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Register a new userCrystalline hydrogenation of graphene by STM tip-induced field dissociation of H$_2$
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We have developed a novel method for crystalline hydrogenation of graphene on the nanoscale. Molecular hydrogen was physisorbed at 5 K onto pristine graphene islands grown on Cu(111) in ultrahigh vacuum. Field emission local to the tip of a scanning tunneling microscope dissociates H$_2$ and results in hydrogenated graphene. At lower coverage, isolated point defects are found on the graphene and are attributed to chemisorbed H on top and bottom surfaces. Repeated H$_2$ exposure and field emission yielded patches and then complete coverage of a crystalline $sqrt{3}$ $times$ $sqrt{3}$ R30{deg} phase, as well as less densely packed 3 $times$ 3 and 4 $times$ 4 structures. The hydrogenation can be reversed by imaging with higher bias voltage.
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Graphite surfaces can be manipulated by several methods to create graphene structures of different shapes and sizes. Scanning tunneling microscopy (STM) can be used to create these structures either through mechanical contact between the tip and the surface or through electro-exfoliation. In the latter, the mechanisms involved in the process of exfoliation with an applied voltage are not fully understood. Here we show how a graphite surface can be locally exfoliated in a systematic manner by applying an electrostatic force with a STM tip at the edge of a terrace, forming triangular flakes several nanometers in length. We demonstrate, through experiments and simulations, how these flakes are created by a two-step process: first a voltage ramp must be applied at the edge of the terrace, and then the tip must be scanned perpendicularly to the edge. Ab-initio electrostatic calculations reveal that the presence of charges on the graphite surface weakens the interaction between layers allowing for exfoliation at voltages in the same range as those used experimentally. Molecular dynamics simulations show that a force applied locally on the edge of a step produces triangular flakes such as those observed under STM. Our results provide new insights towards surface modification that can be extended to other layered materials.
Monolayer graphene epitaxially grown on SiC(0001) was etched by H-plasma and studied by scanning tunneling microscopy and spectroscopy. The etching created partly hexagonal nanopits of monatomic depth as well as elevated regions with a height of about 0.12 nm which are stable at $T$ = 78 K. The symmetric tunnel spectrum about the Femi energy and the absence of a $6times6$ corrugation on the elevated regions suggest that in these regions the carbon buffer layer is decoupled from the SiC substrate and quasi-free-standing bilayer graphene appears at originally monolayer graphene on the buffer layer. This is a result of passivation of the SiC substrate by intercalated hydrogen as in previous reports for graphene on SiC(0001) heat treated in atomic hydrogen.
Non-equilibrium Greens functions calculations based on density functional theory show a direct link between the initial stages of H$_2$ dissociation on a gold atomic wire and the electronic current supported by the gold wire. The simulations reveal that for biases below the stability threshold of the wire, the minimum-energy path for H$_2$ dissociation is not affected. However, the electronic current presents a dramatic drop when the molecule initiates its dissociation. This current drop is traced back to quantum interference between electron paths when the molecule starts interacting with the gold wire.
We consider the theory of Kondo effect and Fano factor energy dependence for magnetic impurity (Co) on graphene. We have performed a first principles calculation and find that the two dimensional $E_1$ representation made of $d_{xz},d_{yz}$ orbitals is likely to be responsible for the hybridization and ultimately Kondo screening for cobalt on graphene. There are few high symmetry sites where magnetic impurity atom can be adsorbed. For the case of Co atom in the middle of hexagon of carbon lattice we find anomalously large Fano $q$-factor, $qapprox 80$ and strongly suppressed coupling to conduction band. This anomaly is a striking example of quantum mechanical interference related to the Berry phase inherent to graphene band structure.
Introduction of spin-orbit interaction (SOI) into graphene with weak hydrogenation ($sim$0.1%) by dissociation of hydrogen silsesquioxane resist has been confirmed through the appearance of inverse spin Hall effect. The spin current was produced by spin injection from permalloy electrodes excluding non-spin relating experimental artifact.
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