516 research outputs found

    Enantioselective Construction of Acyclic Quaternary Carbon Stereocenters: Palladium-Catalyzed Decarboxylative Allylic Alkylation of Fully-Substituted Amide Enolates

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    We report a divergent and modular protocol for the preparation of acyclic molecular frameworks containing newly created quaternary carbon stereocenters. Central to this approach is a sequence composed of a (1) regioselective and -retentive preparation of allyloxycarbonyl-trapped fully substituted stereodefined amide enolates and of a (2) enantioselective palladium-catalyzed decarboxylative allylic alkylation reaction using a novel bisphosphine ligand

    Probing Trends in Enantioinduction via Substrate Design: Palladium-Catalyzed Decarboxylative Allylic Alkylation of α-Enaminones

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    Herein, we report the palladium-catalyzed decarboxylative asymmetric allylic alkylation of α-enaminones. In addition to serving as valuable synthetic building blocks, we exploit the α-enaminone scaffold and its derivatives as probes to highlight structural and electronic factors that govern enantioselectivity in this asymmetric alkylation reaction. Utilizing the (S)-t-BuPHOX ligand in a variety of nonpolar solvents, the alkylated products are obtained in up to 99% yield and 99% enantiomeric excess

    The association between the food environment and weight status among eastern North Carolina youth

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    Objective: To examine associations between various measures of the food environment and BMI percentile among youth. Design: Cross-sectional, observational. Setting: Pitt County, eastern North Carolina. Subjects:We extracted the electronic medical records for youth receiving well child check-ups from January 2007 to June 2008. We obtained addresses for food venues from two secondary sources and ground-truthing. A geographic information systems database was constructed by geocoding home addresses of 744 youth and food venues. We quantified participants\u27 accessibility to food venues by calculating \u27coverage\u27, number of food venues in buffers of 0●25, 0●5, 1 and 5 miles (0●4, 0●8, 1●6 and 8●0 km) and by calculating \u27proximity\u27 or distance to the closest food venue. We examined associations between BMI percentile and food venue accessibility using correlation and regression analyses. Results:There were negative associations between BMI percentile and coverage of farmers\u27 markets/produce markets in 0●25 and 0●5 mile Euclidean and 0●25, 0●5 and 1 mile road network buffers. There were positive associations between BMI percentile coverage of fast-food and pizza places in the 0●25 mile Euclidean and network buffers. In multivariate analyses adjusted for race, insurance status and rural/urban residence, proximity (network distance) to convenience stores was negatively associated with BMI percentile and proximity to farmers\u27 markets was positively associated with BMI percentile. Conclusions: Accessibility to various types of food venues is associated with BMI percentile in eastern North Carolina youth. Future longitudinal work should examine correlations between accessibility to and use of traditional and non-traditional food venues

    EatWellNow: Formative Development of a Place-Based Behavioral “Nudge” Technology Intervention to Promote Healthier Food Purchases among Army Soldiers

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    Approximately 17% of military service members are obese. Research involving army soldiers suggests a lack of awareness of healthy foods on post. Innovative approaches are needed to change interactions with the military food environment. Two complementary technological methods to raise awareness are geofencing (deliver banner ads with website links) and Bluetooth beacons (real-time geotargeted messages to mobile phones that enter a designated space). There is little published literature regarding the feasibility of this approach to promote healthy behaviors in retail food environments. Thus, we conducted a formative feasibility study of a military post to understand the development, interest in, and implementation of EatWellNow, a multi-layered interactive food environment approach using contextual messaging to improve food purchasing decisions within the military food environment. We measured success based on outcomes of a formative evaluation, including process, resources, management, and scientific assessment. We also report data on interest in the approach from a Fort Bragg community health assessment survey (n = 3281). Most respondents agreed that they were interested in receiving push notifications on their phone about healthy options on post (64.5%) and that receiving these messages would help them eat healthier (68.3%). EatWellNow was successfully developed through cross-sector collaboration and was well received in this military environment, suggesting feasibility in this setting. Future work should examine the impact of EatWellNow on military service food purchases and dietary behaviors

    Vapor phase deposition of perovskite photovoltaics:Short track to commercialization?

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    While perovskite-based photovoltaics (PV) is progressing toward commercialization, it remains an open question which fabrication technology - solution-based, vapor-based, or combinations - will pave the way to faster economic breakthrough. The vast majority of research studies make use of solution-processed perovskite thin films, which benefit from a rapid optimization feedback and inexpensive to procure tools in modern research laboratories, but vapor phase deposition processes dominate today's established thin-film manufacturing. As research and development of vapor phase processed perovskite thin films are still strongly underrepresented in literature, their full potential is yet to be identified. In this collaborative perspective of academic influenced by industrial views, we convey a balanced viewpoint on the prospects of vapor-based processing of perovskite PV at an industrial scale. Our perspective highlights the conceptual advantages of vapor phase deposition, discusses the most crucial process parameters in a technology assessment, contains an overview about relevant global industry clusters, and provides an outlook on the commercialization perspectives of the perovskite technology in general.</p

    Atmospheric Escape Processes and Planetary Atmospheric Evolution

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    The habitability of the surface of any planet is determined by a complex evolution of its interior, surface, and atmosphere. The electromagnetic and particle radiation of stars drive thermal, chemical and physical alteration of planetary atmospheres, including escape. Many known extrasolar planets experience vastly different stellar environments than those in our Solar system: it is crucial to understand the broad range of processes that lead to atmospheric escape and evolution under a wide range of conditions if we are to assess the habitability of worlds around other stars. One problem encountered between the planetary and the astrophysics communities is a lack of common language for describing escape processes. Each community has customary approximations that may be questioned by the other, such as the hypothesis of H-dominated thermosphere for astrophysicists, or the Sun-like nature of the stars for planetary scientists. Since exoplanets are becoming one of the main targets for the detection of life, a common set of definitions and hypotheses are required. We review the different escape mechanisms proposed for the evolution of planetary and exoplanetary atmospheres. We propose a common definition for the different escape mechanisms, and we show the important parameters to take into account when evaluating the escape at a planet in time. We show that the paradigm of the magnetic field as an atmospheric shield should be changed and that recent work on the history of Xenon in Earth's atmosphere gives an elegant explanation to its enrichment in heavier isotopes: the so-called Xenon paradox

    Measurement of χ c1 and χ c2 production with s√ = 7 TeV pp collisions at ATLAS

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    The prompt and non-prompt production cross-sections for the χ c1 and χ c2 charmonium states are measured in pp collisions at s√ = 7 TeV with the ATLAS detector at the LHC using 4.5 fb−1 of integrated luminosity. The χ c states are reconstructed through the radiative decay χ c → J/ÏˆÎł (with J/ψ → ÎŒ + ÎŒ −) where photons are reconstructed from Îł → e + e − conversions. The production rate of the χ c2 state relative to the χ c1 state is measured for prompt and non-prompt χ c as a function of J/ψ transverse momentum. The prompt χ c cross-sections are combined with existing measurements of prompt J/ψ production to derive the fraction of prompt J/ψ produced in feed-down from χ c decays. The fractions of χ c1 and χ c2 produced in b-hadron decays are also measured

    Standalone vertex ïŹnding in the ATLAS muon spectrometer

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    A dedicated reconstruction algorithm to find decay vertices in the ATLAS muon spectrometer is presented. The algorithm searches the region just upstream of or inside the muon spectrometer volume for multi-particle vertices that originate from the decay of particles with long decay paths. The performance of the algorithm is evaluated using both a sample of simulated Higgs boson events, in which the Higgs boson decays to long-lived neutral particles that in turn decay to bbar b final states, and pp collision data at √s = 7 TeV collected with the ATLAS detector at the LHC during 2011

    Measurements of Higgs boson production and couplings in diboson final states with the ATLAS detector at the LHC

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    Measurements are presented of production properties and couplings of the recently discovered Higgs boson using the decays into boson pairs, H →γ Îł, H → Z Z∗ →4l and H →W W∗ →lÎœlÎœ. The results are based on the complete pp collision data sample recorded by the ATLAS experiment at the CERN Large Hadron Collider at centre-of-mass energies of √s = 7 TeV and √s = 8 TeV, corresponding to an integrated luminosity of about 25 fb−1. Evidence for Higgs boson production through vector-boson fusion is reported. Results of combined ïŹts probing Higgs boson couplings to fermions and bosons, as well as anomalous contributions to loop-induced production and decay modes, are presented. All measurements are consistent with expectations for the Standard Model Higgs boson
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