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Register a new userOn-surface synthesis of graphene nanoribbons with zigzag edge topology
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Graphene-based nanostructures exhibit a vast range of exciting electronic properties that are absent in extended graphene. For example, quantum confinement in carbon nanotubes and armchair graphene nanoribbons (AGNRs) leads to the opening of substantial electronic band gaps that are directly linked to their structural boundary conditions. Even more intriguing are nanostructures with zigzag edges, which are expected to host spin-polarized electronic edge states and can thus serve as key elements for graphene-based spintronics. The most prominent example is zigzag graphene nanoribbons (ZGNRs) for which the edge states are predicted to couple ferromagnetically along the edge and antiferromagnetically between them. So far, a direct observation of the spin-polarized edge states for specifically designed and controlled zigzag edge topologies has not been achieved. This is mainly due to the limited precision of current top-down approaches, which results in poorly defined edge structures. Bottom-up fabrication approaches, on the other hand, were so far only successfully applied to the growth of AGNRs and related structures. Here, we describe the successful bottom-up synthesis of ZGNRs, which are fabricated by the surface-assisted colligation and cyclodehydrogenation of specifically designed precursor monomers including carbon groups that yield atomically precise zigzag edges. Using scanning tunnelling spectroscopy we prove the existence of edge-localized states with large energy splittings. We expect that the availability of ZGNRs will finally allow the characterization of their predicted spin-related properties such as spin confinement and filtering, and ultimately add the spin degree of freedom to graphene-based circuitry.
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The influence of periodic edge vacancies and antidot arrays on the thermoelectric properties of zigzag graphene nanoribbons is investigated. Using the Greens function method, the tight-binding approximation for the electron Hamiltonian and the 4th nearest neighbor approximation for the phonon dynamical matrix, we calculate the Seebeck coefficient and the thermoelectric figure of merit. It is found that, at a certain periodic arrangement of vacancies on both edges of zigzag nanoribbon, a finite band gap opens and almost twofold degenerate energy levels appear. As a result, a marked increase in the Seebeck coefficient takes place. It is shown that an additional enhancement of the thermoelectric figure of merit can be achieved by a combination of periodic edge defects with an antidot array.
Here, we demonstrate two reliable routes for the fabrication of armchair-edge graphene nanoribbons (GNRs) on TbAu2/Au(111), belonging to a class of two-dimensional ferromagnetic rare earth-gold intermetallic compounds. On-surface synthesis directly on TbAu2 leads to the formation of GNRs, which are short and interconnected with each other. In contrast, the intercalation approach - on-surface synthesis of GNRs directly on Au(111) followed by rare earth intercalation - yields GNRs on TbAu2/Au(111), where both the ribbons and TbAu2 are of high quality comparable with those directly grown on clean Au(111). Besides, the as-grown ribbons retain the same band gap while changing from p-doping to weak n-doping mainly due to a change in the work function of the substrate after the rare earth intercalation. The intercalation approach might also be employed to fabricate other types of GNRs on various rare earth intermetallic compounds, providing platforms to tailor the electronic and magnetic properties of GNRs on magnetic substrates.
In this article, we report band structure studies of zigzag graphene nanoribbons (ZGNRs) on introducing defects (sp_3 hybridized carbon atoms) in different concentrations at edges by varying the ratio of sp_3 to sp_2 hybridized carbon atoms. On the basis of theoretical analyses, band gap values of ZGNRs are found to be strongly dependent on relative arrangement of sp3 to sp2 hybridized carbon atoms at the edges for a defect concentration; so the findings would greatly help in understanding band gap of nanoribbons for their electronic applications.
It is shown that apart from well-known factors, like temperature, substrate, and edge reconstruction effects, also the presence of external contacts is destructive for the formation of magnetic moments at the edges of graphene nanoribbons. The edge magnetism gradually decreases when graphene/electrode interfaces become more and more transparent for electrons. In addition to the graphene/electrode coupling strength, also the aspect ratio parameter, i.e. a width/length ratio of the graphene nanoribbon, is crucial for the suppression of edge magnetism. The present theory uses a tight-binding method, based on the mean-field Hubbard Hamiltonian for $pi$ electrons, and the Greens function technique within the Landauer-Buttiker approach.
We present Fermis golden rule calculations of the optical carrier injection and the coherent control of current injection in graphene nanoribbons with zigzag geometry, using an envelope function approach. This system possesses strongly localized states (flat bands) with a large joint density of states at low photon energies; for ribbons with widths above a few tens of nanometers, this system also posses large number of (non-flat) states with maxima and minima close to the Fermi level. Consequently, even with small dopings the occupation of these localized states can be significantly altered. In this work, we calculate the relevant quantities for coherent control at different chemical potentials, showing the sensitivity of this system to the occupation of the edge states. We consider coherent control scenarios arising from the interference of one-photon absorption at $2hbaromega$ with two-photon absorption at $hbaromega$, and those arising from the interference of one-photon absorption at $hbaromega$ with stimulated electronic Raman scattering (virtual absorption at $2hbaromega$ followed by emission at $hbaromega$). Although at large photon energies these processes follow an energy-dependence similar to that of 2D graphene, the zigzag nanoribbons exhibit a richer structure at low photon energies, arising from divergences of the joint density of states and from resonant absorption processes, which can be strongly modified by doping. As a figure of merit for the injected carrier currents, we calculate the resulting swarm velocities. Finally, we provide estimates for the limits of validity of our model.
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