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  1. Abstract

    Biocatalytic processes are highly selective and specific. However, their utility is limited by the comparatively narrow scope of enzyme‐catalysed transformations. To expand product scope, we are developing biocompatible processes that combine biocatalytic reactions with chemo‐catalysis in single‐flask processes. Here, we show that a chemocatalysed Pictet‐Spengler annulation can be interfaced with biocatalysed alcohol oxidation. This two‐step, one‐pot cascade reaction converts tyramine and aliphatic alcohols to tetrahydroisoquinoline alkaloids in aqueous buffer at mild pH. Tryptamine derivatives are also efficiently converted to tryptolines. Optimization of stoichiometry, pH, reaction time, and whole‐cell catalyst deliver the tetrahydroisouinolines and tryptolines in >90 % and >40 % isolated yield, respectively, with excellent regioselectivity.

     
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    Free, publicly-accessible full text available December 14, 2024
  2. Dinitroalkanes are powerful synthetic building blocks because of the versatility of the 1,3-dinitro motif. Here, we show that dinitroalkanes can be synthesized from aliphatic aldehydes in a three-step cascade reaction catalysed by phosphate buffer and the amino acid lysine. We further show that this methodology can be expanded to limited alcohol substrates (1-butanol and 1-pentanol) with the inclusion of a biocatalysed alcohol oxidation. Simultaneous addition of all reagents gives a maximal yield of 52% of 3-(nitromethyl)hexane, derived from 1-butanol and nitromethane, whereas staggering the introduction of the amino acid catalyst and nitromethane substrate boosts the yield to 71% of 3-(nitromethyl)hexane with near-quantitative consumption of the n-butyraldehyde intermediate. Taken together, this work presents a mild synthetic method that couples multi-step catalytic cascades generate 1,3-dinitroalkanes. 
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  3. The geographical ranges of many mammals and their associated parasites are dynamic. Comprehensive documentation of these communities over time provides a foundation for interpreting how changing environmental conditions, driven by accelerating climate change, other anthropogenic disturbances, and natural events, may influence host-parasite interactions. Fleas (Order Siphonaptera) are obligate, hematophagous parasites of birds and mammals with medical interest because of their role in transmitting pathogens. From 2016 to 2019, we sampled the small mammal and associated flea communities in El Malpais National Conservation Area (El Malpais) in Cibola County, New Mexico. Among 898 mammalian specimens, 925 fleas representing 29 species were collected from 18 host species. Pleochaetis exilis was the most abundant flea species, composing 27% of the total fleas collected, whereas Aetheca wagneri was the most prevalent flea species, parasitizing 8% of the community sampled. Across a total of 284 hosts recorded with fleas, A. wagneri, Malaraeus eremicus, and Peromyscopsylla hesperomys adelpha parasitized the most host species (n = 6 each). Onychomys leucogaster (Wied-Neuwied, 1841), the northern grasshopper mouse, a rodent highly implicated in plague dynamics, was host for the highest number of flea species (n = 15), followed by Peromyscus truei (Shufeldt, 1885) (n = 10). Our aims are to (a) describe the flea-mammal assemblage of a central New Mexico site, creating a baseline for diversity against which changing patterns of association can be assessed over time; (b) identify previously unrecognized host associations; and (c) examine infestation parameters, including the relationships of flea prevalence and mean abundance to host sex, host abundance, and seasonality. As such, our study exemplifies the Documentation and Assessment phases of the DAMA protocol (Document, Assess, Monitor, Act), a central component of exploring distribution and diversity of complex pathogen-host communities across space and time that are essential to a proactive understanding of emerging disease. 
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    Free, publicly-accessible full text available April 10, 2024
  4. The Breakthrough Starshot Initiative aims to send a gram-scale probe to our nearest extrasolar neighbors using a laser-accelerated lightsail traveling at relativistic speeds. Thermal management is a key lightsail design objective because of the intense laser powers required but has generally been considered secondary to accelerative performance. Here, we demonstrate nanophotonic photonic crystal slab reflectors composed of 2H-phase molybdenum disulfide and crystalline silicon nitride, highlight the inverse relationship between the thermal band extinction coefficient and the lightsail’s maximum temperature, and examine the trade-off between minimizing acceleration distance and setting realistic sail thermal limits, ultimately realizing a thermally endurable acceleration minimum distance of 23.3 Gm. We additionally demonstrate multiscale photonic structures featuring thermal-wavelength-scale Mie resonant geometries and characterize their broadband Mie resonance-driven emissivity enhancement and acceleration distance reduction. More broadly, our results highlight new possibilities for simultaneously controlling optical and thermal response over broad wavelength ranges in ultralight nanophotonic structures. 
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  5. Abstract A search for highly electrically charged objects (HECOs) and magnetic monopoles is presented using 2.2 $$\hbox {fb}{^{-1}}$$ fb - 1 of $$p-p$$ p - p collision data taken at a centre of mass energy (E $$_{CM}$$ CM ) of 8 TeV by the MoEDAL detector during LHC’s Run-1. The data were collected using MoEDAL’s prototype Nuclear Track Detectord array and the Trapping Detector array. The results are interpreted in terms of Drell–Yan pair production of stable HECO and monopole pairs with three spin hypotheses (0, 1/2 and 1). The search provides constraints on the direct production of magnetic monopoles carrying one to four Dirac magnetic charges and with mass limits ranging from 590 GeV/c $$^{2}$$ 2 to 1 TeV/c $$^{2}$$ 2 . Additionally, mass limits are placed on HECOs with charge in the range 10 e to 180 e , where e is the charge of an electron, for masses between 30 GeV/c $$^{2}$$ 2 and 1 TeV/c $$^{2}$$ 2 . 
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  6. Free, publicly-accessible full text available June 1, 2024
  7. null (Ed.)