Search

Spin-valley properties in two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDC) has attracted significant interest due to the possible applications in quantum computing. Spin-valley properties can be exploited in TMDC quantum dot (QD) with well-resolved energy levels. This requires smaller QDs, especially in material systems with heavy carrier effective mass e.g. TMDCs and silicon. Device architectures employed for TMDC QDs so far have difficulty achieving smaller QDs. Therefore, an alternative approach in the device architecture is needed. Here, we propose a multilayer device architecture to achieve a gate-defined QD in TMDC with a relatively large energy splitting on the QD. We provide a range of device dimensions and dielectric thicknesses and its correlation with the QD energy splitting. The device architecture is modeled realistically. Moreover, we show that all the device parameters used in modeling are experimentally achievable. These studies lay the foundation for future work toward spin-valley qubits in TMDCs. The successful implementation of these device architectures will drive the technological development of 2D materials-based quantum technologies., Comment: main text: 20 pages, 5 figures; supplementary: 9 pages, 7 figures

We report intriguing and hitherto overlooked low-field room temperature extremely large magnetoresistance (XMR) patterns in graphene/hexagonal boron nitride (h-BN) superlattices that emerge due to the existence of open orbits within each miniband. This finding is set against the backdrop of the experimental discovery of the Hofstadter butterfly in moir superlattices, which has sparked considerable interest in the fractal quantum Hall regime. To cope with the challenge of deciphering the low magnetic field dynamics of moir minibands, we utilize a novel semi-classical calculation method, grounded in zero-field Fermi contours, to predict the nontrivial behavior of the Landau-level spectrum. This is compared with fully quantum simulations, enabling an in-depth and contrasted analysis of transport measurements in high-quality graphene-hBN superlattices. Our results not only highlight the primary observation of the open-orbit induced XMR in this system but also shed new light on other intricate phenomena. These include the nuances of single miniband dynamics, evident through Lifshitz transitions, and the complex interplay of semiclassical and quantum effects between these minibands. Specifically, we document transport anomalies linked to trigonal warping, a semiclassical deviation from the expected linear characteristics of Landau levels, and magnetic breakdown phenomena indicative of quantum tunneling, all effects jointly contributing to the intricacies of a rich electronic landscape uncovered at low magnetic fields., Comment: 5 figures

Two-dimensional (2D) tungsten disulfide (WS$_2$), tungsten diselenide (WSe$_2$), and tungsten ditelluride (WTe$_2$) draw increasing attention due to their attractive properties deriving from the heavy tungsten and chalcogenide atoms, but their mechanical properties are still mostly unknown. Here, we determine the intrinsic and air-aged mechanical properties of mono-, bi-, and trilayer (1-3L) WS$_2$, WSe$_2$ and WTe$_2$ using a complementary suite of experiments and theoretical calculations. High-quality 1L WS$_2$ has the highest Young's modulus (302.4+-24.1 GPa) and strength (47.0+-8.6 GPa) of the entire family, overpassing those of 1L WSe$_2$ (258.6+-38.3 and 38.0+-6.0 GPa, respectively) and WTe$_2$ (149.1+-9.4 and 6.4+-3.3 GPa, respectively). However, the elasticity and strength of WS$_2$ decrease most dramatically with increased thickness among the three materials. We interpret the phenomenon by the different tendencies for interlayer sliding in equilibrium state and under in-plane strain and out-of-plane compression conditions in the indentation process, revealed by finite element method (FEM) and density functional theory (DFT) calculations including van der Waals (vdW) interactions. We also demonstrate that the mechanical properties of the high-quality 1-3L WS$_2$ and WSe$_2$ are largely stable in the air for up to 20 weeks. Intriguingly, the 1-3L WSe$_2$ shows increased modulus and strength values with aging in the air. This is ascribed to oxygen doping, which reinforces the structure. The present study will facilitate the design and use of 2D tungsten dichalcogenides in applications, such as strain engineering and flexible field-effect transistors (FETs).

In van der Waals heterostructures, electronic bands of two-dimensional (2D) materials, their nontrivial topology, and electron-electron interactions can be dramatically changed by a moire pattern induced by twist angles between different layers. Such process is referred to as twistronics, where the tuning of twist angle can be realized through mechanical manipulation of 2D materials. Here we demonstrate an experimental technique that can achieve in situ dynamical rotation and manipulation of 2D materials in van der Waals heterostructures. Using this technique we fabricated heterostructures where graphene is perfectly aligned with both top and bottom encapsulating layers of hexagonal boron nitride. Our technique enables twisted 2D material systems in one single stack with dynamically tunable optical, mechanical, and electronic properties.

The pH dependence of emission from graphene oxide is believed to be due to the protonation of surface functional groups. In this study we use transient absorption spectroscopy to study the sub-picosecond charge dynamics in graphene oxide over a range of pH values, observing dynamics consistent with an excited state protonation step for pH < 9.3. The timescale of this process is ~ 1.5 ps, and a corresponding change in recombination dynamics follows. A broad photo-induced absorption peak centred at 530 nm associated with excited state protonation is also observed.

Two-dimensional semiconductors - atomic layers of materials with covalent intra-layer bonding and weak (van der Waals or quadrupole) coupling between the layers - are a new class of materials with great potential for optoelectronic applications. Among those, a special position is now being taken by post-transition metal chalcogenides (PTMC), InSe and GaSe. It has recently been found that the band gap in 2D crystals of InSe more than doubles in the monolayer compared to thick multilayer crystals, while the high mobility of conduction band electrons is promoted by their light in-plane mass. Here, we use Raman and PL measurements of encapsulated few layer samples, coupled with accurate atomic force and transmission electron microscope structural characterisation to reveal new optical properties of atomically thin GaSe preserved by hBN encapsulation. The band gaps we observe complement the spectral range provided by InSe films, so that optical activity of these two almost lattice-matched PTMC films and their heterostructures densely cover the spectrum of photons from violet to infrared. We demonstrate the realisation of the latter by the first observation of interlayer excitonic photoluminescence in few-layer InSe-GaSe heterostructures. The spatially indirect transition is direct in k-space and therefore is bright, while its energy can be tuned in a broad range by the number of layers., Comment: 8 pages 4 figures

The recent discovery of semiconducting two-dimensional materials has led to the prediction of a revolution in the field of optoelectronics, driven by the introduction of a series of new components that are just a few atoms thick. Key remaining challenges for producing practical devices from these materials lie in improving the coupling of light into and out of single atomic layers, and in making these layers robust to the influence of their surrounding environment. We present a solution to tackle both of these problems simultaneously, by deterministically placing a micro-lens directly onto the surface of these materials. These lenses are dynamically tuned to increase the coupling of light, whilst controlling chromatic aberration, before being set in place with UV light. We show that this approach enhances photoluminescence of tungsten diselenide (WSe2) monolayers by up to 300%, and nearly doubles the imaging resolution of the system. Furthermore, this solution fully encapsulates the monolayer, preventing it from physical damage and degradation in air. The optical solution we have developed could become a key enabling technology for the mass production of ultra-thin optical devices, such as quantum light emitting diodes., Comment: 12 pages, 6 figures

Two-dimensional materials are characterised by a number of unique physical properties which can potentially make them useful to a wide diversity of applications. In particular, the large thermal conductivity of graphene and hexagonal boron nitride has already been acknowledged and these materials have been suggested as novel core materials for thermal management in electronics. However, it was not clear if mass produced flakes of hexagonal boron nitride would allow one to achieve an industrially-relevant value of thermal conductivity. Here we demonstrate that laminates of hexagonal boron nitride exhibit thermal conductivity of up to 20 W/mK, which is significantly larger than that currently used in thermal management. We also show that the thermal conductivity of laminates increases with the increasing volumetric mass density, which creates a way of fine-tuning its thermal properties., Comment: 6 pages, 4 figures

Atomically thin layers of two-dimensional (2D) materials such as graphene, MoS2 and h-BN have immense potential as sensors and electronic devices thanks to their highly desirable electronic, mechanical, optical and heat transport properties. In particular their extreme stiffness, tensile strength and low density allows for high frequency electronic devices, resonators and ultra-sensitive detectors providing realistic avenues for down-scaling electronic devices and nanoelectromechanical systems (NEMS). Whilst nanoscale morphology and electronic properties of 2D materials can be studied using existing electron or scanning probe microscopy approaches, time-dependant phenomena on the ns and shorter time-scales cannot be readily explored. Here we use the heterodyne principle to reach into this ns time-scale and create a local nanoscale probe for electrostatically induced actuation of a graphene resonator, with amplitude sensitivity down to pm range and time sensitivity in the ns range. We experimentally observed response times of 20-120 ns for resonators with beam lengths of 180 nm to 2.5 um in line with the theoretical predictions for such NEMS devices.

In electron microscopy, charging of non-conductive biological samples by focused electron beams hinders their high-resolution imaging. Gold or platinum coatings have been commonly used to prevent such sample charging, but it disables further quantitative and qualitative chemical analyses by energy dispersive spectroscopy (EDS). Here we report that graphene-coating on biological samples enables non-destructive high-resolution imaging by scanning electron microscopy (SEM) as well as chemical analysis by EDS, utilizing graphene's transparency to electron beams, high conductivity, outstanding mechanical strength, and flexibility. We believe that the graphene-coated imaging and analysis would provide us a new opportunity to explore various biological phenomena unseen before due to the limitation in sample preparation and image resolution, which will broaden our understanding on the life mechanism of various living organisms.

Formation, evolution, and vanishing of bubbles are common phenomena in our nature, which can be easily observed in boiling or falling waters, carbonated drinks, gas-forming electrochemical reactions, etc. However, the morphology and the growth dynamics of the bubbles at nanoscale have not been fully investigated owing to the lack of proper imaging tools that can visualize nanoscale objects in liquid phase. Here we demonstrate, for the first time, that the nanobubbles in water encapsulated by graphene membrane can be visualized by in situ ultrahigh vacuum transmission electron microscopy (UHV-TEM), showing the critical radius of nanobubbles determining its unusual long-term stability as well as two distinct growth mechanisms of merging nanobubbles (Ostwald ripening and coalescing) depending on their relative sizes. Interestingly, the gas transport through ultrathin water membranes at nanobubble interface is free from dissolution, which is clearly different from conventional gas transport that includes condensation, transmission and evaporation. Our finding is expected to provide a deeper insight to understand unusual chemical, biological and environmental phenomena where nanoscale gas-state is involved., Comment: 10 text pages, 4 figure pages, and 4 page Supplementary Information. Supplementary movies will be provided on request

We demonstrated that chemical vapor deposition of graphene on Cu films strongly enhances their thermal diffusivity and thermal conductivity. Deposition of graphene increases the thermal conductivity of 9 micrometer (25 micrometer) thick Cu films by up to 24% (16%) near room temperature. Interestingly, the observed improvement of thermal properties of graphene coated Cu films is primarily due to changes in Cu morphology during graphene deposition and associated with it temperature treatment rather than graphene's action as an additional heat conducting channel. Enhancement of thermal properties of metal films via graphene coating may lead to applications in electronic circuits and metallurgy., Comment: 16 pages, 3 figures

Nano-holes, etched under an electron beam at room temperature in singlelayer graphene sheets as a result of their interaction with metalimpurities, are shown to heal spontaneously by filling up with either non-hexagon, graphene-like, or perfect hexagon 2D structures. Scanning transmission electron microscopy was employed to capture the healing process and study atom-by-atom the re-grown structure. A combination of these nano-scale etching and re-knitting processes could lead to new graphene tailoring approaches., Comment: 11 pages, 4 figures

Atomic resolution high angle annular dark field imaging of suspended, single-layer graphene, onto which the metals Cr, Ti, Pd, Ni, Al and Au atoms had been deposited was carried out in an aberration corrected scanning transmission electron microscope. In combination with electron energy loss spectroscopy, employed to identify individual impurity atoms, it was shown that nano-scale holes were etched into graphene, initiated at sites where single atoms of all the metal species except for gold come into close contact with the graphene. The e-beam scanning process is instrumental in promoting metal atoms from clusters formed during the original metal deposition process onto the clean graphene surface, where they initiate the hole-forming process. Our observations are discussed in the light of calculations in the literature, predicting a much lowered vacancy formation in graphene when metal ad-atoms are present. The requirement and importance of oxygen atoms in this process, although not predicted by such previous calculations, is also discussed, following our observations of hole formation in pristine graphene in the presence of Si-impurity atoms, supported by new calculations which predict a dramatic decrease of the vacancy formation energy, when SiOx molecules are present., Comment: final version accepted in ACS Nano + supplementary info. 22+6 pages, 4+5 figures

In-situ high pressure Raman spectroscopy is used to study monolayer, bilayer and few-layer graphene samples supported on silicon in a diamond anvil cell to 3.5 GPa. The results show that monolayer graphene adheres to the silicon substrate under compressive stress. A clear trend in this behaviour as a function of graphene sample thickness is observed. We also study unsupported graphene samples in a diamond anvil cell to 8 GPa, and show that the properties of graphene under compression are intrinsically similar to graphite. Our results demonstrate the differing effects of uniaxial and biaxial strain on the electronic bandstructure., Comment: Accepted in Physical Review B with minor changes