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Monolayer WSe2 exhibits luminescence arising from various types of exciton complexes due to strong many-body effects. Here, we demonstrate selective electrical excitation of positive and negative trions in van der Waals metal-insulator-semiconductor (MIS) heterostructure consisting of few-layer graphene (FLG), hexagonal boron nitride (hBN), and monolayer WSe2. Intentional unbalanced injection of electrons and holes is achieved via field-emission tunneling and electrostatic accumulation. The device exhibits planar electroluminescence from either positive trion X+ or negative trion X- depending on the bias conditions. We show that hBN serves as a tunneling barrier material allowing selective injection of electron or holes into WSe2 from FLG layer. Our observation offers prospects for hot carrier injection, trion manipulation, and on-chip excitonic devices based on two-dimensional semiconductors.
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Non-volatile memories will play a decisive role in the next generation of digital technology. Flash memories are currently the key player in the field, yet they fail to meet the commercial demands of scalability and endurance. Resistive memory devices, and in particular memories based on low-cost, solution-processable and chemically tunable organic materials, are promising alternatives explored by the industry. However, to date, they have been lacking the performance and mechanistic understanding required for commercial translation. Here we report a resistive memory device based on a spin-coated active layer of a transition-metal complex, which shows high reproducibility (â¼350 devices), fast switching (≤30 ns), excellent endurance (â¼1012 cycles), stability (>106 s) and scalability (down to â¼60 nm2). In situ Raman and ultraviolet-visible spectroscopy alongside spectroelectrochemistry and quantum chemical calculations demonstrate that the redox state of the ligands determines the switching states of the device whereas the counterions control the hysteresis. This insight may accelerate the technological deployment of organic resistive memories.
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This corrects the article DOI: 10.1038/nmat5009.
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Two-dimensional (2D) transition metal dichalcogenides (TMDCs) possess interesting one-dimensional (1D) properties at its edges and inversion domain boundaries, where properties markedly different from the 2D basal plane, such as 1D metallicity and charge density waves, can be observed. Although 2D TMDCs crystals are widely grown by chemical vapor deposition (CVD), the fabrication of 1D TMDCs ribbons is challenging due to the difficulty to confine growth in only one dimension. Here we report the controlled growth of MoSe2 nanoribbons with an aspect ratio >100 by using prepatterned Se reconstructions on Au(100). Using scanning tunneling microscope and spectroscopy (STM/STS), the atomic and electronic structure of MoSe2 nanoribbons are studied. The ultranarrow ribbons show metallic behavior, while wider ribbons show a crossover from metallic to semiconducting behavior going from the edge to the center of the ribbon. The observed conductance modulations of the ultranarrow ribbons are attributed to 1D Moiré pattern. Remarkably, it shows a different periodicity compared with the 2D Moiré pattern in wider ribbons indicating that the 1D system is softened due to the high ratio of edge to basal plane bonds. Further, we demonstrated that the nanoribbons are stable against ambient conditions, which suggests that 1D TMDCs can be exploited for further applications.
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Topological insulators (TIs) are a new type of electronic materials in which the nontrivial insulating bulk band topology governs conducting boundary states with embedded spin-momentum locking. Such edge states are more robust in a two-dimensional (2D) TI against scattering by nonmagnetic impurities than in its three-dimensional (3D) variant, because in 2D the two helical edge states are protected from the only possible backscattering. This makes the 2D TI family a better candidate for coherent spin transport and related applications. While several 3D TIs are already synthesized experimentally, physical realization of 2D TI is so far limited to hybrid quantum wells with a tiny bandgap that does not survive temperatures above 10 K. Here, combining first-principles calculations and scanning tunneling microscopy/spectroscopy (STM/STS) experimental studies, we report nontrivial 2D TI phases in 2-monolayer (2-ML) and 4-ML Bi(110) films with large and tunable bandgaps determined by atomic buckling of Bi(110) films. The gapless edge states are experimentally detected within the insulating bulk gap at 77 K. The band topology of ultrathin Bi(110) films is sensitive to atomic buckling. Such buckling is sensitive to charge doping and could be controlled by choosing different substrates on which Bi(110) films are grown.
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Recent success in the growth of monolayer MoS2 via chemical vapor deposition (CVD) has opened up prospects for the implementation of these materials into thin film electronic and optoelectronic devices. Here, we investigate the electronic transport properties of individual crystallites of high quality CVD-grown monolayer MoS2. The devices show low temperature mobilities up to 500 cm(2) V(-1) s(-1) and a clear signature of metallic conduction at high doping densities. These characteristics are comparable to the electronic properties of the best mechanically exfoliated monolayers in literature, verifying the high electronic quality of the CVD-grown materials. We analyze the different scattering mechanisms and show that the short-range scattering plays a dominant role in the highly conducting regime at low temperatures. Additionally, the influence of optical phonons as a limiting factor is discussed.
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Graphene is one of the most promising candidates for integrated circuits due to its robustness against short-channel effects, inherent high carrier mobility and desired gapless nature for Ohmic contact, but it is difficult to achieve satisfactory on/off ratios even at the expense of its carrier mobility, limiting its device applications. Here, we present a strategy to realize high back-gate switching ratios in a graphene monolayer with well-maintained high mobility by forming a vertical heterostructure with a black phosphorus multi-layer. By local current annealing, strain is introduced within an established area of the graphene, which forms a reflective interface with the rest of the strain-free area and thus generates a robust off-state via local current depletion. Applying a positive back-gate voltage to the heterostructure can keep the black phosphorus insulating, while a negative back-gate voltage changes the black phosphorus to be conductive because of hole accumulation. Then, a parallel channel is activated within the strain-free graphene area by edge-contacted electrodes, thereby largely inheriting the intrinsic carrier mobility of graphene in the on-state. As a result, the device can provide an on/off voltage ratio of >103 as well as a mobility of â¼8000 cm2 V-1 s-1 at room temperature, meeting the low-power criterion suggested by the International Roadmap for Devices and Systems.
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Electrical field-induced charge modulation in graphene-based devices at the nanoscale with ultrahigh density carrier accumulation is important for various practical applications. In bilayer graphene (BLG), inversion symmetry can simply be broken by an external electric field. However, control over charge carrier density at the nanometer scale is a challenging task. We demonstrate local gating of BLG in the nanometer range by adsorption of AfFtnAA (which is a bioengineered ferritin, an iron-storing globular protein with ∅ = 12 nm). Low-temperature electrical transport measurements with field-effect transistors with these AfFtnAA/BLG surfaces show hysteresis with two Dirac peaks. One peak at a gate voltage V BG = 35 V is associated with pristine BLG, while the second peak at V BG = 5 V results from local doping by ferritin. This charge trapping at the biomolecular length scale offers a straightforward and non-destructive method to alter the local electronic structure of BLG.
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Transition metal dichalcogenides (TMDs) possess intrinsic spin-orbit interaction (SOI) with high potential to be exploited for various quantum phenomena. SOI allows the manipulation of spin degree of freedom by controlling the carrier's orbital motion via mechanical strain. Here, strain modulated spin dynamics in bilayer MoS2 field-effect transistors (FETs) fabricated on crested substrates are demonstrated. Weak antilocalization (WAL) is observed at moderate carrier concentrations, indicating additional spin relaxation path caused by strain fields arising from substrate crests. The spin lifetime is found to be inversely proportional to the momentum relaxation time, which follows the Dyakonov-Perel spin relaxation mechanism. Moreover, the spin-orbit splitting is obtained as 37.5 ± 1.4 meV, an order of magnitude larger than the theoretical prediction for monolayer MoS2 , suggesting the strain enhanced spin-lattice coupling. The work demonstrates strain engineering as a promising approach to manipulate spin degree of freedom toward new functional quantum devices.
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Understanding the mechanisms of charge transport (CT) across biomolecules in solid-state devices is imperative to realize biomolecular electronic devices in a predictive manner. Although it is well-accepted that biomolecule-electrode interactions play an essential role, it is often overlooked. This paper reveals the prominent role of graphene interfaces with Fe-storing proteins in the net CT across their tunnel junctions. Here, ferritin (AfFtn-AA) is adsorbed on the graphene by noncovalent amine-graphene interactions confirmed with Raman spectroscopy. In contrast to junctions with metal electrodes, graphene has a vanishing density of states toward its intrinsic Fermi level ("Dirac point"), which increases away from the Fermi level. Therefore, the amount of charge carriers is highly sensitive to temperature and electrostatic charging (induced doping), as deduced from a detailed analysis of CT as a function of temperature and iron loading. Remarkably, the temperature dependence can be fully explained within the coherent tunneling regime due to excitation of hot carriers. Graphene is not only demonstrated as an alternative platform to study CT across biomolecular tunnel junctions, but it also opens rich possibilities in employing interface electrostatics in tuning CT behavior.
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Grafito , Aminas , Ferritinas , Grafito/química , Hierro , TemperaturaRESUMEN
A nanometer-sized superconducting quantum interference device (nanoSQUID) is fabricated on the apex of a sharp quartz tip and integrated into a scanning SQUID microscope. A simple self-aligned fabrication method results in nanoSQUIDs with diameters down to 100 nm with no lithographic processing. An aluminum nanoSQUID with an effective area of 0.034 microm2 displays flux sensitivity of 1.8 x 10(-6) Phi(0)/Hz(1/2) and operates in fields as high as 0.6 T. With projected spin sensitivity of 65 micro(B)/Hz(1/2) and high bandwidth, the SQUID on a tip is a highly promising probe for nanoscale magnetic imaging and spectroscopy.
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Magnetismo/instrumentación , Microscopía de Sonda de Barrido/instrumentación , Nanotecnología/instrumentación , Transductores , Diseño de Equipo , Análisis de Falla de EquipoRESUMEN
Homoepitaxial growth of SrTiO3 thin films on 0.5 wt% niobium doped SrTiO3 (100) substrates with high structural perfection was developed using liquid-delivery spin metal-organic vapor phase epitaxy (MOVPE). Exploiting the advantage of adjusting the partial pressures of the individual constituents independently, we tuned the Sr/Ti ratio of the gas phase for realizing, stoichiometric, as well as Sr deficient layers. Quantitative energy dispersive X-ray spectroscopy in a scanning transmission electron microscope confirm Sr deficiency of up to 20% in nominally off-stoichiometrically grown films. Our MOVPE process allows to grow such layers in phase pure state and without extended defect formation. Indications for oxygen deficiency could not be identified. Sr deficient layers exhibit an increased permittivity of Ér = 202 and a larger vertical lattice parameter. Current-voltage characteristics (IVCs) of metal-oxide-semiconductor (Pt/SrTiO3/SrTiO3:Nb) structures reveal that Sr deficient SrTiO3 films show an intrinsic resistive switching with on-off ratios of three orders of magnitude at RT and seven orders of magnitude at 10 K. There is strong evidence that a large deviation from stoichiometry pronounces the resistive switching behavior. IVCs conducted at 10 K indicate a defect-based mechanism instead of mass transport by ion diffusion. This is supported by in-situ STEM investigations that show filaments to form at significant higher voltages than those were resistive switching is observed in our samples.
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Sign reversal of Berry curvature across two oppositely gated regions in bilayer graphene can give rise to counter-propagating 1D channels with opposite valley indices. Considering spin and sub-lattice degeneracy, there are four quantized conduction channels in each direction. Previous experimental work on gate-controlled valley polarizer achieved good contrast only in the presence of an external magnetic field. Yet, with increasing magnetic field the ungated regions of bilayer graphene will transit into the quantum Hall regime, limiting the applications of valley-polarized electrons. Here we present improved performance of a gate-controlled valley polarizer through optimized device geometry and stacking method. Electrical measurements show up to two orders of magnitude difference in conductance between the valley-polarized state and gapped states. The valley-polarized state displays conductance of nearly 4e2/h and produces contrast in a subsequent valley analyzer configuration. These results pave the way to further experiments on valley-polarized electrons in zero magnetic field.
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Electronic symmetry breaking by charge disproportionation results in multifaceted changes in the electronic, magnetic and optical properties of a material, triggering ferroelectricity, metal/insulator transition and colossal magnetoresistance. Yet, charge disproportionation lacks technological relevance because it occurs only under specific physical conditions of high or low temperature or high pressure. Here we demonstrate a voltage-triggered charge disproportionation in thin molecular films of a metal-organic complex occurring in ambient conditions. This provides a technologically relevant molecular route for simultaneous realization of a ternary memristor and a binary memcapacitor, scalable down to a device area of 60 nm2. Supported by mathematical modelling, our results establish that multiple memristive states can be functionally non-volatile, yet discrete-a combination perceived as theoretically prohibited. Our device could be used as a binary or ternary memristor, a binary memcapacitor or both concomitantly, and unlike the existing 'continuous state' memristors, its discrete states are optimal for high-density, ultra-low-energy digital computing.
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Ferromagnetism and superconductivity are two antagonistic phenomena since ferromagnetic exchange fields tend to destroy singlet Cooper pairs. Reconciliation of these two competing phases has been achieved in vertically stacked heterostructures where these two orders are confined in different layers. However, controllable integration of these two phases in one atomic layer is a longstanding challenge. Here, an interlayer-space-confined chemical design (ICCD) is reported for the synthesis of dilute single-atom-doped TaS2 molecular superlattice, whereby ferromagnetism is observed in the superconducting TaS2 layers. The intercalation of 2H-TaS2 crystal with bulky organic ammonium molecule expands its van der Waals gap for single-atom doping via co-intercalated cobalt ions, resulting in the formation of quasi-monolayer Co-doped TaS2 superlattices. Isolated Co atoms are decorated in the basal plane of the TaS2 via substituting the Ta atom or anchoring at a hollow site, wherein the orbital-selected p-d hybridization between Co and neighboring Ta and S atoms induces local magnetic moments with strong ferromagnetic coupling. This ICCD approach can be applied to various metal ions, enabling the synthesis of a series of crystal-size TaS2 molecular superlattices.
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Two-dimensional transition metal dichalcogenide (TMD) materials, albeit promising candidates for applications in electronics and optoelectronics1-3, are still limited by their low electrical mobility under ambient conditions. Efforts to improve device performance through a variety of routes, such as modification of contact metals4 and gate dielectrics5-9 or encapsulation in hexagonal boron nitride10, have yielded limited success at room temperature. Here, we report a large increase in the performance of TMD field-effect transistors operating under ambient conditions, achieved by engineering the substrate's surface morphology. For MoS2 transistors fabricated on crested substrates, we observed an almost two orders of magnitude increase in carrier mobility compared to standard devices, as well as very high saturation currents. The mechanical strain in TMDs has been predicted to boost carrier mobility11, and has been shown to influence the local bandgap12,13 and quantum emission properties14 of TMDs. With comprehensive investigation of different dielectric environments and morphologies, we demonstrate that the substrate's increased corrugation, with its resulting strain field, is the dominant factor driving performance enhancement. This strategy is universally valid for other semiconducting TMD materials, either p-doped or n-doped, opening them up for applications in heterogeneous integrated electronics.
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Copper oxides have been of considerable interest as electrocatalysts for CO2 reduction (CO2R) in aqueous electrolytes. However, their role as an active catalyst in reducing the required overpotential and improving the selectivity of reaction compared with that of polycrystalline copper remains controversial. Here, we introduce the use of selected-ion flow tube mass spectrometry, in concert with chronopotentiometry, in situ Raman spectroscopy, and computational modeling, to investigate CO2R on Cu2O nanoneedles, Cu2O nanocrystals, and Cu2O nanoparticles. We show experimentally that the selective formation of gaseous C2 products (i.e., ethylene) in CO2R is preceded by the reduction of the copper oxide (Cu2OR) surface to metallic copper. On the basis of density functional theory modeling, CO2R products are not formed as long as Cu2O is present at the surface because Cu2OR is kinetically and energetically more favorable than CO2R.
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Large polarons have been of significant recent technological interest as they screen and protect electrons from point-scattering centers. Anatase TiO2 is a model system for studying large polarons as they can be studied systematically over a wide range of temperature and carrier density. The electronic and magneto transport properties of reduced anatase TiO2 epitaxial thin films are analyzed considering various polaronic effects. Unexpectedly, with increasing carrier concentration, the mobility increases, which rarely happens in common metallic systems. We find that the screening of the electron-phonon (e-ph) coupling by excess carriers is necessary to explain this unusual dependence. We also find that the magnetoresistance could be decomposed into a linear and a quadratic component, separately characterizing the carrier transport and trapping as a function of temperature, respectively. The various transport behaviors could be organized into a single phase diagram, which clarifies the evolution of large polaron in this material.
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A configurable framework has been developed that can receive, modify, and export images in different picture archiving and communication system scenarios. The framework has three main components: a receiver for Digital Imaging and Communications in Medicine (DICOM) objects, a processing pipeline to apply one or more modifications to these objects, and one or more senders to send the processed objects to predefined addresses. The toolbox programming was implemented as an open source project in Java. The processing pipeline uses the concept of configurable plug-ins. One plug-in is user programmable by means of extensible stylesheet language files and allows conversion of DICOM objects to extensible markup language documents or other file types. Input and output channels are the DICOM Storage service, DICOM compact disks-read-only memory (CD-ROMs), and the local file system. The toolbox has been successfully applied to different clinical scenarios, including the correction of DICOM objects from non-Integrating the Healthcare Enterprise (IHE) conform modalities, pseudonaming of DICOM images, and use of the IHE Portable Data for Imaging profile with import and export of CD-ROMs. The toolbox has proved reliability in the clinical routine. Because of the open programming interfaces, the functionality can easily be adapted to future applications.