Magnetic order emerging in otherwise non-magnetic materials as carbon is a paradigmatic example of a novel type of s-p electron magnetism predicted to be of exceptional hightemperature stability 1 . It has been demonstrated that atomic scale structural defects of graphene can host unpaired spins 2,3 . However, it is still unclear under which conditions longrange magnetic order can emerge from such defect-bound magnetic moments. Here we propose that in contrast to random defect distributions, atomic scale engineering of graphene edges with specific crystallographic orientation -comprising edge atoms only from one sublattice of the bipartite graphene lattice -can give rise to a robust magnetic order. We employ a nanofabrication technique 4 based on Scanning Tunneling Microscopy to define graphene nanoribbons with nanometer precision and well-defined crystallographic edge orientations.While armchair ribbons display quantum confinement gap, zigzag ribbons narrower than 7 nm reveal a bandgap of about 0.2 -0.3 eV, which can be identified as a signature of 2 interaction induced spin ordering along their edges. Moreover, a semiconductor to metal transition is revealed upon increasing the ribbon width, indicating the switching of the magnetic coupling between opposite ribbon edges from antiferromagnetic to ferromagnetic configuration. We found that the magnetic order on graphene edges of controlled zigzag orientation can be stable even at room temperature, raising hope for graphene-based spintronic devices operating under ambient conditions.The intrinsic magnetism of graphite has a long and controversial history 1 . The origin of the measured magnetic signal is generally attributed to atomic scale structural defects locally breaking the sub-lattice balance of the bipartite hexagonal lattice 5,6 . However, the unambiguous identification of the structural sources of the measured magnetic signal has proven challenging as they are buried inside the bulk of the material. The isolation of single graphene layers 7 opens new prospects in this direction 8,9 as their atomic structure is fully accessible for imaging and controlled modification. In particular, graphene edges of specific (zigzag) crystallographic orientation comprising carbon atoms from only one sub-lattice of the bipartite hexagonal lattice are predicted to host magnetic order 10 , in striking contrast to armchair edges incorporating an equal number of carbon atoms from both sublattices.The strong influence of edge orientation on the electronic structure of graphene nanoribbons had However, the random orientation of the edges and the influence of a possible strong edge-substrate hybridization 21 did not allow full access to the nature of edge-magnetism in graphene. Though the 4 magnetic order is expected to persist to some extent on zigzag segments of randomly oriented graphene edges, the mixing of different edge types are expected to substantially weaken the effect 19,22 . Therefore, the lack of experimental control over the edge orientation seems one of the main ...

Perturbations of the two dimensional carbon lattice of graphene, such as grain boundaries, have significant influence on the charge transport and mechanical properties of this material. Scanning tunneling microscopy measurements presented here show that localized states near the Dirac point dominate the local density of states of grain boundaries in graphene grown by chemical vapor deposition. Such low energy states are not reproduced by theoretical models which treat the grain boundaries as periodic dislocation-cores composed of pentagonal-heptagonal carbon rings. Using ab initio calculations, we have extended this model to include disorder, by introducing vacancies into a grain boundary consisting of periodic dislocation-cores. Within the framework of this model we were able to reproduce the measured density of states features. We present evidence that grain boundaries in graphene grown on copper incorporate a significant amount of disorder in the form of two-coordinated carbon atoms.

We have studied the polarity of magnetoresistance (MR) in three types of magnetic junctions. While the NiFe/single layer graphene (SLG)/Co and NiFe/Al2O3/Co junctions showed spin valve signals with positive MR, the NiFe/Al2O3/SLG/Co junction revealed negative MR values.

The edge oxidation effects of chemical-vapor-deposition-grown graphene devices with nanoconstrictions of different sizes are presented. The effects of edge oxidation on the doping level of a nanoconstriction graphene device were identified by Raman spectroscopy and using the back-gate-voltage-dependent resistance. Strong p-type doping was observed as the size of nanoconstriction decreased. The Dirac point of the graphene device shifted toward positive voltage, and the positions of the G and 2D peaks in Raman spectroscopy shifted toward a higher wave number, indicating the p-type doping effect of the graphene device. p-type doping was lifted by deep-ultraviolet light illumination under a nitrogen atmosphere at room temperature. p-type doping was restored by deep-ultraviolet light illumination under an oxygen atmosphere at room temperature. Edge oxidation in the narrow structures explains the origin of the p-type doping effect widely observed in graphene nanodevices.

The electronic properties of graphene can be significantly influenced by mechanical strain. One practical approach to induce strain in graphene is to transfer atomically thin membranes onto pre-patterned substrates with specific corrugations. The possibility of using nanoparticles to impart extrinsic rippling to graphene has not been fully explored yet. Here we study the structure and elastic properties of graphene grown by chemical vapour deposition and transferred onto a continuous layer of SiO2 nanoparticles with diameters of around 25 nm, prepared on a Si substrate by the Langmuir-Blodgett technique. We show that the corrugation of the transferred graphene, and thus the membrane strain, can be modified by annealing at moderate temperatures. The membrane parts bridging the nanoparticles are suspended and can be reversibly lifted by the attractive forces between an atomic force microscope tip and graphene. This allows the dynamic control of the local morphology of graphene nanomembranes.

The properties of graphene nanoribbons are dependent on both the nanoribbon width and the crystallographic orientation of the edges. Scanning tunneling microscope lithography is a method which is able to create graphene nanoribbons with well defined edge orientation, having a width of a few nanometers. However, it has only been demonstrated on the top layer of graphite. In order to allow practical applications of this powerful lithography technique, it needs to be implemented on single layer graphene. We demonstrate the preparation of graphene nanoribbons with well defined crystallographic orientation on top of gold substrates. Our transfer and lithography approach brings one step closer the preparation of well defined graphene nanoribbons on arbitrary substrates for nanoelectronic applications.

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We fabricated artificially stacked double-layer graphene by sequentially transferring graphene grown by chemical vapor deposition. The double-layer graphene was characterized by Raman spectroscopy and transport measurements. A weak localization effect was observed for different charge carrier densities and temperatures. The obtained intervalley scattering rate was unusually high compared to normal Bernal-stacked bilayer or single-layer graphene. The sharp point defects, local deformation, or bending of graphene plane required for intervalley scattering from one Dirac cone to another seemed to be enhanced by the artificially stacked graphene layers.