Sheng

    2016-08-26

    The controlled exfoliation of hexagonal boron nitride (h-BN) into single- or few-layered nanosheets remains a grand challenge and becomes the bottleneck to essential studies and applications of h-BN. Here, we present an efficient strategy for the scalable synthesis of few-layered h-BN nanosheets (BNNS) using a novel gas exfoliation of bulk h-BN in liquid N2 (L-N2 ). The essence of this strategy lies in the combination of a high temperature triggered expansion of bulk h-BN and the cryogenic L-N2 gasification to exfoliate the h-BN. The produced BNNS after ten cycles (BNNS-10) consisted primarily of fewer than five atomic layers with a high mass yield of 16-20 %. N2 sorption and desorption isotherms show that the BNNS-10 exhibited a much higher specific surface area of 278 m(2)  g(-1) than that of bulk BN (10 m(2)  g(-1) ). Through the investigation of the exfoliated intermediates combined with a theoretical calculation, we found that the huge temperature variation initiates the expansion and curling of the bulk h-BN. Subseqently, the L-N2 penetrates into the interlayers of h-BN along the curling edge, followed by an immediate drastic gasification of L-N2 , further peeling off h-BN. This novel gas exfoliation of high surface area BNNS not only opens up potential opportunities for wide applications, but also can be extended to produce other layered materials in high yields. PMID:27444210

  6. Si-adatom kinetics in defect mediated growth of multilayer epitaxial graphene films on 6H-SiC

    NASA Astrophysics Data System (ADS)

    Shetu, Shamaita S.; Omar, S. U.; Daniels, K. M.; Daas, B.; Andrews, J.; Ma, S.; Sudarshan, T. S.; Chandrashekhar, M. V. S.

    2013-10-01

    We present a quantitative study on the growth of multilayer epitaxial graphene (EG) by solid-state decomposition of SiC on polar (c-plane Si and C-face) and non-polar (a and m planes) 6H-SiC faces, with distinctly different defect profiles. The growth rates are slower than expected from a mechanism that involves Si loss from an open and free surface, and much faster than expected for the nucleation of a defect-free EG layer, implying that defects in the EG play a critical role in determining the growth kinetics. We show that a Deal-Grove growth model, which assumes vertical diffusion of Si through these defects as the limiting factor for EG growth, is unsuitable for describing multilayer growth. Instead, we introduce a lateral "adatom" diffusion mechanism for Si out-diffusion, based on a modified Burton, Cabrera, and Frank model. In this model, defects in epitaxial graphene serve as sinks for Si desorption loss, taking the place of reactive sites, such as step edges for nucleation and growth of crystals produced with external precursors. This analysis shows that the surface diffusion of Si atoms to the grain boundaries of EG limits the growth on c-plane C-face and non-polar faces, rather than the purely vertical diffusion of Si through the grain boundaries described in the Deal-Grove model. However, for Si-face c-plane growth, diffusion of Si to the defects, as well as desorption of Si at the grain boundaries are both relevant, leading to a different temperature trend compared with the other faces. This distinct qualitative difference is ascribed to point-defects in Si-face growth, as contrasted with line defects/grain boundaries on the other faces. The size of the EG grains correlates with the surface diffusion length extracted from this model. The longer a Si adatom diffuses, the higher the quality of the grown EG film, an insight that provides valuable information on Si adatom kinetics for optimizing EG growth. We discuss the applicability of this model to

  7. Few-layer bismuth selenides exfoliated by hemin inhibit amyloid-β1-42 fibril formation

    NASA Astrophysics Data System (ADS)

    Peng, Jian; Xiong, Yunjing; Lin, Zhiqin; Sun, Liping; Weng, Jian

    2015-05-01

    Inhibiting amyloid-β (Aβ) fibril formation is the primary therapeutic strategy for Alzheimer’s disease. Several small molecules and nanomaterials have been used to inhibit Aβ fibril formation. However, insufficient inhibition efficiency or poor metabolization limits their further applications. Here, we used hemin to exfoliate few-layer Bi2Se3 in aqueous solution. Then we separated few-layer Bi2Se3 with different sizes and thicknesses by fractional centrifugation, and used them to attempt to inhibit Aβ1-42 aggregation. The results show that smaller and thinner few-layer Bi2Se3 had the highest inhibition efficiency. We further investigated the interaction between few-layer Bi2Se3 and Aβ1-42 monomers. The results indicate that the inhibition effect may be due to the high adsorption capacity of few-layer Bi2Se3 for Aβ1-42 monomers. Few-layer Bi2Se3 also decreased Aβ-mediated peroxidase-like activity and cytotoxicity according to in vitro neurotoxicity studies under physiological conditions. Therefore, our work shows the potential for applications of few-layer Bi2Se3 in the biomedical field.

  8. Few-layer bismuth selenides exfoliated by hemin inhibit amyloid-β1–42 fibril formation

    PubMed Central

    Peng, Jian; Xiong, Yunjing; Lin, Zhiqin; Sun, Liping; Weng, Jian

    2015-01-01

    Inhibiting amyloid-β (Aβ) fibril formation is the primary therapeutic strategy for Alzheimer’s disease. Several small molecules and nanomaterials have been used to inhibit Aβ fibril formation. However, insufficient inhibition efficiency or poor metabolization limits their further applications. Here, we used hemin to exfoliate few-layer Bi2Se3 in aqueous solution. Then we separated few-layer Bi2Se3 with different sizes and thicknesses by fractional centrifugation, and used them to attempt to inhibit Aβ1-42 aggregation. The results show that smaller and thinner few-layer Bi2Se3 had the highest inhibition efficiency. We further investigated the interaction between few-layer Bi2Se3 and Aβ1-42 monomers. The results indicate that the inhibition effect may be due to the high adsorption capacity of few-layer Bi2Se3 for Aβ1−42 monomers. Few-layer Bi2Se3 also decreased Aβ-mediated peroxidase-like activity and cytotoxicity according to in vitro neurotoxicity studies under physiological conditions. Therefore, our work shows the potential for applications of few-layer Bi2Se3 in the biomedical field. PMID:26018135

  9. Two-photon photoemission from image-potential states of epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Gugel, Dieter; Niesner, Daniel; Eickhoff, Christian; Wagner, Stefanie; Weinelt, Martin; Fauster, Thomas

    2015-12-01

    Using angle- and time-resolved two-photon photoelectron spectroscopy we observe a single series of image-potential states of graphene on monolayer (MLG) and bilayer graphene (BLG) on SiC(0001). The first image-potential state on MLG (BLG) has a binding energy of 0.93 eV (0.84 eV). Lifetimes of the first three image-potential states of MLG are 9, 44 and 110 fs. On hydrogen-intercalated, quasi-freestanding graphene no unoccupied states are observed. We attribute this to the absence of occupied initial states for direct transitions into image-potential states at photon energies below the work function used in two-photon photoemission. The work function varies between 4.14 and 4.79 eV, but the vacuum level stays ∼4.5 eV above the Dirac point for all surfaces studied. This finding suggests that direct excitation of image-potential states cannot be achieved by doping and the electron dynamics for free-standing graphene is not accessible by two-photon photoemission using photon energies below the work function.

  10. A self-powered sensitive ultraviolet photodetector based on epitaxial graphene on silicon carbide

    NASA Astrophysics Data System (ADS)

    Jiao, Huang; Li-Wei, Guo; Wei, Lu; Yong-Hui, Zhang; Zhe, Shi; Yu-Ping, Jia; Zhi-Lin, Li; Jun-Wei, Yang; Hong-Xiang, Chen; Zeng-Xia, Mei; Xiao-Long, Chen

    2016-06-01

    A self-powered graphene-based photodetector with high performance is particularly useful for device miniaturization and to save energy. Here, we report a graphene/silicon carbide (SiC)-based self-powered ultraviolet photodetector that exhibits a current responsivity of 7.4 mA/W with a response frequency of over a megahertz under 325-nm laser irradiation. The built-in photovoltage of the photodetector is about four orders of magnitude higher than previously reported results for similar devices. These favorable properties are ascribed to the ingenious device design using the combined advantages of graphene and SiC, two terminal electrodes, and asymmetric light irradiation on one of the electrodes. Importantly, the photon energy is larger than the band gap of SiC. This self-powered photodetector is compatible with modern semiconductor technology and shows potential for applications in ultraviolet imaging and graphene-based integrated circuits. Project supported by the National Key Basic Research Program of China (Grant Nos. 2011CB932700 and 2013CBA01603) and the National Natural Science Foundation of China (Grant Nos. 51472265 and 51272279).

  11. Effects of aluminum on epitaxial graphene grown on C-face SiC

    SciTech Connect

    Xia, Chao Johansson, Leif I.; Hultman, Lars; Virojanadara, Chariya; Niu, Yuran

    2015-05-21

    The effects of Al layers deposited on graphene grown on C-face SiC substrates are investigated before and after subsequent annealing using low energy electron diffraction (LEED), photoelectron spectroscopy, and angle resolved photoemission. As-deposited layers appear inert. Annealing at a temperature of about 400 °C initiates migration of Al through the graphene into the graphene/SiC interface. Further annealing at temperatures from 500 °C to 700 °C induces formation of an ordered compound, producing a two domain √7× √7R19° LEED pattern and significant changes in the core level spectra that suggest formation of an Al-Si-C compound. Decomposition of this compound starts after annealing at 800 °C, and at 1000 °C, Al is no longer possible to detect at the surface. On Si-face graphene, deposited Al layers did not form such an Al-Si-C compound, and Al was still detectable after annealing above 1000 °C.

  12. Probing the Role of Interlayer Coupling and Coulomb Interactions on Electronic Structure in Few-Layer MoSe2Nanostructures

    NASA Astrophysics Data System (ADS)

    Bradley, Aaron J.; M. Ugeda, Miguel; da Jornada, Felipe H.; Qiu, Diana Y.; Ruan, Wei; Zhang, Yi; Wickenburg, Sebastian; Riss, Alexander; Lu, Jiong; Mo, Sung-Kwan; Hussain, Zahid; Shen, Zhi-Xun; Louie, Steven G.; Crommie, Michael F.

    2015-04-01

    Despite the weak nature of interlayer forces in transition metal dichalcogenide (TMD) materials, their properties are highly dependent on the number of layers in the few-layer two-dimensional (2D) limit. Here, we present a combined scanning tunneling microscopy/spectroscopy and GW theoretical study of the electronic structure of high quality single- and few-layer MoSe2 grown on bilayer graphene. We find that the electronic (quasiparticle) bandgap, a fundamental parameter for transport and optical phenomena, decreases by nearly one electronvolt when going from one layer to three due to interlayer coupling and screening effects. Our results paint a clear picture of the evolution of the electronic wave function hybridization in the valleys of both the valence and conduction bands as the number of layers is changed. This demonstrates the importance of layer number and electron-electron interactions on van der Waals heterostructures, and helps to clarify how their electronic properties might be tuned in future 2D nanodevices.

  13. Probing the Role of Interlayer Coupling and Coulomb Interactions on Electronic Structure in Few-Layer MoSe 2 Nanostructures

    DOE PAGESBeta

    Bradley, Aaron J.; M. Ugeda, Miguel; da Jornada, Felipe H.; Qiu, Diana Y.; Ruan, Wei; Zhang, Yi; Wickenburg, Sebastian; Riss, Alexander; Lu, Jiong; Mo, Sung-Kwan; et al

    2015-03-16

    Despite the weak nature of interlayer forces in transition metal dichalcogenide (TMD) materials, their properties are highly dependent on the number of layers in the few-layer two-dimensional (2D) limit. Here, we present a combined scanning tunneling microscopy/spectroscopy and GW theoretical study of the electronic structure of high quality single- and few-layer MoSe2 grown on bilayer graphene. We find that the electronic (quasiparticle) bandgap, a fundamental parameter for transport and optical phenomena, decreases by nearly one electronvolt when going from one layer to three due to interlayer coupling and screening effects. Our results paint a clear picture of the evolution ofmore » the electronic wave function hybridization in the valleys of both the valence and conduction bands as the number of layers is changed. This demonstrates the importance of layer number and electron-electron interactions on van der Waals heterostructures and helps to clarify how their electronic properties might be tuned in future 2D nanodevices.« less

  14. Direct Growth of Single- and Few-Layer MoS2 on h-BN with Preferred Relative Rotation Angles.

    PubMed

    Yan, Aiming; Velasco, Jairo; Kahn, Salman; Watanabe, Kenji; Taniguchi, Takashi; Wang, Feng; Crommie, Michael F; Zettl, Alex

    2015-10-14

    Monolayer molybdenum disulfide (MoS2) is a promising two-dimensional direct-bandgap semiconductor with potential applications in atomically thin and flexible electronics. An attractive insulating substrate or mate for MoS2 (and related materials such as graphene) is hexagonal boron nitride (h-BN). Stacked heterostructures of MoS2 and h-BN have been produced by manual transfer methods, but a more efficient and scalable assembly method is needed. Here we demonstrate the direct growth of single- and few-layer MoS2 on h-BN by chemical vapor deposition (CVD) method, which is scalable with suitably structured substrates. The growth mechanisms for single-layer and few-layer samples are found to be distinct, and for single-layer samples low relative rotation angles (<5°) between the MoS2 and h-BN lattices prevail. Moreover, MoS2 directly grown on h-BN maintains its intrinsic 1.89 eV bandgap. Our CVD synthesis method presents an important advancement toward controllable and scalable MoS2-based electronic devices.

  15. Probing the Role of Interlayer Coupling and Coulomb Interactions on Electronic Structure in Few-Layer MoSe 2 Nanostructures

    SciTech Connect

    Bradley, Aaron J.; M. Ugeda, Miguel; da Jornada, Felipe H.; Qiu, Diana Y.; Ruan, Wei; Zhang, Yi; Wickenburg, Sebastian; Riss, Alexander; Lu, Jiong; Mo, Sung-Kwan; Hussain, Zahid; Shen, Zhi-Xun; Louie, Steven G.; Crommie, Michael F.

    2015-03-16

    Despite the weak nature of interlayer forces in transition metal dichalcogenide (TMD) materials, their properties are highly dependent on the number of layers in the few-layer two-dimensional (2D) limit. Here, we present a combined scanning tunneling microscopy/spectroscopy and GW theoretical study of the electronic structure of high quality single- and few-layer MoSe2 grown on bilayer graphene. We find that the electronic (quasiparticle) bandgap, a fundamental parameter for transport and optical phenomena, decreases by nearly one electronvolt when going from one layer to three due to interlayer coupling and screening effects. Our results paint a clear picture of the evolution of the electronic wave function hybridization in the valleys of both the valence and conduction bands as the number of layers is changed. This demonstrates the importance of layer number and electron-electron interactions on van der Waals heterostructures and helps to clarify how their electronic properties might be tuned in future 2D nanodevices.

  16. Probing the Role of Interlayer Coupling and Coulomb Interactions on Electronic Structure in Few-Layer MoSe2 Nanostructures

    PubMed Central

    2015-01-01

    Despite the weak nature of interlayer forces in transition metal dichalcogenide (TMD) materials, their properties are highly dependent on the number of layers in the few-layer two-dimensional (2D) limit. Here, we present a combined scanning tunneling microscopy/spectroscopy and GW theoretical study of the electronic structure of high quality single- and few-layer MoSe2 grown on bilayer graphene. We find that the electronic (quasiparticle) bandgap, a fundamental parameter for transport and optical phenomena, decreases by nearly one electronvolt when going from one layer to three due to interlayer coupling and screening effects. Our results paint a clear picture of the evolution of the electronic wave function hybridization in the valleys of both the valence and conduction bands as the number of layers is changed. This demonstrates the importance of layer number and electron–electron interactions on van der Waals heterostructures and helps to clarify how their electronic properties might be tuned in future 2D nanodevices. PMID:25775022

  17. Stacking-dependent electronic property of trilayer graphene epitaxially grown on Ru(0001)

    NASA Astrophysics Data System (ADS)

    Que, Yande; Xiao, Wende; Chen, Hui; Wang, Dongfei; Du, Shixuan; Gao, Hong-Jun

    2015-12-01

    The growth, atomic structure, and electronic property of trilayer graphene (TLG) on Ru(0001) were studied by low temperature scanning tunneling microscopy and spectroscopy in combined with tight-binding approximation (TBA) calculations. TLG on Ru(0001) shows a flat surface with a hexagonal lattice due to the screening effect of the bottom two layers and the AB-stacking in the top two layers. The coexistence of AA- and AB-stacking in the bottom two layers leads to three different stacking orders of TLG, namely, ABA-, ABC-, and ABB-stacking. STS measurements combined with TBA calculations reveal that the density of states of TLG with ABC- and ABB-stacking is characterized by one and two sharp peaks near to the Fermi level, respectively, in contrast to the V-shaped feature of TLG with ABA-stacking. Our work demonstrates that TLG on Ru(0001) might be an ideal platform for exploring stacking-dependent electronic properties of graphene.

  18. Stacking-dependent electronic property of trilayer graphene epitaxially grown on Ru(0001)

    SciTech Connect

    Que, Yande; Xiao, Wende E-mail: hjgao@iphy.ac.cn; Chen, Hui; Wang, Dongfei; Du, Shixuan; Gao, Hong-Jun E-mail: hjgao@iphy.ac.cn

    2015-12-28

    The growth, atomic structure, and electronic property of trilayer graphene (TLG) on Ru(0001) were studied by low temperature scanning tunneling microscopy and spectroscopy in combined with tight-binding approximation (TBA) calculations. TLG on Ru(0001) shows a flat surface with a hexagonal lattice due to the screening effect of the bottom two layers and the AB-stacking in the top two layers. The coexistence of AA- and AB-stacking in the bottom two layers leads to three different stacking orders of TLG, namely, ABA-, ABC-, and ABB-stacking. STS measurements combined with TBA calculations reveal that the density of states of TLG with ABC- and ABB-stacking is characterized by one and two sharp peaks near to the Fermi level, respectively, in contrast to the V-shaped feature of TLG with ABA-stacking. Our work demonstrates that TLG on Ru(0001) might be an ideal platform for exploring stacking-dependent electronic properties of graphene.

  19. Epitaxial graphene on SiC(0001): functional electrical microscopy studies and effect of atmosphere.

    PubMed

    Kazakova, O; Burnett, T L; Patten, J; Yang, L; Yakimova, R

    2013-05-31

    Surface potential distribution, V(CPD), and evolution of atmospheric adsorbates on few and multiple layers (FLG and MLG) of graphene grown on SiC(0001) substrate have been investigated by electrostatic and Kelvin force microscopy techniques at T = 20-120 °C. The change of the surface potential distribution, ΔV(CPD), between FLG and MLG is shown to be temperature dependent. The enhanced ΔV(CPD) value at 120 °C is associated with desorption of adsorbates at high temperatures and the corresponding change of the carrier balance. The nature of the adsorbates and their evolution with temperature are considered to be related to the process of adsorption and desorption of the atmospheric water on MLG domains. We demonstrate that both the nano- and microscale wettability of the material are strongly dependent on the number of graphene layers.

  20. Theory of the Dirac half metal and quantum anomalous Hall effect in Mn-intercalated epitaxial graphene

    NASA Astrophysics Data System (ADS)

    Li, Yuanchang; West, Damien; Huang, Huaqing; Li, Jia; Zhang, S. B.; Duan, Wenhui

    2015-11-01

    The prospect of a Dirac half metal, a material which is characterized by a band structure with a gap in one spin channel but a Dirac cone in the other, is of both fundamental interest and a natural candidate for use in spin-polarized current applications. However, while the possibility of such a material has been reported based on model calculations [H. Ishizuka and Y. Motome, Phys. Rev. Lett. 109, 237207 (2012), 10.1103/PhysRevLett.109.237207], it remains unclear what material system might realize such an exotic state. Using first-principles calculations, we show that the experimentally accessible Mn-intercalated epitaxial graphene on SiC(0001) transits to a Dirac half metal when the coverage is >1 /3 monolayer. This transition results from an orbital-selective breaking of quasi-two-dimensional inversion symmetry, leading to symmetry breaking in a single spin channel which is robust against randomness in the distribution of Mn intercalates. Furthermore, the inclusion of spin-orbit interaction naturally drives the system into the quantum anomalous Hall (QAH) state. Our results thus not only demonstrate the practicality of realizing the Dirac half metal beyond a toy model, but also open up an avenue to the realization of the QAH effect.