Interplay of Landau Quantization and Interminivalley Scatterings in a Weakly Coupled Moiré Superlattice.

Double-layer quantum systems are promising platforms for realizing novel quantum phases. Here, we report a study of quantum oscillations (QOs) in a weakly coupled double-layer system composed of a large-angle twisted-double-bilayer graphene (TDBG). We quantify the interlayer coupling strength by measuring the interlayer capacitance from the QOs pattern at low temperatures, revealing electron-hole asymmetry. At high temperatures when SdHOs are thermally smeared, we observe resistance peaks when Landau levels (LLs) from two moiré minivalleys are aligned, regardless of carrier density; eventually, it results in a 2-fold increase of oscillating frequency in D, serving as compelling evidence of the magneto-intersub-band oscillations (MISOs) in double-layer systems. The temperature dependence of MISOs suggests that electron-electron interactions play a crucial role and the scattering times obtained from MISO thermal damping are correlated with the interlayer coupling strength. Our study reveals intriguing interplays among Landau quantization, moiré band structure, and scatterings.

MoS2-Thin Film Transistor Based Flexible 2T1C Driving Circuits for Active-Matrix Displays.

Two-dimensional (2D) semiconductors offer great potential as high-performance materials for thin film transistors (TFTs) in displays. Their thin, stable, and flexible nature, along with excellent electrical properties, makes them suitable for flexible displays. However, previous demonstrations lacked clear superiority in pixel resolution and TFT performance. Here we present the flexible 2T1C pixel driving circuit for active-matrix displays based on high-quality large-scale monolayer MoS2. A gate-first fabrication process was developed for flexible MoS2-TFTs, showing a remarkable carrier mobility (average at 52.8 cm2 V-1 s-1), high on/off ratio (average at 1.5 × 108), and negligible hysteresis. The driving current can be modulated by pulsed input voltages and demonstrates a stable and prompt response to both frequency and amplitude. We also demonstrated a 10 × 10 active-matrix with high resolution of 508 pixels per inch, exhibiting 100% yield and high uniformity. The driving circuit works well under bending up to ∼0.91% strain, highlighting its normal functions in flexible displays.

Scaling of MoS2 Transistors and Inverters to Sub-10 nm Channel Length with High Performance.

Two-dimensional (2D) semiconductors such as monolayer molybdenum disulfide (MoS2) are promising building blocks for ultrascaled field effect transistors (FETs), benefiting from their atomic thickness, dangling-bond-free flat surface, and excellent gate controllability. However, despite great prospects, the fabrication of 2D ultrashort channel FETs with high performance and uniformity remains a challenge. Here, we report a self-encapsulated heterostructure undercut technique for the fabrication of sub-10 nm channel length MoS2 FETs. The fabricated 9 nm channel MoS2 FETs exhibit superior performances compared with sub-15 nm channel length including the competitive on-state current density of 734/433 µA/µm at VDS = 2/1 V, record-low DIBL of ∼50 mV/V, and superior on/off ratio of 3 × 107 and low subthreshold swing of ∼100 mV/dec. Furthermore, the ultrashort channel MoS2 FETs fabricated by this new technique show excellent homogeneity. Thanks to this, we scale the monolayer inverter down to sub-10 nm channel length.

UItra-low friction and edge-pinning effect in large-lattice-mismatch van der Waals heterostructures.

Two-dimensional heterostructures are excellent platforms to realize twist-angle-independent ultra-low friction due to their weak interlayer van der Waals interactions and natural lattice mismatch. However, for finite-size interfaces, the effect of domain edges on the friction process remains unclear. Here we report the superlubricity phenomenon and the edge-pinning effect at MoS2/graphite and MoS2/hexagonal boron nitride van der Waals heterostructure interfaces. We found that the friction coefficients of these heterostructures are below 10-6. Molecular dynamics simulations corroborate the experiments, which highlights the contribution of edges and interface steps to friction forces. Our experiments and simulations provide more information on the sliding mechanism of finite low-dimensional structures, which is vital to understand the friction process of laminar solid lubricants.

Giant Correlated Gap and Possible Room-Temperature Correlated States in Twisted Bilayer MoS_{2}.

Moiré superlattices have emerged as an exciting condensed-matter quantum simulator for exploring the exotic physics of strong electronic correlations. Notable progress has been witnessed, but such correlated states are achievable usually at low temperatures. Here, we report evidence of possible room-temperature correlated electronic states and layer-hybridized SU(4) model simulator in AB-stacked MoS_{2} homobilayer moiré superlattices. Correlated insulating states at moiré band filling factors v=1, 2, 3 are unambiguously established in twisted bilayer MoS_{2}. Remarkably, the correlated electronic state at v=1 shows a giant correlated gap of ∼126 meV and may persist up to a record-high critical temperature over 285 K. The realization of a possible room-temperature correlated state with a large correlated gap in twisted bilayer MoS_{2} can be understood as the cooperation effects of the stacking-specific atomic reconstruction and the resonantly enhanced interlayer hybridization, which largely amplify the moiré superlattice effects on electronic correlations. Furthermore, extreme large nonlinear Hall responses up to room temperature are uncovered near correlated electronic states, demonstrating the quantum geometry of moiré flat conduction band.

Wafer-Scale Highly Oriented Monolayer MoS2 with Large Domain Sizes.

Two-dimensional molybdenum disulfide (MoS2) is an emergent semiconductor with great potential in next-generation scaled-up electronics, but the production of high-quality monolayer MoS2 wafers still remains a challenge. Here, we report an epitaxy route toward 4 in. monolayer MoS2 wafers with highly oriented and large domains on sapphire. Benefiting from a multisource design for our chemical vapor deposition setup and the optimization of the growth process, we successfully realized material uniformity across the entire 4 in. wafer and greater than 100 µm domain size on average. These monolayers exhibit the best electronic quality ever reported, as evidenced from our spectroscopic and transport characterizations. Our work moves a step closer to practical applications of monolayer MoS2.

In Situ Oxygen Doping of Monolayer MoS2 for Novel Electronics.

In 2D semiconductors, doping offers an effective approach to modulate their optical and electronic properties. Here, an in situ doping of oxygen atoms in monolayer molybdenum disulfide (MoS2 ) is reported during the chemical vapor deposition process. Oxygen concentrations up to 20-25% can be reliable achieved in these doped monolayers, MoS2- x Ox . These oxygen dopants are in a form of substitution of sulfur atoms in the MoS2 lattice and can reduce the bandgap of intrinsic MoS2 without introducing in-gap states as confirmed by photoluminescence spectroscopy and scanning tunneling spectroscopy. Field effect transistors made of monolayer MoS2- x Ox show enhanced electrical performances, such as high field-effect mobility (≈100 cm2 V-1 s-1 ) and inverter gain, ultrahigh devices' on/off ratio (>109 ) and small subthreshold swing value (≈80 mV dec-1 ). This in situ oxygen doping technique holds great promise on developing advanced electronics based on 2D semiconductors.

Employing defected monolayer MoS2 as charge storage materials.

Recently, various two-dimensional (2D) materials have been employed in charge trapping memories as the charge trapping layer instead of conventional metal/semiconductor thin films or discrete particles. Such ultra-thin charge trapping layers are beneficial to the development of miniaturized devices, which is a trend in modern semiconductor technology. 2D MoS2 is an alternative charge trapping material, but previous investigations have been limited to their multilayers. Here, we present the study on employing monolayer MoS2 as charge trapping layer in charge trapping devices. We found that intrinsic monolayer MoS2 is less effective for charge trapping; while defective monolayer MoS2 shows enhanced charge storage capacity. By employing argon plasma treatments, we are able to control the defect density in monolayer MoS2 and the memory window of monolayer MoS2 based charge trapping devices can vary from 1.01 to 5.14 V at a sweeping voltage of ±20 V and program/erase slope from 0.06 to 0.32. Optimized devices show ∼1 ms program/erase speed, >70% charge retention after ∼7000 s and good endurance properties with >1000 cycles. The enhancement of the memory window is attributed to the localized charge tapping sites in defected monolayer MoS2. This work would provide insights for the improvement of storage capacity through defects engineering in the atomically thin 2D materials.

Epitaxial Growth of Flat Antimonene Monolayer: A New Honeycomb Analogue of Graphene.

Group-V elemental monolayers were recently predicted to exhibit exotic physical properties such as nontrivial topological properties, or a quantum anomalous Hall effect, which would make them very suitable for applications in next-generation electronic devices. The free-standing group-V monolayer materials usually have a buckled honeycomb form, in contrast with the flat graphene monolayer. Here, we report epitaxial growth of atomically thin flat honeycomb monolayer of group-V element antimony on a Ag(111) substrate. Combined study of experiments and theoretical calculations verify the formation of a uniform and single-crystalline antimonene monolayer without atomic wrinkles, as a new honeycomb analogue of graphene monolayer. Directional bonding between adjacent Sb atoms and weak antimonene-substrate interaction are confirmed. The realization and investigation of flat antimonene honeycombs extends the scope of two-dimensional atomically-thick structures and provides a promising way to tune topological properties for future technological applications.

Magnetotransport Properties of Graphene Nanoribbons with Zigzag Edges.

The determination of the electronic structure by edge geometry is unique to graphene. In theory, an evanescent nonchiral edge state is predicted at the zigzag edges of graphene. Up to now, the approach used to study zigzag-edged graphene has mostly been limited to scanning tunneling microscopy. The transport properties have not been revealed. Recent advances in hydrogen plasma-assisted "top-down" fabrication of zigzag-edged graphene nanoribbons (Z-GNRs) have allowed us to investigate edge-related transport properties. In this Letter, we report the magnetotransport properties of Z-GNRs down to ∼70 nm wide on an h-BN substrate. In the quantum Hall effect regime, a prominent conductance peak is observed at Landau ν=0, which is absent in GNRs with nonzigzag edges. The conductance peak persists under perpendicular magnetic fields and low temperatures. At a zero magnetic field, a nonlocal voltage signal, evidenced by edge conduction, is detected. These prominent transport features are closely related to the observable density of states at the hydrogen-etched zigzag edge of graphene probed by scanning tunneling spectroscopy, which qualitatively matches the theoretically predicted electronic structure for zigzag-edged graphene. Our study gives important insights for the design of new edge-related electronic devices.

Argon Plasma Induced Phase Transition in Monolayer MoS2.

In this work, we report a facile, clean, controllable and scalable phase engineering technique for monolayer MoS2. We found that weak Ar-plasma bombardment can locally induce 2H→1T phase transition in monolayer MoS2 to form mosaic structures. These 2H→1T phase transitions are stabilized by point defects (single S-vacancies) and the sizes of induced 1T domains are typically a few nanometers, as revealed by scanning tunneling microscopy measurements. On the basis of a selected-area phase patterning process, we fabricated MoS2 FETs inducing 1T phase transition within the metal contact areas, which exhibit substantially improved device performances. Our results open up a new route for phase engineering in monolayer MoS2 and other transition metal dichalcogenide (TMD) materials.

Precisely Aligned Monolayer MoS2 Epitaxially Grown on h-BN basal Plane.

Control of the precise lattice alignment of monolayer molybdenum disulfide (MoS2 ) on hexagonal boron nitride (h-BN) is important for both fundamental and applied studies of this heterostructure but remains elusive. The growth of precisely aligned MoS2 domains on the basal plane of h-BN by a low-pressure chemical vapor deposition technique is reported. Only relative rotation angles of 0° or 60° between MoS2 and h-BN basal plane are present. Domains with same orientation stitch and form single-crystal, domains with different orientations stitch and from mirror grain boundaries. In this way, the grain boundary is minimized and a continuous film stitched by these two types of domains with only mirror grain boundaries is obtained. This growth strategy is also applicable to other 2D materials growth.

Hofstadter Butterfly and Many-Body Effects in Epitaxial Graphene Superlattice.

Graphene placed on hexagonal boron nitride (h-BN) has received a wide range of interest due to the improved electrical performance and rich physics from the interface, especially the emergence of superlattice Dirac points as well as Hofstadter butterfly in high magnetic field. Instead of transferring graphene onto h-BN, epitaxial growth of graphene directly on a single-crystal h-BN provides an alternative and promising way to study these interesting superlattice effects due to their precise lattice alignment. Here we report an electrical transport study on epitaxial graphene superlattice on h-BN with a period of ∼15.6 nm. The epitaxial graphene superlattice is clean, intrinsic, and of high quality with a carrier mobility of ∼27 000 cm(2) V(-1) s(-1), which enables the observation of Hofstadter butterfly features originated from the superlattice at a magnetic field as low as 6.4 T. A metal-insulator transition and magnetic field dependent Fermi velocity were also observed, suggesting prominent electron-electron interaction-induced many-body effects.

Rolling Up a Monolayer MoS2 Sheet.

MoS2 nanoscrolls are formed by argon plasma treatment on monolayer MoS2 sheet. The nanoscale scroll formation is attributed to the partial removal of top sulfur layer in MoS2 during the argon plasma treatment process. This convenient, solvent-free, and high-yielding nanoscroll formation technique is also feasible for other 2D transition metal dichalcogenides.

Thermally Induced Graphene Rotation on Hexagonal Boron Nitride.

In this Letter, we report the observation of thermally induced rotation of graphene on hexagonal boron nitride (h-BN). After the rotation, two thermally stable configurations of graphene on h-BN with a relative lattice twisting angle of 0° (most stable) and 30° (metastable), respectively, were found. Graphene on h-BN with a twisting angle below (above) a critical angle of ∼12±2° tends to rotate towards 0° (30°) at a temperature of >100 °C, which is in line with our theoretical simulations. In addition, by manipulating the annealing temperature and the flake sizes of graphene, moiré superlattices with large spatial periods of graphene on h-BN are achieved. Our studies provide a detailed understanding of the thermodynamic properties of graphene on h-BN and a feasible approach to obtaining van der Waals heterostructures with aligned lattices.

Oxygen-Assisted Chemical Vapor Deposition Growth of Large Single-Crystal and High-Quality Monolayer MoS2.

Monolayer molybdenum disulfide (MoS2) has attracted great interest due to its potential applications in electronics and optoelectronics. Ideally, single-crystal growth over a large area is necessary to preserve its intrinsic figure of merit but is very challenging to achieve. Here, we report an oxygen-assisted chemical vapor deposition method for growth of single-crystal monolayer MoS2. We found that the growth of MoS2 domains can be greatly improved by introducing a small amount of oxygen into the growth environment. Triangular monolayer MoS2 domains can be achieved with sizes up to ∼350 µm and a room-temperature mobility up to ∼90 cm(2)/(V·s) on SiO2. The role of oxygen is not only to effectively prevent the poisoning of precursors but also to eliminate defects during the growth. Our work provides an advanced method for high-quality single-crystal monolayer MoS2 growth.

Nanographene charge trapping memory with a large memory window.

Nanographene is a promising alternative to metal nanoparticles or semiconductor nanocrystals for charge trapping memory. In general, a high density of nanographene is required in order to achieve high charge trapping capacity. Here, we demonstrate a strategy of fabrication for a high density of nanographene for charge trapping memory with a large memory window. The fabrication includes two steps: (1) direct growth of continuous nanographene film; and (2) isolation of the as-grown film into high-density nanographene by plasma etching. Compared with directly grown isolated nanographene islands, abundant defects and edges are formed in nanographene under argon or oxygen plasma etching, i.e. more isolated nanographene islands are obtained, which provides more charge trapping sites. As-fabricated nanographene charge trapping memory shows outstanding memory properties with a memory window as wide as ∼9 V at a relative low sweep voltage of ±8 V, program/erase speed of ∼1 ms and robust endurance of >1000 cycles. The high-density nanographene charge trapping memory provides an outstanding alternative for downscaling technology beyond the current flash memory.

A general route towards defect and pore engineering in graphene.

Defect engineering in graphene is important for tailoring graphene's properties thus applicable in various applications such as porous membranes and ultra-capacitors. In this paper, we report a general route towards defect- and pore- engineering in graphene through remote plasma treatments. Oxygen plasma irradiation was employed to create homogenous defects in graphene with controllable density from a few to ≈10(3) (µm(-2)). The created defects can be further enlarged into nanopores by hydrogen plasma anisotropic etching with well-defined pore size of a few nm or above. The achieved smallest nanopores are ≈2 nm in size, showing the potential for ultra-small graphene nanopores fabrication.

Epitaxial growth of single-domain graphene on hexagonal boron nitride.

Hexagonal boron nitride (h-BN) has recently emerged as an excellent substrate for graphene nanodevices, owing to its atomically flat surface and its potential to engineer graphene's electronic structure. Thus far, graphene/h-BN heterostructures have been obtained only through a transfer process, which introduces structural uncertainties due to the random stacking between graphene and h-BN substrate. Here we report the epitaxial growth of single-domain graphene on h-BN by a plasma-assisted deposition method. Large-area graphene single crystals were successfully grown for the first time on h-BN with a fixed stacking orientation. A two-dimensional (2D) superlattice of trigonal moiré pattern was observed on graphene by atomic force microscopy. Extra sets of Dirac points are produced as a result of the trigonal superlattice potential and the quantum Hall effect is observed with the 2D-superlattice-related feature developed in the fan diagram of longitudinal and Hall resistance, and the Dirac fermion physics near the original Dirac point is unperturbed. The macroscopic epitaxial graphene is in principle limited only by the size of the h-BN substrate and our synthesis method is potentially applicable on other flat surfaces. Our growth approach could thus open new ways of graphene band engineering through epitaxy on different substrates.

Observation of phonon Stark effect.

Stark effect, the electric-field analogue of magnetic Zeeman effect, is one of the celebrated phenomena in modern physics and appealing for emergent applications in electronics, optoelectronics, as well as quantum technologies. While in condensed matter it has prospered only for excitons, whether other collective excitations can display Stark effect remains elusive. Here, we report the observation of phonon Stark effect in a two-dimensional quantum system of bilayer 2H-MoS2. The longitudinal acoustic phonon red-shifts linearly with applied electric fields and can be tuned over ~1 THz, evidencing giant Stark effect of phonons. Together with many-body ab initio calculations, we uncover that the observed phonon Stark effect originates fundamentally from the strong coupling between phonons and interlayer excitons (IXs). In addition, IX-mediated electro-phonon intensity modulation up to ~1200% is discovered for infrared-active phonon A2u. Our results unveil the exotic phonon Stark effect and effective phonon engineering by IX-mediated mechanism, promising for a plethora of exciting many-body physics and potential technological innovations.