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1.
The coupling of phonons to electrons and other phonons plays a defining role in material properties, such as charge and energy transport, light emission, and superconductivity. In atomic solids, phonons are delocalized over the 3D lattice, in contrast to molecular solids where localized vibrations dominate. Here, a hierarchical semiconductor that expands the phonon space by combining localized 0D modes with delocalized 2D and 3D modes is described. This material consists of superatomic building blocks (Re6Se8) covalently linked into 2D sheets that are stacked into a layered van der Waals lattice. Using transient reflectance spectroscopy, three types of coherent phonons are identified: localized 0D breathing modes of isolated superatom, 2D synchronized twisting of superatoms in layers, and 3D acoustic interlayer deformation. These phonons are coupled to the electronic degrees of freedom to varying extents. The presence of local phonon modes in an extended crystal opens the door to controlling material properties from hierarchical phonon engineering.  相似文献   
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An increasing number of individuals work in jobs with little standardization and repetition, that is, with high levels of job non‐routinization. At the same time, demands for creativity are high, which raises the question of how employees can use job non‐routinization to develop creativity. Acknowledging the importance of social processes for creativity, we propose that transformational leaders raise feelings of organizational identification in followers and that this form of identification then helps individuals to develop creativity in jobs with little routinization. This is because organizational members evaluate and promote those ideas as more creative, which are in line with a shared understanding of creativity within the organization. To investigate these relationships, we calculated a mediated moderation model with 173 leader–follower dyads from China. Results confirm our hypotheses that transformational leadership moderates the relationship between job non‐routinization on employee creativity through organizational identification. We conclude that raising feelings of social identity is a key task for leaders today, especially when working in uncertain and fast developing environments with little repetition and the constant need to develop creative ideas.  相似文献   
4.
Traditionally, prodrug activation has been limited to enzymatic triggers or gross physiological aberrations, such as pH, that offer low selectivity and control over dosage. In recent years, the field of prodrug activation chemistry has been transformed by the use of bioorthogonal reactions that can be carried out under biological conditions at sub-millimolar concentrations, with the tetrazine-mediated inverse electron demand Diels–Alder reaction amongst the most recognised. Their high reaction rates, chemoselectivity and excellent biocompatibility make tetrazines ideal small molecules for activating prodrugs. Recently the tetrazine moiety has been used as a prodrug for a pyridazine thus broadening the scope of prodrug systems. This article discusses the concept of using tetrazines as small-molecule activators for prodrugs, and provides an overview of tetrazine-based prodrug systems, with a particular focus on the recently reported prodrug–prodrug activation strategy.  相似文献   
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Combined photochemical arylation, “nuisance effect” (SNAr) reaction sequences have been employed in the design of small arrays for immediate deployment in medium-throughput X-ray protein–ligand structure determination. Reactions were deliberately allowed to run “out of control” in terms of selectivity; for example the ortho-arylation of 2-phenylpyridine gave five products resulting from mono- and bisarylations combined with SNAr processes. As a result, a number of crystallographic hits against NUDT7, a key peroxisomal CoA ester hydrolase, have been identified.  相似文献   
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Four samples of paper and board (P/B) of a type used for packaging dry foods were subjected to migration experiments using raisins and the polymeric powder Tenax as a food simulant. The P/B samples contained only low levels of diisopropylnaphthalene (DiPN) and diisobutyl phthalate (DiBP), and so, experiments were also conducted after spiking the P/B with added model substances. These were o‐xylene, acetophenone, dodecane, benzophenone, DiPN and DiBP. Migration experiments into raisins and Tenax were conducted for 10 days at 40°C. Migration levels depended strongly on the nature of the substance. Migration from spiked P/B samples was more extensive (as a percentage of that available) than migration of intrinsic migratable substances, and so, studying spiked samples tends to be conservative. It is considered likely that this is because of binding of substances, especially aromatics with pi‐electrons such as DiPN and DiBP, to active sites on the surface of P/B fibres, resulting in non‐linear absorption isotherms. However, further work would be needed to prove this conclusively. Considering the results overall and also that raisins packed in P/B can have a shelf life of up to 1 year at ambient temperatures, the test results using Tenax as a food simulant are considered to be appropriate without application of a correction factor. Copyright © 2014 John Wiley & Sons, Ltd.  相似文献   
7.
In a study of conversion from CH4 to H2, jet flame characteristics of these gases and their blends are compared on a burner diameter scale of mm. Low velocity H2 and CH4 jets, burned on pipes of different diameters, indicate higher blow-off limits for H2, but lower heat release rates, a consequence of its lower specific energy. Compensation for this might be obtained through increased H2 flow velocity, or a small increase in pipe diameter. Blended CH4/H2 flames have lower heat release rates than CH4 alone, yet small proportions of H2, with CH4 might still be burned, on a CH4 burner. Throughout, fundamental understanding is enhanced through two dimensionless groups: laminar flame thickness normalised by burner diameter, δk/D, and the dimensionless flow number, U1. These suggest an optimal role for H2 combustion, utilizing its high acoustic and blow-off velocities, in high intensity, subsonic, combustors, at low δk/D, and high U1.  相似文献   
8.
The Asian clam Corbicula fluminea is among the most prolific aquatic invaders in the world; but in colder mid-latitude areas, like the Laurentian Great Lakes, their population expansion has likely been limited by poor overwinter survival. In these areas, Asian clams are typically found in thermal refugia like warmwater discharges from industrial facilities. We sought to identify the current extent of Asian clam populations in Lake Michigan and waters immediately adjacent to it, specifically at locations most likely to harbor overwintering populations – industrial warmwater discharges. During April–May 2017, we surveyed 17 locations around Lake Michigan. Evidence of Asian clam populations was found at four sites, though live specimens (n?=?3) were only found at the Indiana Harbor Ship Canal in East Chicago, IN. Shells or fragments of shells were found at Green Bay, WI, Waukegan, IL, and Port Sheldon, MI. Our findings indicate that although Asian clams are present in Lake Michigan, they are relatively rare, and remain isolated to a few small pockets of over-wintering habitat.  相似文献   
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The gastrointestinal nematode Ostertagia ostertagi is an important cause of lost production, health, and welfare in cattle. Detailed records were obtained over a 5-yr period (2010–2015) by questionnaires and qualitative interviews to investigate the practices adopted by dairy farmers to control cattle helminth infections and the factors associated with heifer exposure to O. ostertagi on pasture. In total, 1,454 heifers' individual milk samples were collected over a 1-yr period (2014–2015) in 43 dairy farms in England and tested for O. ostertagi antibody by ELISA. Multilevel linear regression models were used to investigate the association between individual milk optical density ratio (ODR) against O. ostertagi and heifer management from birth to time of sampling. Farm and heifer median ODR against O. ostertagi were 0.98 (interquartile range = 0.76–1.02) and 0.64 (interquartile range = 0.42–0.84), respectively. The majority of heifers (88%) received an anthelmintic treatment before sampling in this study. After controlling for the effect of anthelmintic treatments, heifer individual milk ODR against O. ostertagi significantly increased with high stocking rate at first grazing and co-grazing with adult cows before calving. Conversely, heifer individual milk ODR against O. ostertagi significantly decreased when heifers had co-grazed with sheep and pasture grass had frequently been mowed. Overall, these results provide evidence to support targeting grazing management toward limiting the use of anthelmintics in dairy young stock to enable sustainable control of cattle helminth infections in England. However, to be accepted and adopted by farmers, these best practices would need to take into account farmers' perspectives and contextual challenges.  相似文献   
10.
Nutrient management on US dairy farms must balance an array of priorities, some of which conflict. To illustrate nutrient management challenges and opportunities across the US dairy industry, the USDA Agricultural Research Service Dairy Agroecosystems Working Group (DAWG) modeled 8 confinement and 2 grazing operations in the 7 largest US dairy-producing states using the Integrated Farm System Model (IFSM). Opportunities existed across all of the dairies studied to increase on-farm feed production and lower purchased feed bills, most notably on large dairies (>1,000 cows) with the highest herd densities. Purchased feed accounted for 18 to 44% of large dairies' total operating costs compared with 7 to 14% on small dairies (<300 milk cows) due to lower stocking rates. For dairies with larger land bases, in addition to a reduction in environmental impact, financial incentives exist to promote prudent nutrient management practices by substituting manure nutrients or legume nutrients for purchased fertilizers. Environmental priorities varied regionally and were principally tied to facility management for dry-lot dairies of the semi-arid western United States (ammonia-N emissions), to manure handling and application for humid midwestern and eastern US dairies (nitrate-N leaching and P runoff), and pasture management for dairies with significant grazing components (nitrous oxide emissions). Many of the nutrient management challenges identified by DAWG are beyond slight modifications in management and require coordinated solutions to ensure an environmentally and economically sustainable US dairy industry.  相似文献   
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