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Understanding the phase transition mechanisms in two-dimensional (2D) materials is a key to precisely tailor their properties at the nanoscale. Molybdenum ditelluride (MoTe2) exhibits multiple phases at room temperature, making it a promising candidate for phase-change applications. Here, we fabricate lateral 2H-Td interfaces with laser irradiation and probe their phase transitions from micro- to atomic scales with in situ heating in the transmission electron microscope (TEM). By encapsulating the MoTe2 with graphene protection layers, we create an in situ reaction cell compatible with atomic resolution imaging. We find that the Td-to-2H phase transition initiates at phase boundaries at low temperatures (200-225 degree C) and propagates anisotropically along the b-axis in a layer-by-layer fashion. We also demonstrate a fully reversible 2H-Td-2H phase transition cycle, which generates a coherent 2H lattice containing inversion domain boundaries. Our results provide insights on fabricating 2D hetero-phase devices with atomically sharp and coherent interfaces., Comment: 38 pages, 5 figures, 9 supplementary figures, and supplementary information

Scanning transmission electron microscopy (STEM) is an indispensable tool for atomic-resolution structural analysis for a wide range of materials. The conventional analysis of STEM images is an extensive hands-on process, which limits efficient handling of high-throughput data. Here we apply a fully convolutional network (FCN) for identification of important structural features of two-dimensional crystals. ResUNet, a type of FCN, is utilized in identifying sulfur vacancies and polymorph types of ${MoS_2}$ from atomic resolution STEM images. Efficient models are achieved based on training with simulated images in the presence of different levels of noise, aberrations, and carbon contamination. The accuracy of the FCN models toward extensive experimental STEM images is comparable to that of careful hands-on analysis. Our work provides a guideline on best practices to train a deep learning model for STEM image analysis and demonstrates FCN's application for efficient processing of a large volume of STEM data., Comment: 24 pages, 5 figures

The properties of metal-semiconductor junctions are often unpredictable because of non-ideal interfacial structures, such as interfacial defects or chemical reactions introduced at junctions. Black phosphorus (BP), an elemental two-dimensional (2D) semiconducting crystal, possesses the puckered atomic structure with high chemical reactivity, and the establishment of a realistic atomic-scale picture of BP's interface toward metallic contact has remained elusive. Here we examine the interfacial structures and properties of physically-deposited metals of various kinds on BP. We find that Au, Ag, and Bi form single-crystalline films with (110) orientation through guided van der Waals epitaxy. Transmission electron microscopy and X-ray photoelectron spectroscopy confirm that atomically sharp van der Waals metal-BP interfaces forms with exceptional rotational alignment. Under a weak metal-BP interaction regime, the BP's puckered structure play an essential role in the adatom assembly process and can lead to the formation of a single crystal, which is supported by our theoretical analysis and calculations. The experimental survey also demonstrates that the BP-metal junctions can exhibit various types of interfacial structures depending on metals, such as the formation of polycrystalline microstructure or metal phosphides. This study provides a guideline for obtaining a realistic view on metal-2D semiconductor interfacial structures, especially for atomically puckered 2D crystals., Comment: 27 pages, 5 figures

Previous studies indicate that the properties of graphene oxide (GO) can be significantly improved by enhancing its graphitic domain size through thermal diffusion and clustering of functional groups. Remarkably, this transition takes place below the decomposition temperature of the functional groups and thus allows fine-tuning of graphitic domains without compromising with the functionality of GO. By studying the transformation of GO under mild thermal treatment, we directly observe this size enhancement of graphitic domains from originally 40 nm2 to 200 nm2 through an extensive transmission electron microscopy (TEM) study. Additionally, we confirm the integrity of the functional groups during this process by comprehensive chemical analysis. A closer look into the process confirms the theoretically predicted relevance for the room temperature stability of GO. We further investigate the influence of enlarged graphitic domains on the hydration behaviour of GO and catalytic performance of single-atom catalysts supported by GO.

A finite Schottky barrier and large contact resistance between monolayer MoS2 and electrodes are the major bottlenecks in developing high-performance field-effect transistors (FETs) that hinder the study of intrinsic quantum behaviors such as valley-spin transport at low temperature. A gate-tunable graphene electrode platform has been developed to improve the performance of MoS2 FETs. However, intrinsic misalignment between the work function of pristine graphene and the conduction band of MoS2 results in a large threshold voltage for the FETs, because of which Ohmic contact behaviors are observed only at very high gate voltages and carrier concentrations (~1013 cm-2). Here, we present high-performance monolayer MoS2 FETs with Ohmic contact at a modest gate voltage by using a chemical-vapor-deposited (CVD) nitrogen-doped graphene with a high intrinsic electron carrier density. The CVD nitrogen-doped graphene and monolayer MoS2 hybrid FETs platform exhibited a large negative shifted threshold voltage of -54.2 V and barrier-free Ohmic contact under zero gate voltage. Transparent contact by nitrogen-doped graphene led to a 214% enhancement in the on-current and a four-fold improvement in the field-effect carrier mobility of monolayer MoS2 FETs compared with those of a pristine graphene electrode platform. The transport measurements, as well as Raman and X-ray photoelectron spectroscopy analyses before and after thermal annealing, reveal that the atomic C-N bonding in the CVD nitrogen-doped graphene is responsible for the dominant effects of electron doping. Large-scale nitrogen-doped graphene electrodes provide a promising device platform for the development of high-performance devices and the study of unique quantum behaviors., Comment: 25 pages, 4 figures

Graphene mechanical resonators are the ultimate two-dimensional nanoelectromechanical systems (NEMS) with applications in sensing and signal processing. While initial devices have shown promising results, an ideal graphene NEMS resonator should be strain engineered, clamped at the edge without trapping gas underneath, and electrically integratable. In this letter, we demonstrate fabrication and direct electrical measurement of circular SU-8 polymer-clamped chemical vapor deposition (CVD) graphene drum resonators. The clamping increases device yield and responsivity, while providing a cleaner resonance spectrum from eliminated edge modes. Furthermore, this resonator is highly strained, indicating its potential in strain engineering for performance enhancement., Comment: 15 pages, 5 figures

Oscillators, which produce continuous periodic signals from direct current power, are central to modern communications systems, with versatile applications such as timing references and frequency modulators. However, conventional oscillators typically consist of macroscopic mechanical resonators such as quartz crystals, which require excessive off-chip space. Here we report oscillators built on micron-size, atomically-thin graphene nanomechanical resonators, whose frequencies can be electrostatically tuned by as much as 14\%. The self-sustaining mechanical motion of the oscillators is generated and transduced at room temperature by simple electrical circuitry. The prototype graphene voltage controlled oscillators exhibit frequency stability and modulation bandwidth sufficient for modulation of radio-frequency carrier signals. As a demonstration, we employ a graphene oscillator as the active element for frequency modulated signal generation, and achieve efficient audio signal transmission., Comment: 18 pages, 4 figures

Atomically thin materials such as graphene and semiconducting transition metal dichalcogenides (TMDCs) have attracted extensive interest in recent years, motivating investigation into multiple properties. In this work, we demonstrate a refined version of the optothermal Raman technique to measure the thermal transport properties of two TMDC materials, MoS2 and MoSe2, in single-layer (1L) and bi-layer (2L) forms. This new version incorporates two crucial improvements over previous implementations. First, we utilize more direct measurements of the optical absorption of the suspended samples under study and find values ~40% lower than previously assumed. Second, by comparing the response of fully supported and suspended samples using different laser spot sizes, we are able to independently measure the interfacial thermal conductance to the substrate and the lateral thermal conductivity of the supported and suspended materials. The approach is validated by examining the response of a suspended film illuminated in different radial positions. For 1L MoS2 and MoSe2, the room-temperature thermal conductivities are (84+/-17) W/mK and (59+/-18) W/mK, respectively. For 2L MoS2 and MoSe2, we obtain values of (77+/-25) W/mK and (42+/-13) W/mK. Crucially, the interfacial thermal conductance is found to be of order 0.1-1 MW/m2K, substantially smaller than previously assumed, a finding that has important implications for design and modeling of electronic devices.

Atomically thin two-dimensional (2D) semiconductors such as molybdenum disulphide (MoS2) hold great promise in electrical, optical, and mechanical devices and display novel physical phenomena such as coupled spin-valley physics and the valley Hall effect. However, the electron mobility of mono- and few-layer MoS2 has so far been substantially below theoretically predicted limits, particularly at low temperature (T), which has hampered efforts to observe its intrinsic quantum transport behaviors. Potential sources of disorder and scattering include both defects such as sulfur vacancies in the MoS2 itself, and extrinsic sources such as charged impurities and remote optical phonons from oxide dielectrics. To reduce extrinsic scattering and approach the intrinsic limit, we developed a van der Waals (vdW) heterostructure device platform where MoS2 layers are fully encapsulated within hexagonal boron nitride (hBN), and electrically contacted in a multi-terminal geometry using gate-tunable graphene electrodes. Multi-terminal magneto-transport measurements show dramatic improvements in performance, including a record-high Hall mobility reaching 34,000 cm2/Vs for 6-layer MoS2 at low T. Comparison to theory shows a decrease of 1-2 orders of magnitude in the density of charged impurities, indicating that performance at low T in previous studies was limited by extrinsic factors rather than defects in the MoS2. We also observed Shubnikov-de Haas (SdH) oscillations for the first time in high-mobility monolayer and few-layer MoS2. This novel device platform therefore opens up a new way toward measurements of intrinsic properties and the study of quantum transport phenomena in 2D semiconducting materials., Comment: 21 pages, 4 figures, 1 table; fix the affiliation and acknowledgements;remove the refs. 36 on page 7

Semiconductor p-n junctions are essential building blocks for modern electronics and optoelectronics. In conventional semiconductors, a p-n junction produces depletion regions of free charge carriers at equilibrium and built-in potentials associated with uncompensated dopant atoms. Carrier transport across the junction occurs by diffusion and drift processes defined by the spatial extent of this region. With the advent of atomically thin van der Waals (vdW) materials and their heterostructures, we are now able to realize a p-n junction at the ultimate quantum limit. In particular, vdW 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 junctions. Here we report the electronic and optoelectronic characterization of atomically thin p-n heterojunctions fabricated using vdW assembly of transition metal dichalcogenides (TMDCs). Across the p-n interface, we observe gate-tuneable diode-like current rectification and photovoltaic response. 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 collection of the photoexcited carriers. The atomically scaled vdW p-n heterostructures presented here constitute the ultimate quantum limit for functional electronic and optoelectronic components., Comment: 29 pages, 3 figures in main & 10 figures in supplementary information

High stress stoichiometric silicon nitride resonators, whose quality factors exceed one million, have shown promise for applications in sensing and signal processing. Yet, electrical integration of the insulating silicon nitride resonators has been challenging, as depositing even a thin layer of metal degrades the quality factor significantly. In this work, we show that graphene used as a conductive coating for Si3N4 membranes reduces the quality factor by less than 30 % on average, which is minimal when compared to the effect of conventional metallization layers such as chromium or aluminum. The electrical integration of Si3N4-Graphene (SiNG) heterostructure resonators is demonstrated with electrical readout and electro-static tuning of the frequency by up to 1 % per volt. These studies demonstrate the feasibility of hybrid graphene/nitride mechanical resonators in which the electrical properties of graphene are combined with the superior mechanical performance of silicon nitride., Comment: 8 pages, 5 figures, journal

Recent progress in large-area synthesis of monolayer molybdenum disulfide, 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 vapor deposition synthesis to grow highly crystalline islands of monolayer molybdenum disulfide up to 120 um 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 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 boundaries cause strong photoluminescence quenching while tilt boundaries cause strong enhancement. In contrast, the boundaries only slightly increase the measured in-plane electrical conductivity.

Two-dimensional (2D) atomic crystals, such as graphene and transition-metal dichalcogenides, have emerged as a new class of materials with remarkable physical properties. In contrast to graphene, monolayer MoS2 is a non-centrosymmetric material with a direct energy gap. Strong photoluminescence, a current on-off ratio exceeding 10^8 in field-effect transistors, and efficient valley and spin control by optical helicity have recently been demonstrated in this material. Here we report the spectroscopic identification in doped monolayer MoS2 of tightly bound negative trions, a quasi-particle composed of two electrons and a hole. These quasi-particles, which can be created with valley and spin polarized holes, have no analogue in other semiconducting 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 opto-electronic and valleytronic applications in 2D atomic crystals., Comment: 18 pages including supplementary information