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The first heterodinuclear ruthenium(II) complexes of the 1,6,7,12-tetraazaperylene (tape) bridging ligand with iron(II), cobalt(II), and nickel(II) were synthesized and characterized. The metal coordination sphere in this complexes is filled by the tetradentate N,N-dimethyl-2,11-diaza[3.3](2,6)-pyridinophane (L-N4Me2) ligand, yielding complexes of the general formula [(L-N4Me2)Ru(mu-tape)M(L-N4Me2)](ClO4)(2)(PF6)(2) with M = Fe {[2](ClO4)(2)(PF6)(2)}, Co {[3](ClO4)(2)(PF6)(2)}, and Ni {[4](ClO4)(2)(PF6)(2)}. Furthermore, the heterodinuclear tape ruthenium(II) complexes with palladium(II)- and platinum(II)-dichloride [(bpy)(2)Ru(-tape)PdCl2](PF6)(2) {[5](PF6)(2)} and [(dmbpy)(2)Ru(-tape)PtCl2](PF6)(2) {[6](PF6)(2)}, respectively were also prepared. The molecular structures of the complex cations [2](4+) and [4](4+) were discussed on the basis of the X-ray structures of [2](ClO4)(4)MeCN and [4](ClO4)(4)MeCN. The electrochemical behavior and the UV/Vis absorption spectra of the heterodinuclear tape ruthenium(II) complexes were explored and compared with the data of the analogous mono- and homodinuclear ruthenium(II) complexes of the tape bridging ligand.
Complementary to the well-established zwitterionic monomer 3-((3-methacrylamidopropyl) dimethylammonio) propane-1-sulfonate (SPP), the closely related monomers 2-hydroxy-3-((3-methacrylamidopropyl) dimethylammonio) propane-1-sulfonate (SHPP) and 4-((3-methacrylamidopropyl) dimethylammonio)butane- 1-sulfonate (SBP) were synthesised and polymerised by reversible addition-fragmentation chain transfer (RAFT) polymerisation, using a fluorophore labeled RAFT agent. The polyzwitterions of systematically varied molar masses were characterised with respect to their solubility in water and aqueous salt solutions. Both poly(sulfobetaine)s show thermoresponsive behaviour in water, exhibiting phase separation at low temperatures and upper critical solution temperatures (UCST). For both polySHPP and polySBP, cloud points depend notably on the molar mass, and are much higher in D2O than in H2O. Also, the cloud points are effectively modulated by the addition of salts. The individual effects can be in parts correlated to the Hofmeister series for the anions studied. Still, they depend in a complex way on the concentration and the nature of the added electrolytes, on the one hand, and on the detailed nature of the spacer group separating the anionic and the cationic charges of the betaine moiety, on the other hand. As anticipated, the cloud points of polySBP are much higher than the ones of the analogous polySPP of identical molar mass. Surprisingly, the cloud points of polySHPP are also somewhat higher than the ones of their polySPP analogues, despite the additional hydrophilic hydroxyl group present in the spacer separating the ammonium and the sulfonate moieties. These findings point to a complicated interplay of the various hydrophilic components in polyzwitterions with respect to their overall hydrophilicity. Thus, the spacer group in the betaine moiety proves to be an effective additional molecular design parameter, apparently small variations of which strongly influence the phase behaviour of the polyzwitterions in specific aqueous environments.
A unique fabrication process of low molar mass, crystalline polypeptoid fibers is described. Thermoresponsive fiber mats are prepared by electrospinning a homogeneous blend of semicrystalline poly(N-(n-propyl) glycine) (PPGly; 4.1 kDa) with high molar mass poly(ethylene oxide) (PEO). Annealing of these fibers at approximate to 100 degrees C selectively removes the PEO and produces stable crystalline fiber mats of pure PPGly, which are insoluble in aqueous solution but can be redissolved in methanol or ethanol. The formation of water-stable polypeptoid fiber mats is an important step toward their utilization in biomedical applications such as tissue engineering or wound dressing.
Warming and eutrophication are two of the most important global change stressors for natural ecosystems, but their interaction is poorly understood. We used a dynamic model of complex, size-structured food webs to assess interactive effects on diversity and network structure. We found antagonistic impacts: Warming increases diversity in eutrophic systems and decreases it in oligotrophic systems. These effects interact with the community size structure: Communities of similarly sized species such as parasitoid-host systems are stabilized by warming and destabilized by eutrophication, whereas the diversity of size-structured predator-prey networks decreases strongly with warming, but decreases only weakly with eutrophication. Nonrandom extinction risks for generalists and specialists lead to higher connectance in networks without size structure and lower connectance in size-structured communities. Overall, our results unravel interactive impacts of warming and eutrophication and suggest that size structure may serve as an important proxy for predicting the community sensitivity to these global change stressors.
Skipping a grade, one specific form of acceleration, is an intervention used for gifted students. Quantitative research has shown acceleration to be a highly successful intervention regarding academic achievement, but less is known about the social–emotional outcomes of grade-skipping. In the present study, the authors used the grounded theory approach to examine the experiences of seven gifted students aged 8 to 16 years who skipped a grade. The interviewees perceived their “feeling of being in the wrong place” before the grade-skipping as strongly influenced by their teachers, who generally did not respond adequately to their needs. We observed a close interrelationship between the gifted students’ intellectual fit and their social situation in class. Findings showed that the grade-skipping in most of the cases bettered the situation in school intellectually as well as socially, but soon further interventions, for instance, a specialized and demanding class- or subject-specific acceleration were added to provide sufficiently challenging learning opportunities.
1. Plant-plant interactions may critically modify the impact of climate change on plant communities. However, the magnitude and even direction of potential future interactions remains highly debated, especially for water-limited ecosystems. Predictions range from increasing facilitation to increasing competition with future aridification. 2. The different methodologies used for assessing plant-plant interactions under changing environmental conditions may affect the outcome but they are not equally represented in the literature. Mechanistic experimental manipulations are rare compared with correlative approaches that infer future patterns from current observations along spatial climatic gradients. 3. Here, we utilize a unique climatic gradient in combination with a large-scale, long-term experiment to test whether predictions about plant-plant interactions yield similar results when using experimental manipulations, spatial gradients or temporal variation. We assessed shrub-annual interactions in three different sites along a natural rainfall gradient (spatial) during 9 years of varying rainfall (temporal) and 8 years of dry and wet manipulations of ambient rainfall (experimental) that closely mimicked regional climate scenarios. 4. The results were fundamentally different among all three approaches. Experimental water manipulations hardly altered shrub effects on annual plant communities for the assessed fitness parameters biomass and survival. Along the spatial gradient, shrub effects shifted from clearly negative to mildly facilitative towards drier sites, whereas temporal variation showed the opposite trend: more negative shrub effects in drier years. 5. Based on our experimental approach, we conclude that shrub-annual interaction will remain similar under climate change. In contrast, the commonly applied space-for-time approach based on spatial gradients would have suggested increasing facilitative effects with climate change. We discuss potential mechanisms governing the differences among the three approaches. 6. Our study highlights the critical importance of long-term experimental manipulations for evaluating climate change impacts. Correlative approaches, for example along spatial or temporal gradients, may be misleading and overestimate the response of plant-plant interactions to climate change.
In nature, plants often encounter chronic or recurring stressful conditions. Recent results indicate that plants can remember a past exposure to stress to be better prepared for a future stress incident. However, the molecular basis of this is poorly understood. Here, we report the involvement of chromatin modifications in the maintenance of acquired thermotolerance (heat stress [HS] memory). HS memory is associated with the accumulation of histone H3 lysine 4 di- and trimethylation at memory-related loci. This accumulation outlasts their transcriptional activity and marks them as recently transcriptionally active. High accumulation of H3K4 methylation is associated with hyper-induction of gene expression upon a recurring HS. This transcriptional memory and the sustained accumulation of H3K4 methylation depend on HSFA2, a transcription factor that is required for HS memory, but not initial heat responses. Interestingly, HSFA2 associates with memory-related loci transiently during the early stages following HS. In summary, we show that transcriptional memory after HS is associated with sustained H3K4 hyper-methylation and depends on a hit-and-run transcription factor, thus providing a molecular framework for HS memory.
The competitive extraction of Cr(III) onto Nauclea diderrichii seed epicarp doped with MnO2 nanoparticles (MnO2 nano-bioextractant (MNB)) in a single and binary batch system was studied. For validity of experimental data, chi square test, root mean square error, sum of the square errors, hybrid fractional error function, Marquart’s percent standard deviation and standard absolute error were used. Among the kinetic models used, pseudo-second-order and Langmuir equations gave the best fits for the experimental data, with qe (mg g) for the uptake of Cr(III) in single metal system onto MNB, then Cr(III) with Cd(II), Pb(II), Hg(II), KCl and CaCl2 in binary metal systems onto MNB were 2.611, then 1.989, 1.016, 2.208, 1.249 and 1.868 from kinetic standpoint, respectively. The initial sorption rates, h (mg/g/min), and half lives, t1/2 (min), for the uptake of Cr(III) in single metal system onto MNB, then Cr(III) with Cd(II), Pb(II), Hg(II), KCl and CaCl2 in binary metal system onto MNB were 3.497, then 2.311, 2.274, 0.242, 2.956, 45.568 and 0.747, then 5.769, 1.766, 12.144, 1.762, and 2.415, respectively. Physicochemical surface analyses such as pH of point of zero charge, Brunauer–Emmett–Teller single point and multi-point techniques for surface area analyses, scanning electron microscopy and transmission electron microscopy were done on MNB and MnO2 nanoparticles in order to understand their surface microstructures. Desorption study showed that MNB can be recycled and used for future study. Hence, MNB showed good potential to remediate Cr(III) from wastewaters and polluted water.
Mediated bioelectrochemical system for biosensing the cell viability of Staphylococcus aureus
(2016)
Staphylococcus aureus is one of the most dangerous human pathogens and is the cause of numerous illnesses ranging from moderate skin infections to life-threatening diseases. Despite advances made in identifying microorganisms, rapid detection methods for the viability of bacteria are still missing. Here, we report a rapid electrochemical assay for cell viability combining the use of double redox mediators and multiwall carbon nanotubes-screen printed electrodes (MWCNTs-SPE), ferricyanide (FCN) and 2,6-dichlorophenolindophenol (DCIP), which served as electron shuttle to enable the bacterial-electrode communications. The current originating from the metabolically active cells was recorded for probing the activity of the intracellular redox centers. Blocking of the respiratory chain pathways with electron transfer inhibitors demonstrated the involvement of the electron transport chain in the reaction. A good correlation between the number of the metabolically active cells and the current was obtained. The proposed assay has been exploited for monitoring cell proliferation of S. aureus during the growth. The sensitivity of the detection method reached 0.1 OD600. Therefore, the technique described is promising for estimating the cell number, measuring the cell viability, and probing intracellular redox center(s).
Previous work on spatial-numerical association (SNAs) included either spatially distributed stimuli or responses. This raises the possibility that the inferred spatial nature of number concepts was a methodological artifact. We present results from a novel task that involves two categories (spatially oriented objects and number magnitudes) and dissociates spatial classification from number classification. The results reveal SNAs without inferential limitations of previous work and point to a working memory mechanism that transfers spatial coding across categories.
The Alanya Massif, which is located to the south of central Taurides in Turkey, presents a typical nappe pile consisting of thrust sheets with contrasting metamorphic histories. In two thrust sheets, Sugozu and GundogmuAY nappes, HP metamorphism under eclogite (550-567 A degrees C/14-18 kbar) and blueschist facies (435-480 A degrees C/11-13 kbar) conditions have been recognized, respectively. Whereas the rest of the Massif underwent MP metamorphism under greenschist to amphibolite facies (525-555 A degrees C/6.5-7.5 kbar) conditions. Eclogite facies metamorphism in Sugozu nappe, which consists of homogeneous garnet-glaucophane-phengite schists with eclogite lenses is dated at 84.8 +/- A 0.8, 84.7 +/- A 1.5 and 82 +/- A 3 Ma (Santonian-Campanian) by Ar-40/Ar-39 phengite, U/Pb zircon and rutile dating methods, respectively. Similarly, phengites in GundogmuAY nappe representing an accretionary complex yield 82-80 Ma (Campanian) ages for blueschist facies metamorphism. During the exhumation, the retrograde overprint of the HP units under greenschist-amphibolite facies conditions and tectonic juxtaposition with the Barrovian units occurred during Campanian (75-78 Ma). Petrological and geochronological data clearly indicate a similar Late Cretaceous tectonometamorphic evolution for both Alanya (84-75 Ma) and Bitlis (84-72 Ma) Massifs. They form part of a single continental sliver (Alanya-Bitlis microcontinent), which was rifted from the southern part of the Anatolide-Tauride platform. The P-T-t coherence between two Massifs suggests that both Massifs have been derived from the closure of the same ocean (Alanya-Bitlis Ocean) located to the south of the Anatolide-Tauride block by a northward subduction. The boundary separating the autochthonous Tauride platform to the north from both the Alanya and Bitlis Massifs to the south represents a suture zone, the Pamphylian-Alanya-Bitlis suture.
Anatolia’s high-pressure metamorphic belts are characterized in part by a Neotethyan stratigraphic succession that includes a mid-Cretaceous hemi-pelagic marble sequence. This unit contains, towards its stratigraphic top, dm-to-m-long radiating calcitic rods forming rosette-like textures. Here, we refer to these features as “Rosetta Marble”. The remarkable textural similarity of non-metamorphic selenite crystals and radiating calcite rods in the Rosetta Marble strongly suggests that these textures represent pseudomorphs after selenites. Metamorphosed hemi-pelagic limestones, dominated by Rosetta selenite pseudomorphs, are alternating with siliceous meta-sediments containing relictic radiolaria tests. This stratigraphic pattern is indicative of transient phases characterized by evaporites precipitated from basinal brines alternating with non-evaporative hemi-pelagic deposition from normal-marine seawater. The regional distribution of Rosetta Marble exposures over 600 km is indicative of basin-scale evaporitic intervals. High-pressure, low-temperature metamorphism of these rocks is witnessed by Sr-rich (up to 3500 ppm), fibrous calcite pseudomorphs after aragonite and isolated aragonite inclusions in quartz. Peak metamorphic conditions of 1.2 GPa and 300–350 °C are attested by high-Si white mica thermobarometry. The Rosetta Marble case example examines the potential to unravel the complete history from deposition to diagenesis and metamorphism of meta-sedimentary rocks.
This paper addresses the lithosphere-scale subduction-collision history of the eastern termination of the Aegean retreating subduction system, i.e. western Anatolia. Although there is some general consensus on the protracted subduction evolution of the Aegean since the early Cenozoic at least, correlation with western Anatolia has been widely debated for more than several decades. In western Anatolia, three main tectonic configurations have been envisaged in the past years to reconstruct slab dynamics during the closure of the Neotethyan oceanic realm since the Late Cretaceous. Some authors have suggested an Aegean-type scenario, with the continuous subduction of a single lithospheric slab, punctuated by episodic slab roll-back and trench retreat, whereas others assumed a discontinuous subduction history marked by intermittent slab break-off during either the Campanian (ca. 75 Ma) or the Early Eocene (ca. 55-50 Ma). The third view implies three partly contemporaneous subduction zones. Our review of these models points to key debated aspects that can be re-evaluated in the light of multidisciplinary constraints from the literature. Our discussion leads us to address the timing of subduction initiation, the existence of hypothetical ocean basins, the number of intervening subduction zones between the Taurides and the Pontides, the palaeogeographic origin of tectonic units and the possibility for slab break-off during either the Campanian or the Early Eocene. Thence, we put forward a favoured tectonic scenario featuring two successive phases of subduction of a single lithospheric slab and episodic accretion of two continental domains separated by a continental trough, representing the eastern end of the Cycladic Ocean of the Aegean. The lack of univocal evidence for slab break-off in western Anatolia and southward-younging HP/LT metamorphism in continental tectonic units (from similar to 85, 70 to 50 Ma) in the Late Cretaceous-Palaeogene period suggests continuous subduction since similar to 110 Ma, marked by roll-back episodes in the Palaeocene and the Oligo-Miocene, and slab tearing below western Anatolia during the Miocene.
A unique assemblage including kumdykolite and kokchetavite, polymorphs of albite and K-feldspar, respectively, together with cristobalite, micas, and calcite has been identified in high-pressure granulites of the Orlica-Snieznik dome (Bohemian Massif) as the product of partial melt crystallization in preserved nanogranites. Previous reports of both kumdykolite and kokchetavite in natural rocks are mainly from samples that passed through the diamond stability field. However, because the maximum pressure recorded in these host rocks is <3 GPa, our observations indicate that high pressure is not required for the formation of kumdykolite and kokchetavite, and their presence is not therefore an indicator of ultrahigh-pressure conditions. Detailed microstructural and microchemical investigation of these inclusions indicates that such phases should instead be regarded as (1) a direct mineralogical criteria to identify former melt inclusions with preserved original compositions, including H2O and CO2 contents and (2) indicators of rapid cooling of the host rocks. Thus, the present study provides novel criteria for the interpretation of melt inclusions in natural rocks and allows a more rigorous characterization of partial melts during deep subduction to mantle depth as well as their behavior on exhumation.
The ground-state classical path approximation is utilized to compute molecular absorption spectra in a mixed quantum-classical frame. To improve the description for high-frequency vibrational satellites, related quantum correction factors are introduced. The improved method is demonstrated for the Q(y),and Q(x)-bands of pheophorbide a. (C) 2015 Elsevier B.V. All rights reserved.
Catalytic amounts of a weak base are sufficient to induce the decomposition of anthracene endoperoxides to anthraquinone. The mechanism has been elucidated by isolation of intermediates in combination with DFT calculations. The whole process is suitable for the convenient generation of hydrogen peroxide under very mild conditions.
Polychlorinated biphenyls (PCBs) can cause endocrine disruption, cancer, immunosuppression, or reproductive failure in animals. We used an individual-based model to explore whether and how PCB-associated reproductive failure could affect the dynamics of a hypothetical polar bear (Ursus maritimus) population exposed to PCBs to the same degree as the East Greenland subpopulation. Dose-response data from experimental studies on a surrogate species, the mink (Mustela vision), were used in the absence of similar data for polar bears. Two alternative types of reproductive failure in relation to maternal sum-PCB concentrations were considered: increased abortion rate and increased cub mortality. We found that the quantitative impact of PCB-induced reproductive failure on population growth rate depended largely on the actual type of reproductive failure involved. Critical potencies of the dose-response relationship for decreasing the population growth rate were established for both modeled types of reproductive failure. Comparing the model predictions of the age-dependent trend of sum-PCBs concentrations in females with actual field measurements from East Greenland indicated that it was unlikely that PCB exposure caused a high incidence of abortions in the subpopulation. However, on the basis of this analysis, it could not be excluded that PCB exposure contributes to higher cub mortality. Our results highlight the necessity for further research on the possible influence of PCBs on polar bear reproduction regarding their physiological pathway. This includes determining the exact cause of reproductive failure, i.e., in utero exposure versus lactational exposure of offspring; the timing of offspring death; and establishing the most relevant reference metrics for the dose-response relationship.
Objectives: To reanalyze the between-population variance in height, weight, and body mass index (BMI), and to provide a globally applicable technique for generating synthetic growth reference charts. Methods: Using a baseline set of 196 female and 197 male growth studies published since 1831, common factors of height, weight, and BMI are extracted via Principal Components separately for height, weight, and BMI. Combining information from single growth studies and the common factors using in principle a Bayesian rationale allows for provision of completed reference charts. Results: The suggested approach can be used for generating synthetic growth reference charts with LMS values for height, weight, and BMI, from birth to maturity, from any limited set of height and weight measurements of a given population. Conclusion: Generating synthetic growth reference charts by incorporating information from a large set of reference growth studies seems suitable for populations with no autochthonous references at hand yet. (C) 2015 Wiley Periodicals, Inc.
Natural vision is characterized by alternating sequences of rapid gaze shifts (saccades) and fixations. During fixations, microsaccades and slower drift movements occur spontaneously, so that the eye is never motionless. Theoretical models of fixational eye movements predict that microsaccades are dynamically coupled to slower drift movements generated immediately before microsaccades, which might be used as a criterion to distinguish microsaccades from small voluntary saccades. Here we investigate a sequential scanning task, where participants generate goal-directed saccades and microsaccades with overlapping amplitude distributions. We show that properties of microsaccades are correlated with precursory drift motion, while amplitudes of goal-directed saccades do not dependent on previous drift epochs. We develop and test a mathematical model that integrates goal-directed and fixational eye movements, including microsaccades. Using model simulations, we reproduce the experimental finding of correlations within fixational eye movement components (i.e., between physiological drift and microsaccades) but not between goal-directed saccades and fixational drift motion. These results lend support to a functional difference between microsaccades and goal-directed saccades, while, at the same time, both types of behavior may be part of an oculomotor continuum that is quantitatively described by our mathematical model. (C) 2015 Elsevier Ltd. All rights reserved.