Tunable moiré bands and strong correlations in small-twist-angle bilayer graphene.

According to electronic structure theory, bilayer graphene is expected to have anomalous electronic properties when it has long-period moiré patterns produced by small misalignments between its individual layer honeycomb lattices. We have realized bilayer graphene moiré crystals with accurately controlled twist angles smaller than 1° and studied their properties using scanning probe microscopy and electron transport. We observe conductivity minima at charge neutrality, satellite gaps that appear at anomalous carrier densities for twist angles smaller than 1°, and tunneling densities-of-states that are strongly dependent on carrier density. These features are robust up to large transverse electric fields. In perpendicular magnetic fields, we observe the emergence of a Hofstadter butterfly in the energy spectrum, with fourfold degenerate Landau levels, and broken symmetry quantum Hall states at filling factors ±1, 2, 3. These observations demonstrate that at small twist angles, the electronic properties of bilayer graphene moiré crystals are strongly altered by electron-electron interactions.

Spin-Conserving Resonant Tunneling in Twist-Controlled WSe2-hBN-WSe2 Heterostructures.

We investigate interlayer tunneling in heterostructures consisting of two tungsten diselenide (WSe2) monolayers with controlled rotational alignment, and separated by hexagonal boron nitride. In samples where the two WSe2 monolayers are rotationally aligned we observe resonant tunneling, manifested by a large conductance and negative differential resistance in the vicinity of zero interlayer bias, which stem from energy- and momentum-conserving tunneling. Because the spin-orbit coupling leads to coupled spin-valley degrees of freedom, the twist between the two WSe2 monolayers allows us to probe the conservation of spin-valley degree of freedom in tunneling. In heterostructures where the two WSe2 monolayers have a 180° relative twist, such that the Brillouin zone of one layer is aligned with the time-reversed Brillouin zone of the opposite layer, the resonant tunneling between the layers is suppressed. These findings provide evidence that, in addition to momentum, the spin-valley degree of freedom is also conserved in vertical transport.

Tunable Γ-K Valley Populations in Hole-Doped Trilayer WSe_{2}.

We present a combined experimental and theoretical study of valley populations in the valence bands of trilayer WSe_{2}. Shubnikov-de Haas oscillations show that trilayer holes populate two distinct subbands associated with the K and Γ valleys, with effective masses 0.5m_{e} and 1.2m_{e}, respectively; m_{e} is the bare electron mass. At a fixed total hole density, an applied transverse electric field transfers holes from Γ orbitals to K orbitals. We are able to explain this behavior in terms of the larger layer polarizability of the K orbital subband.

Density-Dependent Quantum Hall States and Zeeman Splitting in Monolayer and Bilayer WSe_{2}.

We report a study of the quantum Hall states (QHS) of holes in mono- and bilayer WSe_{2}. The QHS sequence transitions between predominantly even and predominantly odd filling factors as the hole density is tuned in the range 1.6-12×10^{12} cm^{-2}. Measurements in tilted magnetic fields reveal an insensitivity of the QHS to the in-plane magnetic field, evincing that the hole spin is locked perpendicular to the WSe_{2} plane. Furthermore, the QHS sequence is insensitive to an applied electric field. These observations imply that the QHS sequence is controlled by the Zeeman-to-cyclotron energy ratio, which remains constant as a function of perpendicular magnetic field at a fixed carrier density, but changes as a function of density due to strong electron-electron interaction.

van der Waals Heterostructures with High Accuracy Rotational Alignment.

We describe the realization of van der Waals (vdW) heterostructures with accurate rotational alignment of individual layer crystal axes. We illustrate the approach by demonstrating a Bernal-stacked bilayer graphene formed using successive transfers of monolayer graphene flakes. The Raman spectra of this artificial bilayer graphene possess a wide 2D band, which is best fit by four Lorentzians, consistent with Bernal stacking. Scanning tunneling microscopy reveals no moiré pattern on the artificial bilayer graphene, and tunneling spectroscopy as a function of gate voltage reveals a constant density of states, also in agreement with Bernal stacking. In addition, electron transport probed in dual-gated samples reveals a band gap opening as a function of transverse electric field. To illustrate the applicability of this technique to realize vdW heterostructuctures in which the functionality is critically dependent on rotational alignment, we demonstrate resonant tunneling double bilayer graphene heterostructures separated by hexagonal boron-nitride dielectric.

Shubnikov-de Haas Oscillations of High-Mobility Holes in Monolayer and Bilayer WSe_{2}: Landau Level Degeneracy, Effective Mass, and Negative Compressibility.

We study the magnetotransport properties of high-mobility holes in monolayer and bilayer WSe_{2}, which display well defined Shubnikov-de Haas (SdH) oscillations, and quantum Hall states in high magnetic fields. In both mono- and bilayer WSe_{2}, the SdH oscillations and the quantum Hall states occur predominantly at even filling factors, evincing a twofold Landau level degeneracy. The Fourier transform analysis of the SdH oscillations in bilayer WSe_{2} reveals the presence of two subbands localized in the top or the bottom layer, as well as negative compressibility. From the temperature dependence of the SdH oscillations we determine a hole effective mass of 0.45m_{0} for both mono- and bilayer WSe_{2}.

Intrinsic disorder in graphene on transition metal dichalcogenide heterostructures.

Semiconducting transition metal dichalchogenides (TMDs) are a family of van der Waals bonded materials that have recently received interest as alternative substrates to hexagonal boron nitride (hBN) for graphene, as well as for components in novel graphene-based device heterostructures. We elucidate the local structural and electronic properties of graphene on TMD heterostructures through scanning tunneling microscopy and spectroscopy measurements. We find that crystalline defects intrinsic to TMDs induce substantial electronic scattering and charge carrier density fluctuations in the graphene. These signatures of local disorder explain the significant degradation of graphene device mobilities using TMD substrates, particularly compared to similar graphene on hBN devices.

Air Stable Doping and Intrinsic Mobility Enhancement in Monolayer Molybdenum Disulfide by Amorphous Titanium Suboxide Encapsulation.

To reduce Schottky-barrier-induced contact and access resistance, and the impact of charged impurity and phonon scattering on mobility in devices based on 2D transition metal dichalcogenides (TMDs), considerable effort has been put into exploring various doping techniques and dielectric engineering using high-κ oxides, respectively. The goal of this work is to demonstrate a high-κ dielectric that serves as an effective n-type charge transfer dopant on monolayer (ML) molybdenum disulfide (MoS2). Utilizing amorphous titanium suboxide (ATO) as the "high-κ dopant", we achieved a contact resistance of ∼180 Ω·µm that is the lowest reported value for ML MoS2. An ON current as high as 240 µA/µm and field effect mobility as high as 83 cm(2)/V-s were realized using this doping technique. Moreover, intrinsic mobility as high as 102 cm(2)/V-s at 300 K and 501 cm(2)/V-s at 77 K were achieved after ATO encapsulation that are among the highest mobility values reported on ML MoS2. We also analyzed the doping effect of ATO films on ML MoS2, a phenomenon that is absent when stoichiometric TiO2 is used, using ab initio density functional theory (DFT) calculations that shows excellent agreement with our experimental findings. On the basis of the interfacial-oxygen-vacancy mediated doping as seen in the case of high-κ ATO-ML MoS2, we propose a mechanism for the mobility enhancement effect observed in TMD-based devices after encapsulation in a high-κ dielectric environment.

Gate-tunable resonant tunneling in double bilayer graphene heterostructures.

We demonstrate gate-tunable resonant tunneling and negative differential resistance in the interlayer current-voltage characteristics of rotationally aligned double bilayer graphene heterostructures separated by hexagonal boron nitride (hBN) dielectric. An analysis of the heterostructure band alignment using individual layer densities, along with experimentally determined layer chemical potentials indicates that the resonance occurs when the energy bands of the two bilayer graphene are aligned. We discuss the tunneling resistance dependence on the interlayer hBN thickness, as well as the resonance width dependence on mobility and rotational alignment.

Band offset and negative compressibility in graphene-MoS2 heterostructures.

We use electron transport to characterize monolayer graphene-multilayer MoS2 heterostructures. Our samples show ambipolar characteristics and conductivity saturation on the electron branch that signals the onset of MoS2 conduction band population. Surprisingly, the carrier density in graphene decreases with gate bias once MoS2 is populated, demonstrating negative compressibility in MoS2. We are able to interpret our measurements quantitatively by accounting for disorder and using the random phase approximation (RPA) for the exchange and correlation energies of both Dirac and parabolic-band two-dimensional electron gases. This interpretation allows us to extract the energetic offset between the conduction band edge of MoS2 and the Dirac point of graphene.

Reconfigurable Complementary Monolayer MoTe2 Field-Effect Transistors for Integrated Circuits.

Transition metal dichalcogenides are of interest for next generation switches, but the lack of low resistance electron and hole contacts in the same material has hindered the development of complementary field-effect transistors and circuits. We demonstrate an air-stable, reconfigurable, complementary monolayer MoTe2 field-effect transistor encapsulated in hexagonal boron nitride, using electrostatically doped contacts. The introduction of a multigate design with prepatterned bottom contacts allows us to independently achieve low contact resistance and threshold voltage tuning, while also decoupling the Schottky contacts and channel gating. We illustrate a complementary inverter and a p-i-n diode as potential applications.

Band Alignment in WSe2-Graphene Heterostructures.

Using different types of WSe2 and graphene-based heterostructures, we experimentally determine the offset between the graphene neutrality point and the WSe2 conduction and valence band edges, as well as the WSe2 dielectric constant along the c-axis. In a first heterostructure, consisting of WSe2-on-graphene, we use the WSe2 layer as the top dielectric in dual-gated graphene field-effect transistors to determine the WSe2 capacitance as a function of thickness, and the WSe2 dielectric constant along the c-axis. In a second heterostructure consisting of graphene-on-WSe2, the lateral electron transport shows ambipolar behavior characteristic of graphene combined with a conductivity saturation at sufficiently high positive (negative) gate bias, associated with carrier population of the conduction (valence) band in WSe2. By combining the experimental results from both heterostructures, we determine the band offset between the graphene charge neutrality point, and the WSe2 conduction and valence band edges.