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We report the study of a tri-axial vector magnetoresistance (MR) in nonmagnetic (Bi1-xInx)2Se3 nanodevices at the composition of x = 0.08. We show a dumbbell-shaped in-plane negative MR up to room temperature as well as a large out-of-plane positive MR. MR at three directions is about in a -3%: -1%: 225% ratio at 2 K. Through both the thickness and composition-dependent magnetotransport measurements, we show that the in-plane negative MR is due to the topological phase transition enhanced intersurface coupling near the topological critical point. Our devices suggest the great potential for room-temperature spintronic applications, for example, vector magnetic sensors., Comment: 23 pages, 12 figures

Van der Waals heterostructure based on layered two-dimensional (2D) materials offers unprecedented opportunities to create materials with atomic precision by design. By combining superior properties of each component, such heterostructure also provides possible solutions to address various challenges of the electronic devices, especially those with vertical multilayered structures. Here, we report the realization of robust memristors for the first time based on van der Waals heterostructure of fully layered 2D materials (graphene/MoS2-xOx/graphene) and demonstrate a good thermal stability lacking in traditional memristors. Such devices have shown excellent switching performance with endurance up to 107 and a record-high operating temperature up to 340oC. By combining in situ high-resolution TEM and STEM studies, we have shown that the MoS2-xOx switching layer, together with the graphene electrodes and their atomically sharp interfaces, are responsible for the observed thermal stability at elevated temperatures. A well-defined conduction channel and a switching mechanism based on the migration of oxygen ions were also revealed. In addition, the fully layered 2D materials offer a good mechanical flexibility for flexible electronic applications, manifested by our experimental demonstration of a good endurance against over 1000 bending cycles. Our results showcase a general and encouraging pathway toward engineering desired device properties by using 2D van der Waals heterostructures., Comment: To appear on Nature Electronics; 31 pages, 6 figures, 8 supplementary figures

Superconductors at the atomic two-dimensional (2D) limit are the focus of an enduring fascination in the condensed matter community. This is because, with reduced dimensions, the effects of disorders, fluctuations, and correlations in superconductors become particularly prominent at the atomic 2D limit; thus such superconductors provide opportunities to tackle tough theoretical and experimental challenges. Here, based on the observation of ultrathin 2D superconductivity in mono- and bilayer molybdenum disulfide (MoS$_2$) with electric-double-layer (EDL) gating, we found that the critical sheet carrier density required to achieve superconductivity in a monolayer MoS$_2$ flake can be as low as 0.55*10$^{14}$cm$^{-2}$, which is much lower than those values in the bilayer and thicker cases in previous report and also our own observations. Further comparison of the phonon dispersion obtained by ab initio calculations indicated that the phonon softening of the acoustic modes around the M point plays a key role in the gate-induced superconductivity within the Bardeen-Cooper Schrieffer (BCS) theory framework. This result might help enrich the understanding of 2D superconductivity with EDL gating.

Two-dimensional (2D) transition metal dichalcogenides (TMDs) have recently emerged as promising candidates for future electronics and optoelectronics. While most of TMDs are intrinsic n-type semiconductors due to electron donating which originates from chalcogen vacancies, obtaining intrinsic high-quality p-type semiconducting TMDs has been challenging. Here, we report an experimental approach to obtain intrinsic p-type Tungsten (W)-based TMDs by substitutional Ta-doping. The obtained few-layer Ta-doped WSe2 (Ta0.01W0.99Se2) field-effect transistor (FET) devices exhibit competitive p-type performances, including ~10^6 current on/off at room temperature. We also demonstrate high quality van der Waals (vdW) p-n heterojunctions based on Ta0.01W0.99Se2/MoS2 structure, which exhibit nearly ideal diode characteristics (with an ideality factor approaching 1 and a rectification ratio up to 10^5) and excellent photodetecting performance. Our study suggests that substitutional Ta-doping holds great promise to realize intrinsic p-type W-based TMDs for future electronic and photonic applications., Comment: To appear in Applied Physics Letters; 31 pages, 4 pages, 7 supplementary figures; submitted on May 1st, 2017

The mid-infrared (MIR) spectral range, pertaining to important applications such as molecular 'fingerprint' imaging, remote sensing, free space telecommunication and optical radar, is of particular scientific interest and technological importance. However, state-of-the-art materials for MIR detection are limited by intrinsic noise and inconvenient fabrication processes, resulting in high cost photodetectors requiring cryogenic operation. We report black arsenic-phosphorus-based long wavelength infrared photodetectors with room temperature operation up to 8.2 um, entering the second MIR atmospheric transmission window. Combined with a van der Waals heterojunction, room temperature specific detectivity higher than 4.9*10^9 Jones was obtained in the 3-5 um range. The photodetector works in a zero-bias photovoltaic mode, enabling fast photoresponse and low dark noise. Our van der Waals heterojunction photodector not only exemplify black arsenic-phosphorus as a promising candidate for MIR opto-electronic applications, but also pave the way for a general strategy to suppress 1/f noise in photonic devices., Comment: To appear in Science Advances; 27 pages, 3 figures, 9 supplementary figures; submitted on Feb. 24th, 2017

Among the family of TMDs, ReS2 takes a special position, which crystalizes in a unique distorted low-symmetry structure at ambient conditions. The interlayer interaction in ReS2 is rather weak, thus its bulk properties are similar to that of monolayer. However, how does compression change its structure and electronic properties is unknown so far. Here using ab initio crystal structure searching techniques, we explore the high-pressure phase transitions of ReS2 extensively and predict two new high-pressure phases. The ambient pressure phase transforms to a "distorted-1T" structure at very low pressure and then to a tetragonal I41/amd structure at around 90 GPa. The "distorted-1T" structure undergoes a semiconductor-metal transition (SMT) at around 70 GPa with a band overlap mechanism. Electron-phonon calculations suggest that the I41/amd structure is superconducting and has a critical superconducting temperature of about 2 K at 100 GPa. We further perform high-pressure electrical resistance measurements up to 102 GPa. Our experiments confirm the SMT and the superconducting phase transition of ReS2 under high pressure. These experimental results are in good agreement with our theoretical predictions., Comment: 25 pages, 6 figures, accepted by npj Quantum Materials

Two dimensional (2D) materials, e.g. graphene, transition metal dichalcogenides (TMDs), black phosphorus (BP), have demonstrated fascinating electrical and optical characteristics and exhibited great potential in optoelectronic applications. High performance and multifunctional devices were achieved by employing diverse designs of architectures, such as hybrid systems with nanostructured materials, bulk semiconductors and organics, forming 2D heterostructures. In this review, we mainly discuss the recent progresses of 2D materials in high responsive photodetectors, light-emitting devices and single photon emitters. Hybrid systems and van der Waals heterostructures based devices are emphasized, which exhibit great potential in state-of-the-art applications., Comment: 31 pages, 11 figures, to appear in Chinese Physics B

The progress in exploiting new electronic materials and devices has been a major driving force in solid-state physics. As a new state of matter, a Weyl semimetal (WSM), particularly a type-II WSM, hosts Weyl fermions as emergent quasiparticles and may harbor novel electrical transport properties because of the exotic Fermi surface. Nevertheless, such a type-II WSM material has not been experimentally observed in nature. In this work, by performing systematic magneto-transport studies on thin films of a predicted material candidate WTe2, we observe notable angle-sensitive (between the electric and magnetic fields) negative longitudinal magnetoresistance (MR), which can likely be attributed to the chiral anomaly in WSM. This phenomenon also exhibits strong planar orientation dependence with the absence of negative longitudinal MR along the tungsten chains (a axis), which is consistent with the distinctive feature of a type-II WSM. By applying a gate voltage, we demonstrate that the Fermi energy can be tuned through the Weyl points via the electric field effect; this is the first report of controlling the unique transport properties in situ in a WSM system. Our results have important implications for investigating simulated quantum field theory in solid-state systems and may open opportunities for implementing new types of electronic applications, such as field-effect chiral electronic devices., Comment: accepted by Nature Communications; 27 pages, 3 figures, 9 supplementary figures; submitted on May 1st, 2016

Van der Waals junctions of two-dimensional materials with an atomically sharp interface open up unprecedented opportunities to design and study functional heterostructures. Semiconducting transition metal dichalcogenides have shown tremendous potential for future applications due to their unique electronic properties and strong light-matter interaction. However, many important optoelectronic applications, such as broadband photodetection, are severely hindered by their limited spectral range and reduced light absorption. Here, we present a p-g-n heterostructure formed by sandwiching graphene with a gapless bandstructure and wide absorption spectrum in an atomically thin p-n junction to overcome these major limitations. We have successfully demonstrated a MoS2-graphene-WSe2 heterostructure for broadband photodetection in the visible to short-wavelength infrared range at room temperature that exhibits competitive device performance, including a specific detectivity of up to 1011 Jones in the near-infrared region. Our results pave the way toward the implementation of atomically thin heterostructures for broadband and sensitive optoelectronic applications., Comment: Submitted to Nano Letters; 25 pages, 4 figures, 7 supplementary figures

Two-dimensional transition metal dichalcogenides are emerging with tremendous potential in many optoelectronic applications due to their strong light-matter interactions. To fully explore their potential in photoconductive detectors, high responsivity and weak signal detection are required. Here, we present high responsivity phototransistors based on few-layer rhenium disulfide (ReS2). Depending on the back gate voltage, source drain bias and incident optical light intensity, the maximum attainable photoresponsivity can reach as high as 88,600 A W-1, which is a record value compared to other two-dimensional materials with similar device structures and two orders of magnitude higher than that of monolayer MoS2. Such high photoresponsivity is attributed to the increased light absorption as well as the gain enhancement due to the existence of trap states in the few-layer ReS2 flakes. It further enables the detection of weak signals, as successfully demonstrated with weak light sources including a lighter and limited fluorescent lighting. Our studies underscore ReS2 as a promising material for future sensitive optoelectronic applications., Comment: Accepted by Advanced Functional Materials; 25 pages, 4 figures, 2 supplementary figures

As the thinnest conductive and elastic material, graphene is expected to play a crucial role in post-Moore era. Besides applications on electronic devices, graphene has shown great potential for nano-electromechanical systems. While interlayer interactions play a key role in modifying the electronic structures of layered materials, no attention has been given to their impact on electromechanical properties. Here we report the positive piezoconductive effect observed in suspended bi- and multi-layer graphene. The effect is highly layer number dependent and shows the most pronounced response for tri-layer graphene. The effect, and its dependence on the layer number, can be understood as resulting from the strain-induced competition between interlayer coupling and intralayer transport, as confirmed by the numerical calculations based on the non-equilibrium Green's function method. Our results enrich the understanding of graphene and point to layer number as a powerful tool for tuning the electromechanical properties of graphene for future applications., Comment: Accepted by Nature Communications; 36 pages, 4 figures, 11 supplementary figures

Semiconducting two-dimensional (2D) transition metal dichalcogenides (TMDs) are emerging as top candidates for post-silicon electronics. While most of 2D TMDs exhibit isotropic behavior, lowering the lattice symmetry could induce anisotropic properties, which are both scientifically interesting and potentially useful. Here, we present atomically thin rhenium disulfide (ReS2) flakes with a unique distorted 1T structure, which exhibit in-plane anisotropic properties. We fabricated mono- and few-layer ReS2 field effect transistors (FETs), which exhibit competitive performance with large current on/off ratios (~107) and low subthreshold swings (100 mV dec-1). The observed anisotropic ratio along two principle axes reaches 3.1, which is the highest among all known 2D semiconducting materials. Furthermore, we successfully demonstrated an integrated digital inverter with good performance by utilizing two ReS2 anisotropic FETs, suggesting the promising implementation of large-scale 2D logic circuits. Our results underscore the unique properties of 2D semiconducting materials with low crystal symmetry for future electronic applications., Comment: accepted by Nature Communications; 23 pages, 4 figures

Lattice structure and symmetry of two-dimensional (2D) layered materials are of key importance to their fundamental mechanical, thermal, electronic and optical properties. Raman spectroscopy, as a convenient and nondestructive tool, however has its limitations on identifying all symmetry allowing Raman modes and determining the corresponding crystal structure of 2D layered materials with high symmetry like graphene and MoS2. Due to lower structural symmetry and extraordinary weak interlayer coupling of ReS2, we successfully identified all 18 first-order Raman active modes for bulk and monolayer ReS2. Without van der Waals (vdW) correction, our local density approximation (LDA) calculations successfully reproduce all the Raman modes. Our calculations also suggest no surface reconstruction effect and the absence of low frequency rigid-layer Raman modes below 100 cm-1. Combining with Raman and LDA thus provides a general approach for studying the vibrational and structural properties of 2D layered materials with lower symmetry., Comment: accepted by Physical Review B; 23 pages, 3 figures, 4 tables

Two-dimensional atomic crystals are extensively studied in recent years due to their exciting physics and device applications. However, a molecular counterpart, with scalable processability and competitive device performance, is still challenging. Here, we demonstrate that high-quality few-layer dioctylbenzothienobenzothiophene molecular crystals can be grown on graphene or boron nitride substrate via van der Waals epitaxy, with precisely controlled thickness down to monolayer, large-area single crystal, low process temperature and patterning capability. The crystalline layers are atomically smooth and effectively decoupled from the substrate due to weak van der Waals interactions, affording a pristine interface for high-performance organic transistors. As a result, monolayer dioctylbenzothienobenzothiophene molecular crystal field-effect transistors on boron nitride show record-high carrier mobility up to 10cm2V-1s-1 and aggressively scaled saturation voltage around 1V. Our work unveils an exciting new class of two-dimensional molecular materials for electronic and optoelectronic applications., Comment: 68 pages, 4 figures

We report on a strong photoluminescence (PL) enhancement of monolayer MoS2 through defect engineering and oxygen bonding. Micro- PL and Raman images clearly reveal that the PL enhancement occurs at cracks/defects formed during high temperature vacuum annealing. The PL enhancement at crack/defect sites could be as high as thousands of times after considering the laser spot size. The main reasons of such huge PL enhancement include: (1) the oxygen chemical adsorption induced heavy p doping and the conversion from trion to exciton; (2) the suppression of non-radiative recombination of excitons at defect sites as verified by low temperature PL measurements. First principle calculations reveal a strong binding energy of ~2.395 eV for oxygen molecule adsorbed on an S vacancy of MoS2. The chemical adsorbed oxygen also provides a much more effective charge transfer (0.997 electrons per O2) compared to physical adsorbed oxygen on ideal MoS2 surface. We also demonstrate that the defect engineering and oxygen bonding could be easily realized by oxygen plasma irradiation. X-ray photoelectron spectroscopy further confirms the formation of Mo-O bonding. Our results provide a new route for modulating the optical properties of two dimensional semiconductors. The strong and stable PL from defects sites of MoS2 may have promising applications in optoelectronic devices., Comment: 23 pages, 9 figures, to appear in ACS Nano

We report on the observation of the two-dimensional weak antilocalization in (Cu0.1Bi0.9)2Te3.06 crystals relying on measurements of the magnetoresistance in a tilted field. The dephasing analysis and scanning tunneling spectroscopy corroborate the transport of the topological surface states (SS). The SSs contribute 3.3% conductance in 30{\mu}m-thick material and become dominant in the 100nm-thick flakes. Such optimized topological SS transport is achieved by an intense aging process, when the bulk conductance is suppressed by four orders of magnitude in the long period. Scanning tunneling microscopy reveals that Cu atoms are initially inside the quintuple layers and migrate to the layer gaps to form Cu clusters during the aging. In combination with first-principles calculations, an atomic tunneling-clustering procedure across a diffusion barrier of 0.57eV is proposed.