Spatially resolved electronic structure of twisted graphene

We have used scanning tunneling microscopy and spectroscopy to resolve the spatial variation of the density of states of twisted graphene layers on top of a highly oriented pyrolytic graphite substrate. Owing to the twist a moire pattern develops with a periodicity that is substantially larger than the periodicity of a single layer graphene. The twisted graphene layer has electronic properties that are distinctly different from that of a single layer graphene due to the nonzero interlayer coupling. For small twist angles (about 1-3.5 degree) the integrated differential conductivity spectrum exhibits two well-defined Van Hove singularities. Spatial maps of the differential conductivity that are recorded at energies near the Fermi level exhibit a honeycomb structure that is comprised of two inequivalent hexagonal sub-lattices. For energies |E-E_F|>0.3 eV the hexagonal structure in the differential conductivity maps vanishes. We have performed tight-binding calculations of the twisted graphene system using the propagation method, in which a third graphene layer is added to mimic the substrate. This third layer lowers the symmetry and explains the development of the two hexagonal sub-lattices in the moire pattern. Our experimental results are in excellent agreement with the tight-binding calculations.Comment: To appear in Phys. Rev.

Growth of silicon on tungsten diselenide

Here, we report a scanning tunneling microscopy and spectroscopy study of the growth of silicon on a tungsten diselenide (WSe2) substrate. We have found convincing experimental evidence that silicon does not remain on the WSe2 substrate but rather intercalates between the top layers of WSe2. Upon silicon deposition, the flat WSe2 surface converts into a surface with a hill-and-valley structure. The lattice constant of the hill-and-valley structure is identical to the lattice constant of WSe2 and the transition from hills to valleys is very gradual, suggesting that the top layer is composed of pristine WSe2. In order to verify this conjecture, we have removed the height information from our scanning tunneling microscopy signal and obtained chemical contrast of the surface by recording dI/dz, rather than the conventional regulation voltage of the z-piezo. The spatially resolved dI/dz maps provide compelling evidence that the deposited silicon does indeed not reside on top of the WSe2 substrate

Control of the metal/WS2 contact properties using 2-dimensional buffer layers

Transition metal dichalcogenides (TMDC) have recently attracted much attention as a promising platform for the realization of 2-dimensional (2D) electronic devices. One of the major challenges for their wide-scale application is the control of the potential barrier at the metal/TMDC junction. Using conductive atomic force microscopy (c-AFM) we have investigated modifications of the Schottky barrier height (SBH) across a Pt/WS2 junction by the introduction of thin buffer layers of graphene and MoSe2. While graphene greatly reduces the contact resistance in both bias directions, thin layers of MoSe2 lower the Schottky barrier and leave the rectifying properties of the junction intact. We have studied the dependence of the transport properties on the thickness of the graphene and MoSe2 buffer layers. In both cases, the charge transport characteristics can be tailored by varying the buffer layer thickness. The edge of single layer graphene is observed to form an ohmic contact to the underlying WSe2 substrate. This study demonstrates that the introduction of atomically thin MoSe2 and graphene buffer layers is a feasible and elegant method to control the Schottky barrier when contacting TMDCs. The results are important for the fabrication of devices utilizing 2D materials

Environmentally Controlled Charge Carrier Injection Mechanisms of Metal/WS2 Junctions

Here we report on a novel, noninvasive route for operando tailoring of the charge transport properties of metal/WS2 contacts without the negative impacts to two-dimensional materials arising from conventional doping methods. The doping level of thin WS2 flakes supported on insulating mica is susceptible to local charge variations induced by the presence of a hydration layer between mica and WS2. We demonstrate, via the use of several complementary scanning probe techniques, that the direct control of the state and thickness of this intercalated water film controls the charge injection properties of Pt/WS2 nanocontacts. A switch from unipolar to ambipolar transport was achieved by environmentally controlling the thickness of the intercalated water. We show that the effect persists even for multilayer flakes and that it is completely reversible, opening a new route toward the realization of novel electronics with environmentally controllable functionalities

Singularities and topologically protected states in twisted bilayer graphene

We have studied the structural and electronic properties of twisted bilayer graphene by scanning tunneling microscopy (STM). For twist angles in the range of about 1° to 4°, the twisted bilayer graphene possesses two Van Hove singularities in the vicinity of the Fermi level. We use the exact location of these Van Hove singularities to determine the twist angle dependent interlayer hopping energy. For a twist angle of 0.6°, we found a hexagonal network of topologically protected one-dimensional channels that run along the boundaries of the AB/BA domains. The electric field in the tunnel junction is responsible for the breaking of the symmetry of the AB and BA domains and the development of the hexagonal network of topologically protected states. The latter shows that the electric field in the tunneling junction can significantly affect the topological nature of two-dimensional materials, and therefore, one should be cautious when interpreting scanning tunneling microscopy and spectroscopy experiments of this class of materials

Intercalation of Si between MoS2 layers

We report a combined experimental and theoretical study of the growth of sub-monolayer amounts of silicon (Si) on molybdenum disulfide (MoS2). At room temperature and low deposition rates we have found compelling evidence that the deposited Si atoms intercalate between the MoS2 layers. Our evidence relies on several experimental observations: (1) Upon the deposition of Si on pristine MoS2 the morphology of the surface transforms from a smooth surface to a hill-and-valley surface. The lattice constant of the hill-and-valley structure amounts to 3.16 Å, which is exactly the lattice constant of pristine MoS2. (2) The transitions from hills to valleys are not abrupt, as one would expect for epitaxial islands growing on-top of a substrate, but very gradual. (3) I(V) scanning tunneling spectroscopy spectra recorded at the hills and valleys reveal no noteworthy differences. (4) Spatial maps of dI/dz reveal that the surface exhibits a uniform work function and a lattice constant of 3.16 Å. (5) X-ray photo-electron spectroscopy measurements reveal that sputtering of the MoS2/Si substrate does not lead to a decrease, but an increase of the relative Si signal. Based on these experimental observations we have to conclude that deposited Si atoms do not reside on the MoS2 surface, but rather intercalate between the MoS2 layers. Our conclusion that Si intercalates upon the deposition on MoS2 is at variance with the interpretation by Chiappe et al. (Adv. Mater. 2014, 26, 2096-2101) that silicon forms a highly strained epitaxial layer on MoS2. Finally, density functional theory calculations indicate that silicene clusters encapsulated by MoS2 are stable