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Showing papers by "Oak Ridge National Laboratory published in 2016"


Journal ArticleDOI
TL;DR: In this article, a review of additive manufacturing (AM) techniques for producing metal parts are explored, with a focus on the science of metal AM: processing defects, heat transfer, solidification, solid-state precipitation, mechanical properties and post-processing metallurgy.
Abstract: Additive manufacturing (AM), widely known as 3D printing, is a method of manufacturing that forms parts from powder, wire or sheets in a process that proceeds layer by layer. Many techniques (using many different names) have been developed to accomplish this via melting or solid-state joining. In this review, these techniques for producing metal parts are explored, with a focus on the science of metal AM: processing defects, heat transfer, solidification, solid-state precipitation, mechanical properties and post-processing metallurgy. The various metal AM techniques are compared, with analysis of the strengths and limitations of each. Only a few alloys have been developed for commercial production, but recent efforts are presented as a path for the ongoing development of new materials for AM processes.

1,713 citations


Journal ArticleDOI
TL;DR: In this paper, the authors used three long-term satellite leaf area index (LAI) records and ten global ecosystem models to investigate four key drivers of LAI trends during 1982-2009.
Abstract: Global environmental change is rapidly altering the dynamics of terrestrial vegetation, with consequences for the functioning of the Earth system and provision of ecosystem services(1,2). Yet how global vegetation is responding to the changing environment is not well established. Here we use three long-term satellite leaf area index (LAI) records and ten global ecosystem models to investigate four key drivers of LAI trends during 1982-2009. We show a persistent and widespread increase of growing season integrated LAI (greening) over 25% to 50% of the global vegetated area, whereas less than 4% of the globe shows decreasing LAI (browning). Factorial simulations with multiple global ecosystem models suggest that CO2 fertilization effects explain 70% of the observed greening trend, followed by nitrogen deposition (9%), climate change (8%) and land cover change (LCC) (4%). CO2 fertilization effects explain most of the greening trends in the tropics, whereas climate change resulted in greening of the high latitudes and the Tibetan Plateau. LCC contributed most to the regional greening observed in southeast China and the eastern United States. The regional effects of unexplained factors suggest that the next generation of ecosystem models will need to explore the impacts of forest demography, differences in regional management intensities for cropland and pastures, and other emerging productivity constraints such as phosphorus availability.

1,534 citations


Journal ArticleDOI
TL;DR: In this paper, the authors demonstrate the possibility to precipitate a coherent reinforcing phase in a fcc-FeCoNiCr HEA matrix using minor additions of Ti and Al, and demonstrate that extraordinary balanced tensile properties at room temperature were achieved, which was due to a well combination of various hardening mechanisms, particularly precipitation hardening.

1,486 citations


Journal ArticleDOI
University of East Anglia1, University of Oslo2, Commonwealth Scientific and Industrial Research Organisation3, University of Exeter4, Oak Ridge National Laboratory5, National Oceanic and Atmospheric Administration6, Woods Hole Research Center7, University of California, San Diego8, Karlsruhe Institute of Technology9, Cooperative Institute for Marine and Atmospheric Studies10, Centre national de la recherche scientifique11, University of Maryland, College Park12, National Institute of Water and Atmospheric Research13, Woods Hole Oceanographic Institution14, Flanders Marine Institute15, Alfred Wegener Institute for Polar and Marine Research16, Netherlands Environmental Assessment Agency17, University of Illinois at Urbana–Champaign18, Leibniz Institute of Marine Sciences19, Max Planck Society20, University of Paris21, Hobart Corporation22, University of Bern23, Oeschger Centre for Climate Change Research24, National Center for Atmospheric Research25, University of Miami26, Council of Scientific and Industrial Research27, University of Colorado Boulder28, National Institute for Environmental Studies29, Joint Institute for the Study of the Atmosphere and Ocean30, Geophysical Institute, University of Bergen31, Goddard Space Flight Center32, Montana State University33, University of New Hampshire34, Bjerknes Centre for Climate Research35, Imperial College London36, Lamont–Doherty Earth Observatory37, Auburn University38, Wageningen University and Research Centre39, VU University Amsterdam40, Met Office41
TL;DR: In this article, the authors quantify all major components of the global carbon budget, including their uncertainties, based on the combination of a range of data, algorithms, statistics, and model estimates and their interpretation by a broad scientific community.
Abstract: . Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere – the “global carbon budget” – is important to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe data sets and methodology to quantify all major components of the global carbon budget, including their uncertainties, based on the combination of a range of data, algorithms, statistics, and model estimates and their interpretation by a broad scientific community. We discuss changes compared to previous estimates and consistency within and among components, alongside methodology and data limitations. CO2 emissions from fossil fuels and industry (EFF) are based on energy statistics and cement production data, respectively, while emissions from land-use change (ELUC), mainly deforestation, are based on combined evidence from land-cover change data, fire activity associated with deforestation, and models. The global atmospheric CO2 concentration is measured directly and its rate of growth (GATM) is computed from the annual changes in concentration. The mean ocean CO2 sink (SOCEAN) is based on observations from the 1990s, while the annual anomalies and trends are estimated with ocean models. The variability in SOCEAN is evaluated with data products based on surveys of ocean CO2 measurements. The global residual terrestrial CO2 sink (SLAND) is estimated by the difference of the other terms of the global carbon budget and compared to results of independent dynamic global vegetation models. We compare the mean land and ocean fluxes and their variability to estimates from three atmospheric inverse methods for three broad latitude bands. All uncertainties are reported as ±1σ, reflecting the current capacity to characterise the annual estimates of each component of the global carbon budget. For the last decade available (2006–2015), EFF was 9.3 ± 0.5 GtC yr−1, ELUC 1.0 ± 0.5 GtC yr−1, GATM 4.5 ± 0.1 GtC yr−1, SOCEAN 2.6 ± 0.5 GtC yr−1, and SLAND 3.1 ± 0.9 GtC yr−1. For year 2015 alone, the growth in EFF was approximately zero and emissions remained at 9.9 ± 0.5 GtC yr−1, showing a slowdown in growth of these emissions compared to the average growth of 1.8 % yr−1 that took place during 2006–2015. Also, for 2015, ELUC was 1.3 ± 0.5 GtC yr−1, GATM was 6.3 ± 0.2 GtC yr−1, SOCEAN was 3.0 ± 0.5 GtC yr−1, and SLAND was 1.9 ± 0.9 GtC yr−1. GATM was higher in 2015 compared to the past decade (2006–2015), reflecting a smaller SLAND for that year. The global atmospheric CO2 concentration reached 399.4 ± 0.1 ppm averaged over 2015. For 2016, preliminary data indicate the continuation of low growth in EFF with +0.2 % (range of −1.0 to +1.8 %) based on national emissions projections for China and USA, and projections of gross domestic product corrected for recent changes in the carbon intensity of the economy for the rest of the world. In spite of the low growth of EFF in 2016, the growth rate in atmospheric CO2 concentration is expected to be relatively high because of the persistence of the smaller residual terrestrial sink (SLAND) in response to El Nino conditions of 2015–2016. From this projection of EFF and assumed constant ELUC for 2016, cumulative emissions of CO2 will reach 565 ± 55 GtC (2075 ± 205 GtCO2) for 1870–2016, about 75 % from EFF and 25 % from ELUC. This living data update documents changes in the methods and data sets used in this new carbon budget compared with previous publications of this data set (Le Quere et al., 2015b, a, 2014, 2013). All observations presented here can be downloaded from the Carbon Dioxide Information Analysis Center ( doi:10.3334/CDIAC/GCP_2016 ).

1,224 citations


Journal ArticleDOI
01 Aug 2016-Carbon
TL;DR: An in-depth historical and current review is presented on the science of lithium-ion battery (LIB) solid electrolyte interphase (SEI) formation on the graphite anode, including structure, morphology, composition, electrochemistry, and formation mechanism.

1,217 citations



Journal ArticleDOI
TL;DR: This work examines an equiatomic medium-entropy alloy containing only three elements, CrCoNi, as a single-phase face-centred cubic solid solution, which displays strength-toughness properties that exceed those of all high-ENTropy alloys and most multi-phase alloys.
Abstract: High-entropy alloys are an intriguing new class of metallic materials that derive their properties from being multi-element systems that can crystallize as a single phase, despite containing high concentrations of five or more elements with different crystal structures. Here we examine an equiatomic medium-entropy alloy containing only three elements, CrCoNi, as a single-phase face-centred cubic solid solution, which displays strength-toughness properties that exceed those of all high-entropy alloys and most multi-phase alloys. At room temperature, the alloy shows tensile strengths of almost 1 GPa, failure strains of ∼70% and KJIc fracture-toughness values above 200 MPa m(1/2); at cryogenic temperatures strength, ductility and toughness of the CrCoNi alloy improve to strength levels above 1.3 GPa, failure strains up to 90% and KJIc values of 275 MPa m(1/2). Such properties appear to result from continuous steady strain hardening, which acts to suppress plastic instability, resulting from pronounced dislocation activity and deformation-induced nano-twinning.

1,101 citations


Journal ArticleDOI
TL;DR: This work demonstrates that oxygen plasma exposure and hydrogen treatment on pristine monolayer MoS2 could introduce more active sites via the formation of defects within the monolayers, leading to a high density of exposed edges and a significant improvement of the hydrogen evolution activity.
Abstract: MoS2 is a promising and low-cost material for electrochemical hydrogen production due to its high activity and stability during the reaction. However, the efficiency of hydrogen production is limited by the amount of active sites, for example, edges, in MoS2. Here, we demonstrate that oxygen plasma exposure and hydrogen treatment on pristine monolayer MoS2 could introduce more active sites via the formation of defects within the monolayer, leading to a high density of exposed edges and a significant improvement of the hydrogen evolution activity. These as-fabricated defects are characterized at the scale from macroscopic continuum to discrete atoms. Our work represents a facile method to increase the hydrogen production in electrochemical reaction of MoS2 via defect engineering, and helps to understand the catalytic properties of MoS2.

961 citations


Journal ArticleDOI
TL;DR: A survey of techniques for approximate computing (AC), which discusses strategies for finding approximable program portions and monitoring output quality, techniques for using AC in different processing units, processor components, memory technologies, and so forth, as well as programming frameworks for AC.
Abstract: Approximate computing trades off computation quality with effort expended, and as rising performance demands confront plateauing resource budgets, approximate computing has become not merely attractive, but even imperative. In this article, we present a survey of techniques for approximate computing (AC). We discuss strategies for finding approximable program portions and monitoring output quality, techniques for using AC in different processing units (e.g., CPU, GPU, and FPGA), processor components, memory technologies, and so forth, as well as programming frameworks for AC. We classify these techniques based on several key characteristics to emphasize their similarities and differences. The aim of this article is to provide insights to researchers into working of AC techniques and inspire more efforts in this area to make AC the mainstream computing approach in future systems.

890 citations


Journal ArticleDOI
TL;DR: The excitation spectrum of α-RuCl3 is proposed as a prime candidate for fractionalized Kitaev physics, and dynamical response measurements above interlayer energy scales are naturally accounted for in terms of deconfinement physics expected for QSLs.
Abstract: Inelastic neutron scattering characterization shows that α-RuCl3 is close to an experimental realization of a Kitaev quantum spin liquid on a honeycomb lattice. The collective excitations provide evidence for deconfined Majorana fermions.

867 citations


Journal ArticleDOI
TL;DR: In this article, large scale synthesis and delamination of 2D Mo2CTx (where T is a surface termination group) has been achieved by selectively etching gallium from the recently discovered nanolaminated, ternary tra...
Abstract: Large scale synthesis and delamination of 2D Mo2CTx (where T is a surface termination group) has been achieved by selectively etching gallium from the recently discovered nanolaminated, ternary tra ...

Journal ArticleDOI
TL;DR: This work attempts to rationalize the high activities of La1−xSrxCoO3−δ through the electronic structure and participation of lattice oxygen in the mechanism of water electrolysis as revealed through ab initio modelling.
Abstract: Perovskite oxides are attractive candidates as catalysts for the electrolysis of water in alkaline energy storage and conversion systems. However, the rational design of active catalysts has been hampered by the lack of understanding of the mechanism of water electrolysis on perovskite surfaces. Key parameters that have been overlooked include the role of oxygen vacancies, B-O bond covalency, and redox activity of lattice oxygen species. Here we present a series of cobaltite perovskites where the covalency of the Co-O bond and the concentration of oxygen vacancies are controlled through Sr(2+) substitution into La(1-x)Sr(x)CoO(3-δ) . We attempt to rationalize the high activities of La(1-x)Sr(x)CoO(3-δ) through the electronic structure and participation of lattice oxygen in the mechanism of water electrolysis as revealed through ab initio modelling. Using this approach, we report a material, SrCoO2.7, with a high, room temperature-specific activity and mass activity towards alkaline water electrolysis.

Journal ArticleDOI
TL;DR: In this article, the authors identify specific mechanisms through which automation may affect travel and energy demand and resulting GHG emissions and bring them together using a coherent energy decomposition framework, and explore the net effects of automation on emissions through several illustrative scenarios.
Abstract: Experts predict that new automobiles will be capable of driving themselves under limited conditions within 5–10 years, and under most conditions within 10–20 years. Automation may affect road vehicle energy consumption and greenhouse gas (GHG) emissions in a host of ways, positive and negative, by causing changes in travel demand, vehicle design, vehicle operating profiles, and choices of fuels. In this paper, we identify specific mechanisms through which automation may affect travel and energy demand and resulting GHG emissions and bring them together using a coherent energy decomposition framework. We review the literature for estimates of the energy impacts of each mechanism and, where the literature is lacking, develop our own estimates using engineering and economic analysis. We consider how widely applicable each mechanism is, and quantify the potential impact of each mechanism on a common basis: the percentage change it is expected to cause in total GHG emissions from light-duty or heavy-duty vehicles in the U.S. Our primary focus is travel related energy consumption and emissions, since potential lifecycle impacts are generally smaller in magnitude. We explore the net effects of automation on emissions through several illustrative scenarios, finding that automation might plausibly reduce road transport GHG emissions and energy use by nearly half – or nearly double them – depending on which effects come to dominate. We also find that many potential energy-reduction benefits may be realized through partial automation, while the major energy/emission downside risks appear more likely at full automation. We close by presenting some implications for policymakers and identifying priority areas for further research.

Journal ArticleDOI
12 Feb 2016-Science
TL;DR: This work created interlayer exciton spin-valley polarization by means of circularly polarized optical pumping and determined a valley lifetime of 40 nanoseconds, which enables the visualization of the expansion of a valley-polarized exciton cloud over several micrometers.
Abstract: Heterostructures comprising different monolayer semiconductors provide an attractive setting for fundamental science and device technologies, such as in the emerging field of valleytronics. We realized valley-specific interlayer excitons in monolayer WSe2-MoSe2 vertical heterostructures. We created interlayer exciton spin-valley polarization by means of circularly polarized optical pumping and determined a valley lifetime of 40 nanoseconds. This long-lived polarization enables the visualization of the expansion of a valley-polarized exciton cloud over several micrometers. The spatial pattern of the polarization evolves into a ring with increasing exciton density, a manifestation of valley exciton exchange interactions. Our work introduces van der Waals heterostructures as a promising platform from which to study valley exciton physics.

Journal ArticleDOI
TL;DR: Before QKD can be widely adopted, it faces a number of important challenges such as secret key rate, distance, size, cost and practical security, according to a survey of key challenges.
Abstract: Quantum key distribution (QKD) promises unconditional security in data communication and is currently being deployed in commercial applications. Nonetheless, before QKD can be widely adopted, it faces a number of important challenges such as secret key rate, distance, size, cost and practical security. Here, we survey those key challenges and the approaches that are currently being taken to address them.

Proceedings ArticleDOI
01 Jun 2016
TL;DR: A novel Expectation-Maximization (EM) based method is formulated that automatically locates discriminative patches robustly by utilizing the spatial relationships of patches and applies it to the classification of glioma and non-small-cell lung carcinoma cases into subtypes.
Abstract: Convolutional Neural Networks (CNN) are state-of-theart models for many image classification tasks. However, to recognize cancer subtypes automatically, training a CNN on gigapixel resolution Whole Slide Tissue Images (WSI) is currently computationally impossible. The differentiation of cancer subtypes is based on cellular-level visual features observed on image patch scale. Therefore, we argue that in this situation, training a patch-level classifier on image patches will perform better than or similar to an image-level classifier. The challenge becomes how to intelligently combine patch-level classification results and model the fact that not all patches will be discriminative. We propose to train a decision fusion model to aggregate patch-level predictions given by patch-level CNNs, which to the best of our knowledge has not been shown before. Furthermore, we formulate a novel Expectation-Maximization (EM) based method that automatically locates discriminative patches robustly by utilizing the spatial relationships of patches. We apply our method to the classification of glioma and non-small-cell lung carcinoma cases into subtypes. The classification accuracy of our method is similar to the inter-observer agreement between pathologists. Although it is impossible to train CNNs on WSIs, we experimentally demonstrate using a comparable non-cancer dataset of smaller images that a patch-based CNN can outperform an image-based CNN.

Journal ArticleDOI
TL;DR: The High-ResMIP (High-resolution Model Intercomparison Project) as mentioned in this paper is a multi-model approach to the systematic investigation of the impact of horizontal resolution on the simulated mean climate and its variability.
Abstract: . Robust projections and predictions of climate variability and change, particularly at regional scales, rely on the driving processes being represented with fidelity in model simulations. The role of enhanced horizontal resolution in improved process representation in all components of the climate system is of growing interest, particularly as some recent simulations suggest both the possibility of significant changes in large-scale aspects of circulation as well as improvements in small-scale processes and extremes. However, such high-resolution global simulations at climate timescales, with resolutions of at least 50 km in the atmosphere and 0.25° in the ocean, have been performed at relatively few research centres and generally without overall coordination, primarily due to their computational cost. Assessing the robustness of the response of simulated climate to model resolution requires a large multi-model ensemble using a coordinated set of experiments. The Coupled Model Intercomparison Project 6 (CMIP6) is the ideal framework within which to conduct such a study, due to the strong link to models being developed for the CMIP DECK experiments and other model intercomparison projects (MIPs). Increases in high-performance computing (HPC) resources, as well as the revised experimental design for CMIP6, now enable a detailed investigation of the impact of increased resolution up to synoptic weather scales on the simulated mean climate and its variability. The High Resolution Model Intercomparison Project (HighResMIP) presented in this paper applies, for the first time, a multi-model approach to the systematic investigation of the impact of horizontal resolution. A coordinated set of experiments has been designed to assess both a standard and an enhanced horizontal-resolution simulation in the atmosphere and ocean. The set of HighResMIP experiments is divided into three tiers consisting of atmosphere-only and coupled runs and spanning the period 1950–2050, with the possibility of extending to 2100, together with some additional targeted experiments. This paper describes the experimental set-up of HighResMIP, the analysis plan, the connection with the other CMIP6 endorsed MIPs, as well as the DECK and CMIP6 historical simulations. HighResMIP thereby focuses on one of the CMIP6 broad questions, “what are the origins and consequences of systematic model biases?”, but we also discuss how it addresses the World Climate Research Program (WCRP) grand challenges.

Journal ArticleDOI
TL;DR: Room-temperature ferroelectricity in 2D CuInP2S6 (CIPS) with a transition temperature of ∼320 K is reported and switchable polarization is observed in thin CIPS of ∼4 nm.
Abstract: Two-dimensional (2D) materials have emerged as promising candidates for various optoelectronic applications based on their diverse electronic properties, ranging from insulating to superconducting. However, cooperative phenomena such as ferroelectricity in the 2D limit have not been well explored. Here, we report room-temperature ferroelectricity in 2D CuInP2S6 (CIPS) with a transition temperature of ∼320 K. Switchable polarization is observed in thin CIPS of ∼4 nm. To demonstrate the potential of this 2D ferroelectric material, we prepare a van der Waals (vdW) ferroelectric diode formed by CIPS/Si heterostructure, which shows good memory behaviour with on/off ratio of ∼100. The addition of ferroelectricity to the 2D family opens up possibilities for numerous novel applications, including sensors, actuators, non-volatile memory devices, and various vdW heterostructures based on 2D ferroelectricity. Two dimensional materials are promising for electronic applications, which await the exploration of cooperative phenomena. Here, Liu et al. report switchable ferroelectric polarization in thin CuInP2S6film at room temperature, demonstrating good memory behaviour with on/off ratio of ∼100 based on two-dimensional ferroelectricity.

Journal ArticleDOI
TL;DR: Mechanistic analyses showed that NK cells were mobilized by epinephrine, and blockade of β-adrenergic signaling blunted training-dependent tumor inhibition, and IL-6-blocking antibodies bluned training-induced tumor suppression, intratumoral NK cell infiltration, and NK cell activation.

Journal ArticleDOI
TL;DR: This study demonstrates enhancement of radiation tolerance with the suppression of void formation by two orders magnitude at elevated temperatures in equiatomic single-phase concentrated solid solution alloys, and reveals its controlling mechanism through a detailed analysis of the depth distribution of defect clusters and an atomistic computer simulation.
Abstract: A grand challenge in material science is to understand the correlation between intrinsic properties and defect dynamics. Radiation tolerant materials are in great demand for safe operation and advancement of nuclear and aerospace systems. Unlike traditional approaches that rely on microstructural and nanoscale features to mitigate radiation damage, this study demonstrates enhancement of radiation tolerance with the suppression of void formation by two orders magnitude at elevated temperatures in equiatomic single-phase concentrated solid solution alloys, and more importantly, reveals its controlling mechanism through a detailed analysis of the depth distribution of defect clusters and an atomistic computer simulation. The enhanced swelling resistance is attributed to the tailored interstitial defect cluster motion in the alloys from a long-range one-dimensional mode to a short-range three-dimensional mode, which leads to enhanced point defect recombination. The results suggest design criteria for next generation radiation tolerant structural alloys.

Journal ArticleDOI
TL;DR: In this paper, the authors presented a system modeling framework for additive manufacturing in the U.S. aircraft industry, with integrated engineering criteria, life-cycle environmental data, aircraft fleet stock and fuel use models under different AM adoption scenarios.

Journal ArticleDOI
TL;DR: The design of a gas–solid interface reaction to achieve delicate control of oxygen activity through uniformly creating oxygen vacancies without affecting structural integrity of Li-rich layered oxides is reported.
Abstract: Lattice oxygen can play an intriguing role in electrochemical processes, not only maintaining structural stability, but also influencing electron and ion transport properties in high-capacity oxide cathode materials for Li-ion batteries. Here, we report the design of a gas-solid interface reaction to achieve delicate control of oxygen activity through uniformly creating oxygen vacancies without affecting structural integrity of Li-rich layered oxides. Theoretical calculations and experimental characterizations demonstrate that oxygen vacancies provide a favourable ionic diffusion environment in the bulk and significantly suppress gas release from the surface. The target material is achievable in delivering a discharge capacity as high as 301 mAh g(-1) with initial Coulombic efficiency of 93.2%. After 100 cycles, a reversible capacity of 300 mAh g(-1) still remains without any obvious decay in voltage. This study sheds light on the comprehensive design and control of oxygen activity in transition-metal-oxide systems for next-generation Li-ion batteries.

Journal ArticleDOI
TL;DR: This work identifies the Weyl points and demonstrates that they are connected by different sets of Fermi arcs for each of the two surface terminations and finds new surface 'track states' that form closed loops and are unique to type II Weyl semimetals.
Abstract: In a type I Dirac or Weyl semimetal, the low-energy states are squeezed to a single point in momentum space when the chemical potential μ is tuned precisely to the Dirac/Weyl point. Recently, a type II Weyl semimetal was predicted to exist, where the Weyl states connect hole and electron bands, separated by an indirect gap. This leads to unusual energy states, where hole and electron pockets touch at the Weyl point. Here we present the discovery of a type II topological Weyl semimetal state in pure MoTe2, where two sets of Weyl points (, ) exist at the touching points of electron and hole pockets and are located at different binding energies above EF. Using angle-resolved photoemission spectroscopy, modelling, density functional theory and calculations of Berry curvature, we identify the Weyl points and demonstrate that they are connected by different sets of Fermi arcs for each of the two surface terminations. We also find new surface 'track states' that form closed loops and are unique to type II Weyl semimetals. This material provides an exciting, new platform to study the properties of Weyl fermions.

Journal ArticleDOI
TL;DR: It is demonstrated that the phase transition was in fact first-order, although still very close to tricritical, according to the variation of the order parameter Q for this transition scaled with temperature T as Q ∼ (Tc−T)β.
Abstract: We have examined the crystal structures and structural phase transitions of the deuterated, partially deuterated and hydrogenous organic-inorganic hybrid perovskite methyl ammonium lead iodide (MAPbI3) using time-of-flight neutron and synchrotron X-ray powder diffraction. Near 330 K the high temperature cubic phases transformed to a body-centered tetragonal phase. The variation of the order parameter Q for this transition scaled with temperature T as Q ∼ (Tc−T)β, where Tc is the critical temperature and the exponent β was close to ¼, as predicted for a tricritical phase transition. However, we also observed coexistence of the cubic and tetragonal phases over a range of temperature in all cases, demonstrating that the phase transition was in fact first-order, although still very close to tricritical. Upon cooling further, all the tetragonal phases transformed into a low temperature orthorhombic phase around 160 K, again via a first-order phase transition. Based upon these results, we discuss the impact of the structural phase transitions upon photovoltaic performance of MAPbI3 based solar cells.

Journal ArticleDOI
TL;DR: In this article, a comprehensive set of evidence of how hydrolase and oxidase activities respond to N fertilization in various ecosystems was provided. But the relationship between response ratios (RRs) of EEA and SOC, soil N (TN), and soil microbial biomass carbon (MBC) were explored when they were reported simultaneously.
Abstract: Nitrogen (N) fertilization affects the rate of soil organic carbon (SOC) decomposition by regulating extracellular enzyme activities (EEA). Extracellular enzymes have not been represented in global biogeochemical models. Understanding the relationships among EEA and SOC, soil N (TN), and soil microbial biomass carbon (MBC) under N fertilization would enable modeling of the influence of EEA on SOC decomposition. Based on 65 published studies, we synthesized the activities of α-1,4-glucosidase (AG), β-1,4-glucosidase (BG), β- d -cellobiosidase (CBH), β-1,4-xylosidase (BX), β-1,4-N-acetyl-glucosaminidase (NAG), leucine amino peptidase (LAP), urease (UREA), acid phosphatase (AP), phenol oxidase (PHO), and peroxidase (PEO) in response to N fertilization. The proxy variables for hydrolytic C acquisition enzymes (C-acq), N acquisition (N-acq), and oxidative decomposition (OX) were calculated as the sum of AG, BG, CBH and BX; AG and LAP; PHO and PEO, respectively. The relationships between response ratios (RRs) of EEA and SOC, TN, or MBC were explored when they were reported simultaneously. Results showed that N fertilization significantly increased CBH, C-acq, AP, BX, BG, AG, and UREA activities by 6.4, 9.1, 10.6, 11.0, 11.2, 12.0, and 18.6%, but decreased PEO, OX and PHO by 6.1, 7.9 and 11.1%, respectively. N fertilization enhanced SOC and TN by 7.6% and 15.3%, respectively, but inhibited MBC by 9.5%. Significant positive correlations were found only between the RRs of C-acq and MBC, suggesting that changes in combined hydrolase activities might act as a proxy for MBC under N fertilization. In contrast with other variables, the RRs of AP, MBC, and TN showed unidirectional trends under different edaphic, environmental, and physiological conditions. Our results provide the first comprehensive set of evidence of how hydrolase and oxidase activities respond to N fertilization in various ecosystems. Future large-scale model projections could incorporate the observed relationship between hydrolases and microbial biomass as a proxy for C acquisition under global N enrichment scenarios in different ecosystems.

Journal ArticleDOI
08 Dec 2016
TL;DR: Lin et al. as mentioned in this paper reviewed the most recent breakthrough discoveries as well as emerging opportunities and remaining challenges in the field of 2D materials, including transition metal dichalcogenides, mono-elemental 2D sheets, and several carbide-and nitride-based materials.
Abstract: Author(s): Lin, Z; McCreary, A; Briggs, N; Subramanian, S; Zhang, K; Sun, Y; Li, X; Borys, NJ; Yuan, H; Fullerton-Shirey, SK; Chernikov, A; Zhao, H; McDonnell, S; Lindenberg, AM; Xiao, K; Le Roy, BJ; Drndic, M; Hwang, JCM; Park, J; Chhowalla, M; Schaak, RE; Javey, A; Hersam, MC; Robinson, J; Terrones, M | Abstract: The rise of two-dimensional (2D) materials research took place following the isolation of graphene in 2004. These new 2D materials include transition metal dichalcogenides, mono-elemental 2D sheets, and several carbide- and nitride-based materials. The number of publications related to these emerging materials has been drastically increasing over the last five years. Thus, through this comprehensive review, we aim to discuss the most recent groundbreaking discoveries as well as emerging opportunities and remaining challenges. This review starts out by delving into the improved methods of producing these new 2D materials via controlled exfoliation, metal organic chemical vapor deposition, and wet chemical means. We look into recent studies of doping as well as the optical properties of 2D materials and their heterostructures. Recent advances towards applications of these materials in 2D electronics are also reviewed, and include the tunnel MOSFET and ways to reduce the contact resistance for fabricating high-quality devices. Finally, several unique and innovative applications recently explored are discussed as well as perspectives of this exciting and fast moving field.

Journal ArticleDOI
26 Feb 2016-Science
TL;DR: It is shown that the addition of tin to palladium catalysts coupled with an appropriate heat treatment cycle switches off the sequential hydrogenation and decomposition reactions, enabling selectivities of >95% toward H2O2.
Abstract: The direct synthesis of hydrogen peroxide (H2O2) from H2 and O2 represents a potentially atom-efficient alternative to the current industrial indirect process. We show that the addition of tin to palladium catalysts coupled with an appropriate heat treatment cycle switches off the sequential hydrogenation and decomposition reactions, enabling selectivities of >95% toward H2O2. This effect arises from a tin oxide surface layer that encapsulates small Pd-rich particles while leaving larger Pd-Sn alloy particles exposed. We show that this effect is a general feature for oxide-supported Pd catalysts containing an appropriate second metal oxide component, and we set out the design principles for producing high-selectivity Pd-based catalysts for direct H2O2 production that do not contain gold.

Journal ArticleDOI
Dorothee C. E. Bakker1, Benjamin Pfeil2, Benjamin Pfeil3, Camilla S. Landa2, Camilla S. Landa3, Nicolas Metzl4, K. O'Brien, Are Olsen3, Are Olsen2, K. Smith, Catherine E Cosca, S. Harasawa, Stephen D. Jones2, Stephen D. Jones3, Shin-Ichiro Nakaoka, Yukihiro Nojiri, Ute Schuster5, Tobias Steinhoff6, Colm Sweeney7, Colm Sweeney8, Taro Takahashi9, Bronte Tilbrook10, Bronte Tilbrook11, Chisato Wada, Rik Wanninkhof12, Simone R. Alin, Carlos F. Balestrini, Leticia Barbero13, Leticia Barbero12, Nicholas R. Bates14, Alejandro A. Bianchi, Frédéric Bonou15, Jacqueline Boutin4, Yann Bozec4, Eugene Burger, Wei-Jun Cai, R. D. Castle12, Liqi Chen16, Melissa Chierici17, Kim I. Currie, Wiley Evans18, Charles Featherstone12, Richard A. Feely, Agneta Fransson19, Catherine Goyet20, Naomi Greenwood, Luke Gregor21, S. Hankin, Nick J. Hardman-Mountford22, Jérôme Harlay23, Judith Hauck24, Mario Hoppema24, Matthew P. Humphreys14, Christopher W. Hunt25, Betty Huss12, J. Severino P. Ibánhez26, J. Severino P. Ibánhez15, Truls Johannessen2, Truls Johannessen3, Ralph F. Keeling, Vassilis Kitidis27, Arne Körtzinger6, Alex Kozyr28, Evangelia Krasakopoulou29, Akira Kuwata, Peter Landschützer30, Siv K. Lauvset2, Nathalie Lefèvre4, Claire Lo Monaco4, Ansley Manke, Jeremy T. Mathis, Liliane Merlivat4, Frank J. Millero13, Pedro M. S. Monteiro21, David R. Munro8, Akihiko Murata31, Timothy Newberger7, Timothy Newberger8, Abdirahman M Omar2, Tsuneo Ono, K. Paterson11, David A. Pearce, Denis Pierrot12, Denis Pierrot13, Lisa L. Robbins32, S. Saito33, Joe Salisbury25, Reiner Schlitzer24, Bernd Schneider34, Roland Schweitzer, Rainer Sieger24, Ingunn Skjelvan2, Kevin F. Sullivan12, Kevin F. Sullivan13, Stewart C Sutherland9, Adrienne J. Sutton, Kazuaki Tadokoro, Maciej Telszewski, Matthias Tuma35, Steven van Heuven, Doug Vandemark25, Brian Ward36, Andrew J. Watson5, Suqing Xu16 
TL;DR: This ESSD "living data" publication documents the methods and data sets used for the assembly of this new version of the SOCAT data collection and compares these with those used for earlier versions of the data collection.
Abstract: . The Surface Ocean CO2 Atlas (SOCAT) is a synthesis of quality-controlled fCO2 (fugacity of carbon dioxide) values for the global surface oceans and coastal seas with regular updates. Version 3 of SOCAT has 14.7 million fCO2 values from 3646 data sets covering the years 1957 to 2014. This latest version has an additional 4.6 million fCO2 values relative to version 2 and extends the record from 2011 to 2014. Version 3 also significantly increases the data availability for 2005 to 2013. SOCAT has an average of approximately 1.2 million surface water fCO2 values per year for the years 2006 to 2012. Quality and documentation of the data has improved. A new feature is the data set quality control (QC) flag of E for data from alternative sensors and platforms. The accuracy of surface water fCO2 has been defined for all data set QC flags. Automated range checking has been carried out for all data sets during their upload into SOCAT. The upgrade of the interactive Data Set Viewer (previously known as the Cruise Data Viewer) allows better interrogation of the SOCAT data collection and rapid creation of high-quality figures for scientific presentations. Automated data upload has been launched for version 4 and will enable more frequent SOCAT releases in the future. High-profile scientific applications of SOCAT include quantification of the ocean sink for atmospheric carbon dioxide and its long-term variation, detection of ocean acidification, as well as evaluation of coupled-climate and ocean-only biogeochemical models. Users of SOCAT data products are urged to acknowledge the contribution of data providers, as stated in the SOCAT Fair Data Use Statement. This ESSD (Earth System Science Data) "living data" publication documents the methods and data sets used for the assembly of this new version of the SOCAT data collection and compares these with those used for earlier versions of the data collection (Pfeil et al., 2013; Sabine et al., 2013; Bakker et al., 2014). Individual data set files, included in the synthesis product, can be downloaded here: doi:10.1594/PANGAEA.849770 . The gridded products are available here: doi:10.3334/CDIAC/OTG.SOCAT_V3_GRID .

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TL;DR: In this paper, the stability and kinetics of the Li-7La3Zr2O12 (LLZO) interface were characterized as a function of temperature and current density.

Journal ArticleDOI
26 May 2016-Nature
TL;DR: The topological magneto-electric response originating in such an engineered topological insulator could allow efficient manipulation of the magnetization dynamics by an electric field, providing an energy-efficient topological control mechanism for future spin-based technologies.
Abstract: Topological insulators are insulating materials that display conducting surface states protected by time-reversal symmetry, wherein electron spins are locked to their momentum. This unique property opens up new opportunities for creating next-generation electronic, spintronic and quantum computation devices. Introducing ferromagnetic order into a topological insulator system without compromising its distinctive quantum coherent features could lead to the realization of several predicted physical phenomena. In particular, achieving robust long-range magnetic order at the surface of the topological insulator at specific locations without introducing spin-scattering centres could open up new possibilities for devices. Here we use spin-polarized neutron reflectivity experiments to demonstrate topologically enhanced interface magnetism by coupling a ferromagnetic insulator (EuS) to a topological insulator (Bi2Se3) in a bilayer system. This interfacial ferromagnetism persists up to room temperature, even though the ferromagnetic insulator is known to order ferromagnetically only at low temperatures (<17 K). The magnetism induced at the interface resulting from the large spin-orbit interaction and the spin-momentum locking of the topological insulator surface greatly enhances the magnetic ordering (Curie) temperature of this bilayer system. The ferromagnetism extends ~2 nm into the Bi2Se3 from the interface. Owing to the short-range nature of the ferromagnetic exchange interaction, the time-reversal symmetry is broken only near the surface of a topological insulator, while leaving its bulk states unaffected. The topological magneto-electric response originating in such an engineered topological insulator could allow efficient manipulation of the magnetization dynamics by an electric field, providing an energy-efficient topological control mechanism for future spin-based technologies.