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Register a new userElectronic structure, imaging contrast and chemical reactivity of graphene moire on metals
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Realization of graphene moire superstructures on the surface of 4d and 5d transition metals offers templates with periodically modulated electron density, which is responsible for a number of fascinating effects, including the formation of quantum dots and the site selective adsorption of organic molecules or metal clusters on graphene. Here, applying the combination of scanning probe microscopy/spectroscopy and the density functional theory calculations, we gain a profound insight into the electronic and topographic contributions to the imaging contrast of the epitaxial graphene/Ir(111) system. We show directly that in STM imaging the electronic contribution is prevailing compared to the topographic one. In the force microscopy and spectroscopy experiments we observe a variation of the interaction strength between the tip and high-symmetry places within the graphene moire supercell, which determine the adsorption cites for molecules or metal clusters on graphene/Ir(111).
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Here, we examine the influence of surface chemical reactivity toward ambient gases on the performance of nanodevices based on two-dimensional materials beyond graphene and novel topological phases of matter. While surface oxidation in ambient conditions was observed for silicene and phosphorene with subsequent reduction of the mobility of charge carriers, nanodevices with active channels of indium selenide, bismuth chalcogenides and transition-metal dichalcogenides are stable in air. However, air-exposed indium selenide suffers of p-type doping due to water decomposition on Se vacancies, whereas the low mobility of charge carriers in transition-metal dichalcogenides increases the response time of nanodevices. Conversely, bismuth chalcogenides require a control of crystalline quality, which could represent a serious hurdle for up scaling.
Epitaxial graphene grown on transition metal surfaces typically exhibits a moire pattern due to the lattice mismatch between graphene and the underlying metal surface. We use both scanning tunneling microscopy (STM) and atomic force microscopy (AFM) experiments to probe the electronic and topographic contrast of the graphene moire on the Ir(111) surface. While STM topography is influenced by the local density of states close to the Fermi energy and the local tunneling barrier height, AFM is capable of yielding the true surface topography once the background force arising from the van der Waals (vdW) interaction between the tip and the substrate is taken into account. We observe a moire corrugation of 35$pm$10 pm, where the graphene-Ir(111) distance is the smallest in the areas where the graphene honeycomb is atop the underlying iridium atoms and larger on the fcc or hcp threefold hollow sites.
The atomic structure at the interface between a two-dimensional (2D) and a three-dimensional (3D) material influences properties such as contact resistance, photo-response, and high-frequency performance. Moire engineering has yet to be explored for tailoring this 2D/3D interface, despite its success in enabling correlated physics at 2D/2D twisted van der Waals interfaces. Using epitaxially aligned MoS$_2$ /Au{111} as a model system, we apply a geometric convolution technique and four-dimensional scanning transmission electron microscopy (4D STEM) to show that the 3D nature of the Au structure generates two coexisting moire periods (18 Angstroms and 32 Angstroms) at the 2D/3D interface that are otherwise hidden in conventional electron microscopy imaging. We show, via ab initio electronic structure calculations, that charge density is modulated with the longer of these moire periods, illustrating the potential for (opto-)electronic modulation via moire engineering at the 2D/3D interface.
We review progress in developing epitaxial graphene as a material for carbon electronics. In particular, improvements in epitaxial graphene growth, interface control and the understanding of multilayer epitaxial graphenes electronic properties are discussed. Although graphene grown on both polar faces of SiC is addressed, our discussions will focus on graphene grown on the (000-1) C-face of SiC. The unique properties of C-face multilayer epitaxial graphene have become apparent. These films behave electronically like a stack of nearly independent graphene sheets rather than a thin Bernal-stacked graphite sample. The origin of multilayer graphenes electronic behavior is 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 causes each sheet to behave like an isolated graphene plane.
This manuscript presents the general approach to the understanding of the connection between bonding mechanism and electronic structure of graphene on metals. To demonstrate its validity, two limiting cases of the weakly and strongly bonded graphene on Al(111) and Ni(111) are considered, where the Dirac cone is preserved or fully destroyed, respectively. Furthermore, the electronic structure, i. e. doping level, hybridization effects, as well as a gap formation at the Dirac point of the intermediate system, graphene/Cu(111), is fully understood in the framework of the proposed approach. This work summarises the long-term debates regarding connection of the bonding strength and the valence band modification in the graphene/metal systems and paves a way for the effective control of the electronic states of graphene in the vicinity of the Fermi level.
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