Topological Weyl semimetal (TWS), a new state of quantum matter, has sparked enormous research interest recently. Possessing unique Weyl fermions in the bulk and Fermi arcs on the surface, TWSs offer a rare platform for realizing many exotic physical phenomena. TWSs can be classified into type-I that respect Lorentz symmetry and type-II that do not. Here, we directly visualize the electronic structure of MoTe2, a recently proposed type-II TWS. Using angle-resolved photoemission spectroscopy (ARPES), we unravel the unique surface Fermi arcs, in good agreement with our ab initio calculations that have nontrivial topological nature. Our work not only leads to new understandings of the unusual properties discovered in this family of compounds, but also allows for the further exploration of exotic properties and practical applications of type-II TWSs, as well as the interplay between superconductivity (MoTe2 was discovered to be superconducting recently) and their topological order.
Chalcogen vacancies are generally considered to be the most common point defects in transition metal dichalcogenide (TMD) semiconductors because of their low formation energy in vacuum and their frequent observation in transmission electron microscopy studies. Consequently, unexpected optical, transport, and catalytic properties in 2D-TMDs have been attributed to in-gap states associated with chalcogen vacancies, even in the absence of direct experimental evidence. Here, we combine low-temperature non-contact atomic force microscopy, scanning tunneling microscopy and spectroscopy, and state-of-the-art ab initio density functional theory and GW calculations to determine both the atomic structure and electronic properties of an abundant chalcogen-site point defect common to MoSe 2 and WS 2 monolayers grown by molecular beam epitaxy and chemical vapor deposition, respectively. Surprisingly, we observe no in-gap states. Our results strongly suggest that the common chalcogen defects in the described 2D-TMD semiconductors, measured in vacuum environment after gentle annealing, are oxygen substitutional defects, rather than vacancies.
Recently discovered materials called threedimensional topological insulators 1-5 constitute examples of symmetry protected topological states in the absence of applied magnetic fields and cryogenic temperatures. A hallmark characteristic of these non-magnetic bulk insulators is the protected metallic electronic states confined to the material's surfaces. Electrons in these surface states are spin polarized with their spins governed by their direction of travel (linear momentum), resulting in a helical spin texture in momentum space.6 Spin-and angle-resolved photoemission spectroscopy (spin-ARPES) has been the only tool capable of directly observing this central feature with simultaneous energy, momentum, and spin sensitivity.6-12 By using an innovative photoelectron spectrometer 13 with a highflux laser-based light source, we discovered another surprising property of these surface electrons which behave like Dirac fermions. We found that the spin polarization of the resulting photoelectrons can be fully manipulated in all three dimensions through selection of the light polarization. These surprising effects are due to the spin-dependent interaction of the helical Dirac fermions with light, which originates from the strong spin-orbit coupling in the material. Our results illustrate unusual scenarios in which the spin polarization of photoelectrons is completely different from the spin state of electrons in the originating initial states. The results also provide the basis for a novel source of highly spinpolarized electrons with tunable polarization in three dimensions.The topological electronic bandstructure of a bulk topological insulator ensures the presence of gapless surface electronic states with Dirac-like dispersions similar to graphene. Unlike graphene, the topological surface states are spin polarized, with their spins locked perpendicular to their momentum, forming helical spinmomentum textures 6 (see Fig. 1(a)). The presence of such 'helical Dirac fermions' forms an operational definition of a 3D topological insulator, and much of the excitement surrounding topological insulators involves the predicted exotic phenomena and potential applications of these metallic states.4,5 These include novel magnetoelectric effects, 14 exotic quasiparticles (in a proximity induced superconducting state) called Majorana fermions which are their own antiparticles, 15 and applications ranging from spintronics to quantum computing. 16Establishing methods that are sensitive to these states and their predicted behaviors have therefore generated much interest. 6,17-20Angle-resolved photoemission spectroscopy (ARPES) directly maps the dispersions and Fermi surfaces of such electronic states in energy-momentum space. Spinresolved ARPES also measures the spin polarization of the corresponding photoelectrons. Following a common assumption that electron spin is conserved in the photoemission process, the technique has been used to identify the presence of the predicted helical spin textures of topological surface states.6-12 Ut...
High quality WSe2 films have been grown on bilayer graphene (BLG) with layer-by-layer control of thickness using molecular beam epitaxy. The combination of angle-resolved photoemission, scanning tunneling microscopy/spectroscopy, and optical absorption measurements reveal the atomic and electronic structures evolution and optical response of WSe2/BLG. We observe that a bilayer of WSe2 is a direct bandgap semiconductor, when integrated in a BLG-based heterostructure, thus shifting the direct-indirect band gap crossover to trilayer WSe2. In the monolayer limit, WSe2 shows a spin-splitting of 475 meV in the valence band at the K point, the largest value observed among all the MX2 (M = Mo, W; X = S, Se) materials. The exciton binding energy of monolayer-WSe2/BLG is found to be 0.21 eV, a value that is orders of magnitude larger than that of conventional three-dimensional semiconductors, yet small as compared to other two-dimensional transition metal dichalcogennides (TMDCs) semiconductors. Finally, our finding regarding the overall modification of the electronic structure by an alkali metal surface electron doping opens a route to further control the electronic properties of TMDCs.
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