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The numerous grainboundaries solid electrolyte interface, whether naturally occurring or artificially designed, leads to non-uniform Li metal deposition and consequently results in poor full-battery performance. Herein, a lithium-ion selective transport layer is reported to achieve a highly efficient and dendrite-free lithium metal anode. The layer-by-layer assembled protonated carbon nitride nanosheets present uniform macroscopical structure without grainboundaries. The carbon nitride with ordered pores in basal plane provides high-speed lithium-ion transport channels with low tortuosity. Consequently, the assembled 324 Wh kg−1 pouch cell exhibits 300 stable cycles with a capacity retention of 90.0% and an average Coulombic efficiency up to 99.7%. The ultra-dense Li metal anode makes current collector-free anode possible, achieving high energy density and long cycle life of a 7 Ah cell (506 Wh kg−1, 160 cycles). Thus, it is proved that a macroscopically uniform interface layer with lithium-ion conductive channels could achieve Li metal battery with promising application potential. Here, authors report a macroscopical grain boundary-free interface layer with microscopic Li + -selective conductive channels enables the ultra-dense Li metal deposition, resulting in a high energy density (506 Wh kg−1) and long cycle life (160 cycles) pouch cell performance. [ABSTRACT FROM AUTHOR]

Two-dimensional (2D) layered materials have been studied in depth during the past two decades due to their unique structure and properties. Transition metal (TM) intercalation of layered materials have been proven as an effective way to introduce new physical properties, such as tunable 2D magnetism, but the direct growth of atomically thin heteroatoms-intercalated layered materials remains untapped. Herein, we directly synthesize various ultrathin heteroatoms-intercalated 2D layered materials (UHI-2DMs) through flux-assisted growth (FAG) approach. Eight UHI-2DMs (V1/3NbS2, Cr1/3NbS2, Mn1/3NbS2, Fe1/3NbS2, Co1/3NbS2, Co1/3NbSe2, Fe1/3TaS2, Fe1/4TaS2) were successfully synthesized. Their thickness can be reduced to the thinnest limit (bilayer 2D material with monolayer intercalated TM), and magnetic ordering can be induced in the synthesized structures. Interestingly, due to the possible anisotropy-stabilized long-range ferromagnetism in Fe1/3TaS2 with weak interlayer coupling, the layer-independent magnetic ordering temperature of Fe1/3TaS2 was revealed by magneto-transport properties. This work establishes a general method for direct synthesis of heteroatom-intercalated ultrathin 2D materials with tunable chemical and physical properties. The intercalation of heteroatoms has been demonstrated to be an effective approach to introduce new physical properties in 2D layered materials (2DMs). Here, the authors report a flux-assisted growth method to synthesize various ultrathin heteroatoms-intercalated 2DMs, showing evidence of anisotropy-stabilized long-range ferromagnetism in Fe1/3TaS2. [ABSTRACT FROM AUTHOR]

Domain boundaries have been intensively investigated in bulk ferroelectric materials and two-dimensional materials. Many methods such as electrical, mechanical and optical approaches have been utilized to probe and manipulate domain boundaries. So far most research focuses on the initial and final states of domain boundaries before and after manipulation, while the microscopic understanding of the evolution of domain boundaries remains elusive. In this paper, we report controllable manipulation of the domain boundaries in two-dimensional ferroelectric In2Se3 with atomic precision using scanning tunneling microscopy. We show that the movements of the domain boundaries can be driven by the electric field from a scanning tunneling microscope tip and proceed by the collective shifting of atoms at the domain boundaries. Our density functional theory calculations reveal the energy path and evolution of the domain boundary movement. The results provide deep insight into domain boundaries in two-dimensional ferroelectric materials and will inspire inventive applications of these materials. Here, the authors realize controllable manipulation of polar domain boundaries in a two-dimensional ferroelectric material In2Se3. It reveals the origin of distinct behaviors for different domain boundaries in combination with density functional theory calculations. [ABSTRACT FROM AUTHOR]

Developing efficient (co-)catalysts with optimized interfacial mass and charge transport properties is essential for enhanced oxygen evolution reaction (OER) via electrochemical water splitting. Here we report one-atom-thick hexagonal boron nitride (hBN) as an attractive co-catalyst with enhanced OER efficiency. Various electrocatalytic electrodes are encapsulated with centimeter-sized hBN films which are dense and impermeable so that only the hBN surfaces are directly exposed to reactive species. For example, hBN covered Ni-Fe (oxy)hydroxide anodes show an ultralow Tafel slope of ~30 mV dec−1 with improved reaction current by about 10 times, reaching ~2000 mA cm−2 (at an overpotential of ~490 mV) for over 150 h. The mass activity of hBN co-catalyst is found exceeding that of commercialized catalysts by up to five orders of magnitude. Using isotope experiments and simulations, we attribute the results to the adsorption of oxygen-containing intermediates at the insulating co-catalyst, where localized electrons facilitate the deprotonation processes at electrodes. Little impedance to electron transfer is observed from hBN film encapsulation due to its ultimate thickness. Therefore, our work also offers insights into mechanisms of interfacial reactions at the very first atomic layer of electrodes. Developing efficient (co-)catalysts with optimized interfacial mass and charge transport properties is essential for enhanced electrochemical oxygen evolution reaction. Here, the authors report one-atom-thick hexagonal boron nitride co-catalyst with enhanced oxygen evolution reaction efficiency. [ABSTRACT FROM AUTHOR]

Single-atom catalysts provide efficiently utilized active sites to improve catalytic activities while improving the stability and enhancing the activities to the level of their bulk metallic counterparts are grand challenges. Herein, we demonstrate a family of single-atom catalysts with different interaction types by confining metal single atoms into the van der Waals gap of two-dimensional SnS2. The relatively weak bonding between the noble metal single atoms and the host endows the single atoms with more intrinsic catalytic activity compared to the ones with strong chemical bonding, while the protection offered by the layered material leads to ultrahigh stability compared to the physically adsorbed single-atom catalysts on the surface. Specifically, the trace Pt-intercalated SnS2 catalyst has superior long-term durability and comparable performance to that of commercial 10 wt% Pt/C catalyst in hydrogen evolution reaction. This work opens an avenue to explore high-performance intercalated single-atom electrocatalysts within various two-dimensional materials. A family of single-atom catalysts synthesized by intercalating metal single atoms into the van der Waals gap of two-dimensional SnS2 is reported. The materials are applied as hydrogen evolving catalysts with good durability and overpotential. [ABSTRACT FROM AUTHOR]

Monolayer (1L) transition metal dichalcogenides (TMDCs) have been attracting tremendous interest in recent years as promising candidate materials in atomic-scale optoelectronic devices due to their direct band gaps (1.5–2.2 eV) and strong light—matter interactions. Unfortunately, their practical applications are limited by low visible light absorption stemming from atomic thickness and negligible infrared response. Here, we report the triangular Sb2O3 microresonators in wide thickness and lateral size distributions grown on 1L TMDCs and their created significant broadband enhancement of light adsorption and photoresponse in 1L WSe2 crystal via coexisting Fabry—Perot and whispering gallery type resonances. As an example of demonstration, 1L WSe2 crystal coupled to Sb2O3 microresonators with widely distributed sizes exhibits the enhanced visible light absorption by up to 5 folds and the simultaneously extended near infrared (NIR) one of more than 50%. For application of 1L WSe2 in photodetection, incorporation of Sb2O3 microresonators leads to significantly enhanced visible light responsivity by ∼ 104 order and expanded NIR one of more than 400 mA·W−1. Similar results have been observed in the other 1L W(Mo) dichalcogenides coupled to Sb2O3 microresonators. This work provides a new route for development of the high-performance monolayer TMDCs-based optoelectronic devices. [ABSTRACT FROM AUTHOR]

Electrochemical reduction of CO2 to multi-carbon fuels and chemical feedstocks is an appealing approach to mitigate excessive CO2 emissions. However, the reported catalysts always show either a low Faradaic efficiency of the C2+ product or poor long-term stability. Herein, we report a facile and scalable anodic corrosion method to synthesize oxygen-rich ultrathin CuO nanoplate arrays, which form Cu/Cu2O heterogeneous interfaces through self-evolution during electrocatalysis. The catalyst exhibits a high C2H4 Faradaic efficiency of 84.5%, stable electrolysis for ~55 h in a flow cell using a neutral KCl electrolyte, and a full-cell ethylene energy efficiency of 27.6% at 200 mA cm−2 in a membrane electrode assembly electrolyzer. Mechanism analyses reveal that the stable nanostructures, stable Cu/Cu2O interfaces, and enhanced adsorption of the *OCCOH intermediate preserve selective and prolonged C2H4 production. The robust and scalable produced catalyst coupled with mild electrolytic conditions facilitates the practical application of electrochemical CO2 reduction. Oxide-derived copper has been extensively studied as catalysts for CO2 electroreduction but its catalytic stability and selectivity still need to be improved. Here, the authors report ultrathin CuO nanoplate arrays for CO2 reduction with high ethylene selectivity and enhanced long-term stability. [ABSTRACT FROM AUTHOR]

Emerging two-dimensional (2D) layered materials have been attracting great attention as sensing materials for next-generation high-performance biological and chemical sensors. The sensor performance of 2D materials is strongly dependent on the structural defects as indispensable active sites for analyte adsorption. However, controllable defect engineering in 2D materials is still challenging. In the present work, we propose exploitation of controllably grown polycrystalline films of 2D layered materials with high-density grain boundaries (GBs) for design of ultra-sensitive ion sensors, where abundant structural defects on GBs act as favorable active sites for ion adsorption. As a proof-of-concept, our fabricated surface plasmon resonance sensors with GB-rich polycrystalline monolayer WS2 films have exhibited high selectivity and superior attomolar-level sensitivity in Hg2+ detection owing to high-density GBs. This work provides a promising avenue for design of ultra-sensitive sensors based on GB-rich 2D layered materials. Here, the authors report the controlled growth of polycrystalline WS2 films with high density of grain boundaries to realize surface plasmon Hg2+ ion sensors exhibiting attomolar sensitivity and enhanced selectivity. [ABSTRACT FROM AUTHOR]

The development of magnetic two-dimensional (2D) materials in its infancy has generated an enormous amount of attention as it offers an ideal platform for the exploration of magnetic properties down to the 2D limit, paving the way for spintronic devices. Due to the nonnegligible advantages including time efficiency and simplified process, the facile bottom-up chemical vapor deposition (CVD) is regarded as a robust method to fabricate ultrathin magnetic nanosheets. Recently, some ultrathin magnets possessing fascinating properties have been successfully synthesized via CVD. Here, the recent researches toward magnetic 2D materials grown by CVD are systematically summarized with special emphasis on the fabrication methods. Then, heteroatoms doping and phase transition induced in CVD growth to bring or tune the magnetic properties in 2D materials are discussed. Characterizations and applications of these magnetic materials are also discussed and reviewed. Finally, some perspectives in need of urgent attention regarding the development of CVD-grown magnetic 2D materials are proposed. [ABSTRACT FROM AUTHOR]

Exploration of structure-property relationships as a function of dopant concentration is commonly based on mean field theories for solid solutions. However, such theories that work well for semiconductors tend to fail in materials with strong correlations, either in electronic behavior or chemical segregation. In these cases, the details of atomic arrangements are generally not explored and analyzed. The knowledge of the generative physics and chemistry of the material can obviate this problem, since defect configuration libraries as stochastic representation of atomic level structures can be generated, or parameters of mesoscopic thermodynamic models can be derived. To obtain such information for improved predictions, we use data from atomically resolved microscopic images that visualize complex structural correlations within the system and translate them into statistical mechanical models of structure formation. Given the significant uncertainties about the microscopic aspects of the material's processing history along with the limited number of available images, we combine model optimization techniques with the principles of statistical hypothesis testing. We demonstrate the approach on data from a series of atomically-resolved scanning transmission electron microscopy images of MoxRe1-xS2 at varying ratios of Mo/Re stoichiometries, for which we propose an effective interaction model that is then used to generate atomic configurations and make testable predictions at a range of concentrations and formation temperatures. [ABSTRACT FROM AUTHOR]

The discovery of ferromagnetic two-dimensional van der Waals materials has opened up opportunities to explore intriguing physics and to develop innovative spintronic devices. However, controllable synthesis of these 2D ferromagnets and enhancing their stability under ambient conditions remain challenging. Here, we report chemical vapor deposition growth of air-stable 2D metallic 1T-CrTe2 ultrathin crystals with controlled thickness. Their long-range ferromagnetic ordering is confirmed by a robust anomalous Hall effect, which has seldom been observed in other layered 2D materials grown by chemical vapor deposition. With reducing the thickness of 1T-CrTe2 from tens of nanometers to several nanometers, the easy axis changes from in-plane to out-of-plane. Monotonic increase of Curie temperature with the thickness decreasing from ~130.0 to ~7.6 nm is observed. Theoretical calculations indicate that the weakening of the Coulomb screening in the two-dimensional limit plays a crucial role in the change of magnetic properties. Here, the authors report chemical vapor deposition growth of metallic 1T-CrTe2 ultrathin crystals with controlled thickness and long-range ferromagnetic ordering, and observe a monotonic increase of the Curie temperature with decreasing thickness. [ABSTRACT FROM AUTHOR]

Valley pseudospin in transition metal dichalcogenides monolayers intrinsically provides additional possibility to control valley carriers, raising a great impact on valleytronics in following years. The spin-valley locking directly contributes to optical selection rules which allow for valley-dependent addressability of excitons by helical optical pumping. As a binary photonic addressable route, manipulation of valley polarization states is indispensable while effective control methods at deep-subwavelength scale are still limited. Here, we report the excitation and control of valley polarization in h-BN/WSe2/h-BN and Au nanoantenna hybrid structure by electron beam. Near-field circularly polarized dipole modes can be excited via precise stimulation and generate the valley polarized cathodoluminescence via near-field interaction. Effective manipulation of valley polarization degree can be realized by variation of excitation position. This report provides a near-field excitation methodology of valley polarization, which offers exciting opportunities for deep-subwavelength valleytronics investigation, optoelectronic circuits integration and future quantum information technologies. Here, the authors generate near-field circularly polarized dipole modes in a hBN/WSe2/hBN–Au nanoantenna hybrid structure by electron beam excitation, and show nanoscale control of the valley polarization through spatial variation of the electron beam excitation position. [ABSTRACT FROM AUTHOR]

Although two-dimensional (2D) atomic layers, such as transition-metal chalcogenides, have been widely synthesized using techniques such as exfoliation1–3 and vapour-phase growth4,5, it is still challenging to obtain phase-controlled 2D structures6–8. Here we demonstrate an effective synthesis strategy via the progressive transformation of non-van der Waals (non-vdW) solids to 2D vdW transition-metal chalcogenide layers with identified 2H (trigonal prismatic)/1T (octahedral) phases. The transformation, achieved by exposing non-vdW solids to chalcogen vapours, can be controlled using the enthalpies and vapour pressures of the reaction products. Heteroatom-substituted (such as yttrium and phosphorus) transition-metal chalcogenides can also be synthesized in this way, thus enabling a generic synthesis approach to engineering phase-selected 2D transition-metal chalcogenide structures with good stability at high temperatures (up to 1,373 kelvin) and achieving high-throughput production of monolayers. We anticipate that these 2D transition-metal chalcogenides will have broad applications for electronics, catalysis and energy storage. A synthetic approach is described, for efficiently converting non-van der Waals solids into two-dimensional van der Waals transition-metal chalcogenide layers with specific phases, enabling the high-throughput production of monolayers. [ABSTRACT FROM AUTHOR]

Through the integration of a strongly coupled plasmonic nanoantenna array with a monolayer MoSe, spatial maps of the photoluminescence (PL) are acquired on- and off-resonance to exhibit the role of the lattice plasmon modes on the enhancement of the PL from the MoSe monolayer. The on-resonance excitation of the hybrid nanostructure at 785 nm reveals a significant PL enhancement of more than 25 (compared to the PL enhancement factor that a Fabry-Perot resonance provides), while the off-resonance excitation at 488 nm only results in an enhancement factor of five. Polarization-resolved optical reflection spectroscopy is also experimented to verify the role of the coupled nanoantenna array on the PL enhancement. Full-wave numerical simulations of the complete structure are also performed to support the observed experimental results. These findings enrich our knowledge regarding the light interaction with 2D materials mediated by plasmonic nanostructures and pave the way for the design of a new class of hybrid 2D material plasmonic devices that utilize enhanced light-matter interaction. [ABSTRACT FROM AUTHOR]

Two-dimensional layers of metal dichalcogenides have attracted much attention because of their ultrathin thickness and potential applications in electronics and optoelectronics. Monolayer SnS, with a band gap of ~2.6 eV, has an octahedral lattice made of two atomic layers of sulfur and one atomic layer of tin. Till date, there have been limited reports on the growth of large-scale and high quality SnS atomic layers and the investigation of their properties as a semiconductor. Here, we report the chemical vapor deposition (CVD) growth of atomic-layer SnS with a large crystal size and uniformity. In addition, the number of layers can be changed from a monolayer to few layers and to bulk by changing the growth time. Scanning transmission electron microscopy was used to analyze the atomic structure and demonstrate the 2H stacking poly-type of different layers. The resultant SnS crystals is used as a photodetector with external quantum efficiency as high as 150%, suggesting promise for optoelectronic applications. [ABSTRACT FROM AUTHOR]

The fast growth of information technology has been sustained by continuous scaling down of the silicon-based metal-oxide field-effect transistor. However, such technology faces two major challenges to further scaling. First, the device electrostatics (the ability of the transistor's gate electrode to control its channel potential) are degraded when the channel length is decreased, using conventional bulk materials such as silicon as the channel. Recently, two-dimensional semiconducting materials have emerged as promising candidates to replace silicon, as they can maintain excellent device electrostatics even at much reduced channel lengths. The second, more severe, challenge is that the supply voltage can no longer be scaled down by the same factor as the transistor dimensions because of the fundamental thermionic limitation of the steepness of turn-on characteristics, or subthreshold swing. To enable scaling to continue without a power penalty, a different transistor mechanism is required to obtain subthermionic subthreshold swing, such as band-to-band tunnelling. Here we demonstrate band-to-band tunnel field-effect transistors (tunnel-FETs), based on a two-dimensional semiconductor, that exhibit steep turn-on; subthreshold swing is a minimum of 3.9 millivolts per decade and an average of 31.1 millivolts per decade for four decades of drain current at room temperature. By using highly doped germanium as the source and atomically thin molybdenum disulfide as the channel, a vertical heterostructure is built with excellent electrostatics, a strain-free heterointerface, a low tunnelling barrier, and a large tunnelling area. Our atomically thin and layered semiconducting-channel tunnel-FET (ATLAS-TFET) is the only planar architecture tunnel-FET to achieve subthermionic subthreshold swing over four decades of drain current, as recommended in ref. 17, and is also the only tunnel-FET (in any architecture) to achieve this at a low power-supply voltage of 0.1 volts. Our device is at present the thinnest-channel subthermionic transistor, and has the potential to open up new avenues for ultra-dense and low-power integrated circuits, as well as for ultra-sensitive biosensors and gas sensors. [ABSTRACT FROM AUTHOR]

Layer-by-layer stacking or lateral interfacing of atomic monolayers has opened up unprecedented opportunities to engineer two-dimensional heteromaterials. Fabrication of such artificial heterostructures with atomically clean and sharp interfaces, however, is challenging. Here, we report a one-step growth strategy for the creation of high-quality vertically stacked as well as in-plane interconnected heterostructures of WS2/MoS2 via control of the growth temperature. Vertically stacked bilayers with WS2 epitaxially grown on top of the MoS2 monolayer are formed with preferred stacking order at high temperature. A strong interlayer excitonic transition is observed due to the type II band alignment and to the clean interface of these bilayers. Vapour growth at low temperature, on the other hand, leads to lateral epitaxy of WS2 on MoS2 edges, creating seamless and atomically sharp in-plane heterostructures that generate strong localized photoluminescence enhancement and intrinsic p-n junctions. The fabrication of heterostructures from monolayers, using simple and scalable growth, paves the way for the creation of unprecedented two-dimensional materials with exciting properties. [ABSTRACT FROM AUTHOR]

Graphene and hexagonal boron nitride (h-BN) have similar crystal structures with a lattice constant difference of only 2%. However, graphene is a zero-bandgap semiconductor with remarkably high carrier mobility at room temperature, whereas an atomically thin layer of h-BN is a dielectric with a wide bandgap of ?5.9 eV. Accordingly, if precise two-dimensional domains of graphene and h-BN can be seamlessly stitched together, hybrid atomic layers with interesting electronic applications could be created. Here, we show that planar graphene/h-BN heterostructures can be formed by growing graphene in lithographically patterned h-BN atomic layers. Our approach can create periodic arrangements of domains with size ranging from tens of nanometres to millimetres. The resulting graphene/h-BN atomic layers can be peeled off the growth substrate and transferred to various platforms including flexible substrates. We also show that the technique can be used to fabricate two-dimensional devices, such as a split closed-loop resonator that works as a bandpass filter. [ABSTRACT FROM AUTHOR]