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For the first time, 2D ultrathin Te flakes (5 nm) are successfully realized by hydrogen‐assisted chemical vapor deposition method. The density functional theory calculations and experiments confirm that two volatile intermediates increase the vapor pressure of the source and promote the reaction. Impressively, the Te‐flake‐based phototransistor shows giant gate‐dependent photoresponse.

Abstract

Tellurium (Te), as an elementary material, has attracted intense attention due to its potentially novel properties. However, it is still a great challenge to realize high‐quality 2D Te due to its helical chain structure. Here, ultrathin Te flakes (5 nm) are synthesized via hydrogen‐assisted chemical vapor deposition method. The density functional theory calculations and experiments confirm the growth mechanism, which can be ascribed to the formation of volatile intermediates increasing vapor pressure of the source and promoting the reaction. Impressively, the Te flake‐based transistor shows high on/off ratio ≈10⁴, ultralow off‐state current ≈8 × 10⁻¹³ A, as well as a negligible hysteresis due to reducing thermally activated defects at 80 K. Moreover, Te‐flake‐based phototransistor demonstrates giant gate‐dependent photoresponse: when gate voltage varies from −70 to 70 V, I _on/I _off is increased by ≈40‐fold. The hydrogen‐assisted strategy may provide a new approach for synthesizing other high quality 2D elementary materials.

The diverse properties of van der Waals heterostructures open unprecedented opportunities for various types of device applications inaccessible in conventional heterostructure materials. Research progress of vertical heterostructure device applications in vertical transistors, infrared photodetectors, and spintronic devices is reviewed, together with a discussion on the challenges and opportunities in the future development of multifunctional devices.

Abstract

The discovery of two‐dimensional (2D) materials with unique electronic, superior optoelectronic, or intrinsic magnetic order has triggered worldwide interest in the fields of material science, condensed matter physics, and device physics. Vertically stacking 2D materials with distinct electronic and optical as well as magnetic properties enables the creation of a large variety of van der Waals heterostructures. The diverse properties of the vertical heterostructures open unprecedented opportunities for various kinds of device applications, e.g., vertical field‐effect transistors, ultrasensitive infrared photodetectors, spin‐filtering devices, and so on, which are inaccessible in conventional material heterostructures. Here, the current status of vertical heterostructure device applications in vertical transistors, infrared photodetectors, and spintronic memory/transistors is reviewed. The relevant challenges for achieving high‐performance devices are presented. An outlook into the future development of vertical heterostructure devices with integrated electronic and optoelectronic as well as spintronic functionalities is also provided.

Elemental 2D materials are some of the more exciting nanomaterials of interest due to their unique and tailorable properties. Recent progress in these exciting materials relative to their potential impact in applications including electronics, optoelectronics, and energy systems is presented.

Abstract

As elemental main group materials (i.e., silicon and germanium) have dominated the field of modern electronics, their monolayer 2D analogues have shown great promise for next‐generation electronic materials as well as potential game‐changing properties for optoelectronics, energy, and beyond. These atomically thin materials composed of single atomic variants of group III through group VI elements on the periodic table have already demonstrated exciting properties such as near‐room‐temperature topological insulation in bismuthene, extremely high electron mobilities in phosphorene and silicone, and substantial Li‐ion storage capability in borophene. Isolation of these materials within the postgraphene era began with silicene in 2010 and quickly progressed to the experimental identification or theoretical prediction of 15 of the 18 main group elements existing as solids at standard pressure and temperatures. This review first focuses on the significance of defects/functionalization, discussion of different allotropes, and overarching structure–property relationships of 2D main group elemental materials. Then, a complete review of emerging applications in electronics, sensing, spintronics, plasmonics, photodetectors, ultrafast lasers, batteries, supercapacitors, and thermoelectrics is presented by application type, including detailed descriptions of how the material properties may be tailored toward each specific application.

Nature Reviews Materials, Published online: 24 October 2019; doi:10.1038/s41578-019-0146-8

Lead-based organic-inorganic hybrid perovskite (OIHP) solar cells can attain efficiencies over 20%. However, the impact of ion mobility and/or organic depletion, structural changes, and segregation under operating conditions urge for decisive and more accurate investigations. Hence, the development of analytical tools for accessing the grain-to-grain OIHP chemistry is of great relevance. Here, we used synchrotron infrared nanospectroscopy (nano-FTIR) to map individual nanograins in OIHP films. Our results reveal a spatial heterogeneity of the vibrational activity associated to the nanoscale chemical diversity of isolated grains. It was possible to map the chemistry of individual grains in CsFAMA [Cs_0.05FA_0.79MA_0.16Pb(I_0.83Br_0.17)₃] and FAMA [FA_0.83MA_0.17Pb(I_0.83Br_0.17)₃] films, with information on their local composition. Nanograins with stronger nano-FTIR activity in CsFAMA and FAMA films can be assigned to PbI₂ and hexagonal polytype phases, respectively. The analysis herein can be extended to any OIHP films where organic cation depletion/accumulation can be used as a chemical label to study composition.

Integration of dissimilar two-dimensional (2D) materials is essential for nanoelectronic applications. Compared to vertical stacking, covalent lateral stitching requires bottom-up synthesis, resulting in rare realizations of 2D lateral heterostructures. Because of its polymorphism and diverse bonding geometries, borophene is a promising candidate for 2D heterostructures, although suitable synthesis conditions have not yet been demonstrated. Here, we report lateral and vertical integration of borophene with graphene. Topographic and spatially resolved spectroscopic measurements reveal nearly atomically sharp lateral interfaces despite imperfect crystallographic lattice and symmetry matching. In addition, boron intercalation under graphene results in rotationally commensurate vertical heterostructures. The rich bonding configurations of boron suggest that borophene can be integrated into a diverse range of 2D heterostructures.

Monitoring and controlling the neutral and charged excitons (trions) in two-dimensional (2D) materials are essential for the development of high-performance devices. However, nanoscale control is challenging because of diffraction-limited spatial resolution of conventional far-field techniques. Here, we extend the classical tip-enhanced photoluminescence based on tip-substrate nanocavity to quantum regime and demonstrate controlled nano-optical imaging, namely, tip-enhanced quantum plasmonics. In addition to improving the spatial resolution, we use the scanning probe to control the optoelectronic response of monolayer WS₂ by varying the neutral/charged exciton ratio via charge tunneling in Au-Ag picocavity. We observe trion "hot spots" generated by varying the picometer-scale probe-sample distance and show the effects of weak and strong coupling, which depend on the spatial location. Our experimental results are in agreement with simulations and open an unprecedented view of a new range of quantum plasmonic phenomena with 2D materials that will help to design new quantum optoelectronic devices.

Ceramic materials have been widely used for structural applications. However, most ceramics have rather limited plasticity at low temperatures and fracture well before the onset of plastic yielding. The brittle nature of ceramics arises from the lack of dislocation activity and the need for high stress to nucleate dislocations. Here, we have investigated the deformability of TiO₂ prepared by a flash-sintering technique. Our in situ studies show that the flash-sintered TiO₂ can be compressed to ~10% strain under room temperature without noticeable crack formation. The room temperature plasticity in flash-sintered TiO₂ is attributed to the formation of nanoscale stacking faults and nanotwins, which may be assisted by the high-density preexisting defects and oxygen vacancies introduced by the flash-sintering process. Distinct deformation behaviors have been observed in flash-sintered TiO₂ deformed at different testing temperatures, ranging from room temperature to 600°C. Potential mechanisms that may render ductile ceramic materials are discussed.

The design of single-molecule photoswitchable emitters was the first milestone toward the advent of single-molecule localization microscopy, setting a new paradigm in the field of optical imaging. Several photoswitchable emitters have been developed, but they all fluoresce in the visible or far-red ranges, missing the desirable near-infrared window where biological tissues are most transparent. Moreover, photocontrol of individual emitters in the near-infrared would be highly desirable for elementary optical molecular switches or information storage elements since most communication data transfer protocols are established in this spectral range. Here, we introduce a type of hybrid nanomaterials consisting of single-wall carbon nanotubes covalently functionalized with photoswitching molecules that are used to control the intrinsic luminescence of the single nanotubes in the near-infrared (beyond 1 μm). Through the control of photoswitching, we demonstrate super-localization imaging of nanotubes unresolved by diffraction-limited microscopy.

Two-dimensional boron, borophene, was realized in recent experiments but still lacks an adequate growth theory for guiding its controlled synthesis. Combining ab initio calculations and experimental characterization, we study edges and growth kinetics of borophene on Ag(111). In equilibrium, the borophene edges are distinctly reconstructed with exceptionally low energies, in contrast to those of other two-dimensional materials. Away from equilibrium, sequential docking of boron feeding species to the reconstructed edges tends to extend the given lattice out of numerous polymorphic structures. Furthermore, each edge can grow via multiple energy pathways of atomic row assembly due to variable boron-boron coordination. These pathways reveal different degrees of anisotropic growth kinetics, shaping borophene into diverse elongated hexagonal islands in agreement with experimental observations in terms of morphology as well as edge orientation and periodicity. These results further suggest that ultrathin borophene ribbons can be grown at low temperature and low boron chemical potential.

The presence and configurations of defects are primary components determining materials functionality. Their population and distribution are often nonergodic and dependent on synthesis history, and therefore rarely amenable to direct theoretical prediction. Here, dynamic electron beam–induced transformations in Si deposited on a graphene monolayer are used to create libraries of possible Si and carbon vacancy defects. Deep learning networks are developed for automated image analysis and recognition of the defects, creating a library of (meta) stable defect configurations. Density functional theory is used to estimate atomically resolved scanning tunneling microscopy (STM) signatures of the classified defects from the created library, allowing identification of several defect types across imaging platforms. This approach allows automatic creation of defect libraries in solids, exploring the metastable configurations always present in real materials, and correlative studies with other atomically resolved techniques, providing comprehensive insight into defect functionalities.

The emergence of flat bands and correlated behaviors in "magic angle" twisted bilayer graphene (tBLG) has sparked tremendous interest, though its many aspects are under intense debate. Here we report observation of both superconductivity and the Mott-like insulating state in a tBLG device with a twist angle of ~0.93°, which is smaller than the magic angle by 15%. At an electron concentration of ±5 electrons/moiré unit cell, we observe a narrow resistance peak with an activation energy gap ~0.1 meV. This indicates additional correlated insulating state, and is consistent with theory predicting a high-energy flat band. At doping of ±12 electrons/moiré unit cell we observe resistance peaks arising from the Dirac points in the spectrum. Our results reveal that the "magic" range of tBLG is in fact larger than what is previously expected, and provide a wealth of new information to help decipher the strongly correlated phenomena observed in tBLG.