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 hightemperature stability 1 . It has been demonstrated that atomic scale structural defects of graphene can host unpaired spins 2,3 . However, it is still unclear under which conditions longrange 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 sublattice of the bipartite graphene lattice -can give rise to a robust magnetic order. We employ a nanofabrication technique 4 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 2 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.The intrinsic magnetism of graphite has a long and controversial history 1 . The origin of the measured magnetic signal is generally attributed to atomic scale structural defects locally breaking the sub-lattice balance of the bipartite hexagonal lattice 5,6 . However, the unambiguous identification of the structural sources of the measured magnetic signal has proven challenging as they are buried inside the bulk of the material. The isolation of single graphene layers 7 opens new prospects in this direction 8,9 as their atomic structure is fully accessible for imaging and controlled modification. In particular, graphene edges of specific (zigzag) crystallographic orientation comprising carbon atoms from only one sub-lattice of the bipartite hexagonal lattice are predicted to host magnetic order 10 , in striking contrast to armchair edges incorporating an equal number of carbon atoms from both sublattices.The strong influence of edge orientation on the electronic structure of graphene nanoribbons had However, the random orientation of the edges and the influence of a possible strong edge-substrate hybridization 21 did not allow full access to the nature of edge-magnetism in graphene. Though the 4 magnetic order is expected to persist to some extent on zigzag segments of randomly oriented graphene edges, the mixing of different edge types are expected to substantially weaken the effect 19,22 . Therefore, the lack of experimental control over the edge orientation seems one of the main ...

MoS2 single layers have recently emerged as strong competitors of graphene in electronic and optoelectronic device applications due to their intrinsic direct bandgap. However, transport measurements reveal the crucial role of defect-induced electronic states, pointing out the fundamental importance of characterizing their intrinsic defect structure. Transmission Electron Microscopy (TEM) is able to image atomic scale defects in MoS2 single layers, but the imaged defect structure is far from the one probed in the electronic devices, as the defect density and distribution are substantially altered during the TEM imaging. Here, we report that under special imaging conditions, STM measurements can fully resolve the native atomic scale defect structure of MoS2 single layers. Our STM investigations clearly resolve a high intrinsic concentration of individual sulfur atom vacancies, and experimentally identify the nature of the defect induced electronic mid-gap states, by combining topographic STM images with ab intio calculations. Experimental data on the intrinsic defect structure and the associated defect-bound electronic states that can be directly used for the interpretation of transport measurements are essential to fully understand the operation, reliability and performance limitations of realistic electronic devices based on MoS2 single layers.

Theory has predicted rich and very distinct physics for graphene devices with boundaries that follow either the armchair or zigzag crystallographic directions. A prerequisite to disclose this physics in experiment is to be able to produce devices with boundaries of pure chirality. Exfoliated flakes frequently exhibit corners with an odd multiple of 30°, which raised expectations that their boundaries follow pure zigzag and armchair directions. The predicted Raman behavior at such crystallographic edges however failed to confirm pure edge chirality. Here, we perform confocal Raman spectroscopy on hexagonal holes obtained after the anisotropic etching of prepatterned pits using carbothermal decomposition of SiO 2 . The boundaries of the hexagonal holes are aligned along the zigzag

Isolating large-areas of atomically thin transition metal chalcogenide crystals is an important but challenging task. The mechanical exfoliation technique can provide single layers of the highest structural quality, enabling to study their pristine properties and ultimate device performance. However, a major drawback of the technique is the low yield and small (typically < 10 μm) lateral size of the produced single layers. Here, we report a novel mechanical exfoliation technique, based on chemically enhanced adhesion, yielding MoS2 single layers with typical lateral sizes of several hundreds of microns. The idea is to exploit the chemical affinity of the sulfur atoms that can bind more strongly to a gold surface than the neighboring layers of the bulk MoS2 crystal. Moreover, we found that our exfoliation process is not specific to MoS2, but can be generally applied for various layered chalcogenides including selenites and tellurides, providing an easy access to large-area 2D crystals for the whole class of layered transition metal chalcogenides.