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The title compounds, [(1R,3R,4R,5R,6S)-4,5-bis(acetyloxy)-7-oxo-2-oxabicyclo[4.2.0]octan-3-yl]methyl acetate, C14H18O8, (I), [(1S,4R,5S,6R)-5-acetyloxy-7-hydroxyimino-2-oxobicyclo[4.2.0]octan-4-yl acetate, C11H15NO6, (II), and [(3aR,5R,6R,7R,7aS)-6,7-bis(acetyloxy)-2-oxooctahydropyrano[3,2-b]pyrrol-5-yl]methyl acetate, C14H19NO8, (III), are stable bicyclic carbohydrate derivatives. They can easily be synthesized in a few steps from commercially available glycals. As a result of the ring strain from the four-membered rings in (I) and (II), the conformations of the carbohydrates deviate strongly from the ideal chair form. Compound (II) occurs in the boat form. In the five-membered lactam (III), on the other hand, the carbohydrate adopts an almost ideal chair conformation. As a result of the distortion of the sugar rings, the configurations of the three bicyclic carbohydrate derivatives could not be determined from their NMR coupling constants. From our three crystal structure determinations, we were able to establish for the first time the absolute configurations of all new stereocenters of the carbohydrate rings.
Volunteered geographical information (VGI) and citizen science have become important sources data for much scientific research. In the domain of land cover, crowdsourcing can provide a high temporal resolution data to support different analyses of landscape processes. However, the scientists may have little control over what gets recorded by the crowd, providing a potential source of error and uncertainty. This study compared analyses of crowdsourced land cover data that were contributed by different groups, based on nationality (labelled Gondor and Non-Gondor) and on domain experience (labelled Expert and Non-Expert). The analyses used a geographically weighted model to generate maps of land cover and compared the maps generated by the different groups. The results highlight the differences between the maps how specific land cover classes were under-and over-estimated. As crowdsourced data and citizen science are increasingly used to replace data collected under the designed experiment, this paper highlights the importance of considering between group variations and their impacts on the results of analyses. Critically, differences in the way that landscape features are conceptualised by different groups of contributors need to be considered when using crowdsourced data in formal scientific analyses. The discussion considers the potential for variation in crowdsourced data, the relativist nature of land cover and suggests a number of areas for future research. The key finding is that the veracity of citizen science data is not the critical issue per se. Rather, it is important to consider the impacts of differences in the semantics, affordances and functions associated with landscape features held by different groups of crowdsourced data contributors.
We study the adsorption–desorption transition of polyelectrolyte chains onto planar, cylindrical and spherical surfaces with arbitrarily high surface charge densities by massive Monte Carlo computer simulations. We examine in detail how the well known scaling relations for the threshold transition—demarcating the adsorbed and desorbed domains of a polyelectrolyte near weakly charged surfaces—are altered for highly charged interfaces. In virtue of high surface potentials and large surface charge densities, the Debye–Hückel approximation is often not feasible and the nonlinear Poisson–Boltzmann approach should be implemented. At low salt conditions, for instance, the electrostatic potential from the nonlinear Poisson–Boltzmann equation is smaller than the Debye–Hückel result, such that the required critical surface charge density for polyelectrolyte adsorption σc increases. The nonlinear relation between the surface charge density and electrostatic potential leads to a sharply increasing critical surface charge density with growing ionic strength, imposing an additional limit to the critical salt concentration above which no polyelectrolyte adsorption occurs at all. We contrast our simulations findings with the known scaling results for weak critical polyelectrolyte adsorption onto oppositely charged surfaces for the three standard geometries. Finally, we discuss some applications of our results for some physical–chemical and biophysical systems.
Coupling of attention and saccades when viewing scenes with central and peripheral degradation
(2016)
Degrading real-world scenes in the central or the peripheral visual field yields a characteristic pattern: Mean saccade amplitudes increase with central and decrease with peripheral degradation. Does this pattern reflect corresponding modulations of selective attention? If so, the observed saccade amplitude pattern should reflect more focused attention in the central region with peripheral degradation and an attentional bias toward the periphery with central degradation. To investigate this hypothesis, we measured the detectability of peripheral (Experiment 1) or central targets (Experiment 2) during scene viewing when low or high spatial frequencies were gaze-contingently filtered in the central or the peripheral visual field. Relative to an unfiltered control condition, peripheral filtering induced a decrease of the detection probability for peripheral but not for central targets (tunnel vision). Central filtering decreased the detectability of central but not of peripheral targets. Additional post hoc analyses are compatible with the interpretation that saccade amplitudes and direction are computed in partial independence. Our experimental results indicate that task-induced modulations of saccade amplitudes reflect attentional modulations.
This article first outlines different ways of how psycholinguists have dealt with linguistic diversity and illustrates these approaches with three familiar cases from research on language processing, language acquisition, and language disorders. The second part focuses on the role of morphology and morphological variability across languages for psycholinguistic research. The specific phenomena to be examined are to do with stem-formation morphology and inflectional classes; they illustrate how experimental research that is informed by linguistic typology can lead to new insights.
Climate change increases riverine carbon outgassing, while export to the ocean remains uncertain
(2016)
Any regular interaction of land and river during flooding affects carbon pools within the terrestrial system, riverine carbon and carbon exported from the system. In the Amazon basin carbon fluxes are considerably influenced by annual flooding, during which terrigenous organic material is imported to the river. The Amazon basin therefore represents an excellent example of a tightly coupled terrestrial-riverine system. The processes of generation, conversion and transport of organic carbon in such a coupled terrigenous-riverine system strongly interact and are climate-sensitive, yet their functioning is rarely considered in Earth system models and their response to climate change is still largely unknown. To quantify regional and global carbon budgets and climate change effects on carbon pools and carbon fluxes, it is important to account for the coupling between the land, the river, the ocean and the atmosphere. We developed the RIVerine Carbon Model (RivCM), which is directly coupled to the well-established dynamic vegetation and hydrology model LPJmL, in order to account for this large-scale coupling. We evaluate RivCM with observational data and show that some of the values are reproduced quite well by the model, while we see large deviations for other variables. This is mainly caused by some simplifications we assumed. Our evaluation shows that it is possible to reproduce large-scale carbon transport across a river system but that this involves large uncertainties. Acknowledging these uncertainties, we estimate the potential changes in riverine carbon by applying RivCM for climate forcing from five climate models and three CO2 emission scenarios (Special Report on Emissions Scenarios, SRES). We find that climate change causes a doubling of riverine organic carbon in the southern and western basin while reducing it by 20% in the eastern and northern parts. In contrast, the amount of riverine inorganic carbon shows a 2- to 3-fold increase in the entire basin, independent of the SRES scenario. The export of carbon to the atmosphere increases as well, with an average of about 30 %. In contrast, changes in future export of organic carbon to the Atlantic Ocean depend on the SRES scenario and are projected to either decrease by about 8.9% (SRES A1B) or increase by about 9.1% (SRES A2). Such changes in the terrigenous-riverine system could have local and regional impacts on the carbon budget of the whole Amazon basin and parts of the Atlantic Ocean. Changes in riverine carbon could lead to a shift in the riverine nutrient supply and pH, while changes in the exported carbon to the ocean lead to changes in the supply of organic material that acts as a food source in the Atlantic. On larger scales the increased outgassing of CO2 could turn the Amazon basin from a sink of carbon to a considerable source. Therefore, we propose that the coupling of terrestrial and riverine carbon budgets should be included in subsequent analysis of the future regional carbon budget.
Children’s interpretations of sentences containing focus particles do not seem adult-like until school age. This study investigates how German 4-year-old children comprehend sentences with the focus particle ‘nur’ (only) by using different tasks and controlling for the impact of general cognitive abilities on performance measures. Two sentence types with ‘only’ in either pre-subject or pre-object position were presented. Eye gaze data and verbal responses were collected via the visual world paradigm combined with a sentence-picture verification task. While the eye tracking data revealed an adult-like pattern of focus particle processing, the sentence-picture verification replicated previous findings of poor comprehension, especially for ‘only’ in pre-subject position. A second study focused on the impact of general cognitive abilities on the outcomes of the verification task. Working memory was related to children’s performance in both sentence types whereas inhibitory control was selectively related to the number of errors for sentences with ‘only’ in pre-subject position. These results suggest that children at the age of 4 years have the linguistic competence to correctly interpret sentences with focus particles, which–depending on specific task demands–may be masked by immature general cognitive abilities.
Exosomes are small membrane vesicles released by different cell types, including hepatocytes, that play important roles in intercellular communication. We have previously demonstrated that hepatocyte-derived exosomes contain the synthetic machinery to form sphingosine-1-phosphate (S1P) in target hepatocytes resulting in proliferation and liver regeneration after ischemia/reperfusion (I/R) injury. We also demonstrated that the chemokine receptors, CXCR1 and CXCR2, regulate liver recovery and regeneration after I/R injury. In the current study, we sought to determine if the regulatory effects of CXCR1 and CXCR2 on liver recovery and regeneration might occur via altered release of hepatocyte exosomes. We found that hepatocyte release of exosomes was dependent upon CXCR1 and CXCR2. CXCR1-deficient hepatocytes produced fewer exosomes, whereas CXCR2-deficient hepatocytes produced more exosomes compared to their wild-type controls. In CXCR2-deficient hepatocytes, there was increased activity of neutral sphingomyelinase (Nsm) and intracellular ceramide. CXCR1-deficient hepatocytes had no alterations in Nsm activity or ceramide production. Interestingly, exosomes from CXCR1-deficient hepatocytes had no effect on hepatocyte proliferation, due to a lack of neutral ceramidase and sphingosine kinase. The data demonstrate that CXCR1 and CXCR2 regulate hepatocyte exosome release. The mechanism utilized by CXCR1 remains elusive, but CXCR2 appears to modulate Nsm activity and resultant production of ceramide to control exosome release. CXCR1 is required for packaging of enzymes into exosomes that mediate their hepatocyte proliferative effect.
The interaction of water with α-alumina (i.e. α-Al2O3) surfaces is important in a variety of applications and a useful model for the interaction of water with environmentally abundant aluminosilicate phases. Despite its significance, studies of water interaction with α-Al2O3 surfaces other than the (0001) are extremely limited. Here we characterize the interaction of water (D2O) with a well defined α-Al2O3(1[1 with combining macron]02) surface in UHV both experimentally, using temperature programmed desorption and surface-specific vibrational spectroscopy, and theoretically, using periodic-slab density functional theory calculations. This combined approach makes it possible to demonstrate that water adsorption occurs only at a single well defined surface site (the so-called 1–4 configuration) and that at this site the barrier between the molecularly and dissociatively adsorbed forms is very low: 0.06 eV. A subset of OD stretch vibrations are parallel to this dissociation coordinate, and thus would be expected to be shifted to low frequencies relative to an uncoupled harmonic oscillator. To quantify this effect we solve the vibrational Schrödinger equation along the dissociation coordinate and find fundamental frequencies red-shifted by more than 1500 cm−1. Within the context of this model, at moderate temperatures, we further find that some fraction of surface deuterons are likely delocalized: dissociatively and molecularly absorbed states are no longer distinguishable.
Changes in free symptom attributions in hypochondriasis after cognitive therapy and exposure therapy
(2016)
Background: Cognitive-behavioural therapy can change dysfunctional symptom attributions in patients with hypochondriasis. Past research has used forced-choice answer formats, such as questionnaires, to assess these misattributions; however, with this approach, idiosyncratic attributions cannot be assessed. Free associations are an important complement to existing approaches that assess symptom attributions. Aims: With this study, we contribute to the current literature by using an open-response instrument to investigate changes in freely associated attributions after exposure therapy (ET) and cognitive therapy (CT) compared with a wait list (WL). Method: The current study is a re-examination of a formerly published randomized controlled trial (Weck, Neng, Richtberg, Jakob and Stangier, 2015) that investigated the effectiveness of CT and ET. Seventy-three patients with hypochondriasis were randomly assigned to CT, ET or a WL, and completed a 12-week treatment (or waiting period). Before and after the treatment or waiting period, patients completed an Attribution task in which they had to spontaneously attribute nine common bodily sensations to possible causes in an open-response format. Results: Compared with the WL, both CT and ET reduced the frequency of somatic attributions regarding severe diseases (CT: Hedges's g = 1.12; ET: Hedges's g = 1.03) and increased the frequency of normalizing attributions (CT: Hedges's g = 1.17; ET: Hedges's g = 1.24). Only CT changed the attributions regarding moderate diseases (Hedges's g = 0.69). Changes in somatic attributions regarding mild diseases and psychological attributions were not observed. Conclusions: Both CT and ET are effective for treating freely associated misattributions in patients with hypochondriasis. This study supplements research that used a forced-choice assessment.