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Rhombohedral graphite (RG) shows strong correlations in its topological flat band and is pivotal for exploring emergent, correlated electronic phenomena. One key advantage is the enhancement of electronic interactions with the increase in the number of rhombohedrally stacked graphene layers. Increasing thickness also leads to an exponential increase in the number of stacking faults, necessitating a precise method to identify flawless rhombohedral stacking. Overcoming this challenge is difficult because the established technique for stacking sequence identification, based on the Raman 2D peak, fails in thick RG samples. We demonstrate that the strong layer dependence of the band structure can be harnessed to identify RG without stacking faults, or alternatively, to detect their presence. For thicknesses ranging from 3 to 12 layers, we show that each perfect RG structure presents distinctive peak positions in electronic Raman scattering (ERS). This measurement can be carried out using a conventional confocal Raman spectrometer at room temperature, using visible excitation wavelengths. Consequently, this overcomes the identification challenge by providing a simple and fast optical measurement technique, thereby helping to establish RG as a platform for studying strong correlations in one of the simplest crystals possible., Comment: 20 pages, 6 figures

The behavior of single layer van der Waals (vdW) materials is profoundly influenced by the immediate atomic environment at their surface, a prime example being the myriad of emergent properties in artificial heterostructures. Equally significant are adsorbates deposited onto their surface from ambient. While vdW interfaces are well understood, our knowledge regarding atmospheric contamination is severely limited. Here we show that the common ambient contamination on the surface of: graphene, graphite, hBN and MoS2 is composed of a self-organized molecular layer, which forms during a few days of ambient exposure. Using low-temperature STM measurements we image the atomic structure of this adlayer and in combination with infrared spectroscopy identify the contaminant molecules as normal alkanes with lengths of 20-26 carbon atoms. Through its ability to self-organize, the alkane layer displaces the manifold other airborne contaminant species, capping the surface of vdW materials and possibly dominating their interaction with the environment.

Topological materials host robust properties, unaffected by microscopic perturbations, owing to the global topological properties of the bulk electron system. Materials in which the topological invariant can be changed by easily tuning external parameters are especially sought after. Zirconium pentatelluride (ZrTe$_5$) is one of a few experimentally available materials that reside close to the boundary of a topological phase transition, allowing the switching of its invariant by mechanical strain. Here, we unambiguously identify a topological insulator - metal transition as a function of strain, by a combination of ab initio calculations and direct measurements of the local charge density. Our model quantitatively describes the response to complex strain patterns found in bubbles of few layer ZrTe$_5$ without fitting parameters, reproducing the mechanical deformation dependent closing of the band gap observed using scanning tunneling microscopy. We calculate the topological phase diagram of ZrTe$_5$ and identify the phase at equilibrium, enabling the design of device architectures which exploit the unique topological switching characteristics of the system., Comment: 18 pages, 4 figures

In crystalline solids the interactions of charge and spin can result in a variety of emergent quantum ground states, especially in partially filled, topological flat bands such as Landau levels or in 'magic-angle' bilayer graphene. Much less explored is rhombohedral graphite (RG), perhaps the simplest and structurally most perfect condensed matter system to host a flat band protected by symmetry. By scanning tunneling microscopy we map the flat band charge density of 8, 10 and 17 layers and identify a domain structure emerging from a competition between a sublattice antiferromagnetic insulator and a gapless correlated paramagnet. Our density-matrix renormalization group calculations explain the observed features and demonstrate that the correlations are fundamentally different from graphene based magnetism identified until now, forming the ground state of a quantum magnet. Our work establishes RG as a new platform to study many-body interactions beyond the mean-field approach, where quantum fluctuations and entanglement dominate., Comment: supplementary information included

Quantum confinement of graphene carriers is an effective way to engineer its properties. It is commonly realized through physical edges that are associated with the deterioration of mobility and strong suppression of plasmon resonances. Here, we demonstrate a simple, large-area, edge-free nanostructuring technique, based on amplifying random nanoscale structural corrugations to a level where they efficiently confine carriers, without inducing significant inter-valley scattering. This soft confinement, allows the low-loss lateral ultra-confinement of graphene plasmons, scaling up their resonance frequency from native terahertz to commercially relevant visible range. Visible graphene plasmons localized into nanocorrugations mediate several orders of magnitude stronger light-matter interactions (Raman enhancement) than those previously achieved with graphene, enabling the detection of specific molecules from femtomolar solutions or ambient air. Moreover, nanocorrugated graphene sheets also support propagating visible plasmon modes revealed by scanning near-field optical microscopy observation of their interference patterns.

Molybdenum disulfide nanoribbons with zigzag edges show ferromagnetic and metallic properties based on previous \emph{ab-initio} calculations. The investigation of the role of disorder on the magnetic properties is, however, still lacking due to the computational costs of these methods. In this work we fill this gap by studying the magnetic and electronic properties of several nanometer long MoS$_2$ zigzag nanoribbons using tight-binding and Hubbard Hamiltonians. Our results reveal that proper tight-binding parameters for the edge atoms are crucial to obtain quantitatively the metallic states and the magnetic properties of MoS$_2$ nanoribbons. With the help of the fine-tuned parameters, we perform large-scale calculations and predict the spin domain-wall energy along the edges, which is found to be significantly lower compared to that of the zigzag graphene nanoribbons. The tight-binding approach allows us to address the effect of edge disorder on the magnetic properties. Our results open the way for investigating electron-electron effects in realistic-size nanoribbon devices in MoS$_2$ and also provide valuable information for spintronic applications., Comment: 8 pages, 7 figures

The chemical inertness of the defect-free basal plane confers environmental stability to MoS2 single-layers, but it also limits their chemical versatility and catalytic activity. The stability of the pristine MoS2 basal plane against oxidation under ambient conditions is a widely accepted assumption in the interpretation of various studies and applications. However, single-atom level structural investigations reported here reveal that oxygen atoms spontaneously incorporate into the basal plane of MoS2 single layers during ambient exposure. Our scanning tunneling microscopy investigations reveal a slow oxygen substitution reaction, upon which individual sulfur atoms are one by one replaced by oxygen, giving rise to solid solution type 2D MoS2-xOx crystals. O substitution sites present all over the basal plane act as single-atomic active reaction centers, substantially increasing the catalytic activity of the entire MoS2 basal plane for the electrochemical H2 evolution reaction., Comment: 6 pages, 5 figures

Quantum spin Hall (QSH) insulators are materials that feature an insulating bulk and host edge states protected by time-reversal symmetry. The helical locking of spin and momentum in these states suppresses backscattering of charge carriers, promising applications from low-power electronics to quantum computing. A major challenge for applications is the identification of large gap QSH materials, which would enable room temperature dissipationless transport in their edge states. Here we show that the layered mineral jacutingaite (Pt$_2$HgSe$_3$) is a candidate QSH material, realizing the long sought after the Kane-Mele insulator. Using scanning tunneling microscopy, we measure a band gap of 110 meV, above room temperature, and identify the hallmark edge states. By calculating the $\mathbb{Z}_2$ invariant, we confirm the topological nature of the gap. Being a layered mineral, it is stable in air and can be thinned down to a few atomic layers by mechanical exfoliation. Furthermore, we demonstrate that it can be integrated into heterostructures with other two-dimensional materials. This adds a topological insulator to the 2D quantum material library, greatly expanding the possibilities for tuning 2D electron systems using stacks of layered materials.

Graphene nanoribbons (GNRs) have been proposed as potential building blocks for field effect transistor (FET) devices due to their quantum confinement bandgap. Here, we propose a novel GNR device concept, enabling the control of both charge and spin signals, integrated within the simplest three-terminal device configuration. In a conventional FET device, a gate electrode is employed to tune the Fermi level of the system in and out of a static bandgap. By contrast, in the switching mechanism proposed here, the applied gate voltage can dynamically open and close an interaction gap, with only a minor shift of the Fermi level. Furthermore, the strong interplay of the band structure and edge spin configuration in zigzag ribbons enables such transistors to carry spin polarized current without employing an external magnetic field or ferromagnetic contacts. Using an experimentally validated theoretical model, we show that such transistors can switch at low voltages and high speed, and the spin polarization of the current can be tuned from 0% to 50% by using the same back gate electrode. Furthermore, such devices are expected to be robust against edge irregularities and can operate at room temperature. Controlling both charge and spin signal within the simplest FET device configuration could open up new routes in data processing with graphene based devices., Comment: 16 pages, 5 figures, accepted for publication in 2D Materials

We investigate the local electronic structure of a Sinai-like, quadrilateral graphene quantum billiard with zigzag and armchair edges using scanning tunneling microscopy at room temperature. It is revealed that besides the $(\sqrt{3}\times\sqrt{3})R30${\deg} superstructure, which is caused by the intervalley scattering, its overtones also appear in the STM measurements, which are attributed to the Umklapp processes. We point out that these results can be well understood by taking into account the Coulomb interaction in the quantum billiard, accounting for both the measured density of state values and the experimentally observed topography patterns. The analysis of the level-spacing distribution substantiates the experimental findings as well. We also reveal the magnetic properties of our system which should be relevant in future graphene based electronic and spintronic applications., Comment: 8 pages, 8 figures, accepted for publication in PRB

Magnetic order emerging in otherwise non-magnetic materials as carbon is a paradigmatic example of a novel type of s-p electron magnetism predicted to be of exceptional high-temperature stability. It has been demonstrated that atomic scale structural defects of graphene can host unpaired spins. However, it is still unclear under which conditions long-range magnetic order can emerge from such defect-bound magnetic moments. Here we propose that in contrast to random defect distributions, atomic scale engineering of graphene edges with specific crystallographic orientation, comprising edge atoms only from one sub-lattice of the bipartite graphene lattice, can give rise to a robust magnetic order. We employ a nanofabrication technique based on Scanning Tunneling Microscopy to define graphene nanoribbons with nanometer precision and well-defined crystallographic edge orientations. While armchair ribbons display quantum confinement gap, zigzag ribbons narrower than 7 nm reveal a bandgap of about 0.2 - 0.3 eV, which can be identified as a signature of interaction induced spin ordering along their edges. Moreover, a semiconductor to metal transition is revealed upon increasing the ribbon width, indicating the switching of the magnetic coupling between opposite ribbon edges from antiferromagnetic to ferromagnetic configuration. We found that the magnetic order on graphene edges of controlled zigzag orientation can be stable even at room temperature, raising hope for graphene-based spintronic devices operating under ambient conditions.

Chemical vapor deposition (CVD) on Cu foil is one of the most promising methods to produce graphene samples despite of introducing numerous grain boundaries into the perfect graphene lattice. A rich variety of GB structures can be realized experimentally by controlling the parameters in the CVD method. Grain boundaries contain non-hexagonal carbon rings (4,5,7,8 membered rings) and vacancies in various ratios and arrangements. Using wave packet dynamic (WPD) simulations and tight-binding electronic structure calculations, we have studied the effect of the structure of GBs on the transport properties. Three model GBs with increasing disorder were created in the computer: a periodic 5-7 GB, a "serpentine" GB, and a disordered GB containing 4,8 membered rings and vacancies. It was found that for small energies (E=EF+-1eV) the transmission decreases with increasing disorder. Four membered rings and vacancies are identified as the principal scattering centres. Revealing the connection between the properties of GBs and the CVD growth method may open new opportunities in the graphene based nanoelectronics., Comment: Applied Surface Science (2013)

The evolution of electronic wave packets (WPs) through grain boundaries (GBs) of various structures in graphene was investigated by the numerical solution of the time-dependent Schroedinger equation. WPs were injected from a simulated STM tip placed above one of the grains. Electronic structure of the GBs was calculated by ab-initio and tight-binding methods. Two main factors governing the energy dependence of the transport have been identified: the misorientation angle of the two adjacent graphene grains and the atomic structure of the GB. In case of an ordered GB made of a periodic repetition of pentagon-heptagon pairs, it was found that the transport at high and low energies is mainly determined by the misorientation angle, but the transport around the Fermi energy is correlated with the electronic structure of the GB. A particular line defect with zero misorientation angle (Lahiri et al, Nat Nanotechnol 2010,5:326) behaves as a metallic nanowire and shows electron-hole asymmetry for hot electrons or holes. To generate disordered GBs, found experimentally in CVD graphene samples, a Monte-Carlo-like procedure has been developed. Results show a reduced transport for the disordered GBs, primarily attributed to electronic localized states caused by C atoms with only two covalent bonds., Comment: Carbon (2013)

Perturbations of the two dimensional carbon lattice of graphene, such as grain boundaries, have significant influence on the charge transport and mechanical properties of this material. Scanning tunneling microscopy measurements presented here show that localized states near the Dirac point dominate the local density of states of grain boundaries in graphene grown by chemical vapor deposition. Such low energy states are not reproduced by theoretical models which treat the grain boundaries as periodic dislocation-cores composed of pentagonal-heptagonal carbon rings. Using ab initio calculations, we have extended this model to include disorder, by introducing vacancies into a grain boundary consisting of periodic dislocation-cores. Within the framework of this model we were able to reproduce the measured density of states features. We present evidence that grain boundaries in graphene grown on copper incorporate a significant amount of disorder in the form of two-coordinated carbon atoms.