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Showing papers in "Nature Communications in 2015"


Journal ArticleDOI
TL;DR: The results of this combined computational and experimental study suggest that hybrid halide perovskites are mixed ionic–electronic conductors, a finding that has major implications for solar cell device architectures.
Abstract: Understanding the mechanism of ionic transport in organic–inorganic halide perovskites is crucial for the design of future solar cells. Here, Eames et al. undertake a combined experimental and computational study to elucidate the ion conducting species and help rationalize the unusual behaviour observed in these perovskite-based devices.

2,050 citations


Journal ArticleDOI
TL;DR: It is reported that the use of highly concentrated electrolytes composed of ether solvents and the lithium bis(fluorosulfonyl)imide salt enables the high-rate cycling of a lithium metal anode at high Coulombic efficiency (up to 99.1%) without dendrite growth.
Abstract: Lithium metal is an ideal battery anode. However, dendrite growth and limited Coulombic efficiency during cycling have prevented its practical application in rechargeable batteries. Herein, we report that the use of highly concentrated electrolytes composed of ether solvents and the lithium bis(fluorosulfonyl)imide salt enables the high-rate cycling of a lithium metal anode at high Coulombic efficiency (up to 99.1%) without dendrite growth. With 4 M lithium bis(fluorosulfonyl)imide in 1,2-dimethoxyethane as the electrolyte, a lithium|lithium cell can be cycled at 10 mA cm(-2) for more than 6,000 cycles, and a copper|lithium cell can be cycled at 4 mA cm(-2) for more than 1,000 cycles with an average Coulombic efficiency of 98.4%. These excellent performances can be attributed to the increased solvent coordination and increased availability of lithium ion concentration in the electrolyte. Further development of this electrolyte may enable practical applications for lithium metal anode in rechargeable batteries.

1,824 citations


Journal ArticleDOI
TL;DR: A strategy to entrap polysulfides in the cathode that relies on a chemical process, whereby a host--manganese dioxide nanosheets serve as the prototype--reacts with initially formed lithium polysolfides to form surface-bound intermediates, which are among the best reported to date.
Abstract: The lithium-sulfur battery is receiving intense interest because its theoretical energy density exceeds that of lithium-ion batteries at much lower cost, but practical applications are still hindered by capacity decay caused by the polysulfide shuttle. Here we report a strategy to entrap polysulfides in the cathode that relies on a chemical process, whereby a host--manganese dioxide nanosheets serve as the prototype--reacts with initially formed lithium polysulfides to form surface-bound intermediates. These function as a redox shuttle to catenate and bind 'higher' polysulfides, and convert them on reduction to insoluble lithium sulfide via disproportionation. The sulfur/manganese dioxide nanosheet composite with 75 wt% sulfur exhibits a reversible capacity of 1,300 mA h g(-1) at moderate rates and a fade rate over 2,000 cycles of 0.036%/cycle, among the best reported to date. We furthermore show that this mechanism extends to graphene oxide and suggest it can be employed more widely.

1,625 citations


Journal ArticleDOI
TL;DR: The as-prepared three-dimensional structured electrodes developed by electrodepositing amorphous mesoporous nickel–iron composite nanosheets directly onto macroporous nickel foam substrates is the most efficient oxygen evolution electrode in alkaline electrolytes reported to the best of the knowledge.
Abstract: Development of efficient and affordable oxygen evolution catalysts is essential for large-scale electrolytic water splitting. Here, the authors report mesoporous nickel–iron composite nanosheets loaded on macroporous nickel foam substrates, and evaluate their electrocatalytic oxygen evolution in basic media.

1,583 citations


Journal ArticleDOI
TL;DR: A rapid crystal growth process to obtain MAPbX3 single crystals, an order of magnitude faster than previous reports, and the grown crystals exhibit transport properties and trap densities comparable to the highest quality MAPb X3 reported to date.
Abstract: Single crystals of methylammonium lead trihalide perovskites (MAPbX3; MA=CH3NH3+, X=Br− or I−) have shown remarkably low trap density and charge transport properties; however, growth of such high-quality semiconductors is a time-consuming process. Here we present a rapid crystal growth process to obtain MAPbX3 single crystals, an order of magnitude faster than previous reports. The process is based on our observation of the substantial decrease of MAPbX3 solubility, in certain solvents, at elevated temperatures. The crystals can be both size- and shape-controlled by manipulating the different crystallization parameters. Despite the rapidity of the method, the grown crystals exhibit transport properties and trap densities comparable to the highest quality MAPbX3 reported to date. The phenomenon of inverse or retrograde solubility and its correlated inverse temperature crystallization strategy present a major step forward for advancing the field on perovskite crystallization. Hybrid perovskites are a promising class of materials for photovoltaic applications. Here, addressing the need for high-quality hybrid perovskite materials, the authors achieve the rapid growth of hybrid perovskite single crystals of high quality by inverse temperature crystallization.

1,448 citations


Journal ArticleDOI
TL;DR: A use of carbon dioxide as a renewable one-carbon (C1) building block in organic synthesis could contribute to a more sustainable use of resources.
Abstract: Carbon dioxide exits in the atmosphere and is produced by the combustion of fossil fuels, the fermentation of sugars and the respiration of all living organisms. An active goal in organic synthesis is to take this carbon--trapped in a waste product--and re-use it to build useful chemicals. Recent advances in organometallic chemistry and catalysis provide effective means for the chemical transformation of CO₂ and its incorporation into synthetic organic molecules under mild conditions. Such a use of carbon dioxide as a renewable one-carbon (C1) building block in organic synthesis could contribute to a more sustainable use of resources.

1,423 citations


Journal ArticleDOI
TL;DR: The results show that in the TaAs-type materials the WeylSemimetal state does not depend on fine-tuning of chemical composition or magnetic order, which opens the door for the experimental realization of Weyl semimetals and Fermi arc surface states in real materials.
Abstract: Weyl fermions are massless chiral fermions that play an important role in quantum field theory but have never been observed as fundamental particles. A Weyl semimetal is an unusual crystal that hosts Weyl fermions as quasiparticle excitations and features Fermi arcs on its surface. Such a semimetal not only provides a condensed matter realization of the anomalies in quantum field theories but also demonstrates the topological classification beyond the gapped topological insulators. Here, we identify a topological Weyl semimetal state in the transition metal monopnictide materials class. Our first-principles calculations on TaAs reveal its bulk Weyl fermion cones and surface Fermi arcs. Our results show that in the TaAs-type materials the Weyl semimetal state does not depend on fine-tuning of chemical composition or magnetic order, which opens the door for the experimental realization of Weyl semimetals and Fermi arc surface states in real materials. Proposals for the realization of Weyl semimetals, topologically non-trivial materials which host Weyl fermion quasiparticles, have faced demanding experimental requirements. Here, the authors predict such a state in stoichiometric TaAs, arising due to the breaking of inversion symmetry.

1,375 citations


Journal ArticleDOI
TL;DR: It is demonstrated beyond reasonable doubt that entropy predominates the thermodynamic landscape, and drives a reversible solid-state transformation between a multiphase and single-phase state.
Abstract: Configurational disorder can be compositionally engineered into mixed oxide by populating a single sublattice with many distinct cations. The formulations promote novel and entropy-stabilized forms of crystalline matter where metal cations are incorporated in new ways. Here, through rigorous experiments, a simple thermodynamic model, and a five-component oxide formulation, we demonstrate beyond reasonable doubt that entropy predominates the thermodynamic landscape, and drives a reversible solid-state transformation between a multiphase and single-phase state. In the latter, cation distributions are proven to be random and homogeneous. The findings validate the hypothesis that deliberate configurational disorder provides an orthogonal strategy to imagine and discover new phases of crystalline matter and untapped opportunities for property engineering.

1,343 citations


Journal ArticleDOI
TL;DR: A genome-wide association study in the Nordic region identifying a novel MM risk locus at ELL2 that encodes a stoichiometrically limiting component of the super-elongation complex that drives secretory-specific immunoglobulin mRNA production and transcriptional regulation in plasma cells is reported.
Abstract: Multiple myeloma (MM) is characterized by an uninhibited, clonal growth of plasma cells. While first-degree relatives of patients with MM show an increased risk of MM, the genetic basis of inherited MM susceptibility is incompletely understood. Here we report a genome-wide association study in the Nordic region identifying a novel MM risk locus at ELL2 (rs56219066T; odds ratio (OR)=1.25; P=9.6 × 10(-10)). This gene encodes a stoichiometrically limiting component of the super-elongation complex that drives secretory-specific immunoglobulin mRNA production and transcriptional regulation in plasma cells. We find that the MM risk allele harbours a Thr298Ala missense variant in an ELL2 domain required for transcription elongation. Consistent with a hypomorphic effect, we find that the MM risk allele also associates with reduced levels of immunoglobulin A (IgA) and G (IgG) in healthy subjects (P=8.6 × 10(-9) and P=6.4 × 10(-3), respectively) and, potentially, with an increased risk of bacterial meningitis (OR=1.30; P=0.0024).

1,342 citations


Journal ArticleDOI
TL;DR: Low-threshold amplified spontaneous emission and lasing from ∼10 nm monodisperse colloidal nanocrystals of caesium lead halide perovskites CsPbX3 are reported.
Abstract: Metal halide semiconductors with perovskite crystal structures have recently emerged as highly promising optoelectronic materials. Despite the recent surge of reports on microcrystalline, thin-film and bulk single-crystalline metal halides, very little is known about the photophysics of metal halides in the form of uniform, size-tunable nanocrystals. Here we report low-threshold amplified spontaneous emission and lasing from ∼10 nm monodisperse colloidal nanocrystals of caesium lead halide perovskites CsPbX3 (X=Cl, Br or I, or mixed Cl/Br and Br/I systems). We find that room-temperature optical amplification can be obtained in the entire visible spectral range (440–700 nm) with low pump thresholds down to 5±1 μJ cm−2 and high values of modal net gain of at least 450±30 cm−1. Two kinds of lasing modes are successfully observed: whispering-gallery-mode lasing using silica microspheres as high-finesse resonators, conformally coated with CsPbX3 nanocrystals and random lasing in films of CsPbX3 nanocrystals. Lead halide perovskite colloidal nanocrystals have promising optoelectronic properties, such as high photoluminescence quantum yields and narrow emission linewidths. Here, the authors report low-threshold amplified spontaneous emission and two kinds of lasing in nanostructured caesium lead halide perovskites.

1,305 citations


Journal ArticleDOI
TL;DR: This work demonstrates optical pumping of interlayer electric polarization, which may provoke further exploration of inter layer exciton condensation, as well as new applications in two-dimensional lasers, light-emitting diodes and photovoltaic devices.
Abstract: Monolayer transition metal dichalcogenide heterostructures with type II band alignment have generated wide interest in device physics at the two-dimensional limit. Here, Rivera et al. observe interlayer excitons in vertically stacked MoSe2–WSe2 heterostructures and demonstrate tunability of the energy and luminescence.

Journal ArticleDOI
TL;DR: An electrocatalyst for hydrogen generation based on very small amounts of cobalt dispersed as individual atoms on nitrogen-doped graphene is reported, which is robust and highly active in aqueous media with very low overpotentials.
Abstract: Reduction of water to hydrogen through electrocatalysis holds great promise for clean energy, but its large-scale application relies on the development of inexpensive and efficient catalysts to replace precious platinum catalysts. Here we report an electrocatalyst for hydrogen generation based on very small amounts of cobalt dispersed as individual atoms on nitrogen-doped graphene. This catalyst is robust and highly active in aqueous media with very low overpotentials (30 mV). A variety of analytical techniques and electrochemical measurements suggest that the catalytically active sites are associated with the metal centres coordinated to nitrogen. This unusual atomic constitution of supported metals is suggestive of a new approach to preparing extremely efficient single-atom catalysts.

Journal ArticleDOI
TL;DR: The reduced grain boundary area and improved crystallinity dramatically reduce the charge recombination in OTP thin films to the level in OTB single crystals.
Abstract: Large-aspect-ratio grains are needed in polycrystalline thin-film solar cells for reduced charge recombination at grain boundaries; however, the grain size in organolead trihalide perovskite (OTP) films is generally limited by the film thickness. Here we report the growth of OTP grains with high average aspect ratio of 2.3-7.9 on a wide range of non-wetting hole transport layers (HTLs), which increase nucleus spacing by suppressing heterogeneous nucleation and facilitate grain boundary migration in grain growth by imposing less drag force. The reduced grain boundary area and improved crystallinity dramatically reduce the charge recombination in OTP thin films to the level in OTP single crystals. Combining the high work function of several HTLs, a high stabilized device efficiency of 18.3% in low-temperature-processed planar-heterojunction OTP devices under 1 sun illumination is achieved. This simple method in enhancing OTP morphology paves the way for its application in other optoelectronic devices for enhanced performance.

Journal ArticleDOI
TL;DR: It is demonstrated that a stable and uniform solid electrolyte interphase layer is formed due to a synergetic effect of both lithium polysulfide and lithium nitrate as additives in ether-based electrolyte, preventing dendrite growth and minimizing electrolyte decomposition.
Abstract: Lithium dendrite growth is a serious hazard in battery operations. Here, the authors show that when using lithium polysulfide and lithium nitrate as additives in ether-based electrolyte, a stable and uniform solid electrolyte interphase forms on the lithium surface, which prevents dendrite growth.

Journal ArticleDOI
TL;DR: It is shown that a 3D current collector with a submicron skeleton and high electroactive surface area can significantly improve the electrochemical deposition behaviour of Li and reveals a new avenue for developing Li anodes with a long lifespan.
Abstract: Lithium metal is one of the most attractive anode materials for electrochemical energy storage. However, the growth of Li dendrites during electrochemical deposition, which leads to a low Coulombic efficiency and safety concerns, has long hindered the application of rechargeable Li-metal batteries. Here we show that a 3D current collector with a submicron skeleton and high electroactive surface area can significantly improve the electrochemical deposition behaviour of Li. Li anode is accommodated in the 3D structure without uncontrollable Li dendrites. With the growth of Li dendrites being effectively suppressed, the Li anode in the 3D current collector can run for 600 h without short circuit and exhibits low voltage hysteresis. The exceptional electrochemical performance of the Li-metal anode in the 3D current collector highlights the importance of rational design of current collectors and reveals a new avenue for developing Li anodes with a long lifespan.

Journal ArticleDOI
TL;DR: A metal-organic frameworks-assisted strategy for synthesizing nanostructured transition metal carbide nano-octahedrons composed of ultrafine nanocrystallites exhibited remarkable electrocatalytic performance for hydrogen production from both acidic and basic solutions is demonstrated.
Abstract: Electrochemical water splitting has been considered as a promising approach to produce clean and sustainable hydrogen fuel. However, the lack of high-performance and low-cost electrocatalysts for hydrogen evolution reaction hinders the large-scale application. As a new class of porous materials with tunable structure and composition, metal-organic frameworks have been considered as promising candidates to synthesize various functional materials. Here we demonstrate a metal-organic frameworks-assisted strategy for synthesizing nanostructured transition metal carbides based on the confined carburization in metal-organic frameworks matrix. Starting from a compound consisting of copper-based metal-organic frameworks host and molybdenum-based polyoxometalates guest, mesoporous molybdenum carbide nano-octahedrons composed of ultrafine nanocrystallites are successfully prepared as a proof of concept, which exhibit remarkable electrocatalytic performance for hydrogen production from both acidic and basic solutions. The present study provides some guidelines for the design and synthesis of nanostructured electrocatalysts. There is extensive research into non-platinum electrocatalysts for hydrogen evolution. Here, the authors report a molybdenum carbide catalyst, prepared via the carburization of a copper metal-organic framework host/molybdenum-based polyoxometalates guest system, and demonstrate its catalytic activity.

Journal ArticleDOI
TL;DR: This study uses detailed crop statistics time series for ~13,500 political units to examine how recent climate variability led to variations in maize, rice, wheat and soybean crop yields worldwide.
Abstract: Many studies have examined the role of mean climate change in agriculture, but an understanding of the influence of inter-annual climate variations on crop yields in different regions remains elusive. We use detailed crop statistics time series for ~13,500 political units to examine how recent climate variability led to variations in maize, rice, wheat and soybean crop yields worldwide. While some areas show no significant influence of climate variability, in substantial areas of the global breadbaskets, >60% of the yield variability can be explained by climate variability. Globally, climate variability accounts for roughly a third (~32-39%) of the observed yield variability. Our study uniquely illustrates spatial patterns in the relationship between climate variability and crop yield variability, highlighting where variations in temperature, precipitation or their interaction explain yield variability. We discuss key drivers for the observed variations to target further research and policy interventions geared towards buffering future crop production from climate variability.

Journal ArticleDOI
TL;DR: A comprehensive joint experiment–theory investigation of point defects in monolayer molybdenum disulphide prepared by mechanical exfoliation, physical and chemical vapour deposition and influence of defects on electronic structure and charge-carrier mobility is predicted by calculation and observed by electric transport measurement.
Abstract: Defects usually play an important role in tailoring various properties of two-dimensional materials. Defects in two-dimensional monolayer molybdenum disulphide may be responsible for large variation of electric and optical properties. Here we present a comprehensive joint experiment–theory investigation of point defects in monolayer molybdenum disulphide prepared by mechanical exfoliation, physical and chemical vapour deposition. Defect species are systematically identified and their concentrations determined by aberration-corrected scanning transmission electron microscopy, and also studied by ab-initio calculation. Defect density up to 3.5 × 1013 cm−2 is found and the dominant category of defects changes from sulphur vacancy in mechanical exfoliation and chemical vapour deposition samples to molybdenum antisite in physical vapour deposition samples. Influence of defects on electronic structure and charge-carrier mobility are predicted by calculation and observed by electric transport measurement. In light of these results, the growth of ultra-high-quality monolayer molybdenum disulphide appears a primary task for the community pursuing high-performance electronic devices. Imperfections can greatly alter a material’s properties. Here, the authors investigate the influence of point defects on the electronic structure, charge-carrier mobility and optical absorption of molybdenum disulphide prepared by mechanical exfoliation, physical and chemical vapour deposition.

Journal ArticleDOI
TL;DR: This article used three daily global climate data sets and three fire danger indices to develop a simple annual metric of fire weather season length, and map spatio-temporal trends from 1979 to 2013.
Abstract: Climate strongly influences global wildfire activity, and recent wildfire surges may signal fire weather-induced pyrogeographic shifts. Here we use three daily global climate data sets and three fire danger indices to develop a simple annual metric of fire weather season length, and map spatio-temporal trends from 1979 to 2013. We show that fire weather seasons have lengthened across 29.6 million km 2 (25.3%) of the Earth’s vegetated surface, resulting in an 18.7% increase in global mean fire weather season length. We also show a doubling (108.1% increase) of global burnable area affected by long fire weather seasons (41.0 s above the historical mean) and an increased global frequency of long fire weather seasons across 62.4 million km 2 (53.4%) during the second half of the study period. If these fire weather changes are coupled with ignition sources and available fuel, they could markedly impact global ecosystems, societies, economies and climate.

Journal ArticleDOI
TL;DR: An anion exchange method is reported to synthesize a complex ternary metal sulfides hollow structure, namely nickel cobalt sulfide ball-in-ball hollow spheres that show long-term cycling performance and potential application in high-performance electrochemical capacitors.
Abstract: While the synthesis of hollow structures of transition metal oxides is well established, it is extremely challenging to fabricate complex hollow structures for mixed transition metal sulfides. Here we report an anion exchange method to synthesize a complex ternary metal sulfides hollow structure, namely nickel cobalt sulfide ball-in-ball hollow spheres. Uniform nickel cobalt glycerate solid spheres are first synthesized as the precursor and subsequently chemically transformed into nickel cobalt sulfide ball-in-ball hollow spheres. When used as electrode materials for electrochemical capacitors, these nickel cobalt sulfide hollow spheres deliver a specific capacitance of 1,036 F g(-1) at a current density of 1.0 A g(-1). An asymmetric supercapacitor based on these ball-in-ball structures shows long-term cycling performance with a high energy density of 42.3 Wh kg(-1) at a power density of 476 W kg(-1), suggesting their potential application in high-performance electrochemical capacitors.

Journal ArticleDOI
TL;DR: In Fig. 4c of this Article, the y axis values were wrongly given as 0, 20, 40, 60 and 80 in the middle and the lower panels.
Abstract: Nature Communications 6: Article number: 6081 (2015); Published 20 January 2015; Updated 3 June 2015. In Fig. 4c of this Article, the y axis values were wrongly given as 0, 20, 40, 60 and 80 in the middle and the lower panels. The correct values should read 0, 10, 20, 30 and 40 for the middle and 0,1, 2, 3 and 4 for the lower panels.

Journal ArticleDOI
TL;DR: This work calculates and map recent change over 5 years in cumulative impacts to marine ecosystems globally from fishing, climate change, and ocean- and land-based stressors and affirm the importance of addressing climate change to maintain and improve the condition of marine ecosystems.
Abstract: Human pressures on the ocean are thought to be increasing globally, yet we know little about their patterns of cumulative change, which pressures are most responsible for change, and which places are experiencing the greatest increases. Managers and policymakers require such information to make strategic decisions and monitor progress towards management objectives. Here we calculate and map recent change over 5 years in cumulative impacts to marine ecosystems globally from fishing, climate change, and ocean- and land-based stressors. Nearly 66% of the ocean and 77% of national jurisdictions show increased human impact, driven mostly by climate change pressures. Five percent of the ocean is heavily impacted with increasing pressures, requiring management attention. Ten percent has very low impact with decreasing pressures. Our results provide large-scale guidance about where to prioritize management efforts and affirm the importance of addressing climate change to maintain and improve the condition of marine ecosystems.

Journal ArticleDOI
TL;DR: It is demonstrated that the Na(+) intercalation pseudocapacitance in TiO2/graphene nanocomposites enables high-rate capability and long cycle life in a sodium-ion battery.
Abstract: Sodium-ion batteries are emerging as a highly promising technology for large-scale energy storage applications. However, it remains a significant challenge to develop an anode with superior long-term cycling stability and high-rate capability. Here we demonstrate that the Na(+) intercalation pseudocapacitance in TiO2/graphene nanocomposites enables high-rate capability and long cycle life in a sodium-ion battery. This hybrid electrode exhibits a specific capacity of above 90 mA h g(-1) at 12,000 mA g(-1) (∼36 C). The capacity is highly reversible for more than 4,000 cycles, the longest demonstrated cyclability to date. First-principle calculations demonstrate that the intimate integration of graphene with TiO2 reduces the diffusion energy barrier, thus enhancing the Na(+) intercalation pseudocapacitive process. The Na-ion intercalation pseudocapacitance enabled by tailor-deigned nanostructures represents a promising strategy for developing electrode materials with high power density and long cycle life.

Journal ArticleDOI
TL;DR: It is shown that proteins, enzymes and DNA rapidly induce the formation of protective metal-organic framework coatings under physiological conditions by concentrating the framework building blocks and facilitating crystallization around the biomacromolecules.
Abstract: Robust biomacromolecules could be used for a wide range of biotechnological applications. Here the authors report a biomimetic mineralization process, in which biomolecules are encapsulated within metal-organic frameworks, and their stability is subsequently increased without significant bioactivity loss.

Journal ArticleDOI
TL;DR: The first perovskite–PCBM hybrid solid with significantly reduced hysteresis and recombination loss achieved in a single step is reported, and it is posited that PCBM, by tying up both halide-rich antisites and unincorporated halides, reduces electric field-induced anion migration that may give rise to hysteResis and unstable diode behaviour.
Abstract: Solution-processed planar perovskite devices are highly desirable in a wide variety of optoelectronic applications; however, they are prone to hysteresis and current instabilities. Here we report the first perovskite-PCBM hybrid solid with significantly reduced hysteresis and recombination loss achieved in a single step. This new material displays an efficient electrically coupled microstructure: PCBM is homogeneously distributed throughout the film at perovskite grain boundaries. The PCBM passivates the key PbI3(-) antisite defects during the perovskite self-assembly, as revealed by theory and experiment. Photoluminescence transient spectroscopy proves that the PCBM phase promotes electron extraction. We showcase this mixed material in planar solar cells that feature low hysteresis and enhanced photovoltage. Using conductive AFM studies, we reveal the memristive properties of perovskite films. We close by positing that PCBM, by tying up both halide-rich antisites and unincorporated halides, reduces electric field-induced anion migration that may give rise to hysteresis and unstable diode behaviour.

Journal ArticleDOI
TL;DR: In this article, the first Weyl semimetal was identified in a class of stoichiometric materials, including TaAs, TaP, NbAs, and NbP, which break crystalline inversion symmetry.
Abstract: The recent discoveries of Dirac fermions in graphene and on the surface of topological insulators have ignited worldwide interest in physics and materials science. A Weyl semimetal is an unusual crystal where electrons also behave as massless quasi-particles but interestingly they are not Dirac fermions. These massless particles, Weyl fermions, were originally considered in massless quantum electrodynamics but have not been observed as a fundamental particle in nature. A Weyl semimetal provides a condensed matter realization of Weyl fermions, leading to unique transport properties with novel device applications. Here, we THEORETICALLY identify the first Weyl semimetal in a class of stoichiometric materials (TaAs, NbAs, NbP, TaP), which break crystalline inversion symmetry, including TaAs, TaP, NbAs and NbP. Our first-principles calculation-based predictions on TaAs reveal the spin-polarized Weyl cones and Fermi arc surface states in this compound. We also observe pairs of Weyl points with the same chiral charge which project onto the same point in the surface Brillouin zone, giving rise to multiple Fermi arcs connecting to a given Weyl point. Our results show that TaAs is the first topological semimetal identified which does not depend on fine-tuning of chemical composition or magnetic order, greatly facilitating an exploration of Weyl physics in real materials. (Note added: This theoretical prediction of November 2014 (see paper in Nature Communications) was the basis for the first experimental discovery of Weyl Fermions and topological Fermi arcs in TaAs recently published in Science (2015) at this http URL)

Journal ArticleDOI
TL;DR: This work presents a novel and scalable approach to genome-based approaches that combines cell reprograming, nanofiltration, and ‘spatially aggregating’ techniques that allow for real-time assessment of the impact of environmental factors on gene expression and disease progression.
Abstract: Nature Communications 6: Article number: 6046 (2015); Published 5 February 2015; Updated 6 July 2015 The affiliation details for Emiliano Giardina are incorrect in this Article. The correct address for this author is given below: Department of Biopathology, Centre of Excellence for Genomic Risk Assessment in Multifactorial and Complex Diseases, School of Medicine, University of Rome ‘Tor Vergata’ and Laboratory of Molecular Genetics UILDM, Fondazione Santa Lucia, Rome 00179, Italy.

Journal ArticleDOI
TL;DR: P polarization-insensitive, micron-thick, high-contrast transmitarray micro-lenses with focal spots as small as 0.57 λ are reported, thus enabling widespread adoption and a rigorous method for ultrathin lens design is discussed.
Abstract: Flat optical devices thinner than a wavelength promise to replace conventional free-space components for wavefront and polarization control. Transmissive flat lenses are particularly interesting for applications in imaging and on-chip optoelectronic integration. Several designs based on plasmonic metasurfaces, high-contrast transmitarrays and gratings have been recently implemented but have not provided a performance comparable to conventional curved lenses. Here we report polarization-insensitive, micron-thick, high-contrast transmitarray micro-lenses with focal spots as small as 0.57 λ. The measured focusing efficiency is up to 82%. A rigorous method for ultrathin lens design, and the trade-off between high efficiency and small spot size (or large numerical aperture) are discussed. The micro-lenses, composed of silicon nano-posts on glass, are fabricated in one lithographic step that could be performed with high-throughput photo or nanoimprint lithography, thus enabling widespread adoption.

Journal ArticleDOI
TL;DR: It is demonstrated that high-quality, few-layer BP nanosheets, with controllable size and observable photoluminescence, can be produced in large quantities by liquid phase exfoliation under ambient conditions in solvents such as N-cyclohexyl-2-pyrrolidone (CHP).
Abstract: Few-layer black phosphorus (BP) is a new two-dimensional material which is of great interest for applications, mainly in electronics. However, its lack of environmental stability severely limits its synthesis and processing. Here we demonstrate that high-quality, few-layer BP nanosheets, with controllable size and observable photoluminescence, can be produced in large quantities by liquid phase exfoliation under ambient conditions in solvents such as N-cyclohexyl-2-pyrrolidone (CHP). Nanosheets are surprisingly stable in CHP, probably due to the solvation shell protecting the nanosheets from reacting with water or oxygen. Experiments, supported by simulations, show reactions to occur only at the nanosheet edge, with the rate and extent of the reaction dependent on the water/oxygen content. We demonstrate that liquid-exfoliated BP nanosheets are potentially useful in a range of applications from ultrafast saturable absorbers to gas sensors to fillers for composite reinforcement.

Journal ArticleDOI
TL;DR: The hetero-doped nitrogen/sulphur sites are demonstrated to show strong binding energy and be capable of anchoring polysulPHides based on first-principles calculations, and a high specific capacity, high-rate capacity and excellent cycling stability are achieved.
Abstract: Lithium–sulphur batteries with a high theoretical energy density are regarded as promising energy storage devices for electric vehicles and large-scale electricity storage. However, the low active material utilization, low sulphur loading and poor cycling stability restrict their practical applications. Herein, we present an effective strategy to obtain Li/polysulphide batteries with high-energy density and long-cyclic life using three-dimensional nitrogen/sulphur codoped graphene sponge electrodes. The nitrogen/sulphur codoped graphene sponge electrode provides enough space for a high sulphur loading, facilitates fast charge transfer and better immobilization of polysulphide ions. The hetero-doped nitrogen/sulphur sites are demonstrated to show strong binding energy and be capable of anchoring polysulphides based on first-principles calculations. As a result, a high specific capacity of 1,200 mAh g−1 at 0.2C rate, a high-rate capacity of 430 mAh g−1 at 2C rate and excellent cycling stability for 500 cycles with ∼0.078% capacity decay per cycle are achieved. There is intensive research underway into the cathode development of lithium–sulphur batteries. Here, the authors report a lithium–sulphur battery using nitrogen/sulphur codoped graphene structure which displays excellent electrochemical performance with high sulphur loading.