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Carbon-based ionogels tuning the properties of the ionic liquid via carbon-ionic liquid interaction
(2012)
The behavior of two ionic liquids (ILs), 1-ethyl-3-methylimidazolium dicyanamide [Emim][DCA] and 1-ethyl-3-methylimidazolium triflate [Emim][TfO], in (meso) porous carbonaceous hosts was investigated. Prior to IL incorporation into the host, the carbon matrix was thermally annealed between 180 and 900 degrees C to control carbon condensation and surface chemistry. The resulting materials have an increasing "graphitic'' carbon character with increasing treatment temperature, reflected in a modified behavior of the ILs when impregnated into the carbon host. The two ILs show significant changes in the thermal behavior as measured from differential scanning calorimetry; these changes can be assigned to anion-pi interaction between the IL anions and the pore wall surfaces of these flexible carbonaceous support materials.
Rates of multiple paternities were investigated in the sailfin molly (Poecilia latipinna), using eight microsatellite loci. Genotyping was performed for offspring and mothers in 40 broods from four allopatric populations from the south-eastern U.S.A. along a geographic stretch of 1200 km in west-east direction and approximately 200 km from north to south. No significant differences regarding rates of multiple paternities were found between populations despite sample populations stemming from ecologically divergent habitats. Even the most conservative statistical approach revealed a minimum of 70% of the broods being sired by at least two males, with an average of 1.80-2.95 putative fathers per brood. Within broods, one male typically sired far more offspring than would be expected under an assumed equal probability of all detected males siring offspring.
Structural kinetic modeling (SKM) enables the analysis of dynamical properties of metabolic networks solely based on topological information and experimental data. Current SKM-based experiments are hampered by the time-intensive process of assigning model parameters and choosing appropriate sampling intervals for MonteCarlo experiments. We introduce a toolbox for the automatic and efficient construction and evaluation of structural kinetic models (SK models). Quantitative and qualitative analyses of network stability properties are performed in an automated manner. We illustrate the model building and analysis process in detailed example scripts that provide toolbox implementations of previously published literature models.
Metabolic networks are characterized by complex interactions and regulatory mechanisms between many individual components. These interactions determine whether a steady state is stable to perturbations. Structural kinetic modeling (SKM) is a framework to analyze the stability of metabolic steady states that allows the study of the system Jacobian without requiring detailed knowledge about individual rate equations. Stability criteria can be derived by generating a large number of structural kinetic models (SK-models) with randomly sampled parameter sets and evaluating the resulting Jacobian matrices. Until now, SKM experiments applied univariate tests to detect the network components with the largest influence on stability. In this work, we present an extended SKM approach relying on supervised machine learning to detect patterns of enzyme-metabolite interactions that act together in an orchestrated manner to ensure stability. We demonstrate its application on a detailed SK-model of the Calvin-Benson cycle and connected pathways. The identified stability patterns are highly complex reflecting that changes in dynamic properties depend on concerted interactions between several network components. In total, we find more patterns that reliably ensure stability than patterns ensuring instability. This shows that the design of this system is strongly targeted towards maintaining stability. We also investigate the effect of allosteric regulators revealing that the tendency to stability is significantly increased by including experimentally determined regulatory mechanisms that have not yet been integrated into existing kinetic models.
The link between numerical magnitude and mechanisms of spatial orienting has been underlined in an increasing number of studies. Similarly, the relationship between numerical magnitude and grasping actions has started to be investigated. The present study focuses on the influence of numerical magnitude processing in the free choice of the position of an object. Participants were presented with a digit (1-9 without 5) and were required to decide whether it was smaller or larger than 5. Then, they had to grasp a small cube and change its position before vocally responding "higher" or "lower". Results showed that in the initial phase of the grasp movement, the grip aperture was modulated by the numerical magnitude. Moreover, participants shifted the position of the cube more leftward with smaller digits compared with larger ones, and they tended to position the object closer to themselves with smaller digits compared with larger ones. These results extend the previous findings indicating that the processing of magnitude is tightly related to the mechanisms of spatial orienting that subserve action execution.
Aim: The hydrolytic degradation behavior of degradable aliphatic polyester-based polymers is strongly influenced by the uptake or transport of water into the polymer matrix and also the hydrolysis rate of ester bonds.
Methods: We examined the volumetric swelling behavior of poly[(rac-lactide)-co-glycolide] (PLGA) and PLGA-based polyurethanes (PLGA-PU) with water contents of 0 wt%, 2 wt% and 7 wt% water at 310 K using a molecular modeling approach. Polymer systems with a number average molecular weight of M-n = 10,126 g.mol(-1) were constructed from PLGA with a lactide content of 67 mol%, whereby PLGA-PU systems were composed of five PLGA segments with M-n = 2052 g.mol(-1), which were connected via urethane linkers originated from 2,2,4-trimethyl hexamethylene-1,6-diisocyanate (TMDI), hexamethyl-1,6-diisocyanate (HDI), or L-lysine-1,6-diisocyanate (LDI).
Results: The calculated densities of the dry PLGA-PU systems were found to be lower than for pure PLGA. The obtained volumetric swelling of the PLGA-PU was depending on the type of urethane linker, whereby all swollen PLGA-PUs contained larger free volume distribution compared to pure PLGA. The mean square displacement curves for dry PLGA and PLGA-PUs showed that urethane linker units reduce the mobility of the polymer chains, while an increase in backbone atoms mobility was found, when water was added to these systems. Consequently, an increased water uptake of PLGA-PU matrices combined with a higher mobility of the chain segments should result in an accelerated hydrolytic chain scission rate in comparison to PLGA.
Conclusions: It can be anticipated that the incorporation of urethane linkers might be a helpful tool to adjust the degradation behavior of polyesters.
Aim: Multifunctional polymer-based biomaterials, which combine degradability with a shape-memory capability and in this way enable the design of actively moving implants such as self-anchoring implants or controlled release systems, have been recently introduced. Of particular interest are approved degradable polymers such as poly(L-lactide) (PLLA), which can be easily functionalized with a shape-memory effect. In the case of semicrystalline PLLA, the glass transition can be utilized as shape-memory switching domain.
Methods: In this work we applied a fully atomistic molecular dynamics simulation to study the shape-memory behavior of PLLA. A heating-deformation-cooling programming procedure was applied to atomistic PLLA packing models followed by a recovery module under stress-free conditions allowing the shape recovery. The recovery was simulated by heating the samples from T-low = 250 K to T-high = 500 K with different heating rates beta of 125, 40 and 4 K.ns(-1).
Results: We could demonstrate that the obtained strain recovery rate (R-r) was strongly influenced by the applied simulation time and heating rate, whereby R-r values in the range from 46% to 63% were achieved. On its own the application of a heating rate of 4 K.ns(-1) enabled us to determine a characteristic switching temperature of T-sw = 473 K for the modeled samples.
Conclusions: We anticipate that the atomistic modeling approach presented should be capable of enabling further study of T-sw with respect to the molecular structure of the investigated SMP and therefore could be applied in the context of design and development of new shape-memory (bio) materials.
Inhalt: - Verschiedene Dimensionen der Nachhaltigkeit - Das Gemeinsame der verschiedenen Dimensionen - Das Streben nach einem besseren Verständnis der Welt - Nachhaltigkeit - Ein allgemeines Modell der Nachhaltigkeit: Das »Existenzraum-Modell« - Das Metasystem Erde - Die Zukunftsfähigkeit der Gesellschaft
Disproportionate single-species contribution to canopy-soil nutrient flux in an Amazonian rainforest
(2012)
Rainfall, throughfall and stemflow were monitored on an event basis in an undisturbed open tropical rainforest with a large number of palm trees located in the southwestern Amazon basin of Brazil. Stemflow samples were collected from 24 trees with a diameter at breast height (DBH) > 5 cm, as well as eight young and four full-grown babassu palms (Attalea speciosa Mart.) for 5 weeks during the peak of the wet season. We calculated rainfall, throughfall and stemflow concentrations and fluxes of Na+, K+, Ca2+, Mg2+,, Cl-, SO42-, NO3- and H+ and stemflow volume-weighted mean concentrations and fluxes for three size classes of broadleaf trees and three size classes of palms. The concentrations of most solutes were higher in stemflow than in rainfall and increased with increasing tree and palm size. Concentration enrichments from rainfall to stemflow and throughfall were particularly high (81-fold) for NO3-. Stemflow fluxes of NO3- and H+ exceeded throughfall fluxes but stemflow fluxes of other solutes were less than throughfall fluxes. Stemflow solute fluxes to the forest soil were dominated by fluxes on babassu palms, which represented only 4% of total stem number and 10% of total basal area. For NO3-, stemflow contributed 51% of the total mass of nitrogen delivered to the forest floor (stemflow + throughfall) and represented more than a 2000-fold increase in NO3- flux compared what would have been delivered by rainfall alone on the equivalent area. Because these highly localized fluxes of both water and NO3- persist in time and space, they have the potential to affect patterns of soil moisture, microbial populations and other features of soil biogeochemistry conducive to the creation of hotspots for nitrogen leaching and denitrification, which could amount to an important fraction of total ecosystem fluxes. Because these hotspots occur over very small areas, they have likely gone undetected in previous studies and need to be considered as an important feature of the biogeochemistry of palm-rich tropical forest.
In landscapes which are predominately characterised by agriculture, natural ecosystems are often reduced to a mosaic of scattered patches of natural vegetation. Species with formerly connected distribution ranges now have restricted gene flow among populations. This has isolating effects upon population structure, because species are often confined by their limited dispersal capabilities. In this study, we test the effects of habitat fragmentation, precipitation, and isolation of populations on the genetic structure (AFLP) and fitness of the Asteraceae Catananche lutea. Our study area is an agro-dominated ecosystem in the desert-Mediterranean transition zone of the Southern Judea Lowlands in Israel. Our analysis revealed an intermediate level of intra-population genetic diversity across the study site with reduced genetic diversity on smaller scale. Although the size of the whole study area was relatively small (20 x 45 km), we found isolation by distance to be effective. We detected a high level of genetic differentiation among populations but genetic structure did not reflect spatial patterns. Population genetic diversity was correlated neither with position along the precipitation gradient nor with different seed types or other plant fitness variables in C. lutea.
Time-resolved emission data (fluorescence decay and fluorescence depolarization) of two three-color Forster resonance energy transfer (tc-FRET) systems consisting of a carbostyril donor (D), a ruthenium complex (Ru) as relay dye, and a Cy5 derivative (Cy) or, optionally, an anthraquinone quencher (Q) were carefully analyzed using advanced distribution analysis models. Thereby, it is possible to get information on the flexibility and mobility of the chromophores which are bound to double stranded (ds) DNA. Especially the distance distribution based on the analysis of the fluorescence depolarization is an attractive approach to complement data of fluorescence decay time analysis. The distance distributions extracted from the experimental data were in excellent agreement with those determined from accessible volume (AV) simulations. Moreover, the study showed that for tc-FRET systems the combination of dyes emitting on different time scales (e.g., nanoseconds vs microseconds) is highly beneficial in the distribution analysis of time-resolved luminescence data in cases where macromolecules such as DNA are involved. Here, the short lifetimes can yield information on the rotation of the dye molecule itself and the long lifetime can give insight in the overall dynamics of the macromolecule.
We introduce an approach to computing answer sets of logic programs, based on concepts successfully applied in Satisfiability (SAT) checking. The idea is to view inferences in Answer Set Programming (ASP) as unit propagation on nogoods. This provides us with a uniform constraint-based framework capturing diverse inferences encountered in ASP solving. Moreover, our approach allows us to apply advanced solving techniques from the area of SAT. As a result, we present the first full-fledged algorithmic framework for native conflict-driven ASP solving. Our approach is implemented in the ASP solver clasp that has demonstrated its competitiveness and versatility by winning first places at various solver contests.
We present the new multi-threaded version of the state-of-the-art answer set solver clasp. We detail its component and communication architecture and illustrate how they support the principal functionalities of clasp. Also, we provide some insights into the data representation used for different constraint types handled by clasp. All this is accompanied by an extensive experimental analysis of the major features related to multi-threading in clasp.
We show that it is possible to approximate the zeta-function of a curve over a finite field by meromorphic functions which satisfy the same functional equation and moreover satisfy (respectively do not satisfy) an analog of the Riemann hypothesis. In the other direction, it is possible to approximate holomorphic functions by simple manipulations of such a zeta-function. No number theory is required to understand the theorems and their proofs, for it is known that the zeta-functions of curves over finite fields are very explicit meromorphic functions. We study the approximation properties of these meromorphic functions.
Cell-to-cell diversity in a synchronized chlamydomonas culture as revealed by single-cell analyses
(2012)
In a synchronized photoautotrophic culture of Chlamydomonas reinhardtii, cell size, cell number, and the averaged starch content were determined throughout the light-dark cycle. For single-cell analyses, the relative cellular starch was quantified by measuring the second harmonic generation (SHG). In destained cells, amylopectin essentially represents the only biophotonic structure. As revealed by various validation procedures, SHG signal intensities are a reliable relative measure of the cellular starch content. During photosynthesis-driven starch biosynthesis, synchronized Chlamydomonas cells possess an unexpected cell-to-cell diversity both in size and starch content, but the starch-related heterogeneity largely exceeds that of size. The cellular volume, starch content, and amount of starch/cell volume obey lognormal distributions. Starch degradation was initiated by inhibiting the photosynthetic electron transport in illuminated cells or by darkening. Under both conditions, the averaged rate of starch degradation is almost constant, but it is higher in illuminated than in darkened cells. At the single-cell level, rates of starch degradation largely differ but are unrelated to the initial cellular starch content. A rate equation describing the cellular starch degradation
Hydrogen isotope values (delta D) of sedimentary aquatic and terrestrial lipid biomarkers, originating from algae, bacteria, and leaf wax, have been used to record isotopic properties of ancient source water (i.e., precipitation and/or lake water) in several mid-and high-latitude lacustrine environments. In the tropics, however, where both processes associated with isotope fractionation in the hydrologic system and vegetation strongly differ from those at higher latitudes, calibration studies for this proxy are not yet available. To close this gap of knowledge, we sampled surface sediments from 11 lakes in Cameroon to identify those hydro-climatological processes and physiological factors that determine the hydrogen isotopic composition of aquatic and terrestrial lipid biomarkers. Here we present a robust framework for the application of compound-specific hydrogen isotopes in tropical Africa. Our results show that the delta D values of the aquatic lipid biomarker n-C(17) alkane were not correlated with the delta D values of lake water. Carbon isotope measurements indicate that the n-C(17) alkane was derived from multiple source organisms that used different hydrogen pools for biosynthesis. We demonstrate that the delta D values of the n-C(29) alkane were correlated with the delta D values of surface water (i.e., river water and groundwater), which, on large spatial scales, reflect the isotopic composition of mean annual precipitation. Such a relationship has been observed at higher latitudes, supporting the robustness of the leaf-wax lipid delta D proxy on a hemispheric spatial scale. In contrast, the delta D values of the n-C(31) alkane did not show such a relationship but instead were correlated with the evaporative lake water delta D values. This result suggests distinct water sources for both leaf-wax lipids, most likely originating from two different groups of plants. These new findings have important implications for the interpretation of long-chain n-alkane delta D records from ancient lake sediments. In particular, a robust interpretation of palaeohydrological data requires knowledge of the vegetation in the catchment area as different plants may utilise different water sources. Our results also suggest that the combination of carbon and hydrogen isotopes does help to differentiate between the metabolic pathway and/or growth form of organisms and therefore, the source of hydrogen used during lipid biosynthesis.
The 'wet' early to mid-Holocene of tropical Africa, with its enhanced monsoon, ended with an abrupt shift toward drier conditions and was ultimately replaced by a drier climate that has persisted until the present day. The forcing mechanisms, the timing, and the spatial extent of this major climatic transition are not well understood and remain the subject of ongoing research. We have used a detailed palaeo-shoreline record from Lake Turkana (Kenya) to decipher and characterise this marked climatic transition in East Africa. We present a high-precision survey of well-preserved palaeo-shorelines, new radiocarbon ages from shoreline deposits, and oxygen-isotope measurements on freshwater mollusk shells to elucidate the Holocene moisture history from former lake water-levels in this climatically sensitive region. In combination with previously published data our study shows that during the early Holocene the water-level in Lake Turkana was high and the lake overflowed temporarily into the White Nile drainage system. During the mid-Holocene (similar to 5270 +/- 300 cal. yr BP), however, the lake water-level fell by similar to 50 m, coeval with major episodes of aridity on the African continent. A comparison between palaeo-hydrological and archaeological data from the Turkana Basin suggests that the mid-Holocene climatic transition was associated with fundamental changes in prehistoric cultures, highlighting the significance of natural climate variability and associated periods of protracted drought as major environmental stress factors affecting human occupation in the East African Rift System. (
We employ the ultrafast response of a 15.4 nm thin SrRuO3 layer grown epitaxially on a SrTiO3 substrate to perform time-domain sampling of an x-ray pulse emitted from a synchrotron storage ring. Excitation of the sample with an ultrashort laser pulse triggers coherent expansion and compression waves in the thin layer, which turn the diffraction efficiency on and off at a fixed Bragg angle during 5 ps. This is significantly shorter than the duration of the synchrotron x-ray pulse of 100 ps. Cross-correlation measurements of the ultrafast sample response and the synchrotron x-ray pulse allow to reconstruct the x-ray pulse shape.
We present a minimal conceptual model for the Atlantic meridional overturning circulation which incorporates the advection of salinity and the basic dynamics of the oceanic pycnocline. Four tracer transport processes following Gnanadesikan in Science 283(5410):2077-2079, (1999) allow for a dynamical adjustment of the oceanic pycnocline which defines the vertical extent of a mid-latitudinal box. At the same time the model captures the salt-advection feedback (Stommel in Tellus 13(2):224-230, (1961)). Due to its simplicity the model can be solved analytically in the purely wind- and purely mixing-driven cases. We find the possibility of abrupt transition in response to surface freshwater forcing in both cases even though the circulations are very different in physics and geometry. This analytical approach also provides expressions for the critical freshwater input marking the change in the dynamics of the system. Our analysis shows that including the pycnocline dynamics in a salt-advection model causes a decrease in the freshwater sensitivity of its northern sinking up to a threshold at which the circulation breaks down. Compared to previous studies the model is restricted to the essential ingredients. Still, it exhibits a rich behavior which reaches beyond the scope of this study and might be used as a paradigm for the qualitative behaviour of the Atlantic overturning in the discussion of driving mechanisms.
Laser-induced condensed phase reactions are often interpreted as nonequilibrium phenomena that go beyond conventional thermodynamics. Here, we show by Langevin dynamics and for the example of femtosecond-laser desorption of hydrogen from a ruthenium surface that light adsorbates thermalize rapidly due to ultrafast energy redistribution after laser excitation. Despite the complex reaction mechanism involving hot electrons in the surface region, all desorption product properties are characterized by equilibrium distributions associated with a single, unique temperature. This represents an example of ultrahot chemistry on the subpicosecond time scale.
Selective excitation of molecule-surface vibrations in H2 and D2 dissociatively adsorbed on Ru(0001)
(2012)
In this contribution we report about the selective vibrational excitation of H2 and D2 on Ru(0001) as an example for nonadiabatic coupling of an open quantum system to a dissipative environment. We investigate the possibility of achieving state-selective vibrational excitations of H2 and D2 adsorbed on a Ru(0001) surface using picosecond infrared laser pulses. The systems behavior is explored using pulses that are rationally designed and others that are optimized using a time-local variant of Optimal Control Theory. The effects of dissipation on the laser-driven dynamics are studied using the reduced-density matrix formalism. The non-adiabatic couplings between adsorbate and surface are computed perturbatively, for which our recently introduced state-resolved anharmonic rate model is used. It is shown that mode- and state-selective excitation can be achieved in the absence of dissipation when using optimized laser pulses. The inclusion of dissipation in the model reduces the state selectivity and the population transfer yield to highly excited states. In this case, mode activation is most effectively realized by a rational pulse of carefully chosen duration rather than by a locally optimized pulse.
East African paleoenvironments are highly variable, marked by extreme fluctuations in moisture availability, which has far-reaching implications for the origin, evolution and dispersal of Homo sapiens in and beyond the region. This paper presents results from a pilot core from the Chew Bahir basin in southern Ethiopia that records the climatic history of the past 45 ka, with emphasis on the African Humid Period (AHP, similar to 15-5 ka calBP). Geochemical, physical and biological indicators show that Chew Bahir responded to climatic fluctuations on millennial to centennial timescales, and to the precessional cycle, since the Last Glacial Maximum. Potassium content of the sediment appears to be a reliable proxy for aridity, showing that Chew Bahir reacted to the insolation-controlled humidity increase of the AHP with a remarkably abrupt onset and a gradual termination, framing a sharply defined arid phase (similar to 12.8-11.6 ka calBP) corresponding to the Younger Dryas chronozone. The Chew Bahir record correlates well with low- and high-latitude paleoclimate records, demonstrating that the site responded to regional and global climate changes.
Spatially explicit multi-year crop information is required for many environmental applications. The study presented here proposes a hierarchical classification approach for per-plot crop type identification that is based on spectral-temporal profiles and accounts for deviations from the average growth stage timings by incorporating agro-meteorological information in the classification process. It is based on the fact that each crop type has a distinct seasonal spectral behavior and that the weather may accelerate or delay crop development. The classification approach was applied to map 12 crop types in a 14,000 km(2) catchment area in Northeast Germany for several consecutive years. An accuracy assessment was performed and compared to those of a maximum likelihood classification. The 7.1% lower overall classification accuracy of the spectral-temporal profiles approach may be justified by its independence of ground truth data. The results suggest that the number and timing of image acquisition is crucial to distinguish crop types. The increasing availability of optical imagery offering a high temporal coverage and a spatial resolution suitable for per-plot crop type mapping will facilitate the continuous refining of the spectral-temporal profiles for common crop types and different agro-regions and is expected to improve the classification accuracy of crop type maps using these profiles.
The aims of this study were to identify areas of wind erosion and dust deposition and to quantify the effects of different grazing intensities on soil redistribution rates in grasslands based on the Cs-137 technique. Because the method uses a reference inventory as threshold for erosion or deposition, the classification of any other site as source or sink for dust depends on the accurate selection of this reference site.
Measurements of Cs-137 inventories and depth distributions were carried out at pasture sites with predominant species of Stipa grandis and Leymus chinensis which are grazed with different intensities. Additional measurements were made at arable land, plant-covered sand dunes and alluvial plains. Wind-induced soil erosion and dust deposition rates were calculated from Cs-137 inventories by means of the "Profile-Distribution" and the "Mass Balance II" models.
The selection of the reference site was based on fluid dynamical and process-determining parameters. The chosen site should meet the following four conditions: (i) located at a summit position with obviously low deposition rates, (ii) sufficient vegetation cover to prevent wind erosion, (iii) plane to exclude water erosion and (iv) in the wind/dust shadow of a higher elevation. The measured reference inventory of Cs-137 was 1967(+/- 102) Bqm(-2) located at a summit position of moderately grazed Leymus chinensis steppe. The Cs-137 inventories at other sites ranged from 1330 Bqm(-2) at heavily grazed sites to 5119 Bqm(-2) at river deposits, representing annual average soil losses of up to 130 tkm(-2) and deposits of up to 540 tkm(-2), respectively. The calculated annual averages of dust depositions at ungrazed Leymus chinensis sites were related to the dust storm frequencies of the last 50 years resulting in a description of the temporal variability of annual dust depositions from about 154 tkm(-2) in the 1960s to 26 tkm(-2) at recent times. Based on this quantification already 80% of the total dust depositions can be related to the 20 years between the 1960s and the end of the 1970s and only 20% to the time between 1980 and 2001.
Cs-137 technique is a promising method to assess the effect of grazing intensity and land use types on the spatial variability of wind-induced soil and dust redistribution processes in semi-arid grasslands. However, considerable efforts are needed to identify a reliable reference site, because erosion and deposition induced by wind may occur at the same places. The combination of the dust deposition rates derived from Cs-137 profile data with the dust storm frequencies is helpful for a better reconstruction of the temporal variability of dust deposition and wind erosion in this region. The calculated recent deposition rates of about 20 tkm(-2) are in good agreement with data of other authors.
Der Autor diskutiert die Chancen und Risiken bei der Einbindung
des Südens in die internationale Klimapolitik. Lange Zeit hatten die
Entwicklungsländer am wenigsten zum Klimawandel beigetragen,
wären aber am stärksten von ihm betroffen. Mittlerweile jedoch tragen
diese Länder in erheblichem Maße selbst zum Klimawandel bei. Allerdings
setzen deren Regierungen auf Zeit. Sie erwarten Ressourcentransfers.
Dies verstärkt auch alte Probleme des ‚Rent-Seeking‘.
An experimental and computational study on the impact of functional groups on the oxidation stability of higher acenes is presented. We synthesized anthracenes, tetracenes, and pentacenes with various substituents at the periphery, identified their photooxygenation products, and measured the kinetics. Furthermore, the products obtained from thermolysis and the kinetics of the thermolysis are investigated. Density functional theory is applied in order to predict reaction energies, frontier molecular orbital interactions, and radical stabilization energies. The combined results allow us to describe the mechanisms of the oxidations and the subsequent thermolysis. We found that the alkynyl group not only enhances the oxidation stability of acenes but also protects the resulting endoperoxides from thermal decomposition. Additionally, such substituents increase the regioselectivity of the photooxygenation of tetracenes and pentacenes. For the first time, we oxidized alkynylpentacenes by using chemically generated singlet oxygen (O-1(2)) without irradiation and identified a 6,13-endoperoxide as the sole regioisomer. The bimolecular rate constant of this oxidation amounts to only 1 X 10(5) s(-1) M-1. This unexpectedly slow reaction is a result of a physical deactivation of O-1(2). In contrast to unsubstituted or aryl-substituted acenes, photooxygenation of alkynyl-substituted acenes proceeds most likely by a concerted mechanism, while the thermolysis is well explained by the formation of radical intermediates. Our results should be important for the future design of oxidation stable acene-based semiconductors.
Relaxation processes and structural transitions in nonstretched and uniaxially stretched films of poly(vinylidene fluoride-hexafluoropropylene) (P(VDF-HFP)) and its homopolymer polyvinylidene fluoride (PVDF) for comparison were investigated with the aim of understanding the electromechanical properties of this lower-modulus ferroelectric copolymer. The mechanical and the dielectric response at the glass transition ( relaxation) exhibit similar temperature dependence of the relaxation time, whereas mechanical and dielectric processes above the glass transition are not related. They represent a continuous softening process within the amorphous phase and the dielectric relaxation, respectively. The latter is attributed to conformational changes of VDF segments in lamellae of spherulites constituting the nonpolar crystalline phase. Furthermore, there is a contribution from melting of secondary crystallites formed in the amorphous phase during annealing or storage. Mechanically, this transition appears in nonstretched and stretched films as an accelerated decrease of the elastic modulus that terminates the rubber plateau. Dielectrically, this transition becomes visible as a frequency-independent loss peak only in stretched films, because stretching removes the relaxation, which superimposes the transition in nonstretched films. Melting of secondary crystallites is shown to appear in the homopolymer, too, though less pronounced because of more complete primary crystallisation.
Stretching increases the modulus above the glass transition only slightly, and it does not significantly influence the softening process. On the other hand, stretching causes a spontaneous polarisation and introduces order within the amorphous phase, rendering it more polar. Melting of secondary crystallites provides an additional contribution to the polarisation. These findings may explain the relatively high electromechanical activity of P(VDF-HFP) but also its relatively low thermal stability. Moreover, they may be important for correct procedure and analysis of temperature-dependent dielectric measurements on partially crystalline polymers, in particular on those with less favourable sterical conditions for primary crystallisation.
Beringian climate and environmental history are poorly characterized at its easternmost edge. Lake sediments from the northern Yukon Territory have recorded sedimentation, vegetation, summer temperature and precipitation changes since similar to 16 cal ka BP. Herb-dominated tundra persisted until similar to 14.7 cal ka BP with mean July air temperatures <= 5 degrees C colder and annual precipitation 50 to 120 mm lower than today. Temperatures rapidly increased during the Bolling/Allerod interstadial towards modern conditions, favoring establishment of Betula-Salix shrub tundra. Pollen-inferred temperature reconstructions recorded a pronounced Younger Dryas stadial in east Beringia with a temperature drop of similar to 1.5 degrees C (similar to 2.5 to 3.0 degrees C below modern conditions) and low net precipitation (90 to 170 mm) but show little evidence of an early Holocene thermal maximum in the pollen record. Sustained low net precipitation and increased evaporation during early Holocene warming suggest a moisture-limited spread of vegetation and an obscured summer temperature maximum. Northern Yukon Holocene moisture availability increased in response to a retreating Laurentide Ice Sheet, postglacial sea level rise, and decreasing summer insolation that in turn led to establishment of Alnus-Berula shrub tundra from similar to 5 cal ka BP until present, and conversion of a continental climate into a coastal-maritime climate near the Beaufort Sea.
We correlate the morphology and energy level alignment of bilayer structures comprising the donor poly(3-hexylthiophene) (P3HT) and the acceptor polyfluorene copolymer poly(9,90dialklylfluorene-alt-4,7-bis(2,5-thiendiyl)-2,1,3-benzothiadiazole) (PFTBTT) with the performance of these bilayers in organic photovoltaic cells (OPVCs). The conducting polymer poly(ethylenedioxythiophene): poly (styrenesulfonate) (PEDT:PSS) was used as the bottom electrode and Ca as the top electrode. Ultraviolet photoelectron spectroscopy (UPS) revealed that notable interface dipoles occur at all interfaces across the OPVC structure, highlighting that vacuum level alignment cannot reliably be used to estimate the electronic properties for device design. Particularly the effective electrode work function values (after contact formation with the conjugated polymers) differ significantly from those of the pristine electrode materials. Chemical reactions between PEDT: PSS and P3HT on the one hand and Ca and PFTBTT on the other hand are identified as cause for the measured interface dipoles. The vacuum level shift between P3HT and PFTBTT is related to mutual energy level pinning at gap states. Annealing induced morphological changes at the P3HT/PFTBTT interface increased the efficiency of OPVCs, while the electronic structure was not affected by thermal treatment.
Orbitolinids are larger foraminifera widespread in Lower Cretaceous shallow-water carbonates of the Tethyan realm. They are among the most important fossil groups used for Biostratigraphy. Despite this and although the structural features of the group have been described in detail, very little is known about the composition of their agglutinated test and the process by which they selected foreign grains. In this study, the test of Orbitolina d'Orbigny, 1850 (subgenus Mesorbitolina Schroeder, 1962) from Aptian shallow-water carbonate deposits of southern Italy has been studied in detail. We combine petrographic techniques (optical microscope and SEM) with energy-dispersive x-ray spectrometry (EDS), electron probe microanalyzer (EPMA), X-ray diffraction and Raman spectroscopy analyses.
The results show that the test of Mesorbitolina is composed of carbonate and non-carbonate agglutinated grains with the latter distributed across the test with a specific pattern, moving from the marginal to the central zone. In the marginal zone, non-carbonate grains are found only in the epidermis and along the septa which are composed of quartz, with smaller amounts of illite/muscovite and K-feldspar grains. In the central zone of the test, non-carbonate grains are distributed in two ways. Coarse grains of quartz and K-feldspar are abundant and randomly placed in the endoskeleton embedded in a mosaic of minute carbonate grains. Flat grains, mainly of illite/muscovite constitute the external part of the septa. Our observations indicate that Mesorbitolina did select and place agglutinated grains across its test, mainly according to their shape, whereas it did not select particles according to grain size. The distribution of agglutinated particles according to their mineralogical composition shows some contradictory evidence and therefore, at the moment, grain selection in function of mineralogy cannot be completely confirmed or ruled out. Analogies in the test composition of Mesorbitolina specimens from coeval deposits from different areas of southern Italy indicate that the features of their agglutinated test are typical characters of the genus Mesorbitolina. However, it is still unclear what advantage was obtained by the foraminifer by the described test features.
Purpose: Polymer networks with adjustable properties prepared from endgroup-functionalized oligoesters by UV-crosslinking in melt have evolved into versatile multifunctional biomaterials. In addition to the molecular weight or architecture of precursors, the reaction conditions for crosslinking are pivotal for the polymer network properties. Crosslinking of precursors in solution may facilitate low-temperature processes and are compared here to networks synthesized in melt.
Methods: Oligo(epsilon-caprolactone)-(z) methacrylate (oCL-(z) IEMA) precursors with a linear (z = di) or a four-armed star-shaped (z = tetra) architecture were crosslinked by radical polymerization in melt or in solution with UV irradiation. The thermal, mechanical, and swelling properties of the polymer networks obtained were characterized.
Results: Crosslinking in solution resulted in materials with lower Young's moduli (E), lower maximum stress (sigma(max)), and higher elongation at break (epsilon(B)) as determined at 70 degrees C. Polymer networks from 8 kDa star-shaped precursors exhibited poor elasticity when synthesized in the melt, but can be established as stretchable materials with a semi-crystalline morphology, a high gel-content, and a high elongation at break when prepared in solution.
Conclusions: The crosslinking condition of methacrylate functionalized precursors significantly affected network properties. For some types of precursors such as star-shaped telechelics, synthesis in solution provided semi-crystalline elastic materials that were not accessible from crosslinking in melt.
The present study reports a facile approach for sulfite biosensing, based on enhanced direct electron transfer of a human sulfite oxidase (hSO) immobilized on a gold nanoparticles modified electrode. The spherical core shell AuNPs were prepared via a new method by reduction of HAuCl4 with branched poly(ethyleneimine) in an ionic liquids resulting particles with a diameter less than 10 nm. These nanoparticles were covalently attached to a mercaptoundecanoic acid modified Au-electrode where then hSO was adsorbed and an enhanced interfacial electron transfer and electrocatalysis was achieved. UV/Vis and resonance Raman spectroscopy, in combination with direct protein voltammetry, are employed for the characterization of the system and reveal no perturbation of the structural integrity of the redox protein. The proposed biosensor exhibited a quick steady-state current response, within 2 s, a linear detection range between 0.5 and 5.4 mu M with a high sensitivity (1.85 nA mu M-1). The investigated system provides remarkable advantages in the possibility to work at low applied potential and at very high ionic strength. Therefore these properties could make the proposed system useful in the development of bioelectronic devices and its application in real samples.
In this paper, we analytically study a star motif of Stuart-Landau oscillators, derive the bifurcation diagram and discuss the different forms of synchronization arising in such a system. Despite the parameter mismatch between the central node and the peripheral ones, an analytical approach independent of the number of units in the system has been proposed. The approach allows to calculate the separatrices between the regions with distinct dynamical behavior and to determine the nature of the different transitions to synchronization appearing in the system. The theoretical analysis is supported by numerical results.
Grenzen : Einführung
(2012)
With ongoing miniaturization of electronic devices, the need for individually addressable, switchable molecules arises. An example are azobenzenes on surfaces which have been shown to be switchable between trans and cis forms. Here, we examine the "direct" (rather than substrate-mediated) channel of the trans -> cis photoisomerization after pi pi* excitation of tetra-tert-butyl-azobenzene physisorbed on surfaces mimicking Au(111) and Bi(111), respectively. In spirit of the direct channel, the electronic structure of the surface is neglected, the latter merely acting as a rigid platform which weakly interacts with the molecule via Van-der-Waals forces. Starting from thermal ensembles which represent the trans-form, sudden excitations promote the molecules to pi pi*-excited states which are non-adiabatically coupled among themselves and to a n pi*-excited and the ground state, respectively. After excitation, relaxation to the ground state by internal conversion takes place, possibly accompanied by isomerization. The process is described here by "on the fly" semiclassical surface hopping dynamics in conjunction with a semiempirical Hamiltonian (AM1) and configuration-interaction type methods. It is found that steric constraints imposed by the substrate lead to reduced but non-vanishing, trans -> cis reaction yields and longer internal conversion times than for the isolated molecule. Implications for recent experiments for azobenzenes on surfaces are discussed.
There is much recent interest in the idea that we represent our knowledge together with the sensory and motor features that were activated during its acquisition. This paper reviews the evidence for such "embodiment" in the domain of numerical cognition, a traditional stronghold of abstract theories of knowledge representation. The focus is on spatial-numerical associations, such as the SNARC effect (small numbers are associated with left space, larger numbers with right space). Using empirical evidence from behavioral research, I first describe sensory and motor biases induced by SNARC, thus identifying numbers as embodied concepts. Next, I propose a hierarchical relationship between grounded, embodied, and situated aspects of number knowledge. This hierarchical conceptualization helps to understand the variety of SNARC-related findings and yields testable predictions about numerical cognition. I report several such tests, ranging from cross-cultural comparisons of horizontal and vertical SNARC effects (Shaki and Fischer in J Exp Psychol Hum Percept Perform 38(3): 804-809, 2012) to motor cortical activation studies in adults with left- and right-hand counting preferences (Tschentscher et al. in NeuroImage 59: 3139-3148, 2012). It is concluded that the diagnostic features for each level of the proposed hierarchical knowledge representation, together with the spatial associations of numbers, make the domain of numerical knowledge an ideal testing ground for embodied cognition research.
Parenchyma cells from tubers of Solanum tuberosum L. convert several externally supplied sugars to starch but the rates vary largely. Conversion of glucose 1-phosphate to starch is exceptionally efficient. In this communication, tuber slices were incubated with either of four solutions containing equimolar [U-C-14]glucose 1-phosphate, [U-C-14]sucrose, [U-C-14]glucose 1-phosphate plus unlabelled equimolar sucrose or [U-C-14]sucrose plus unlabelled equimolar glucose 1-phosphate. C-14-incorporation into starch was monitored. In slices from freshly harvested tubers each unlabelled compound strongly enhanced C-14 incorporation into starch indicating closely interacting paths of starch biosynthesis. However, enhancement disappeared when the tubers were stored. The two paths (and, consequently, the mutual enhancement effect) differ in temperature dependence. At lower temperatures, the glucose 1-phosphate-dependent path is functional, reaching maximal activity at approximately 20 degrees C but the flux of the sucrose-dependent route strongly increases above 20 degrees C. Results are confirmed by in vitro experiments using [U-C-14]glucose 1-phosphate or adenosine-[U-C-14]glucose and by quantitative zymograms of starch synthase or phosphorylase activity. In mutants almost completely lacking the plastidial phosphorylase isozyme(s), the glucose 1-phosphate-dependent path is largely impeded. Irrespective of the size of the granules, glucose 1-phosphate-dependent incorporation per granule surface area is essentially equal. Furthermore, within the granules no preference of distinct glucosyl acceptor sites was detectable. Thus, the path is integrated into the entire granule biosynthesis. In vitro C-14-incorporation into starch granules mediated by the recombinant plastidial phosphorylase isozyme clearly differed from the in situ results. Taken together, the data clearly demonstrate that two closely but flexibly interacting general paths of starch biosynthesis are functional in potato tuber cells.
We studied the spreading of feature-based attention from attended to ignored motion fields (linear, circular, and combinations). When observers attended one of two superimposed motion fields on one side of the visual midline, sub-threshold priming by an ignored motion field was altered significantly on the opposite side of the midline. This attentional spreading was observed only when attended and ignored motion fields conformed to a complex global flow, not when they shared the same linear motion. These findings corroborate an earlier study (Festman & Braun, 2010), which obtained similar results with a complementary methodology. We conclude that feature-based attention is more complex than hitherto appreciated in that it spreads preferentially in an object-specific manner.
Bilingual speakers are faced with the problem to keep their languages apart, but do so with interindividually varying success. Cognitive control abilities might be an important factor to explain such interindividual differences. Here we compare two late, balanced and highly proficient bilingual groups (mean age 24 years, L1 Russian, L2 German) which were established according to their language control abilities on a bilingual picture-naming task. One group had difficulties to remain in the instructed target language and switched unintentionally to the non-target language ("switchers"), whereas the other group rarely switched unintentionally ("non-switchers"). This group-specific behavior could not be explained by language background, socio-cultural, or demographic variables. Rather, the non-switchers also demonstrated a faster and better performance on four cognitive control tests (Tower of Hanoi, Ruff Figural Fluency Test, Divided Attention, Go/Nogo). Here, we focus on two additional executive function tasks, theWisconsin Card SortingTest (WCST) and the Flanker task requiring conflict monitoring and conflict resolution. Non-switchers outperformed switchers with regard to speed and accuracy, and were better at finding and applying the correct rules in the WCST. Similarly, in the Flanker task non-switchers performed faster and better on conflict trials and had a higher correction rate following an error. Event-related potential recordings furthermore revealed a smaller error-related negativity in the non-switchers, taken as evidence for a more efficient self-monitoring system. We conclude that bilingual language performance, in particular switching behavior, is related to performance on cognitive control tasks. Better cognitive control, including conflict monitoring, results in decreased unintentional switching.
Although all bilinguals encounter cross-language interference (CLI), some bilinguals are more susceptible to interference than others. Here, we report on language performance of late bilinguals (Russian/German) on two bilingual tasks (interview, verbal fluency), their language use and switching habits. The only between-group difference was CLI: one group consistently produced significantly more errors of CLI on both tasks than the other (thereby replicating our findings from a bilingual picture naming task). This striking group difference in language control ability can only be explained by differences in cognitive control, not in language proficiency or language mode.
Using the eye-movement monitoring technique in two reading comprehension experiments, this study investigated the timing of constraints on wh-dependencies (so-called island constraints) in first- and second-language (L1 and L2) sentence processing. The results show that both L1 and L2 speakers of English are sensitive to extraction islands during processing, suggesting that memory storage limitations affect L1 and L2 comprehenders in essentially the same way. Furthermore, these results show that the timing of island effects in L1 compared to L2 sentence comprehension is affected differently by the type of cue (semantic fit versus filled gaps) signaling whether dependency formation is possible at a potential gap site. Even though L1 English speakers showed immediate sensitivity to filled gaps but not to lack of semantic fit, proficient German-speaking learners of English as a L2 showed the opposite sensitivity pattern. This indicates that initial wh-dependency formation in L2 processing is based on semantic feature matching rather than being structurally mediated as in L1 comprehension.
Clustering of gene expression data is often done with the latent aim of dimension reduction, by finding groups of genes that have a common response to potentially unknown stimuli. However, what is poorly understood to date is the behaviour of a low dimensional signal embedded in high dimensions. This paper introduces a multicollinear model which is based on random matrix theory results, and shows potential for the characterisation of a gene cluster's correlation matrix. This model projects a one dimensional signal into many dimensions and is based on the spiked covariance model, but rather characterises the behaviour of the corresponding correlation matrix. The eigenspectrum of the correlation matrix is empirically examined by simulation, under the addition of noise to the original signal. The simulation results are then used to propose a dimension estimation procedure of clusters from data. Moreover, the simulation results warn against considering pairwise correlations in isolation, as the model provides a mechanism whereby a pair of genes with 'low' correlation may simply be due to the interaction of high dimension and noise. Instead, collective information about all the variables is given by the eigenspectrum.
Clusters of codons pairing to low-abundance tRNAs synchronize the translation with co-translational folding of single domains in multidomain proteins. Although proven with some examples, the impact of the ribosomal speed on the folding and solubility on a global, cell-wide level remains elusive. Here we show that upregulation of three low-abundance tRNAs in Escherichia coil increased the aggregation propensity of several cellular proteins as a result of an accelerated elongation rate. Intriguingly, alterations in the concentration of the natural tRNA pool compromised the solubility of various chaperones consequently rendering the solubility of some chaperone-dependent proteins.
This article studies proactive work behavior from a within-person perspective. Building on the broaden-and-build model and the mood-as-information approach, we hypothesized that negative trait affect and positive state affect predict the relative time spent on proactive behavior. Furthermore, based on self-determination theory we argued that persons want to feel competent and that proactive behavior is one way to experience competence. In an experience-sampling study, 52 employees responded to surveys 3 times a day for 5 days. Hierarchical linear modeling confirmed the hypotheses on trait and state affect. Analyses furthermore showed that although a higher level of experienced competence at core task activities was associated with a subsequent increase in time spent on these activities, low experienced competence predicted an increase in time spent on proactive behavior.
The use of CO2 as a massive and polarizable drift gas is shown to greatly improve peak-to-peak resolution (Rp-p), as compared with N2, for the separation of disaccharides in a Synapt G2 traveling wave ion mobility cell. Near or baseline Rp-p was achieved for three pairs of sodiated molecules of disaccharide isomers, that is, cellobiose and sucrose (Rp-p?=?0.76), maltose and sucrose (Rp-p?=?1.04), and maltose and lactose (Rp-p?=?0.74). Ion mobility mass spectrometry using CO2 as the drift gas offers therefore an attractive alternative for fast and efficient separation of isomeric disaccharides.
Piezoelectrets are novel transducer materials which can be widely applied in sensors and actuators. Here, three techniques for determining piezoelectric d(33) coefficients of piezoelectrets are reviewed and compared. Two types of piezoelectrets, polyethylene-naphthalate (PEN) polymer-foam piezoelectrets and fluorinated ethylene-propylene (FEP) copolymer-layer piezoelectrets, have been prepared and measured by means of dynamic, resonance, and acoustical methods. The dynamic measurements show that the d(33) coefficient of PEN-foam samples clearly decreases with increasing stress, but 80% of the initial d(33) can be retained after 1800 cycles of a continuous dynamic measurement in a mechanical fatigue test. The resonance measurements demonstrate that both PEN-foam and FEP-layer samples exhibit clear electro-mechanical resonances. PEN-foam samples show elastic moduli in the range from 1 to 12 MPa and d(33) values up to 500 pC N-1, while FEP-layer samples show homogeneous elastic moduli of about 0.3 MPa and d(33) values of about 280 pC N-1. The acoustical measurements reveal that both PEN-foam and FEP-layer samples exhibit stable frequency responses in the range from 5.7 to 20 kHz. In addition, d(33) coefficients obtained with different experimental methods are in good agreement with each other, which confirms the reliability of all three techniques.
Earthquake-triggered landslide dams are potentially dangerous disrupters of water and sediment flux in mountain rivers, and capable of releasing catastrophic outburst flows to downstream areas. We analyze an inventory of 828 landslide dams in the Longmen Shan mountains, China, triggered by the M-w 7.9 2008 Wenchuan earthquake. This database is unique in that it is the largest of its kind attributable to a single regional-scale triggering event: 501 of the spatially clustered landslides fully blocked rivers, while the remainder only partially obstructed or diverted channels in steep watersheds of the hanging wall of the Yingxiu-Beichuan Fault Zone. The size distributions of the earthquake-triggered landslides, landslide dams, and associated lakes (a) can be modeled by an inverse gamma distribution; (b) show that moderate-size slope failures caused the majority of blockages; and (c) allow a detailed assessment of seismically induced river-blockage effects on regional water and sediment storage. Monte Carlo simulations based on volumetric scaling relationships for soil and bedrock failures respectively indicate that 14% (18%) of the estimated total coseismic landslide volume of 6.4 (14.6) x 10(9) m(3) was contained in landslide dams, representing only 1.4% of the >60,000 slope failures attributed to the earthquake. These dams have created storage capacity of similar to 0.6x 10(9) m(3) for incoming water and sediment. About 25% of the dams containing 2% of the total river-blocking debris volume failed one week after the earthquake; these figures had risen to 60% (similar to 20%), and >90% (>90%) within one month, and one:year, respectively, thus also emptying similar to 92% of the total potential water and sediment storage behind these, dams within one year following the earthquake. Currently only similar to 0.08 x 10(9) m(3) remain available as natural reservoirs for storing water and sediment, while similar to 0.19 x 10(9) m(3), i.e. about a third of the total river-blocking debris volume, has been eroded by rivers. Dam volume and upstream catchment area control to first order the longevity of the barriers, and bivariate domain plots are consistent with the observation that most earthquake-triggered landslide dams were ephemeral. We conclude that the river-blocking portion of coseismic slope failures disproportionately modulates the post-seismic sediment flux in the Longmen Shan on annual to decadal timescales.
Amonchquite dyke, in the vicinity of Loch Roag, Lewis, Outer Hebrides has an unusually enriched chemistry, and contains a unique assemblage of megacrysts and xenoliths from the lithosphere of the Hebridean craton. A Ar-40/Ar-39 plateau age of 45.2 +/- 0.2 Ma (2 sigma) of a phlogopite megacryst from the dyke overlaps an earlier reported K-Ar age, and confirms that the British Palaeogene Igneous Province extended into the Eocene. Similar late low-volume melts were erupted in the Eocene and Oligocene in West and East Greenland, suggesting that such late-stage magmatic rejuvenescence is a widespread feature across the North Atlantic Igneous Province.
Information integration across company borders becomes increasingly important for the success of product lifecycle management in industry and complex supply chains. Semantic technologies are about to play a crucial role in this integrative process. However, cross-company data exchange requires mechanisms to enable fine-grained access control definition and enforcement, preventing unauthorized leakage of confidential data across company borders. Currently available semantic repositories are not sufficiently equipped to satisfy this important requirement. This paper presents an infrastructure for controlled sharing of semantic data between cooperating business partners. First, we motivate the need for access control in semantic data federations by a case study in the industrial service sector. Furthermore, we present an architecture for controlling access to semantic repositories that is based on our newly developed SemForce security service. Finally, we show the practical feasibility of this architecture by an implementation and several performance experiments.
Sk 183 is the visually brightest star in the N90 nebula, a young star-forming region in the Wing of the Small Magellanic Cloud (SMC). We present new optical spectroscopy from the Very Large Telescope which reveals Sk 183 to be one of the most massive O-type stars in the SMC. Classified as an O3-type dwarf on the basis of its nitrogen spectrum, the star also displays broadened He I absorption, which suggests a later type. We propose that Sk 183 has a composite spectrum and that it is similar to another star in the SMC, MPG 324. This brings the number of rare O2- and O3-type stars known in the whole of the SMC to a mere four. We estimate physical parameters for Sk 183 from analysis of its spectrum. For a single-star model, we estimate an effective temperature of 46 +/- 2 kK, a low mass-loss rate of similar to 10(-7) M-circle dot yr(-1), and a spectroscopic mass of 46(-8)(+ 9) M-circle dot (for an adopted distance modulus of 18.7 mag to the young population in the SMC Wing). An illustrative binary model requires a slightly hotter temperature (similar to 47.5 kK) for the primary component. In either scenario, Sk 183 is the earliest-type star known in N90 and will therefore be the dominant source of hydrogen-ionizing photons. This suggests Sk 183 is the primary influence on the star formation along the inner edge of the nebula.
A direct competitive homogeneous immunoassay for progesterone - the Redox Quenching Immunoassay
(2012)
A direct competitive amperometric immunoassay format for the detection of haptens and proteins was developed. The method is based on the quenching of electroactivity of ferrocenium, which is coupled to the antigen and used as the primary reporter, upon binding to a monoclonal anti-ferrocenium antibody, which is coupled to the detection antibody and used as a secondary reporter. A separation-free progesterone immunoassay with a lower detection limit of 1 ng?mL-1 (3.18 nmol?L-1) in 1?:?2 diluted blood serum was realised by combining two bifunctional conjugates, a ferrocenium-PEG-progesterone tracer and a bioconjugate of one anti-progesterone and one anti-ferrocenium antibody. The immune complex is formed within 30 s upon addition of progesterone, resulting in a total analysis time of 1.5 min.
A modo de introducción
(2012)
Wie stark sich im Verlauf des zurückliegenden Vierteljahrhunderts der Bekanntheitsgrad Alexander von Humboldts in der deutschsprachigen Öffentlichkeit verändert hat, zeigen nicht nur Fernsehumfragen zu den berühmtesten Deutschen, in denen Alexander von Humboldt mittlerweile figuriert, oder Fernsehserien, die über aktuelle Expeditionen berichten und auf Humboldts Namen zurückgreifen. Am deutlichsten vielleicht belegt dies der enorme Erfolg von Daniel Kehlmanns Roman Die Vermessung der Welt, der ohne die zuvor skizzierte Entwicklung nicht denkbar gewesen wäre. Es ist vor diesem Hintergrund nicht nur reizvoll, sondern aufschlußreich, sich mit dem großen Erfolg dieses kleinen Romans zu beschäftigen. Worum geht es in Die Vermessung der Welt? Und wie läßt sich das »Phänomen Kehlmann« aus etwas größerer Distanz erklären?
De cómicos e histéricos
(2012)
La popularidad de Alejandro de Humboldt ha cambiado profundamente dentro del último cuarto de siglo en la opinión pública de habla alemana. Prueba de esto son no sólo las encuestas televisivas sobre los alemanes más famosos, dentro de las cuales figura en estos momentos Alejandro de Humboldt, o programas de televisión sobre expediciones actuales, en los que continuamente se retoma el nombre de Humboldt; quizás la comprobación más clara de este cambio es el éxito enorme de la novela Die Vermessung der Welt de Daniel Kehlmann. Éxito que sería impensable sin el proceso esbozado más arriba. Ante este trasfondo, estudiar el gran éxito de esta pequeña novela resulta no sólo atractivo, sino además revelador. ¿De qué se trata Die Vermessung der Welt? ¿Cómo se puede explicar el »fenómeno Kehlmann« desde una distancia relativamente mayor?
Auf der Suche nach dem (sich verlierenden) Leben : Wissenschaft und Schreiben bei Roland Barthes
(2012)
Weltsichten Amerikas : hemisphaerische Konstruktionen in José Lezama Limas "La expresión americana"
(2012)
Veloziferische Exzellenzen
(2012)
Wood has an excellent mechanical performance, but wider utilization of this renewable resource as an engineering material is limited by unfavorable properties such as low dimensional stability upon moisture changes and a low durability. However, some wood species are known to produce a wood of higher quality by inserting mainly phenolic substances in the already formed cell walls a process so-called heartwood formation. In the present study, we used the heartwood formation in black locust (Robinia pseudoacacia) as a source of bioinspiration and transferred principles of the modification in order to improve spruce wood properties (Picea abies) by a chemical treatment with commercially available flavonoids. We were able to effectively insert hydrophobic flavonoids in the cell wall after a tosylation treatment for activation. The chemical treatment reduced the water uptake of the wood cell walls and increased the dimensional stability of the bulk spruce wood. Further analysis of the chemical interaction of the flavonoid with the structural cell wall components revealed the basic principle of this bioinspired modification. Contrary to established modification treatments, which mainly address the hydroxyl groups of the carbohydrates with hydrophilic substances, the hydrophobic flavonoids are effective by a physical bulking in the cell wall most probably stabilized by pi-pi interactions. A biomimetic transfer of the underlying principle may lead to alternative cell wall modification procedures and improve the performance of wood as an engineering material.
During visual fixation on a target object, our eyes are not motionless but generate slow fixational eye movements and microsaccades. Effects of visual attention have been observed in both microsaccade rates and spatial directions. Experimental results, however, range from early (<200 ms) to late (>600 ms) effects combined with cue-congruent as well as cue-incongruent microsaccade directions. On the basis of well characterized neural circuitry in superior colliculus, we construct a dynamical model of neural activation that is modulated by perceptual input and visual attention. Our results show that additive integration of low-level perceptual responses and visual attention can explain microsaccade rate and direction effects across a range of visual cueing tasks. These findings suggest that the patterns of microsaccade direction observed in experiments are compatible with a single dynamical mechanism. The basic principles of the model are highly relevant to the general problem of integration of low-level perception and top-down selective attention.
The class of 2,5 disubstituted-1,3,4-oxadiazoles containing a biphenyl unit on one side is intensively used as electron transport materials to enhance the performance of organic light emitting diodes (OLEDs). In contrast to the ongoing research on these materials insights in their structure-property relationships are still incomplete. To overcome the structural tentativeness and ambiguities the crystal structures of 2-(4-biphenylyl)-5-(4-tert-butylphenyl)-1,3,4-oxadiazole, that of the related compound 2-(4-biphenylyl)-5-phenyl-1,3,4-oxadiazole and of 2-(4-biphenylyl)-5-(2,6-dimethylphenyl)-1,3,4-oxadiazole are determined. A comparison with the results of GAUSSIAN03 calculations and similar compounds in the Cambridge Structural Database leads to a profound characterization.
A transient two-dimensional model describing degenerate four-wave mixing inside saturable gain media is presented. The new model is compared to existing one-dimensional models with their qualitative results confirmed. Large quantitative differences with respect to peak reflectivity and optimum pump fluence are observed. Furthermore, the influence of the beam focus size, the transverse position and the crossing angle on the reflectivity of the grating is investigated using the improved model. It is demonstrated that the phase conjugate reflectivity depends sensitively on the transverse features of the interacting beams with a transverse shift in the position of the pump beams yielding a threefold improvement in reflectivity. (C) 2012 Optical Society of America
To investigate how preschoolers acquire a tool use strategy and how they adapt their tool use to a changed situation, 2- to 4-year-olds were asked to retrieve chips from a transparent box with a rod, either by stabbing and lifting through a top opening or by pushing through a front and a back opening. In both conditions, about 40% of the children acquired effective tool use by individual learning, and 90% of the other children learned this by observing only one demonstration. When confronted with a changed situation (i.e., previous opening covered, alternative opening uncovered), children perseverated with the recently learned, but now ineffective tool use strategy. Neither age nor acquisition type of the first strategy affected preschoolers' perseverations. Results indicate that prior tool use experiences have differential effects in situations that require either transferring known functions to novel objects or using a familiar tool for an alternative purpose.
Movement or goal Goal salience and verbal cues affect preschoolers' imitation of action components
(2012)
The impact of goal salience and verbal cues given by the model on 3- to 5-year-olds' reproduction of action components (movement or goal) was investigated in an imitation choice task. Preschoolers watched an experimenter moving a puppet up or down a ramp, terminating at one of two target objects. The target objects were either differently colored plastic bowls (low-salient group) or sociofunctionally relevant objects (high-salient group). While demonstrating the action in several trials, the model verbalized either the movement, the goal, both the movement and the goal, or none of the components. Children imitated the action on a second ramp with reversed positions of the target objects, so they needed to decide whether to reproduce the observed movement or the observed end state. In the high-salient group, preschoolers preferentially imitated the goal component, whereas in the low-salient group, they did not show a preference for one of the components. Across trials, preschoolers preferentially imitated the goal when this component or both components were verbalized, whereas they showed no preference when the movement or none of the components was emphasized. Yet, verbal cues seemed to have stronger effects in the low-salient condition. We conclude that sociofunctional salience of action goals and communicative cues of the model affect young children's representation of observed actions, leading to a selective reproduction of those action components that are relevant to the child.
Suppression of the near-infrared OH night-sky lines with fibre Bragg gratings - first results
(2012)
The background noise between 1 and 1.8 ?mu m in ground-based instruments is dominated by atmospheric emission from hydroxyl molecules. We have built and commissioned a new instrument, the Gemini Near-infrared OH Suppression Integral Field Unit (IFU) System (GNOSIS), which suppresses 103 OH doublets between 1.47 and 1.7?mu m by a factor of 1000 with a resolving power of 10?000. We present the first results from the commissioning of GNOSIS using the IRIS2 spectrograph at the Anglo-Australian Telescope. We present measurements of sensitivity, background and throughput. The combined throughput of the GNOSIS fore-optics, grating unit and relay optics is 36?per cent, but this could be improved to 46?per cent with a more optimal design. We measure strong suppression of the OH lines, confirming that OH suppression with fibre Bragg gratings will be a powerful technology for low-resolution spectroscopy. The integrated OH suppressed background between 1.5 and 1.7 mu m is reduced by a factor of 9 compared to a control spectrum using the same system without suppression. The potential of low-resolution OH-suppressed spectroscopy is illustrated with example observations of Seyfert galaxies and a low-mass star. The GNOSIS background is dominated by detector dark current below 1.67 mu m and by thermal emission above 1.67 mu m. After subtracting these, we detect an unidentified residual interline component of 860 +/- 210 photons s-1 m-2?arcsec-2?mu m-1, comparable to previous measurements. This component is equally bright in the suppressed and control spectra. We have investigated the possible source of the interline component, but were unable to discriminate between a possible instrumental artefact and intrinsic atmospheric emission. Resolving the source of this emission is crucial for the design of fully optimized OH suppression spectrographs. The next-generation OH suppression spectrograph will be focused on resolving the source of the interline component, taking advantage of better optimization for a fibre Bragg grating feed incorporating refinements of design based on our findings from GNOSIS. We quantify the necessary improvements for an optimal OH suppressing fibre spectrograph design.
This paper introduces and analyses a general statistical model, termed the RAndom RElaxations (RARE) model, of random relaxation processes in disordered systems. The model considers excitations that are randomly scattered around a reaction center in a general embedding space. The model's input quantities are the spatial scattering statistics of the excitations around the reaction center, and the chemical reaction rates between the excitations and the reaction center as a function of their mutual distance. The framework of the RARE model is versatile and a detailed stochastic analysis of the random relaxation processes is established. Analytic results regarding the duration and the range of the random relaxation processes, as well as the model's thermodynamic limit, are obtained in closed form. In particular, the case of power-law inputs, which turn out to yield stretched exponential relaxation patterns and asymptotically Paretian relaxation ranges, is addressed in detail.
Steatotic livers show increased hepatic damage and impaired regeneration after partial hepatectomy (PH) under ischemia/reperfusion (I/R), which is commonly applied in clinical practice to reduce bleeding. The known function of retinol-binding protein 4 (RBP4) is to transport retinol in the circulation. We examined whether modulating RBP4 and/or retinol could protect steatotic and nonsteatotic livers in the setting of PH under I/R. Steatotic and nonsteatotic livers from Zucker rats were subjected to PH (70%) with 60 minutes of ischemia. RBP4 and retinol levels were measured and altered pharmacologically, and their effects on hepatic damage and regeneration were studied after reperfusion. Decreased RBP4 levels were observed in both liver types, whereas retinol levels were reduced only in steatotic livers. RBP4 administration exacerbated the negative consequences of liver surgery with respect to damage and liver regeneration in both liver types. RBP4 affected the mobilization of retinol from steatotic livers, and this revealed actions of RBP4 independent of simple retinol transport. The injurious effects of RBP4 were not due to changes in retinol levels. Treatment with retinol was effective only for steatotic livers. Indeed, retinol increased hepatic injury and impaired liver regeneration in nonsteatotic livers. In steatotic livers, retinol reduced damage and improved regeneration after surgery. These benefits of retinol were associated with a reduced accumulation of hepatocellular fat. Thus, strategies based on modulating RBP4 could be ineffective and possibly even harmful in both liver types in the setting of PH under I/R. In terms of clinical applications, a retinol pretreatment might open new avenues for liver surgery that specifically benefit the steatotic liver. Liver Transpl 18:1198-1208, 2012.
We study the dispersion interaction of the van der Waals and Casimir-Polder (vdW-CP) type between a neutral atom and the surface of a conductor by allowing for nonlocal electrodynamics, i.e. electron diffusion. We consider two models: (i) bulk diffusion, and (ii) diffusion in a surface charge layer. In both cases, we find that the transition to a semiconductor as a function of the conductivity is continuous, unlike the case of a local model. The relevant parameter is the electric screening length and depends on the carrier diffusion constant. We find that for distances comparable to the screening length, vdW-CP data can distinguish between bulk and surface diffusion, hence it can be a sensitive probe for surface states.
Let (M, g) be a complete 3-dimensional asymptotically flat manifold with everywhere positive scalar curvature. We prove that, given a compact subset K subset of M, all volume preserving stable constant mean curvature surfaces of sufficiently large area will avoid K. This complements the results of G. Huisken and S.-T. Yau [17] and of J. Qing and G. Tian [26] on the uniqueness of large volume preserving stable constant mean curvature spheres in initial data sets that are asymptotically close to Schwarzschild with mass m > 0. The analysis in [17] and [26] takes place in the asymptotic regime of M. Here we adapt ideas from the minimal surface proof of the positive mass theorem [32] by R. Schoen and S.-T. Yau and develop geometric properties of volume preserving stable constant mean curvature surfaces to handle surfaces that run through the part of M that is far from Euclidean.
Herzog macht Stadt
(2012)
Prognosen
(2012)
We studied testate amoebae and possible correlated abiotic factors in soils of 31 mature forest ecosystems using an easily applicable and spatially explicit method. Simple counting on soil thin-sections with a light microscope resulted in amoeba densities comparable to previously reported values, i.e. 0.1 x 10(8) to 11.5 x 10(8) individuals m(-2) (upper 3 cm of soil). Soil moisture and soil acidity seem to be correlated with amoeba densities. At sites of moderate soil moisture regimes (SMR 2-7) we found higher densities of testate amoebae at pH < 4.5. At wetter sites (SMR >= 8) higher individual densities were recorded also at less acidic sites. The in situ description of amoebae, based on the analysis of a complete soil thin-section, showed a relatively uniform spatial micro-distribution throughout the organic and mineral soil horizons (no testate amoeba clusters). We discuss the pros and cons of the soil thin-section method and suggest it as an additional tool to improve knowledge of the spatial micro-distribution of testate amoebae.
Graph transformation systems have been studied extensively and applied to several areas of computer science like formal language theory, the modeling of databases, concurrent or distributed systems, and visual, logical, and functional programming. In most kinds of applications it is necessary to have the possibility of restricting the applicability of rules. This is usually done by means of application conditions. In this paper, we continue the work of extending the fundamental theory of graph transformation to the case where rules may use arbitrary (nested) application conditions. More precisely, we generalize the Embedding theorem, and we study how local confluence can be checked in this context. In particular, we define a new notion of critical pair which allows us to formulate and prove a Local Confluence Theorem for the general case of rules with nested application conditions. All our results are presented, not for a specific class of graphs, but for any arbitrary M-adhesive category, which means that our results apply to most kinds of graphical structures. We demonstrate our theory on the modeling of an elevator control by a typed graph transformation system with positive and negative application conditions.
Partitioning cluster algorithms have proven to be powerful tools for data-driven integration of large geoscientific databases. We used fuzzy Gustafson-Kessel cluster analysis to integrate Landsat imagery,. airborne radiometric, and regional geochemical data to aid in the interpretation of a multimethod database. The survey area extends over 3700 km(2) and is located in the Northern Cape Province, South Africa. We carefully selected five variables for cluster analysis to avoid the clustering results being dominated by spatially high-correlated data sets that were present in our database. Unlike other, more popular cluster algorithms, such as k-means or fuzzy c-means, the Gustafson-Kessel algorithm requires no preclustering data processing, such as scaling or adjustment of histographic data distributions. The outcome of cluster analysis was a classified map that delineates prominent near-to-surface structures. To add value to the classified map, we compared the detected structures to mapped geology and additional geophysical ground-truthing data. We were able to associate the structures detected by cluster analysis to geophysical and geological information thus obtaining a pseudolithology map. The latter outlined an area with increased mineral potential where manganese mineralization, i.e., psilomelane, had been located.
Away from active plate boundaries the relationships between spatiotemporal variations in density and geothermal gradient are important for understanding the evolution of topography in continental interiors. In this context the classic concept of the continental lithosphere as comprising three static layers of different densities (upper crust, lower crust, and upper mantle) is not adequate to assess long-term changes in topography and relief in regions associated with pronounced thermal anomalies in the mantle. We have therefore developed a one-dimensional model, which is based on thermodynamic equilibrium assemblage computations and deliberately excludes the effects of melting processes like intrusion or extrusions. Our model calculates the "metamorphic density" of rocks as a function of pressure, temperature, and chemical composition. It not only provides a useful tool for quantifying the influence of petrologic characteristics on density, but also allows the modeled "metamorphic" density to be adjusted to variable geothermal gradients and applied to different geodynamic environments. We have used this model to simulate a scenario in which the lithosphere-asthenosphere boundary is subjected to continuous heating over a long period of time (130 Ma), and demonstrate how an anorogenic plateau with an elevation of 1400 m can be formed solely as a result of heat transfer within the continental lithosphere. Our results show that, beside dynamic topography (of asthenospheric origin), density changes within the lithosphere have an important impact on the evolution of anorogenic plateaus.
Associated heterotrophic bacteria alter the microenvironment of cyanobacteria and potentially influence cyanobacterial development. Therefore, we studied interactions of the unicellular freshwater cyanobacterium Microcystis aeruginosa with heterotrophic bacteria. The associated bacterial community was greatly driven by temperature as seen by DNA fingerprinting. However, the associated microbes also closely interacted with the cyanobacteria indicating changing ecological consequence of the associated bacterial community with temperature. Whereas concentration of dissolved organic carbon in cyanobacterial cultures changed in a temperature-dependent manner, its quality greatly varied under the same environmental conditions, but with different associated bacterial communities. Furthermore, temperature affected quantity and quality of cell-bound microcystins, whereby interactions between M. aeruginosa and their associated community often masked this temperature effect. Both macro- and microenvironment of active cyanobacterial strains were characterized by high pH and oxygen values creating a unique habitat that potentially affects microbial diversity and function. For example, archaea including 'anaerobic' methanogens contributed to the associated microbial community. This implies so far uncharacterized interactions between Microcystis aeruginosa and its associated prokaryotic community, which has unknown ecological consequences in a climatically changing world.