Quasi-free Standing Epitaxial Graphene on SiC by Hydrogen Intercalation

Quasi-free standing epitaxial graphene is obtained on SiC(0001) by hydrogen intercalation. The hydrogen moves between the 6root3 reconstructed initial carbon layer and the SiC substrate. The topmost Si atoms which for epitaxial graphene are covalently bound to this buffer layer, are now saturated by hydrogen bonds. The buffer layer is turned into a quasi-free standing graphene monolayer with its typical linear pi-bands. Similarly, epitaxial monolayer graphene turns into a decoupled bilayer. The intercalation is stable in air and can be reversed by annealing to around 900 degrees Celsius.Comment: Accepted for publication in Physical Review Letter

Intercalation of graphene on SiC(0001) via ion-implantation

Electronic devices based on graphene technology are catching on rapidly and the ability to engineer graphene properties at the nanoscale is becoming, more than ever, indispensable. Here, we present a new procedure of graphene functionalization on SiC(0001) that paves the way towards the fabrication of complex graphene electronic chips. The procedure resides on the well-known ion-implantation technique. The efficiency of the working principle is demonstrated by the intercalation of the epitaxial graphene layer on SiC(0001) with Bi atoms, which was not possible following standard procedures. Our results put forward the ion-beam lithography to nanostructure and functionalize desired graphene chips

LEED Holography applied to a complex superstructure: a direct view of the adatom cluster on SiC(111)-(3x3)

For the example of the SiC(111)-(3x3) reconstruction we show that a holographic interpretation of discrete Low Energy Electron Diffraction (LEED) spot intensities arising from ordered, large unit cell superstructures can give direct access to the local geometry of a cluster around an elevated atom, provided there is only one such prominent atom per surface unit cell. By comparing the holographic images obtained from experimental and calculated data we illuminate validity, current limits and possible shortcomings of the method. In particular, we show that periodic vacancies such as cornerholes may inhibit the correct detection of the atomic positions. By contrast, the extra diffraction intensity due to slight substrate reconstructions, as for example buckling, seems to have negligible influence on the images. Due to the spatial information depth of the method the stacking of the cluster can be imaged down to the fourth layer. Finally, it is demonstrated how this structural knowledge of the adcluster geometry can be used to guide the dynamical intensity analysis subsequent to the holographic reconstruction and necessary to retrieve the full unit cell structure.Comment: 11 pages RevTex, 6 figures, Phys. Rev. B in pres

Tracking primary thermalization events in graphene with photoemission at extreme timescales

Direct and inverse Auger scattering are amongst the primary processes that mediate the thermalization of hot carriers in semiconductors. These two processes involve the annihilation or generation of an electron-hole pair by exchanging energy with a third carrier, which is either accelerated or decelerated. Inverse Auger scattering is generally suppressed, as the decelerated carriers must have excess energies higher than the band gap itself. In graphene, which is gapless, inverse Auger scattering is instead predicted to be dominant at the earliest time delays. Here, $<8$ femtosecond extreme-ultraviolet pulses are used to detect this imbalance, tracking both the number of excited electrons and their kinetic energy with time- and angle-resolved photoemission spectroscopy. Over a time window of approximately 25 fs after absorption of the pump pulse, we observe an increase in conduction band carrier density and a simultaneous decrease of the average carrier kinetic energy, revealing that relaxation is in fact dominated by inverse Auger scattering. Measurements of carrier scattering at extreme timescales by photoemission will serve as a guide to ultrafast control of electronic properties in solids for PetaHertz electronics.Comment: 16 pages, 8 figure

Holographic Image Reconstruction from Electron Diffraction Intensities of Ordered Superstructures

We report on a novel holographic reconstruction of well resolved atomic images from discrete spot intensities appearing in low-energy electron diffraction (LEED) from crystalline surfaces. This opens holographic LEED to the wide field of ordered systems giving access to rather complex surface structures

Graphene formed on SiC under various environments: Comparison of Si-face and C-face

The morphology of graphene on SiC {0001} surfaces formed in various environments including ultra-high vacuum, 1 atm of argon, and 10^-6 to 10^-4 Torr of disilane is studied by atomic force microscopy, low-energy electron microscopy, and Raman spectroscopy. The graphene is formed by heating the surface to 1100 - 1600 C, which causes preferential sublimation of the Si atoms. The argon atmosphere or the background of disilane decreases the sublimation rate so that a higher graphitization temperature is required, thus improving the morphology of the films. For the (0001) surface, large areas of monolayer-thick graphene are formed in this way, with the size of these areas depending on the miscut of the sample. Results on the (000-1) surface are more complex. This surface graphitizes at a lower temperature than for the (0001) surface and consequently the growth is more three-dimensional. In an atmosphere of argon the morphology becomes even worse, with the surface displaying markedly inhomogeneous nucleation, an effect attributed to unintentional oxidation of the surface during graphitization. Use of a disilane environment for the (000-1) surface is found to produce improved morphology, with relatively large areas of monolayer-thick graphene.Comment: 22 pages, 11 figures, Proceedings of STEG-2 Conference; eliminated Figs. 4 and 7 from version 1, for brevity, and added Refs. 18, 29, 30, 31 together with associated discussio

Enhanced electron-phonon coupling in graphene with periodically distorted lattice

Electron-phonon coupling directly determines the stability of cooperative order in solids, including superconductivity, charge and spin density waves. Therefore, the ability to enhance or reduce electron-phonon coupling by optical driving may open up new possibilities to steer materials' functionalities, potentially at high speeds. Here we explore the response of bilayer graphene to dynamical modulation of the lattice, achieved by driving optically-active in-plane bond stretching vibrations with femtosecond mid-infrared pulses. The driven state is studied by two different ultrafast spectroscopic techniques. Firstly, TeraHertz time-domain spectroscopy reveals that the Drude scattering rate decreases upon driving. Secondly, the relaxation rate of hot quasi-particles, as measured by time- and angle-resolved photoemission spectroscopy, increases. These two independent observations are quantitatively consistent with one another and can be explained by a transient three-fold enhancement of the electron-phonon coupling constant. The findings reported here provide useful perspective for related experiments, which reported the enhancement of superconductivity in alkali-doped fullerites when a similar phonon mode was driven.Comment: 12 pages, 4 figure

Deterministic direct growth of WS2 on CVD graphene arrays

The combination of the exciting properties of graphene with those of monolayer tungsten disulfide (WS2) makes this heterostack of great interest for electronic, optoelectronic and spintronic applications. The scalable synthesis of graphene/WS2 heterostructures on technologically attractive substrates like SiO2 would greatly facilitate the implementation of novel two-dimensional (2D) devices. In this work, we report the direct growth of monolayer WS2 via chemical vapor deposition (CVD) on single-crystal graphene arrays on SiO2. Remarkably, spectroscopic and microscopic characterization reveals that WS2 grows only on top of the graphene crystals so that the vertical heterostack is selectively obtained in a bottom-up fashion. Spectroscopic characterization indicates that, after WS2 synthesis, graphene undergoes compressive strain and hole doping. Tailored experiments show that such hole doping is caused by the modification of the SiO2 stoichiometry at the graphene/SiO2 interface during the WS2 growth. Electrical transport measurements reveal that the heterostructure behaves like an electron-blocking layer at large positive gate voltage, which makes it a suitable candidate for the development of unipolar optoelectronic components