Two-dimensional (2D) atomic crystals, such as graphene and transition-metal dichalcogenides, have emerged as a new class of materials with remarkable physical properties 1 . In contrast to graphene, monolayer MoS 2 is a non-centrosymmetric material with a direct energy gap 2-5 . Strong photoluminescence 2,3 , a current on-off ratio exceeding 10 8 in field-effect transistors 6 , and efficient valley and spin control by optical helicity 7-9 have recently been demonstrated in this material. Here we report the spectroscopic identification in doped monolayer MoS 2 of tightly bound negative trions, a quasi-particle composed of two electrons and a hole. These quasiparticles, which can be created with valley and spin polarized holes, have no analogue in other materials. They also possess a large binding energy (~ 20 meV), rendering them significant even at room temperature. Our results open up new avenues both for fundamental studies of many-body interactions and for optoelectronic and valleytronic applications in 2D atomic crystals.The trion binding energy that we observe in monolayer MoS 2 is nearly an order of magnitude larger than that found in conventional quasi-2D systems, such as semiconductor quantum wells (QWs) [10][11][12][13] . This is a consequence of the greatly enhanced Coulomb interactions in monolayer MoS 2 , arising from reduced dielectric screening in gapped 2D crystals and the relatively heavy carrier band masses associated with the Mo d-manifolds 4,5,14 . For an electron density as high as n = 10 11 cm -2 , for instance, the dimensionless interaction parameter r s is ~60 in monolayer MoS 2 (Supplementary Information S1). This value is significantly larger than that for carriers in QWs even at very low doping levels 15 . Monolayer MoS 2 is a strongly interacting system even in the presence of relatively high carrier densities; it thus presents an ideal laboratory for exploring many-body phenomena, such as carrier multiplication and Wigner crystallization 16 .The atomic structure of MoS 2 consists of hexagonal planes of S and Mo atoms in a trigonal prismatic structure (Fig. 1a) 17 . The two sublattices of the hexagonal MoS 2 structure are occupied, respectively, by one Mo and two S atoms (Fig. 1b). Monolayer MoS 2 is a direct gap semiconductor with energy gaps located at the K and K' points of the Brillouin zone (Fig. 1c). Both the highest valence bands and the lowest conduction bands are formed primarily from the Mo d-orbitals 4,17 . The large spin-orbit interaction 2 splits the highest valence bands at the K (K') point by ~ 160 meV 2,3,7,14,18 . The valley and spin (VS) degrees are coupled because of the lack of inversion symmetry in monolayer MoS 2 . As has been recently shown experimentally, this allows optical pumping of a single valley (and spin) with circularly polarized light 7-9 .Here we investigate the optical response of monolayer MoS 2 as a function of carrier density by means of absorption and photoluminescence (PL) spectroscopy. In our investigations we have made use of MoS 2 monolayers p...

Recent progress in large-area synthesis of monolayer molybdenum disulphide, a new two-dimensional direct-bandgap semiconductor, is paving the way for applications in atomically thin electronics. Little is known, however, about the microstructure of this material. Here we have refined chemical vapour deposition synthesis to grow highly crystalline islands of monolayer molybdenum disulphide up to 120 μm in size with optical and electrical properties comparable or superior to exfoliated samples. Using transmission electron microscopy, we correlate lattice orientation, edge morphology and crystallinity with island shape to demonstrate that triangular islands are single crystals. The crystals merge to form faceted tilt and mirror twin boundaries that are stitched together by lines of 8- and 4-membered rings. Density functional theory reveals localized mid-gap states arising from these 8-4 defects. We find that mirror twin boundaries cause strong photoluminescence quenching whereas tilt boundaries cause strong enhancement. Meanwhile, mirror twin boundaries slightly increase the measured in-plane electrical conductivity, whereas tilt boundaries slightly decrease the conductivity.

Semiconductor p-n junctions are essential building blocks for electronic and optoelectronic devices. In conventional p-n junctions, regions depleted of free charge carriers form on either side of the junction, generating built-in potentials associated with uncompensated dopant atoms. Carrier transport across the junction occurs by diffusion and drift processes influenced by the spatial extent of this depletion region. With the advent of atomically thin van der Waals materials and their heterostructures, it is now possible to realize a p-n junction at the ultimate thickness limit. Van der Waals junctions composed of p- and n-type semiconductors--each just one unit cell thick--are predicted to exhibit completely different charge transport characteristics than bulk heterojunctions. Here, we report the characterization of the electronic and optoelectronic properties of atomically thin p-n heterojunctions fabricated using van der Waals assembly of transition-metal dichalcogenides. We observe gate-tunable diode-like current rectification and a photovoltaic response across the p-n interface. We find that the tunnelling-assisted interlayer recombination of the majority carriers is responsible for the tunability of the electronic and optoelectronic processes. Sandwiching an atomic p-n junction between graphene layers enhances the collection of the photoexcited carriers. The atomically scaled van der Waals p-n heterostructures presented here constitute the ultimate functional unit for nanoscale electronic and optoelectronic devices.

Atomically thin two-dimensional semiconductors such as MoS 2 hold great promise in electrical, optical, and mechanical devices and display novel physical phenomena. However, the electron mobility of mono-and few-layer MoS 2 has so far been substantially below theoretically predicted limits, which has hampered efforts to observe its intrinsic quantum transport behaviours. Potential sources of disorder and scattering include both defects such as sulfur vacancies in the MoS 2 itself, and extrinsic sources such as charged impurities and remote optical phonons from oxide dielectrics. To reduce extrinsic scattering, here we developed a van der Waals heterostructure device platform where MoS 2 layers are fully encapsulated within hexagonal boron nitride, and electrically contacted in a multi-terminal geometry using gate-tunable graphene electrodes. Magneto-transport measurements show dramatic improvements in performance, including a record-high Hall mobility reaching 34,000 cm 2 /Vs for 6-layer MoS 2 at low temperature, confirming that low-temperature performance in previous studies was limited by extrinsic interfacial impurities rather than bulk defects in the MoS 2 . We also observed Shubnikov-de Haas oscillations for the first time in high-mobility monolayer and few-layer MoS 2 . Modeling of potential scattering sources and quantum lifetime analysis indicate that a combination of short-ranged and long-ranged interfacial scattering limits low-temperature mobility of MoS 2 . 3Following the many advances in basic science and applications of graphene, other twodimensional (2D) materials, especially transition metal dichalcogenides (TMDCs), have attracted significant interest for their fascinating electrical, optical, and mechanical properties [1][2][3][4][5][6][7][8] . Among the TMDCs, semiconducting MoS 2 has been the mostly widely studied: it shows a thicknessdependent electronic band structure 3,5 , reasonably high carrier mobility 1,2,6-9 , and novel phenomena such as coupled spin-valley physics and the valley Hall effect 10-14 , leading to various applications, such as transistors 1,7,15 , memories 16 , logic circuits 17,18 , light-emitters 19 , and photo-detectors 20 with flexibility and transparency 2,21 . However, as for any 2D material, the electrical and optical properties of MoS 2 are strongly affected by impurities and its dielectric environment 1,2,9,22 , hindering the study of intrinsic physics and limiting the design of 2D-material-based devices. In particular, the theoretical upper bound of the electron mobility of monolayer (1L) MoS 2 is predicted to be from several tens to a few thousands at room temperature (T) and exceed 10 5 cm 2 /Vs at low T depending on the dielectric environment, impurity density and charge carrier density [23][24][25] . In contrast, experimentally measured 1L MoS 2 devices on SiO 2 substrates have exhibited room-T two-terminal field-effect mobility that ranges from 0.1 -55 cm 2 /Vs 1,26,27 . This value increases to 15 -60 cm 2 /Vs with encapsulation by highdielectric materials 1...

Atomically thin forms of layered materials, such as conducting graphene, insulating hexagonal boron nitride (hBN), and semiconducting molybdenum disulfide (MoS2), have generated great interests recently due to the possibility of combining diverse atomic layers by mechanical "stacking" to create novel materials and devices. In this work, we demonstrate field-effect transistors (FETs) with MoS2 channels, hBN dielectric, and graphene gate electrodes. These devices show field-effect mobilities of up to 45 cm(2)/Vs and operating gate voltage below 10 V, with greatly reduced hysteresis. Taking advantage of the mechanical strength and flexibility of these materials, we demonstrate integration onto a polymer substrate to create flexible and transparent FETs that show unchanged performance up to 1.5% strain. These heterostructure devices consisting of ultrathin two-dimensional (2D) materials open up a new route toward high-performance flexible and transparent electronics.

Pristine graphene is the strongest material ever measured. However, large-area graphene films produced by means of chemical vapor deposition (CVD) are polycrystalline and thus contain grain boundaries that can potentially weaken the material. We combined structural characterization by means of transmission electron microscopy with nanoindentation in order to study the mechanical properties of CVD-graphene films with different grain sizes. We show that the elastic stiffness of CVD-graphene is identical to that of pristine graphene if postprocessing steps avoid damage or rippling. Its strength is only slightly reduced despite the existence of grain boundaries. Indentation tests directly on grain boundaries confirm that they are almost as strong as pristine. Graphene films consisting entirely of well-stitched grain boundaries can retain ultrahigh strength, which is critical for a large variety of applications, such as flexible electronics and strengthening components.

Electron tunneling through atomically flat and ultrathin hexagonal boron nitride (h-BN) on gold-coated mica was investigated using conductive atomic force microscopy. Low-bias direct tunneling was observed in mono-, bi-, and tri-layer h-BN. For all thicknesses, Fowler-Nordheim tunneling (FNT) occurred at high bias, showing an increase of breakdown voltage with thickness. Based on the FNT model, the barrier height for tunneling (3.07 eV) and dielectric strength (7.94 MV/cm) of h-BN are obtained; these values are comparable to those of SiO2.

It is important from a fundamental standpoint and for practical applications to understand how the mechanical properties of graphene are influenced by defects. Here we report that the two-dimensional elastic modulus of graphene is maintained even at a high density of sp 3 -type defects. Moreover, the breaking strength of defective graphene is only B14% smaller than its pristine counterpart in the sp 3 -defect regime. By contrast, we report a significant drop in the mechanical properties of graphene in the vacancy-defect regime. We also provide a mapping between the Raman spectra of defective graphene and its mechanical properties. This provides a simple, yet non-destructive methodology to identify graphene samples that are still mechanically functional. By establishing a relationship between the type and density of defects and the mechanical properties of graphene, this work provides important basic information for the rational design of composites and other systems utilizing the high modulus and strength of graphene.