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Monolayer transition metal dichalcogenides have emerged as prominent candidates to explore the complex interplay between the spin and the valleys degrees of freedom. The strong spin-orbit interaction and broken inversion symmetry within these materials lead to the spin-valley locking effect, in which carriers occupying the K and K' valleys of the reciprocal space must have opposite spin depending on which valley they reside. This effect is particularly strong for holes due to a larger spin-orbit gap in the valence band. By reducing the dimensionality of a monolayer of tungsten diselenide to 1D via electrostatic confinement, we demonstrate that spin-valley locking in combination with strong hole-hole interactions lead to a ferromagnetic state in which hole transport through the 1D system is spin-valley polarized, even without an applied magnetic field, and that the persistence of this spin-valley polarized configuration can be tuned by a global back-gate. This observation opens the possibility of implementing a robust and stable valley polarized system, essential for valleytronic applications.

We present a theory of interacting valence holes in a gate-defined one-dimensional quantum channel in a single layer of a transition metal dichalcogenide material WSe$_2$. Based on a microscopic atomistic tight-binding model and Hartree-Fock and exact configuration-interaction tools we demonstrate the possibility of symmetry-broken valley polarized states for strongly interacting holes. The interplay between interactions, perpendicular magnetic field, and the lateral confinement asymmetry together with the strong Rashba spin-orbit coupling present in WSe$_2$ material is analyzed, and its impact on valley polarization is discussed. For weaker interactions, an investigation of the pair correlation function reveals a valley-antiferromagnetic phase. For low hole densities, a formation of a zigzag Wigner crystal phase is predicted. The impact of various hole liquid phases on transport in a high mobility quasi-one dimensional channel is discussed., Comment: 12 pages, 11 figures, 1 table

High-harmonic generation in solids allows probing and controlling electron dynamics in crystals on few femtosecond timescales, paving the way to lightwave electronics. In the spatial domain, recent advances in the real-space interpretation of high-harmonic emission in solids allows imaging the field-free, static, potential of the valence electrons with picometer resolution. The combination of such extreme spatial and temporal resolutions to measure and control strong-field dynamics in solids at the atomic scale is poised to unlock a new frontier of lightwave electronics. Here, we report a strong intensity-dependent anisotropy in the high-harmonic generation from ReS$_2$ that we attribute to angle-dependent interference of currents from the different atoms in the unit cell. Furthermore, we demonstrate how the laser parameters control the relative contribution of these atoms to the high-harmonic emission. Our findings provide an unprecedented atomic perspective on strong-field dynamics in crystals and suggest that crystals with a large number of atoms in the unit cell are not necessarily more efficient harmonic emitters than those with fewer atoms.

Twisting bilayers of transition metal dichalcogenides (TMDs) gives rise to a periodic moir\'{e} potential resulting in flat electronic bands with localized wavefunctions and enhanced correlation effects. In this work, scanning tunneling microscopy is used to image a WS$_{2}$ bilayer twisted approximately $3^{\circ}$ off the antiparallel alignment. Scanning tunneling spectroscopy reveals the presence of localized electronic states in the vicinity of the valence band onset. In particular, the onset of the valence band is observed to occur first in regions with a Bernal stacking in which S atoms are located on top of each other. In contrast, density-functional theory calculations on twisted bilayers which have been relaxed in vacuum predict the highest lying flat valence band to be localized in regions of AA' stacking. However, agreement with the experiment is recovered when the calculations are carried out on bilayers in which the atomic displacements from the unrelaxed positions have been reduced reflecting the influence of the substrate and finite temperature. This demonstrates the delicate interplay of atomic relaxations and the electronic structure of twisted bilayer materials., Comment: 21 pages, 7 figures

Semiconducting ferroelectric materials with low energy polarisation switching offer a platform for next-generation electronics such as ferroelectric field-effect transistors. Ferroelectric domains at symmetry-broken interfaces of transition metal dichalcogenide films provide an opportunity to combine the potential of semiconducting ferroelectrics with the design flexibility of two-dimensional material devices. Here, local control of ferroelectric domains in a marginally twisted WS2 bilayer is demonstrated with a scanning tunneling microscope at room temperature, and their observed reversible evolution understood using a string-like model of the domain wall network. We identify two characteristic regimes of domain evolution: (i) elastic bending of partial screw dislocations separating smaller domains with twin stacking and (ii) formation of perfect screw dislocations by merging pairs of primary domain walls. We also show that the latter act as the seeds for the reversible restoration of the inverted polarisation. These results open the possibility to achieve full control over atomically thin semiconducting ferroelectric domains using local electric fields, which is a critical step towards their technological use.

We report on temperature-dependent size and anisotropy of the Fermi pockets in graphite revealed by magnetotransport measurements. The magnetoresistances obtained in fields along the c-axis obey an extended Kohler's rule, with the carrier density following prediction of a temperature-dependent Fermi energy, indicating a change in the Fermi pocket size with temperature. The angle-dependent magnetoresistivities at a given temperature exhibit a scaling behavior. The scaling factor that reflects the anisotropy of the Fermi surface is also found to vary with temperature. Our results demonstrate that temperature-driven changes in Fermi surface can be ubiquitous and need to be considered in understanding the temperature-dependent carrier density and magnetoresistance anisotropy in semimetals., Comment: To appear in Physical Review B

Detecting single charging events in quantum devices is an important step towards realizing practical quantum circuits for quantum information processing. In this work, we demonstrate that van derWaals heterostructure devices with gated nano-constrictions in monolayer WSe2 can be used as charge detectors for nearby quantum dots. These results open the possibility of implementing charge detection schemes based on 2D materials in complex quantum circuits.

Quantum confinenement and manipulation of charge carriers are critical for achieving devices practical for quantum technologies. The interplay between electron spin and valley, as well as the possibility to address their quantum states electrically and optically, make two-dimensional (2D) transition metal dichalcogenides an emerging platform for the development of quantum devices. In this work, we fabricate devices based on heterostructures of layered 2D materials, in which we realize gate-controlled tungsten diselenide (WSe2) hole quantum dots. We discuss the observed mesoscopic transport features related to the emergence of quantum dots in the WSe2 device channel, and we compare them to a theoretical model., Comment: 6 pages, 4 figures

Fabrication of custom-built heterostructures based on stacked 2D materials provides an effective method to controllably tune electronic and optical properties. To that end, optimizing fabrication techniques for building these heterostructures is imperative. A common challenge in layer-by-layer assembly of 2D materials is the formation of bubbles at the atomically thin interfaces. We propose a technique for addressing this issue by removing the bubbles formed at the heterostructure interface in a custom-defined area using the heat generated by a laser, equipped with raster scanning capabilities. We demonstrate that the density of bubbles formed at graphene-ReS2 interfaces can be controllably reduced using this method. We discuss an understanding of the flattening mechanism by considering the interplay of interface thermal conductivities and adhesion energies between two atomically thin 2D materials.

Vertical stacking of atomically thin materials offers a large platform for realizing novel properties enabled by proximity effects and moir\'e patterns. Here we focus on mechanically assembled heterostructures of graphene and ReS$_2$, a van der Waals layered semiconductor. Using scanning tunneling microscopy and spectroscopy (STM/STS) we image the sharp edge between the two materials as well as areas of overlap. Locally resolved topographic images revealed the presence of a striped superpattern originating in the interlayer interactions between graphene's hexagonal structure and the triclinic, low in-plane symmetry of ReS$_2$. We compare the results with a theoretical model that estimates the shape and angle dependence of the moir\'e pattern between graphene and ReS$_2$. These results shed light on the complex interface phenomena between van der Waals materials with different lattice symmetries., Comment: 8 pages, 4 figures

Atomic scale defects in semiconductors enable their technological applications and realization of novel quantum states. Using scanning tunneling microscopy and spectroscopy complemented by ab-initio calculations we determine the nature of defects in the anisotropic van der Waals layered semiconductor ReS$_2$. We demonstrate the in-plane anisotropy of the lattice by directly visualizing chains of rhenium atoms forming diamond-shaped clusters. Using scanning tunneling spectroscopy we measure the semiconducting gap in the density of states. We reveal the presence of lattice defects and by comparison of their topographic and spectroscopic signatures with ab initio calculations we determine their origin as oxygen atoms absorbed at lattice point defect sites. These results provide an atomic-scale view into the semiconducting transition metal dichalcogenides, paving the way toward understanding and engineering their properties., Comment: 9 pages, 4 figures; Supp 5 pages, 4 figures

Graphene has demonstrated great promise for technological use, yet control over material growth and understanding of how material imperfections affect the performance of devices are challenges that hamper the development of applications. In this work we reveal new insight into the connections between the performance of the graphene devices as environmental sensors and the microscopic details of the interactions at the sensing surface. Specifically, we monitor changes in the resistance of the chemical-vapour deposition grown graphene devices as exposed to different concentrations of ethanol. We perform thermal surface treatments after the devices are fabricated, use scanning probe microscopy to visualize their effects on the graphene sensing surface down to nanometer scale and correlate them with the measured performance of the device as an ethanol sensor. Our observations are compared to theoretical calculations of charge transfers between molecules and the graphene surface. We find that, although often overlooked, the surface cleanliness after device fabrication is responsible for the device performance and reliability. These results further our understanding of the mechanisms of sensing in graphene-based environmental sensors and pave the way to optimizing such devices, especially for their miniaturization, as with decreasing size of the active zone the potential role of contaminants will rise.

In this paper we present the design and fabrication of a portable device for environmental monitoring applications. This novel hand-held apparatus monitors the changes in the resistance of a sensing surface with a high accuracy and resolution and transmits the recorded data wirelessly to a cellphone. Such a design offers a solution for field testing of environmental sensors. The tested sensing surface in this study is based on an ultrathin material: graphene, which is placed on the surface of a Si/SiO2 wafer. This signal transducer and wireless communication system form together an ideal platform to harvest the sensitivity and selectivity of 2D materials for gas sensing applications., Comment: The paper will not be submitted for publication after all. It is not under peer review, and we request it be withdrawn for these reasons

Recent advances in large-scale synthesis of graphene and other 2D materials have underscored the importance of local defects such as dislocations and grain boundaries (GBs), and especially their tendency to alter the electronic properties of the material. Understanding how the polycrystalline morphology affects the electronic properties is crucial for the development of applications such as flexible electronics, energy harvesting devices or sensors. We here report on atomic scale characterization of several GBs and on the structural-dependence of the localized electronic states in their vicinity. Using low temperature scanning tunneling microscopy (STM) and spectroscopy (STS), together with tight binding and ab initio numerical simulations we explore GBs on the surface of graphite and elucidate the interconnection between the local density of states (LDOS) and their atomic structure. We show that the electronic fingerprints of these GBs consist of pronounced resonances which, depending on the relative orientation of the adjacent crystallites, appear either on the electron side of the spectrum or as an electron-hole symmetric doublet close to the charge neutrality point. These two types of spectral features will impact very differently the transport properties allowing, in the asymmetric case to introduce transport anisotropy which could be utilized to design novel growth and fabrication strategies to control device performance.

A hallmark of materials with extremely large magnetoresistance (XMR) is the transformative 'turn-on' temperature behavior: when the applied magnetic field $H$ is above certain value, the resistivity versus temperature $\rho(T)$ curve shows a minimum at a field dependent temperature $T^*$, which has been interpreted as a magnetic-field-driven metal-insulator transition or attributed to an electronic structure change. Here, we demonstrate that $\rho(T)$ curves with turn-on behavior in the newly discovered XMR material WTe$_2$ can be scaled as MR $\sim(H/\rho_0)^m$ with $m\approx 2$ and $\rho_0$ being the resistivity at zero-field. We obtained experimentally and also derived from the observed scaling the magnetic field dependence of the turn-on temperature $T^* \sim (H-H_c)^\nu$ with $\nu \approx 1/2$, which was earlier used as evidence for a predicted metal-insulator transition. The scaling also leads to a simple quantitative expression for the resistivity $\rho^* \approx 2 \rho_0$ at the onset of the XMR behavior, which fits the data remarkably well. These results exclude the possible existence of a magnetic-field-driven metal-insulator transition or significant contribution of an electronic structure change to the low-temperature XMR in WTe$_2$. This work resolves the origin of the turn-on behavior observed in several XMR materials and also provides a general route for a quantitative understanding of the temperature dependence of MR in both XMR and non-XMR materials.

Using temperature dependent Raman spectroscopy we address the question of how the transition from bulk to few atomic layers affects the charge density wave (CDW) phases in 1T-TaS2. We find that for crystals with thickness larger than approx 10nm the transition temperatures between the different phases as well as the hysteresis that occurs in the thermal cycle correspond to the ones expected for a bulk sample. However, when the crystals become thinner than $\approx 10nm$, the commensurate CDW phase is suppressed down to the experimentally accessible temperatures. In addition, the nearly commensurate CDW phase is diminished below approx 4nm. These findings suggest that the interlayer coupling plays a significant role in determining the properties of CDW systems consisting of a few unit cells in the vertical direction.

Extremely large magnetoresistance (XMR) was recently discovered in WTe$_2$, triggering extensive research on this material regarding the XMR origin. Since WTe$_2$ is a layered compound with metal layers sandwiched between adjacent insulating chalcogenide layers, this material has been considered to be electronically two-dimensional (2D). Here we report two new findings on WTe$_2$: (1) WTe$_2$ is electronically 3D with a mass anisotropy as low as $2$, as revealed by the 3D scaling behavior of the resistance $R(H,\theta)=R(\varepsilon_\theta H)$ with $\varepsilon_\theta =(\cos^2 \theta + \gamma^{-2}\sin^2 \theta)^{1/2}$, $\theta$ being the magnetic field angle with respect to c-axis of the crystal and $\gamma$ being the mass anisotropy; (2) the mass anisotropy $\gamma$ varies with temperature and follows the magnetoresistance behavior of the Fermi liquid state. Our results not only provide a general scaling approach for the anisotropic magnetoresistance but also are crucial for correctly understanding the electronic properties of WTe$_2$, including the origin of the remarkable 'turn-on' behavior in the resistance versus temperature curve, which has been widely observed in many materials and assumed to be a metal-insulator transition.

One-atom thick crystalline layers and their vertical heterostructures carry the promise of designer electronic materials that are unattainable by standard growth techniques. In order to realize their potential it is necessary to isolate them from environmental disturbances in particular those introduced by the substrate. But finding and characterizing suitable substrates, and minimizing the random potential fluctuations they introduce, has been a persistent challenge in this emerging field. Here we show that Landau-level (LL) spectroscopy is exquisitely sensitive to potential fluctuations on both local and global length scales. Harnessing this technique we demonstrate that the insertion of an intermediate graphene layer provides superior screening of substrate induced disturbances, more than doubling the electronic mean free path. Furthermore, we find that the proximity of hBN acts as a nano-scale vacuum cleaner, dramatically suppressing the global potential fluctuations. This makes it possible to fabricate high quality devices on standard SiO2 substrates., Comment: 16 pages, 4 figures

We report the observation of an isolated charged impurity in graphene and present direct evidence of the close connection between the screening properties of a 2D electron system and the influence of the impurity on its electronic environment. Using scanning tunneling microscopy and Landau level spectroscopy we demonstrate that in the presence of a magnetic field the strength of the impurity can be tuned by controlling the occupation of Landau-level states with a gate-voltage. At low occupation the impurity is screened becoming essentially invisible. Screening diminishes as states are filled until, for fully occupied Landau-levels, the unscreened impurity significantly perturbs the spectrum in its vicinity. In this regime we report the first observation of Landau-level splitting into discrete states due to lifting the orbital degeneracy., Comment: 13 pages, 4 figures