Two-dimensional layered MoS2 shows great potential for nanoelectronic and optoelectronic devices due to its high photosensitivity, which is the result of its indirect to direct band gap transition when the bulk dimension is reduced to a single monolayer. Here, we present an exhaustive study of the band alignment and relativistic properties of a van der Waals heterostructure formed between single layers of MoS2 and graphene. A sharp, high-quality MoS2-graphene interface was obtained and characterized by micro-Raman spectroscopy, high-resolution X-ray photoemission spectroscopy (HRXPS), and scanning high-resolution transmission electron microscopy (STEM/HRTEM). Moreover, direct band structure determination of the MoS2/graphene van der Waals heterostructure monolayer was carried out using angle-resolved photoemission spectroscopy (ARPES), shedding light on essential features such as doping, Fermi velocity, hybridization, and band-offset of the low energy electronic dynamics found at the interface. We show that, close to the Fermi level, graphene exhibits a robust, almost perfect, gapless, and n-doped Dirac cone and no significant charge transfer doping is detected from MoS2 to graphene. However, modification of the graphene band structure occurs at rather larger binding energies, as the opening of several miniband-gaps is observed. These miniband-gaps resulting from the overlay of MoS2 and the graphene layer lattice impose a superperiodic potential.
Quantum phase transitions (QPTs) are ubiquitous in strongly correlated materials. However, the microscopic complexity of these systems impedes the quantitative understanding of QPTs. We observed and thoroughly analyzed the rich strongly correlated physics in two profoundly dissimilar regimes of quantum criticality. With a circuit implementing a quantum simulator for the three-channel Kondo model, we reveal the universal scalings toward different low-temperature fixed points and along the multiple crossovers from quantum criticality. An unanticipated violation of the maximum conductance for ballistic free electrons is uncovered. The present charge pseudospin implementation of a Kondo impurity opens access to a broad variety of strongly correlated phenomena.
Stacking two-dimensional materials in so-called van der Waals (vdW) heterostructures, like the combination of GaSe and graphene, provides the ability to obtain hybrid systems which are suitable to design optoelectronic devices. Here, we report the structural and electronic properties of the direct growth of multilayered GaSe by Molecular beam Epitaxy (MBE) on graphene. Reflection high-energy electron diffraction (RHEED) images exhibited sharp streaky features indicative of high quality GaSe layer produced via a vdW epitaxy. Micro-Raman spectroscopy showed that, after the vdW hetero-interface formation, the Raman signature of pristine graphene is preserved. However, the GaSe film tuned the charge density of graphene layer by shifting the Dirac point by about 80 meV toward lower binding energies, attesting an electron transfer from graphene to GaSe. Angle-resolved photoemission spectroscopy (ARPES) measurements showed that the maximum of the valence band of few layers of GaSe are located at the Γ point at a binding energy of about -0.73 eV relatively to the Fermi level (p-type doping). From the ARPES measurements, a hole effective mass defined along the ΓM direction and equal to about m*/m0 = -1.1 was determined. By coupling the ARPES data with high resolution X-ray photoemission spectroscopy (HR-XPS) measurements, the Schottky interface barrier height was estimated to be 1.2 eV. These findings allow deeper understanding of the interlayer interactions and the electronic structure of GaSe/graphene vdW heterostructure.
We investigate the magneto-transport properties of epitaxial graphene single-layer on 4H-SiC(0001), grown by atmospheric pressure graphitization in Ar, followed by H2 intercalation. We directly demonstrate the importance of saturating the Si dangling bonds at the graphene/SiC(0001) interface to achieve high carrier mobility. Upon successful Si dangling bonds elimination, carrier mobility increases from 3 000 cm2V−1s−1 to >11 000 cm2V−1s−1 at 0.3 K. Additionally, graphene electron concentration tends to decrease from a few 1012 cm−2 to less than 1012 cm−2. For a typical large (30 × 280 μm2) Hall bar, we report the observation of the integer quantum Hall states at 0.3 K with well developed transversal resistance plateaus at Landau level filling factors of ν = 2, 6, 10, 14… 42 and Shubnikov de Haas oscillation of the longitudinal resistivity observed from about 1 T. In such a device, the Hall state quantization at ν = 2, at 19 T and 0.3 K, can be very robust: the dissipation in electronic transport can stay very low, with the longitudinal resistivity lower than 5 mΩ, for measurement currents as high as 250 μA. This is very promising in the view of an application in metrology.
demonstrate the tunability of the quasiparticle energy gap of few layered gallium selenide (GaSe) directly grown on a bilayer graphene substrate by molecular beam epitaxy (MBE). Our results show that the band gap is about 3.50 ± 0.05 eV for single-tetralayer (1TL), 3.00 ± 0.05 eV for bi-tetralayer (2TL) and 2.30 ± 0.05 eV for tritetralayer (3TL). This band gap evolution of GaSe, in particularly the shift of the valence band with respect to the Fermi level, was confirmed by angle-resolved photoemission spectroscopy (ARPES) measurements and our theoretical calculations. Moreover, we observed a charge transfer in GaSe/graphene van der Waals (vdW) heterostructure using ARPES. These findings demonstrate the high impact on the GaSe electronic band structure and electronic properties that can be obtained by the control of 2D materials layer thickness and the graphene induced doping.
Structural defects in the molybdenum disulfide (MoS) monolayer are widely known for strongly altering its properties. Therefore, a deep understanding of these structural defects and how they affect MoS electronic properties is of fundamental importance. Here, we report on the incorporation of atomic hydrogen in monolayered MoS to tune its structural defects. We demonstrate that the electronic properties of single layer MoS can be tuned from the intrinsic electron (n) to hole (p) doping via controlled exposure to atomic hydrogen at room temperature. Moreover, this hydrogenation process represents a viable technique to completely saturate the sulfur vacancies present in the MoS flakes. The successful incorporation of hydrogen in MoS leads to the modification of the electronic properties as evidenced by high resolution X-ray photoemission spectroscopy and density functional theory calculations. Micro-Raman spectroscopy and angle resolved photoemission spectroscopy measurements show the high quality of the hydrogenated MoS confirming the efficiency of our hydrogenation process. These results demonstrate that the MoS hydrogenation could be a significant and efficient way to achieve tunable doping of transition metal dichalcogenides (TMD) materials with non-TMD elements.
The stacking order of multilayer graphene has a profound influence on its electronic properties. In particular, it has been predicted that a rhombohedral stacking sequence displays a very flat conducting surface state: the longer the sequence, the flatter the band. In such a flat band, the role of electron-electron correlation is enhanced, possibly resulting in high Tc superconductivity, magnetic order, or charge density wave order. Here we demonstrate that rhombohedral multilayers are easily obtained by epitaxial growth on 3C-SiC(111) on a 2° off-axis 6H-SiC(0001). The resulting samples contain rhombohedral sequences of five layers on 70% of the surface. We confirm the presence of the flat band at the Fermi level by scanning tunneling spectroscopy and angle-resolved photoemission spectroscopy, in close agreement with the predictions of density functional theory calculations.
Nitrogen doping of graphene is of great interest for both fundamental research to explore the effect of dopants on a 2D electrical conductor and applications such as lithium storage, composites, and nanoelectronic devices. Here, we report on the modifications of the electronic properties of epitaxial graphene thanks to the introduction, during the growth, of nitrogen-atom substitution in the carbon honeycomb lattice. High-resolution transmission microscopy and low-energy electron microscopy investigations indicate that the nitrogen-doped graphene is uniform at large scale. The substitution of nitrogen atoms in the graphene planes was confirmed by high-resolution X-ray photoelectron spectroscopy, which reveals several atomic configurations for the nitrogen atoms: graphitic-like, pyridine-like, and pyrrolic-like. Angle-resolved photoemission measurements show that the N-doped graphene exhibits large n-type carrier concentrations of 2.6 × 10(13) cm(-2), about 4 times more than what is found for pristine graphene, grown under similar pressure conditions. Our experiments demonstrate that a small amount of dopants (<1%) can significantly tune the electronic properties of graphene by shifting the Dirac cone about 0.3 eV toward higher binding energies with respect to the π band of pristine graphene, which is a key feature for envisioning applications in nanoelectronics.
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