Symmetry Engineering in Twisted Bilayer WTe2.

The fabrication of artificial structures using a twisted van der Waals assembly has been a key technique for recent advancements in the research of two-dimensional (2D) materials. To date, various exotic phenomena have been observed thanks to the modified electron correlation or moiré structure controlled by the twist angle. However, the twisted van der Waals assembly has further potential to modulate the physical properties by controlling the symmetry. In this study, we fabricated twisted bilayer WTe2 and demonstrated that the twist angle successfully controls the spatial inversion symmetry and hence the spin splitting in the band structure. Our results reveal the further potential of a twisted van der Waals assembly, suggesting the feasibility of pursuing new physical phenomena in 2D materials based on the control of symmetry.

Resonant Tunneling between Quantized Subbands in van der Waals Double Quantum Well Structure Based on Few-Layer WSe2.

We demonstrate van der Waals double quantum well (vDQW) devices based on few-layer WSe2 quantum wells and a few-layer h-BN tunnel barrier. Due to the strong out-of-plane confinement, an exfoliated WSe2 exhibits quantized subband states at the Γ point in its valence band. Here, we report resonant tunneling and negative differential resistance in vDQW at room temperature owing to momentum- and energy-conserved tunneling between the quantized subbands in each well. Compared to single quantum well (QW) devices with only one QW layer possessing quantized subbands, superior current peak-to-valley ratios were obtained for the DQWs. Our findings suggest a new direction for utilizing few-layer-thick transition metal dichalcogenides in subband QW devices, bridging the gap between two-dimensional materials and state-of-the-art semiconductor QW electronics.

Resonant Tunneling Due to van der Waals Quantum-Well States of Few-Layer WSe2 in WSe2/h-BN/p+-MoS2 Junction.

Few-layer transition metal dichalcogenides (TMDs) exhibit out-of-plane wave function confinement with subband quantization. This phenomenon is totally absent in monolayer crystals and is regarded as resulting from a naturally existing van der Waals quantum-well state. Because the energy separation between the subbands corresponds to the infrared wavelength range, few-layer TMDs are attractive for their potential to facilitate the application of TMD semiconductors as infrared photodetectors and emitters. Here, we report a few-layer WSe2/h-BN tunnel barrier/multilayer p+-MoS2 tunnel junction to access the quantized subbands of few-layer WSe2 via tunneling spectroscopy measurements. Resonant tunneling and a negative differential resistance were observed when the top of the valence band Γ-point of p+-MoS2 was energetically aligned with one of the empty subbands at the Γ-point of few-layer WSe2. These results demonstrate a critical step toward the utilization of subband quantization in few-layer TMD materials for infrared optoelectronics applications.

3D Manipulation of 2D Materials Using Microdome Polymer.

We demonstrate 3D mechanical manipulations, such as sliding, rotating, folding, flipping, and exfoliating, of 2D materials using a microdome polymer (MDP) via in situ real-time observation with an optical microscope. A dimethylpolysiloxane (PDMS)-based MDP is covered with a poly(vinyl chloride) (PVC) adhesion layer. This PVC-MDP structure enables us to achieve small and adjustable contact areas between the PVC-MDP and a 2D-material flake, which is typically between ∼10 and ∼100 µm in diameter. The adhesion between the PVC polymer and 2D materials is fully tunable with temperature: Strong adhesion at ∼70 °C allows pick-up of the 2D material, and release occurs at ∼130 °C when the adhesion is weak. Thus the PVC-MDP functions as a point-of-contact manipulator for 2D materials, permitting the 3D manipulation of 2D-material flakes. Our method could facilitate the expansion of van der Waals heterostructure fabrication technology and the development of preparation techniques for more complex 3D structures.

Cyclotron Resonance Study of Monolayer Graphene under Double Moiré Potentials.

We report the first cyclotron resonance study of monolayer graphene under double-moiré potentials in which the crystal axis of graphene is nearly aligned to those of both the top and bottom hexagonal boron nitride (h-BN) layers. Under mid-infrared light irradiation, we observe cyclotron resonance absorption with the following unique features: (1) cyclotron resonance magnetic field BCR is entirely different from that of nonaligned monolayer graphene, (2) BCR exhibits strong electron-hole asymmetry, and (3) splitting of BCR is observed for |ν| < 1, with the split maximum at |ν| = 1, resulting in eyeglass-shaped trajectories. These features are well explained by considering the large bandgap induced by the double moiré potentials, the electron-hole asymmetry in the Fermi velocity, and the Fermi-level-dependent enhancement of spin gaps, which suggests a large electron-electron correlation contribution in this system.

Hexagonal Boron Nitride Synthesized at Atmospheric Pressure Using Metal Alloy Solvents: Evaluation as a Substrate for 2D Materials.

Hexagonal boron nitride (h-BN) synthesized under high pressure and high temperature (HPHT) has been used worldwide in two-dimensional (2D) materials research as an essential material for constructing van der Waals heterostructures. Here, we study h-BN synthesized with another method, i.e., via synthesis at atmospheric pressure and high temperature (APHT) using a metal alloy solvent. First, we examine the APHT h-BN in a bulk crystal form using cathodoluminescence and find that it does not have carbon-rich domains that inevitably exist in a core region of all the HPHT h-BN crystals. Next, we statistically compare the size of the crystal flakes exfoliated on a SiO2/Si substrate from APHT and HPHT h-BN crystals by employing our automated 2D material searching system. Finally, we provide direct evidence that APHT h-BN can serve as a high-quality substrate for 2D materials by demonstrating high carrier mobility, ballistic transport, and Hofstadter butterfly in graphene and photoluminescence in WS2.

Electrical Control of Cyclotron Resonance in Dual-Gated Trilayer Graphene.

Landau levels (LLs) of ABA-stacked trilayer graphene (TLG) are described as the combination of monolayer graphene-like LLs and bilayer graphene-like LLs. They are extremely sensitive to the applied perpendicular electric displacement field D. Here, we demonstrate the electrical control of cyclotron resonance (CR) in a dual-gated ABA-stacked TLG. Under the irradiation of mid-infrared light, we observed the photovoltage induced by the CR absorption through the photothermoelectric effect. The resonant magnetic field in CR is changed by applying D while keeping the carrier density constant. Numerical simulations based on the tight-binding model complement the experimental observations. We believe that the present study provides a boost to graphene-based photodetectors and photoemitters with an electrically tunable wavelength in mid-infrared to terahertz spectral ranges.

Carbon-Rich Domain in Hexagonal Boron Nitride: Carrier Mobility Degradation and Anomalous Bending of the Landau Fan Diagram in Adjacent Graphene.

Hexagonal boron nitride (h-BN) crystals grown under ultrahigh pressures and ultrahigh temperatures exhibit a high crystallinity and are used throughout the world as ideal substrates and insulating layers in van der Waals heterostructures. However, in their central region, these crystals have domains which contain a significant density of carbon impurities. In this study, we utilized cathodoluminescence and far-ultraviolet photoluminescence to reveal that the carbon (C)-rich domain can exist even after exfoliation. Then, we studied the carrier transport of graphene in h-BN/graphene/h-BN van der Waals heterostructures, precisely arranging the graphene to straddle the border of the C-rich domain in h-BN. We found that the carrier mobility of graphene on the C-rich h-BN domain was significantly suppressed. In addition, characteristic bending of the Landau fan diagram was observed on the electron-doped side. These results suggest that the C-rich domain in h-BN forms an impurity level and induces extrinsic carrier scattering into adjacent graphene.

Imaging Bulk and Edge Transport near the Dirac Point in Graphene Moiré Superlattices.

Van der Waals structures formed by aligning monolayer graphene with insulating layers of hexagonal boron nitride exhibit a moiré superlattice that is expected to break sublattice symmetry. Despite an energy gap of several tens of millielectronvolts opening in the Dirac spectrum, electrical resistivity remains lower than expected at low temperature and varies between devices. While subgap states are likely to play a role in this behavior, their precise nature is unclear. We present a scanning gate microscopy study of moiré superlattice devices with comparable activation energy but with different charge disorder levels. In the device with higher charge impurity (∼1010 cm-2) and lower resistivity (∼10 kΩ) at the Dirac point we observe current flow along the graphene edges. Combined with simulations, our measurements suggest that enhanced edge doping is responsible for this effect. In addition, a device with low charge impurity (∼109 cm-2) and higher resistivity (∼100 kΩ) shows subgap states in the bulk, consistent with the absence of shunting by edge currents.

Intersubband Landau Level Couplings Induced by In-Plane Magnetic Fields in Trilayer Graphene.

We observed broken-symmetry quantum Hall effects and level crossings between spin- and valley- resolved Landau levels (LLs) in Bernal stacked trilayer graphene. When the magnetic field was tilted with respect to the sample normal from 0° to 66°, the LL crossings formed at intersections of zeroth and second LLs from monolayer-graphene-like and bilayer-graphene-like subbands, respectively, exhibited a sequence of transitions. The results indicate the LLs from different subbands are coupled by in-plane magnetic fields (B_{∥}), which was explained by developing the tight-binding model Hamiltonian of trilayer graphene under B_{∥}.

Cubic Rashba spin-orbit interaction of a two-dimensional hole gas in a strained-Ge/SiGe quantum well.

The spin-orbit interaction (SOI) of a two-dimensional hole gas in the inversion symmetric semiconductor Ge is studied in a strained-Ge/SiGe quantum well structure. We observe weak antilocalization (WAL) in the magnetoconductivity measurement, revealing that the WAL feature can be fully described by the k-cubic Rashba SOI theory. Furthermore, we demonstrate electric field control of the Rashba SOI. Our findings reveal that the heavy hole (HH) in strained Ge is a purely cubic Rashba system, which is consistent with the spin angular momentum m(j) = ± 3/2 nature of the HH wave function.

Cyclic Wear Reliability of 2D Monolayers.

Understanding wear, a critical factor impacting the reliability of mechanical systems, is vital for nano-, meso-, and macroscale applications. Due to the complex nature of nanoscale wear, the behavior of nanomaterials such as two-dimensional materials under cyclic wear and their surface damage mechanism is yet unexplored. In this study, we used atomic force microscopy coupled with molecular dynamic simulations to statistically examine the cyclic wear behavior of monolayer graphene, MoS2, and WSe2. We show that graphene displays exceptional durability and lasts over 3000 cycles at 85% of the applied critical normal load before failure, while MoS2 and WSe2 last only 500 cycles on average. Moreover, graphene undergoes catastrophic failure as a result of stress concentration induced by local out-of-plane deformation. In contrast, MoS2 and WSe2 exhibit intermittent failure, characterized by damage initiation at the edge of the wear track and subsequent propagation throughout the entire contact area. In addition to direct implications for MEMS and NEMS industries, this work can also enable the optimization of the use of 2D materials as lubricant additives on a macroscopic level.

Crossover between rigid and reconstructed moiré lattice in h-BN-encapsulated twisted bilayer WSe2 with different twist angles.

A moiré lattice in a twisted-bilayer transition metal dichalcogenide (tBL-TMD) exhibits a complex atomic reconstruction effect when its twist angle is less than a few degrees. The influence of the atomic reconstruction on material properties of the tBL-TMD has been of particular interest. In this study, we performed scanning transmission electron microscopy (STEM) imaging of a moiré lattice in h-BN-encapsulated twisted bilayer WSe2 with various twist angles. Atomic-resolution imaging of the moiré lattice revealed a reconstructed moiré lattice below a crossover twist angle of ∼4° and a rigid moiré lattice above this angle. Our findings indicate that h-BN encapsulation has a considerable influence on lattice reconstruction, as the crossover twist angle was larger in h-BN-encapsulated devices compared to non-encapsulated devices. We believe that this difference is due to the improved flatness and uniformity of the twisted bilayers with h-BN encapsulation. Our results provide a foundation for a deeper understanding of the lattice reconstruction in twisted TMD materials with h-BN encapsulation.

Super-Ballistic Width Dependence of Thermal Conductivity in Graphite Nanoribbons and Microribbons.

The super-ballistic temperature dependence of thermal conductivity, facilitated by collective phonons, has been widely studied. It has been claimed to be unambiguous evidence for hydrodynamic phonon transport in solids. Alternatively, hydrodynamic thermal conduction is predicted to be as strongly dependent on the width of the structure as is fluid flow, while its direct demonstration remains an unexplored challenge. In this work, we experimentally measured thermal conductivity in several graphite ribbon structures with different widths, from 300 nm to 1.2 µm, and studied its width dependence in a wide temperature range of 10-300 K. We observed enhanced width dependence of the thermal conductivity in the hydrodynamic window of 75 K compared to that in the ballistic limit, which provides indispensable evidence for phonon hydrodynamic transport from the perspective of peculiar width dependence. This will help to find the missing piece to complete the puzzle of phonon hydrodynamics, and guide future attempts at efficient heat dissipation in advanced electronic devices.

Observation of phonon Poiseuille flow in isotopically purified graphite ribbons.

In recent times, the unique collective transport physics of phonon hydrodynamics motivates theoreticians and experimentalists to explore it in micro- and nanoscale and at elevated temperatures. Graphitic materials have been predicted to facilitate hydrodynamic heat transport with their intrinsically strong normal scattering. However, owing to the experimental difficulties and vague theoretical understanding, the observation of phonon Poiseuille flow in graphitic systems remains challenging. In this study, based on a microscale experimental platform and the pertinent occurrence criterion in anisotropic solids, we demonstrate the existence of the phonon Poiseuille flow in a 5.5 µm-wide, suspended and isotopically purified graphite ribbon up to a temperature of 90 K. Our observation is well supported by our theoretical model based on a kinetic theory with fully first-principles inputs. Thus, this study paves the way for deeper insight into phonon hydrodynamics and cutting-edge heat manipulating applications.

Boundary scattering in ballistic graphene.

We report magnetotransport measurements in ballistic graphene mesoscopic wires where the charge carrier mean free path is comparable to the wire width W. Magnetoresistance curves show characteristic peak structures where the peak field scales with the ratio of cyclotron radius R(c) and wire width W as W/R(c)=0.9±0.1, due to diffusive boundary scattering. The obtained proportionality constant between R(c) and W differs from that of a classical semiconductor two-dimensional electron system in which W/R(c)=0.55.

Atomic force microscopy based tunable local anodic oxidation of graphene.

We have fabricated graphene/graphene oxide/graphene (G/GO/G) junctions by local anodic oxidation lithography using atomic force microscopy (AFM). The conductance of the G/GO/G junction decreased with the bias voltage applied to the AFM cantilever V(tip). For G/GO/G junctions fabricated with large and small |V(tip)|. GO was semi-insulating and semiconducting, respectively. AFM-based LAO lithography can be used to locally oxidize graphene with various oxidation levels and achieve tunability from semiconducting to semi-insulating GO.

All-dry flip-over stacking of van der Waals junctions of 2D materials using polyvinyl chloride.

We demonstrated an all-dry polymer-to-polymer transfer technique for two-dimensional (2D) crystal flakes using a polyvinyl chloride (PVC) layer deposited on a piece of polydimethylsiloxane (PDMS). Unexpectedly, the pickup/release temperatures were modified in wider temperature range simply by changing the thickness of the PVC layer than changing the plasticizer ratio. Utilizing the difference in the pickup/release temperatures depending on the PVC film thickness, 2D flakes were transferred from a thicker PVC film to a thinner one. This polymer-to-polymer transfer technique can be utilized to flip over van der Waals heterostructures. As a demonstration, we fabricated a mountain-like stacked structure of hexagonal boron nitride flakes using the flip-over stacking technique. Finally, we compared the results of thermomechanical analysis with the pickup/release temperatures of the PVC/PDMS stamp. The PVC was revealed to be at the glass transition and in the viscoelastic flow regimes when the 2D flakes were picked up and dry released, respectively. Our polymer-to-polymer transfer method facilitates flip-over van der Waals stacking in an all-dry manner, expanding the possibility of 2D materials device fabrications.

Dry pick-and-flip assembly of van der Waals heterostructures for microfocus angle-resolved photoemission spectroscopy.

We present a dry pick-and-flip assembly technique for angle-resolved photoemission spectroscopy (ARPES) of van der Waals heterostructures. By combining Elvacite2552C acrylic resin and 1-ethyl-3-methylimidazolium ionic liquid, we prepared polymers with glass transition temperatures (Tg) ranging from 37 to 100 â„ƒ. The adhesion of the polymer to the 2D crystals was enhanced at [Formula: see text]. By utilizing the difference in [Formula: see text], a 2D heterostructure can be transferred from a high-[Formula: see text] polymer to a lower-[Formula: see text] polymer, which enables flipping its surface upside down. This process is suitable for assembling heterostructures for ARPES, where the top capping layer should be monolayer graphene. The laser-based micro-focused ARPES measurements of 5-layer WTe2, 3-layer MoTe2, 2-layer WTe2/few-layer Cr2Ge2Te6, and twisted double bilayer WTe2 demonstrate that this process can be utilized as a versatile sample fabrication method for investigating the energy spectra of 2D heterostructures.

Emergence of orbital angular moment at van Hove singularity in graphene/h-BN moiré superlattice.

Bloch electrons lacking inversion symmetry exhibit orbital magnetic moments owing to the rotation around their center of mass; this moment induces a valley splitting in a magnetic field. For the graphene/h-BN moiré superlattice, inversion symmetry is broken by the h-BN. The superlattice potential generates a series of Dirac points (DPs) and van Hove singularities (vHSs) within an experimentally accessible low energy state, providing a platform to study orbital moments with respect to band structure. In this work, theoretical calculations and magnetothermoelectric measurements are combined to reveal the emergence of an orbital magnetic moment at vHSs in graphene/h-BN moiré superlattices. The thermoelectric signal for the vHS at the low energy side of the hole-side secondary DP exhibited significant magnetic field-induced valley splitting with an effective g-factor of approximately 130; splitting for other vHSs was negligible. This was attributed to the emergence of an orbital magnetic moment at the second vHS at the hole-side.