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Optical properties of modified diamondoids have been studied theoretically using vibrationally resolved electronic absorption, emission and resonance Raman spectra. A time-dependent correlation function approach has been used for electronic two-state models, comprising a ground state (g) and a bright, excited state (e), the latter determined from linear-response, time-dependent density functional theory (TD-DFT). The harmonic and Condon approximations were adopted. In most cases origin shifts, frequency alteration and Duschinsky rotation in excited states were considered. For other cases where no excited state geometry optimization and normal mode analysis were possible or desired, a short-time approximation was used. The optical properties and spectra have been computed for (i) a set of recently synthesized sp(2)/sp(3) hybrid species with CQC double-bond connected saturated diamondoid subunits, (ii) functionalized (mostly by thiol or thione groups) diamondoids and (iii) urotropine and other C-substituted diamondoids. The ultimate goal is to tailor optical and electronic features of diamondoids by electronic blending, functionalization and substitution, based on a molecular-level understanding of the ongoing photophysics.
The distinction of enantiomers is a key aspect of chemical analysis. In mass spectrometry the distinction of enantiomers has been achieved by ionizing the sample with circularly polarized laser pulses and comparing the ion yields for light of opposite handedness. While resonant excitation conditions are expected to be most efficient, they are not required for the detection of a circular dichroism (CD) in the ion yield. However, the prediction of the size and sign of the circular dichroism becomes challenging if non-resonant multiphoton excitations are used to ionize the sample. Employing femtosecond laser pulses to drive electron wavepacket dynamics based on ab initio calculations, we attempt to reveal underlying mechanisms that determine the CD under non-resonant excitation conditions. Simulations were done for (R)-1,2-propylene oxide, using time-dependent configuration interaction singles with perturbative doubles (TD-CIS(D)) and the aug-cc-pVTZ basis set. Interactions between the electric field and the electric dipole and quadrupole as well as between the magnetic field and the magnetic dipole were explicitly accounted for. The ion yield was determined by treating states above the ionization potential as either stationary or non-stationary with energy-dependent lifetimes based on an approved heuristic approach. The observed population dynamics do not allow for a simple interpretation, because of highly non-linear interactions. Still, the various transition pathways are governed by resonant enantiospecific n-photon excitation, with preferably high transition dipole moments, which eventually dominate the CD in the ionized population.
Albian-Turonian subduction-accretionary complexes are exposed widely in the Central Pontides. A major portion of the accretionary complexes is made up of a metaflysch sequence consisting of slate/phyllite and metasandstone intercalation with blocks of marble, Na-amphibole bearing metabasite, and serpentinite. The metaflysch sequence represents distal parts of a large Lower Cretaceous submarine turbidite fan deposited on the Laurasian active continental margin that was subsequently accreted and metamorphosed during the Albian. Raman spectra of carbonaceous material of the metapelitic rocks revealed that the metaflysch consists of metamorphic packets with distinct peak metamorphic temperatures. The majority of the metapelites are low-temperature (ca. 330 degrees C) slates characterized by lack of differentiation of the graphite (G) and D2 defect bands. They possibly represent offscraped distal turbidites along the toe of the Albian accretionary wedge. Other phyllites are characterized by a slightly pronounced G band with a D2 defect band occurring on its shoulder. Peak metamorphic temperatures of these phyllites are constrained to 370-385 degrees C. The phyllites are associated with a strip of incipient blueschist facies metabasites and are found as a sliver within the offscraped distal turbidites. We interpret the phyllites as underplated continental sediments together with oceanic crustal basalt along the basal decollement. Tectonic emplacement of the underplated rocks into the offscraped distal turbidites was possibly achieved by out-of-sequence thrusting causing tectonic thickening and uplift of the wedge.
cis-Diamminedichloroplatinum(II) (Cisplatin) is one of the most important and frequently used cytostatic drugs for the treatment of various solid tumors. Herein, a laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS) method incorporating a fast and simple sample preparation protocol was developed for the elemental mapping of Cisplatin in the model organism Caenorhabditis elegans (C. elegans). The method allows imaging of the spatially-resolved elemental distribution of platinum in the whole organism with respect to the anatomic structure in L4 stage worms at a lateral resolution of 5 mm. In addition, a dose- and time-dependent Cisplatin uptake was corroborated quantitatively by a total reflection X-ray fluorescence spectroscopy (TXRF) method, and the elemental mapping indicated that Cisplatin is located in the intestine and in the head of the worms. Better understanding of the distribution of Cisplatin in this well-established model organism will be instrumental in deciphering Cisplatin toxicity and pharmacokinetics. Since the cytostatic effect of Cisplatin is based on binding the DNA by forming intra- and interstrand crosslinks, the response of poly(ADP-ribose) metabolism enzyme 1 (pme-1) deletion mutants to Cisplatin was also examined. Loss of pme-1, which is the C. elegans ortholog of human poly(ADP-ribose) polymerase 1 (PARP-1) led to disturbed DNA damage response. With respect to survival and brood size, pme-1 deletion mutants were more sensitive to Cisplatin as compared to wildtype worms, while Cisplatin uptake was indistinguishable.
Fully renewable pyridinium ionic liquids were synthesised via the hydrothermal decarboxylation of pyridinium zwitterions derived from furfural and amino acids in flow. The functionality of the resulting ionic liquid (IL) can be tuned by choice of different amino acids as well as different natural carboxylic acids as the counter-ions. A representative member of this new class of ionic liquids was successfully used for the synthesis of ionogels and as a solvent for the Heck coupling.
Plasma convection in the high-latitude ionosphere provides important information about magnetosphere-ionosphere-thermosphere coupling. In this study we estimate the along-track component of plasma convection within and around the polar cap, using electron density profiles measured by the three Swarm satellites. The velocity values estimated from the two different satellite pairs agree with each other. In both hemispheres the estimated velocity is generally anti-sunward, especially for higher speeds. The obtained velocity is in qualitative agreement with Super Dual Auroral Radar Network data. Our method can supplement currently available instruments for ionospheric plasma velocity measurements, especially in cases where these traditional instruments suffer from their inherent limitations. Also, the method can be generalized to other satellite constellations carrying electron density probes.
1,2-Dithiosquaratonickelates are available by direct synthesis from metal salts with dipotassium-1,2-dithiosquarate and the appropriate counter cations. The synthesis and characterization, including mass spectrometry, of a series 1,2-dithiosquaratonickelates(II), [Ni(dtsq)(2)](2-), with several "onium" cations is reported and the X-ray structures of two diamagnetic complexes, (HexPh(3)P)(2)[Ni(dtsq)(2)] and (BuPh3P)(2)[Ni(dtsq)(2)] with sterically demanding counter ions are presented. The diamagnetic nickel complexes have been doped as host lattices with traces of Cu(II) to measure EPR for additional structural information. The thermal behavior of this series is studied by thermogravimetry and differential thermal analysis (TG/DTA). The thermolysis in air as well as under nitrogen atmosphere of these complexes results in nickel oxide nano-particles in all cases, which are characterized by X-ray powder diffraction.
The role of morphological and syntactic information in non-native second language (L2) comprehension is controversial. Some have argued that late bilinguals rapidly integrate grammatical cues with other information sources during reading or listening in the same way as native speakers. Others claim that structural cues are underused in L2 processing. We examined different kinds of modifiers inside compounds (e.g. singulars vs. plurals, *rat eater vs. rats eater) with respect to this controversy which are subject to both structural and nonstructural constraints. Two offline and two online (eye-movement) experiments were performed examining the role of these constraints in spoken language comprehension of English and German, testing 77 advanced L2 learners. We also compared the L2 groups to corresponding groups of native speakers. Our results suggest that despite native-like sensitivity to the compounding constraints, late bilinguals rely more on non-structural constraints and are less able to revise their initial interpretations than L1 comprehenders.
Upconversion NaYF4:Yb:Er nanoparticles co-doped with Gd3+ and Nd3+ for thermometry on the nanoscale
(2015)
In the present work, the upconversion luminescence properties of oleic acid capped NaYF4:Gd3+:Yb3+:Er3+ upconversion nanoparticles (UCNP) with pure beta crystal phase and Nd3+ ions as an additional sensitizer were studied in the temperature range of 288 K < T < 328 K. The results of this study showed that the complex interplay of different mechanisms and effects, causing the special temperature behavior of the UCNP can be developed into thermometry on the nanoscale, e.g. to be applied in biological systems on a cellular level. The performance was improved by the use of Nd3+ as an additional dopant utilizing the cascade sensitization mechanism in tri-doped UCNP.
This paper examines phonological phrasing in the Kwa language Akan. Regressive [+ATR] vowel harmony between words (RVH) serves as a hitherto unreported diagnostic of phonological phrasing. In this paper I discuss VP-internal and NP-internal structures, as well as SVO(O) and serial verb constructions. RVH is a general process in Akan grammar, although it is blocked in certain contexts. The analysis of phonological phrasing relies on universal syntax-phonology mapping constraints whereby lexically headed syntactic phrases are mapped onto phonological phrases. Blocking contexts call for a domain-sensitive analysis of RVH assuming recursive prosodic structure which makes reference to maximal and non-maximal phonological phrases. It is proposed (i) that phonological phrase structure is isomorphic to syntactic structure in Akan, and (ii) that the process of RVH is blocked at the edge of a maximal phonological phrase; this is formulated in terms of a domain-sensitive CrispEdge constraint.
We compute explicitly, and without any extra regularity assumptions, the large time limit of the fibrewise heat operator for Bismut-Lott type superconnections in the L-2-setting. This is motivated by index theory on certain non-compact spaces (families of manifolds with cocompact group action) where the convergence of the heat operator at large time implies refined L-2-index formulas.
As applications, we prove a local L-2-index theorem for families of signature operators and an L-2-Bismut-Lott theorem, expressing the Becker-Gottlieb transfer of flat bundles in terms of Kamber-Tondeur classes. With slightly stronger regularity we obtain the respective refined versions: we construct L-2-eta forms and L-2-torsion forms as transgression forms.
This is the first attempt at characterizing reading difficulty in Hindi using naturally occurring sentences. We created the Potsdam-Allahabad Hindi Eyetracking Corpus by recording eye-movement data from 30 participants at the University of Allahabad, India. The target stimuli were 153 sentences selected from the beta version of the Hindi-Urdu treebank. We find that word- or low-level predictors (syllable length, unigram and bigram frequency) affect first-pass reading times, regression path duration, total reading time, and outgoing saccade length. An increase in syllable length results in longer fixations, and an increase in word unigram and bigram frequency leads to shorter fixations. Longer syllable length and higher frequency lead to longer outgoing saccades. We also find that two predictors of sentence comprehension difficulty, integration and storage cost, have an effect on reading difficulty. Integration cost (Gibson, 2000) was approximated by calculating the distance (in words) between a dependent and head; and storage cost (Gibson, 2000), which measures difficulty of maintaining predictions, was estimated by counting the number of predicted heads at each point in the sentence. We find that integration cost mainly affects outgoing saccade length, and storage cost affects total reading times and outgoing saccade length. Thus, word-level predictors have an effect in both early and late measures of reading time, while predictors of sentence comprehension difficulty tend to affect later measures. This is, to our knowledge, the first demonstration using eye-tracking that both integration and storage cost influence reading difficulty.
Arsenic-containing fatty acids are a group of fat-soluble arsenic species (arsenolipids) which are present in marine fish and other seafood. Recently, it has been shown that arsenic-containing hydrocarbons, another group of arsenolipids, exert toxicity in similar concentrations comparable to arsenite although the toxic modes of action differ. Hence, a risk assessment of arsenolipids is urgently needed. In this study the cellular toxicity of a saturated (AsFA 362) and an unsaturated (AsFA 388) arsenic-containing fatty acid and three of their proposed metabolites (DMA(V), DMAPr and thio-DMAPr) were investigated in human liver cells (HepG2). Even though both arsenic-containing fatty acids were less toxic as compared to arsenic-containing hydrocarbons and arsenite, significant effects were observable at mu M concentrations. DMA(V) causes effects in a similar concentration range and it could be seen that it is metabolised to its highly toxic thio analogue thio-DMA(V) in HepG2 cells. Nevertheless, DMAPr and thio-DMAPr did not exert any cytotoxicity. In summary, our data indicate that risks to human health related to the presence of arsenic-containing fatty acids in marine food cannot be excluded. This stresses the need for a full in vitro and in vivo toxicological characterisation of these arsenolipids.
Brownian motion is ergodic in the Boltzmann-Khinchin sense that long time averages of physical observables such as the mean squared displacement provide the same information as the corresponding ensemble average, even at out-of-equilibrium conditions. This property is the fundamental prerequisite for single particle tracking and its analysis in simple liquids. We study analytically and by event-driven molecular dynamics simulations the dynamics of force-free cooling granular gases and reveal a violation of ergodicity in this Boltzmann-Khinchin sense as well as distinct ageing of the system. Such granular gases comprise materials such as dilute gases of stones, sand, various types of powders, or large molecules, and their mixtures are ubiquitous in Nature and technology, in particular in Space. We treat-depending on the physical-chemical properties of the inter-particle interaction upon their pair collisions-both a constant and a velocity-dependent (viscoelastic) restitution coefficient epsilon. Moreover we compare the granular gas dynamics with an effective single particle stochastic model based on an underdamped Langevin equation with time dependent diffusivity. We find that both models share the same behaviour of the ensemble mean squared displacement (MSD) and the velocity correlations in the limit of weak dissipation. Qualitatively, the reported non-ergodic behaviour is generic for granular gases with any realistic dependence of epsilon on the impact velocity of particles.
The aim of this work was to verify the processing of pronominal anaphora by children that have attention deficit hyperactivity disorder or dyslexia. The sample studied consisted of 75 children that speak German, which read two texts of 80 words containing pronominal anaphora. The eye movements of all participants were recorded and, to make sure they were reading with attention, two activities that tested reading comprehension were proposed. Through the analysis of eye movements, specifically the fixations, the data indicate that children with disorders have difficulty to process the pronominal anaphora, especially dyslexic children.
This paper does a critical reading of Beyond the Horizon and The Housemaid and observes that the author, Amma Darko, seeks primarily to challenge prevailing and traditional views of motherhood held by African societies; i.e. motherhood and its associated activities such as caring, training and disciplining. Amma Darko sharply condemns this view and calls for a critical analysis of the nature of motherhood, especially in contemporary times. Agreeing with Amma Darko and taking issues raised by her even a little further, with snippets from the books, the paper brings to the fore the fact that the prevailing and traditional views of motherhood have inherent conflict with reality. That is to say, these views are carelessly assumed as problem-free. Within this context, we also critically bring into discussion the running theme of exploiting the exploiter in the two books within the framework of gender studies and queer theory. We also generally question the fixed categories of paradigms generated by normative ideology and conclude with the realisation that almost all mothers (and, for that matter, exhibition of womanhood) in these novels failed because of the wrong choices they made, which were basically and largely fuelled by challenging economic conditions.
Geochemistry and Ar-40/Ar-39 age of Early Carboniferous dolerite sills in the southern Baltic Sea
(2015)
The Early Carboniferous magmatic event in the southern Baltic Sea is manifested by dolerite intrusions. The presumable area in which the dolerite intrusions occur ranges from 30 to 60 km in east-west direction, and is about 100 km in north-south direction. The dolerites were sampled in well D1-1 and investigated by applying chemical analysis and Ar-40/Ar-39 step-heating dating. Dolerites are classified as alkali and sodic, characterized by high TiO2 (3.92, 3.99 wt%) and P2O5 (1.67, 1.77 wt%) and low MgO (4.89, 4.91 wt%) concentrations, enriched in light rare earth elements, originated from an enriched mantle magma source and emplaced in a continental rift tectonic setting. The 351 +/- 11 Ma Ar-40/Ar-39 plateau age for groundmass plagioclase indicates a considerable age gap with the 310-250 Ma magmatism in southern Scandinavia and northern Germany. The magmatic rocks in the Baltic Sedimentary Basin are coeval with alkaline intrusions of NE Poland. Both magmatic provinces lie in the northwestward prolongation of the Pripyat-Dnieper-Donetsk Rift (370-359 Ma) and may constitute a later phase of magmatic activity of this propagating rift system.
Accelerating climate change and increased economic and environmental interests in permafrost-affected regions have resulted in an acute need for more directed permafrost research. In June 2014, 88 early career researchers convened to identify future priorities for permafrost research. This multidisciplinary forum concluded that five research topics deserve greatest attention: permafrost landscape dynamics, permafrost thermal modeling, integration of traditional knowledge, spatial distribution of ground ice, and engineering issues. These topics underline the need for integrated research across a spectrum of permafrost-related domains and constitute a contribution to the Third International Conference on Arctic Research Planning (ICARP III).
Impacts of warming and changes in precipitation frequency on the regeneration of two Acer species
(2015)
The phase behavior of an amphiphilic block copolymer based on a poly(aspartic acid) hydrophilic block and a poly(n-butyl acrylate) hydrophobic block was investigated at the air-water and air-buffer interface. The polymer forms stable monomolecular films on both subphases. At low pH, the isotherms exhibit a plateau. Compression-expansion experiments and infrared reflection absorption spectroscopy suggest that the plateau is likely due to the formation of polymer bi- or multilayers. At high pH the films remain intact upon compression and no multilayer formation is observed. Furthermore, the mineralization of calcium phosphate beneath the monolayer was studied at different pH. The pH of the subphase and thus the polymer charge strongly affects the phase behavior of the film and the mineral formation. After 4 h of mineralization at low pH, atomic force microscopy shows smooth mineral films with a low roughness. With increasing pH the mineral films become inhomogeneous and the roughness increases. Transmission electron microscopy confirms this: at low pH a few small but uniform particles form whereas particles grown at higher pH are larger and highly agglomerated. Energy-dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy confirm the formation of calcium phosphate. The levels of mineralization are higher in samples grown at high pH.
Background: Previous studies have shown that BMP4 may play an important part in the development of auditory neurons (ANs), which are degenerated in sensorineural hearing loss. However, whether BMP4 can promote sensory fate specification from mesenchymal stromal cells (MSCs) is unknown so far.
Methods: MSCs isolated from Sprague-Dawley (SD) rats were confirmed by expression of MSC markers using flow cytometry and adipogenesis/osteogenesis using differentiation assays. MSCs treated with a complex of neurotrophic factors (BMP4 group and non-BMP4 group) were induced into auditory neuron-like cells, then the differences between the two groups were analyzed in morphological observation, cell growth curve, qRT-PCR, and immunofluorescence.
Results: Flow cytometric analysis showed that the isolated cells expressed typical MSC surface markers. After adipogenic and osteogenic induction, the cells were stained by oil red O and Alizarin Red. The neuronal induced cells were in the growth plateau and had special forms of neurons. In the presence of BMP4, the inner ear genes NF-M, Neurog1, GluR4, NeuroD, Calretinin, NeuN, Tau, and GATA3 were up-regulated in MSCs.
Conclusions: MSCs have the capacity to differentiate into auditory neuron-like cells in vitro. As an effective inducer, BMP4 may play a key role in transdifferentiation.
The role of givenness, presupposition, and prosody in Czech word order: An experimental study
(2015)
The zebrafish embryonic heart is composed of only a few hundred cells, representing only a small fraction of the entire embryo. Therefore, to prevent the cardiac transcriptome from being masked by the global embryonic transcriptome, it is necessary to collect sufficient numbers of hearts for further analyses. Furthermore, as zebrafish cardiac development proceeds rapidly, heart collection and RNA extraction methods need to be quick in order to ensure homogeneity of the samples. Here, we present a rapid manual dissection protocol for collecting functional/beating hearts from zebrafish embryos. This is an essential prerequisite for subsequent cardiac-specific RNA extraction to determine cardiac-specific gene expression levels by transcriptome analyses, such as quantitative real-time polymerase chain reaction (RT-qPCR). The method is based on differential adhesive properties of the zebrafish embryonic heart compared with other tissues; this allows for the rapid physical separation of cardiac from extracardiac tissue by a combination of fluidic shear force disruption, stepwise filtration and manual collection of transgenic fluorescently labeled hearts.
Research has shown that learning disabilities are associated with internalizing problems in (pre) adolescents. In order to examine this relationship for math disability (MD), math achievement and internalizing problem scores were measured in a representative group of 1,436 (pre) adolescents. MD was defined by a discrepancy between math achievement and IQ. Internalizing problems were measured through a multi-informant (parents, teachers, self-report) approach. The results revealed that MD puts (pre) adolescents at a higher risk for internalizing problems. External and self-ratings differed between boys and girls, indicating that either they show distinct internalizing symptoms or they are being perceived differently by parents and teachers. Results emphasize the importance of both a multi-informant approach and the consideration of gender differences when measuring internalizing symptomatology of children with MD. For an optimal treatment of MD, depressive and anxious symptoms need to be considered.
Aim - Plant reintroductions and other forms of targeted species translocations will in the future gain growing importance for nature conservation. In fragmented habitats, species reintroductions offer one of the most efficient tools for preserving or restoring plant diversity. In our study, we have compiled available data about plant reintroduction projects in Germany to answer the following questions: (1) What are the characteristics, habitat preferences and ecological strategies of species considered in plant reintroduction trials, and are these representative of the entire class of threatened species in Germany? (2) Is the judgment of the success or failure of plant reintroductions biased by the choice of species used in the experiments? (3) Do reintroduction efforts focus on those species for which Germany has a particularly high responsibility for conservation?
Methods - Information about reintroduction projects in Germany were obtained from published and internet sources as well as unpublished reports. In our search we focused on single-species trials in the framework of scientific or conservation projects. For all threatened species included in our database, we compiled information on their systematics, life form, ecological strategies and habitat preferences. A list of all species being threatened nationally or regionally, comprising both reintroduced and not reintroduced species, served as a reference for statistical analysis.
Results - The list of vascular plants used in conservation-oriented reintroductions consisted of 196 taxa. Species of families with large and conspicuous, mostly insect-pollinated flowers (for example, Orchidaceae) were over-represented among the reintroduced species compared to those threatened species not included in reintroduction trials. Species considered were also more often than expected found in semi-natural open habitats such as heathlands and grasslands. Notably, many projects focused on calcareous grasslands, characterized by dry, high-pH and infertile soils. In contrast, species of more near-natural vegetation (alpine and rocky formations, forests) were under-represented. About 25% of the species that were reintroduced are not threatened on the national scale. Out of 150 species for which Germany has a particularly high responsibility for conservation, only 14 (9.3%) were reintroduced. For only about 1/3 of all reintroduction attempts, success or failure were documented; whereas the success rate appears to be relatively low in nutrient-poor environments, trials with nutrient-demanding and competitive species were more successful.
Conclusions - We conclude that conservation-oriented reintroduction attempts should focus more on species for which the country or a region has a particular high responsibility. Reintroductions, to a larger extent than at present, also need to consider the different chances of success in different habitat types and environments.
Diverse anatomy of the tongue and taste organs in five species of caecilian (Amphibia: Gymnophiona)
(2015)
Limited previous studies on caecilian taste organs have demonstrated the presence of very few taste buds in the oral epithelium, while providing somewhat contradictory reports of their distribution within the oropharynx and across taxa. Here we report on the gross morphology of the tongue and explore the distribution, number and morphology of taste organs of five caecilian species representing five families, focusing upon variation within the group and investigating whether larvae and adults have the same type of taste organs. We find that taste buds are widespread in the oropharynx of caecilians and that they occur both in adults and larvae of a species with a biphasic life history. Thus Gymnophiona differ substantially from Batriachia, which have distinct larval and adult taste organs.
Exposure to organic mercury compounds promotes primarily neurological effects. Although methylmercury is recognized as a potent neurotoxicant, its transfer into the central nervous system (CNS) is not fully evaluated. While methylmercury and thiomersal pass the blood-brain barrier, limited data are available regarding the second brain regulating interface, the blood-cerebrospinal fluid (CSF) barrier. This novel study was designed to investigate the effects of organic as well as inorganic mercury compounds on, and their transfer across, a porcine in vitro model of the blood-CSF barrier for the first time. The barrier system is significantly more sensitive towards organic Hg compounds as compared to inorganic compounds regarding the endpoints cytotoxicity and barrier integrity. Whereas there are low transfer rates from the blood side to the CSF side, our results strongly indicate an active transfer of the organic mercury compounds out of the CSF. These results are the first to demonstrate an efflux of organic mercury compounds regarding the CNS and provide a completely new approach in the understanding of mercury compounds specific transport.
Organic mercury (Hg) species exert their toxicity primarily in the central nervous system. The food relevant Hg species methylmercury (MeHg) has been frequently studied regarding its neurotoxic effects in vitro and in vivo. Neurotoxicity of thiomersal, which is used as a preservative in medical preparations, is to date less characterised. Due to dealkylation of organic Hg or oxidation of elemental Hg, inorganic Hg is present in the brain albeit these species are not able to readily cross the blood brain barrier. This study compared for the first time toxic effects of organic MeHg chloride (MeHgCl) and thiomersal as well as inorganic mercury chloride (HgCl2) in differentiated human neurons (LUHMES) and human astrocytes (CCF-STTG1). The three Hg species differ in their degree and mechanism of toxicity in those two types of brain cells. Generally, neurons are more susceptible to Hg species induced cytotoxicity as compared to astrocytes. This might be due to the massive cellular mercury uptake in the differentiated neurons. The organic compounds exerted stronger cytotoxic effects as compared to inorganic HgCl2. In contrast to HgCl2 exposure, organic Hg compounds seem to induce the apoptotic cascade in neurons following low-level exposure. No indicators for apoptosis were identified for both inorganic and organic mercury species in astrocytes. Our studies clearly demonstrate species-specific toxic mechanisms. A mixed exposure towards all Hg species in the brain can be assumed. Thus, prospectively coexposure studies as well as cocultures of neurons and astrocytes could provide additional information in the investigation of Hg induced neurotoxicity.
Complex biopolymers (BPs) such as chitin and cellulose provide the majority of organic carbon in aquatic ecosystems, but the mechanisms by which communities of bacteria in natural systems exploit them are unclear. Previous degradation experiments in artificial systems predominantly used microcosms containing a single bacterial species, neglecting effects of interspecific interactions. By constructing simplified aquatic microbial communities, we tested how the addition of other bacterial species, of a nanoflagellate protist capable of consuming bacteria, or of both, affect utilization of BPs. Surprisingly, total abundance of resident bacteria in mixed communities increased upon addition of the protist. Concomitantly, bacteria shifted from free-living to aggregated morphotypes that seemed to promote utilization of BPs. In our model system, these interactions significantly increased productivity in terms of overall bacterial numbers and carbon transfer efficiency. This indicates that interactions on microbial aggregates may be crucial for chitin and cellulose degradation. We therefore suggest that interspecific microbial interactions must be considered when attempting to model the turnover of the vast pool of complex biopolymers in aquatic ecosystems.
Inflammation in Cachexia
(2015)
NaYF4:Yb:Er nanoparticles (UCNP) were synthesized under mild experimental conditions to obtain a pure cubic lattice. Upon annealing at different temperatures up to T-an = 700 degrees C phase transitions to the hexagonal phase and back to the cubic phase were induced. The UCNP materials obtained for different T-an were characterized with respect to the lattice phase using standard XRD and Raman spectroscopy as well as steady state and time resolved upconversion luminescence. The standard techniques showed that for the annealing temperature range 300 degrees C < T-an < 600 degrees C the hexagonal lattice phase was dominant. For T-an < 300 degrees C hardly any change in the lattice phase could be deduced, whereas for T-an > 600 degrees C a back transfer to the alpha-phase was observed. Complementarily, the luminescence upconversion properties of the annealed UCNP materials were characterized in steady state and time resolved luminescence measurements. Distinct differences in the upconversion luminescence intensity, the spectral intensity distribution and the luminescence decay kinetics were found for the cubic and hexagonal lattice phases, respectively, corroborating the results of the standard analytical techniques used. In laser power dependent measurements of the upconversion luminescence intensity it was found that the green (G1, G2) and red (R) emission of Er3+ showed different effects of T-an on the number of required photons reflecting the differences in the population routes of different energy levels involved. Furthermore, the intensity ratio of G(full)/R is highly effected by the laser power only when the beta-phase is present, whereas the G1/G2 intensity ratio is only slightly effected regardless of the crystal phase. Moreover, based on different upconversion luminescence kinetics characteristics of the cubic and hexagonal phase time-resolved area normalized emission spectra (TRANES) proved to be a very sensitive tool to monitor the phase transition between cubic and hexagonal phases. Based on the TRANES analysis it was possible to resolve the lattice phase transition in more detail for 200 degrees C < T-an < 300 degrees C, which was not possible with the standard techniques.
The following article aims to show how the Zionist movement defined its loyalty to Zionism, Germany, and German culture, as well as its reaction to the First World War. Central to the Zionist movement was the "creation of a home for Jewish people secured by public law." This is why superficial examinations assume that for Zionists the conflicts of the European powers were important only as they affected the pursuit of their own political agendas, an impression intensified by their posture of reserve towards military service. Crucial for Zionist positions on the First World War are the discourses revolving around the relationship between German culture, patriotism, and loyalty within the movement. This project is conducted with the help of the Judische Rundschau (JR; Jewish Review), which functions as the official organ of the "Zionistische Vereinigung fur Deutschland" (ZVfD; Zionist Association of Germany).
The article describes the history of Jews in Europe from the end of the Middle Ages until the aftermath of the Second World War as a sequence of migrational processes. It thereby demonstrates how the migration paradigm can contribute to a comprehensive understanding of European Jewish history during the given period by better explaining the various types of settlement, as well as other central phenomena of Jewish existence, such as inclusion/exclusion, assimilation/acculturation, and anti-Semitism. The article tries to assess the significance of the "religious factor" within the complex interdependencies between so-called "push" and "pull" factors that determined the individual migrations. In most cases, religious motives played only a minor role, while economic factors tended to dominate, particularly in regard to the functions Jews, as members of a minority, were permitted to carry out in the context of non-Jewish majority societies.
As an example of migration of the Franciscans, this article pursues the effects of their idea of mission: acquisition and transfer of knowledge concerning non-Christians in the communication of missionaries, using the examples of journeys to Mongolia or the encounter with indigenous peoples in the New World (Aztecs).
These friars wanted to teach non-Christians rather than subjugate them. The context of religion and migration resulted in a "boom" of inculturation. And the same context shows the way the Franciscans claimed their identity as well as their struggle, how Franciscans connected pastoral care with recognition of the cultural and religious plurality of Christendom. They embodied what it could mean to say: "our monastery is the world".
X-ray spectroscopy is a powerful tool to study the local charge distribution of chemical systems. Together with the liquid jet it becomes possible to probe chemical systems in their natural environment, the liquid phase. In this work, we present X-ray absorption (XA), X-ray emission (XE) and resonant inelastic X-ray scattering (RIXS) data of pure water and various salt solutions and show the possibilities these methods offer to elucidate the nature of ion-water interaction.
Improving semi-automated glacier mapping with a multi-method approach: applications in central Asia
(2015)
Studies of glaciers generally require precise glacier outlines. Where these are not available, extensive manual digitization in a geographic information system (GIS) must be performed, as current algorithms struggle to delineate glacier areas with debris cover or other irregular spectral profiles. Although several approaches have improved upon spectral band ratio delineation of glacier areas, none have entered wide use due to complexity or computational intensity.
In this study, we present and apply a glacier mapping algorithm in Central Asia which delineates both clean glacier ice and debris-covered glacier tongues. The algorithm is built around the unique velocity and topographic characteristics of glaciers and further leverages spectral and spatial relationship data. We found that the algorithm misclassifies between 2 and 10% of glacier areas, as compared to a similar to 750 glacier control data set, and can reliably classify a given Landsat scene in 3-5 min.
The algorithm does not completely solve the difficulties inherent in classifying glacier areas from remotely sensed imagery but does represent a significant improvement over purely spectral-based classification schemes, such as the band ratio of Landsat 7 bands three and five or the normalized difference snow index. The main caveats of the algorithm are (1) classification errors at an individual glacier level, (2) reliance on manual intervention to separate connected glacier areas, and (3) dependence on fidelity of the input Landsat data.
Dendritic cells (DC) contribute to immunity by presenting antigens to T cells and shape the immune response by the secretion of cytokines. Due to their immune stimulatory potential DC-based therapies are promising approaches to overcome tolerance e.g. against tumors. In order to enforce the immunogenicity of DCs, they have to be matured and activated in vitro, which requires an appropriate cell culture substrate, supporting their survival expansion and activation.
Since most cell culture devices are not optimized for DC growth, it is hypothesized that polymers with certain physicochemical properties can positively influence the DC cultures. With the aim to evaluate the effects that polymers with different chemical compositions have on the survival, the activation status, and the cytokine/chemokine secretion profile of DC, their interaction with polystyrene (PS), polycarbonate (PC), poly(ether imide) (PEI), and poly(styrene-co-acrylonitrile) (PSAN)-based cell culture inserts was investigated. By using this insert system, which fits exactly into 24 well cell culture plates, effects induced from the culture dish material can be excluded. The viability of untreated DC after incubation with the different inserts was not influenced by the different inserts, whereas LPS-activatedDCshowed an increased survival after cultivation on PC, PS, and PSAN compared to tissue culture polystyrene (TCP). The activation status of DC estimated by the expression of CD40, CD80, CD83, CD86 and HLA-DR expression was not altered by the different inserts in untreated DC but slightly reduced when LPS-activated DC were cultivated on PC, PS, PSAN, and PEI compared to TCP. For each polymeric cell culture insert a distinct cytokine profile could be observed.
Since inserts with different chemical compositions of the inserts did not substantially alter the behavior of DC all insert systems could be considered as alternative substrate. The observed increased survival on some polymers, which showed in contrast to TCP a hydrophobic surface, could be beneficial for certain applications such as T cell expansion and activation.
Polyether ether ketone (PEEK) as a high-performance, thermoplastic implant material entered the field of medical applications due to its structural function and commercial availability. In bone tissue engineering, the combination of mesenchymal stem cells (MSCs) with PEEK implants may accelerate the bone formation and promote the osseointegration between the implant and the adjacent bone tissue. In this concept the question how PEEK influences the behaviour and functions of MSCs is of great interest. Here the cellular response of human adipose-derived MSCs to PEEK was evaluated and compared to tissue culture plate (TCP) as the reference material. Viability and morphology of cells were not altered when cultured on the PEEK film. The cells on PEEK presented a high proliferation activity in spite of a relatively lower initial cell adhesion rate. There was no significant difference on cell apoptosis and senescence between the cells on PEEK and TCP. The inflammatory cytokines and VEGF secreted by the cells on these two surfaces were at similar levels. The cells on PEEK showed up-regulated BMP2 and down-regulated BMP4 and BMP6 gene expression, whereas no conspicuous differences were observed in the committed osteoblast markers (BGLAP, COL1A1 and Runx2). With osteoinduction the cells on PEEK and TCP exhibited a similar osteogenic differentiation potential. Our results demonstrate the biofunctionality of PEEK for human MSC cultivation and differentiation. Its clinical benefits in bone tissue engineering may be achieved by combining MSCs with PEEK implants. These data may also provide useful information for further modification of PEEK with chemical or physical methods to regulate the cellular processes of MSCs and to consequently improve the efficacy of MSC-PEEK based therapies.
Silicones are widely used as biomaterials for medical devices such as extracorporeal equipments. However, there is often conflicting evidence about their supposed cell-and histocompatibility. Macrophages could mediate silicone-induced adverse responses such as foreign body reaction and fibrous encapsulation. The polarization behaviour of macrophages could determine the clinical outcome after implantation of biomaterials. Induction of classically activated macrophages (CAM) may induce and support uncontrolled inflammatory responses and undesired material degradation. In contrast, polarization into alternatively activated macrophages (AAM) is assumed to support healing processes and implant integration.
This study compared the interaction of non-polarized macrophages (M0), CAM, and AAM with commercially available tissue culture polystyrene (TCP) and a medical grade silicone-based biomaterial, regarding the secretion of inflammatory mediators such as cytokines and chemokines. Firstly, by using the Limulus amoebocyte lysate (LAL) test the silicone films were shown to be free of soluble endotoxins, which is the prerequisite to investigate their interaction with primary immune cells. Primary human monocyte-derived macrophages (M0) were polarized into CAM and AAM by addition of suitable differentiation factors. These macrophage subsets were incubated on the materials for 24 hours and their viability and cytokine secretion was assessed. In comparison to TCP, cell adhesion was lower on silicone after 24 hours for all three macrophage subsets. However, compared to TCP, silicone induced higher levels of certain inflammatory and chemotactic cytokines in M0, CAM, and AAM macrophage subsets.
Conclusively, it was shown that silicone has the ability to induce a pro-inflammatory state to different magnitudes dependent on the macrophage subsets. This priming of the macrophage phenotype by silicone could explain the incidence of severe foreign body complications observed in vivo.
Background/Aims: To investigate the renal phenotype under conditions of an activated renal ET-1 system in the status of nitric oxide deficiency, we compared kidney function and morphology in wild-type, ET-1 transgenic (ET+/+), endothelial nitric oxide synthase knockout (eNOS-/-) and ET+/+eNOS-/- mice. Methods: We assessed blood pressure, parameters of renal morphology, plasma cystatin C, urinary protein excretion, expression of genes associated with glomerular filtration barrier and tissue remodeling, and plasma metabolites using metabolomics. Results: eNOS-/- and ET+/+eNOS-/- mice developed hypertension. Osteopontin, albumin and protein excretion were increased in eNOS-/- and restored in ET+/+eNOS-/- animals. All genetically modified mice developed renal interstitial fibrosis and glomerulosclerosis. Genes involved in tissue remodeling (serpinel, TIMP1, Collal, CCL2) were up-regulated in eNOS-/-, but not in ET+/+eNOS-/- mice. Plasma levels of free carnitine and acylcarnitines, amino acids, diacyl phosphatidylcholines, lysophosphatidylcholines and hexoses were descreased in eNOS-/- and were in the normal range in ET+/+eNOS-/- mice. Conclusion: eNOS-/- mice developed renal dysfunction, which was partially rescued by ET-1 overexpression in eNOS-/- mice. The metabolomics results suggest that ET-1 overexpression on top of eNOS knockout is associated with a functional recovery of mitochondria (rescue effect in 13-oxidation of fatty acids) and an increase in antioxidative properties (normalization of monounsaturated fatty acids levels). (C) 2015 The Author(s) Published by S. Karger AG, Basel
We investigate the ergodic properties of a random walker performing (anomalous) diffusion on a random fractal geometry. Extensive Monte Carlo simulations of the motion of tracer particles on an ensemble of realisations of percolation clusters are performed for a wide range of percolation densities. Single trajectories of the tracer motion are analysed to quantify the time averaged mean squared displacement (MSD) and to compare this with the ensemble averaged MSD of the particle motion. Other complementary physical observables associated with ergodicity are studied, as well. It turns out that the time averaged MSD of individual realisations exhibits non-vanishing fluctuations even in the limit of very long observation times as the percolation density approaches the critical value. This apparent non-ergodic behaviour concurs with the ergodic behaviour on the ensemble averaged level. We demonstrate how the non-vanishing fluctuations in single particle trajectories are analytically expressed in terms of the fractal dimension and the cluster size distribution of the random geometry, thus being of purely geometrical origin. Moreover, we reveal that the convergence scaling law to ergodicity, which is known to be inversely proportional to the observation time T for ergodic diffusion processes, follows a power-law similar to T-h with h < 1 due to the fractal structure of the accessible space. These results provide useful measures for differentiating the subdiffusion on random fractals from an otherwise closely related process, namely, fractional Brownian motion. Implications of our results on the analysis of single particle tracking experiments are provided.
The plasmon resonance of metal nanoparticles determines their optical response in the visible spectral range. Many details such as the electronic properties of gold near the particle surface and the local environment of the particles influence the spectra. We show how the cheap but highly precise fabrication of composite nanolayers by spin-assisted layer-by-layer deposition of polyelectrolytes can be used to investigate the spectral response of gold nanospheres (GNS) and gold nanorods (GNR) in a self-consistent way, using the established Maxwell-Garnett effective medium (MGEM) theory beyond the limit of homogeneous media. We show that the dielectric function of gold nanoparticles differs from the bulk value and experimentally characterize the shape and the surrounding of the particles thoroughly by SEM, AFM and ellipsometry. Averaging the dielectric functions of the layered surrounding by an appropriate weighting with the electric field intensity yields excellent agreement for the spectra of several nanoparticles and nanorods with various cover-layer thicknesses.
Algorithm selection (AS) techniques - which involve choosing from a set of algorithms the one expected to solve a given problem instance most efficiently - have substantially improved the state of the art in solving many prominent AI problems, such as SAT, CSP, ASP, MAXSAT and QBF. Although several AS procedures have been introduced, not too surprisingly, none of them dominates all others across all AS scenarios. Furthermore, these procedures have parameters whose optimal values vary across AS scenarios. This holds specifically for the machine learning techniques that form the core of current AS procedures, and for their hyperparameters. Therefore, to successfully apply AS to new problems, algorithms and benchmark sets, two questions need to be answered: (i) how to select an AS approach and (ii) how to set its parameters effectively. We address both of these problems simultaneously by using automated algorithm configuration. Specifically, we demonstrate that we can automatically configure claspfolio 2, which implements a large variety of different AS approaches and their respective parameters in a single, highly-parameterized algorithm framework. Our approach, dubbed AutoFolio, allows researchers and practitioners across a broad range of applications to exploit the combined power of many different AS methods. We demonstrate AutoFolio can significantly improve the performance of claspfolio 2 on 8 out of the 13 scenarios from the Algorithm Selection Library, leads to new state-of-the-art algorithm selectors for 7 of these scenarios, and matches state-of-the-art performance (statistically) on all other scenarios. Compared to the best single algorithm for each AS scenario, AutoFolio achieves average speedup factors between 1.3 and 15.4.
The application of electrospray ionization (ESI) ion mobility (IM) spectrometry on the detection end of a high-performance liquid chromatograph has been a subject of study for some time. So far, this method has been limited to low flow rates or has required splitting of the liquid flow. This work presents a novel concept of an ESI source facilitating the stable operation of the spectrometer at flow rates between 10 mu L min(-1) and 1500 mu L min(-1) without flow splitting, advancing the T-cylinder design developed by Kurnin and co-workers. Flow rates eight times faster than previously reported were achieved because of a more efficient dispersion of the liquid at increased electrospray voltages combined with nebulization by a sheath gas. Imaging revealed the spray operation to be in a rotationally symmetric multijet-mode. The novel ESI-IM spectrometer tolerates high water contents (<= 90%) and electrolyte concentrations up to 10 mM, meeting another condition required of high-performance liquid chromatography (HPLC) detectors. Limits of detection of 50 nM for promazine in the positive mode and 1 mu M for 1,3-dinitrobenzene in the negative mode were established. Three mixtures of reduced complexity (five surfactants, four neuroleptics, and two isomers) were separated in the millisecond regime in stand-alone operation of the spectrometer. Separations of two more complex mixtures (five neuroleptics and 13 pesticides) demonstrate the application of the spectrometer as an HPLC detector. The examples illustrate the advantages of the spectrometer over the established diode array detector, in terms of additional IM separation of substances not fully separated in the retention time domain as well as identification of substances based on their characteristic IMs.
The primary motivation for systematic bases in first principles electronic structure simulations is to derive physical and chemical properties of molecules and solids with predetermined accuracy. This requires a detailed understanding of the asymptotic behaviour of many-particle Coulomb systems near coalescence points of particles. Singular analysis provides a convenient framework to study the asymptotic behaviour of wavefunctions near these singularities. In the present work, we want to introduce the mathematical framework of singular analysis and discuss a novel asymptotic parametrix construction for Hamiltonians of many-particle Coulomb systems. This corresponds to the construction of an approximate inverse of a Hamiltonian operator with remainder given by a so-called Green operator. The Green operator encodes essential asymptotic information and we present as our main result an explicit asymptotic formula for this operator. First applications to many-particle models in quantum chemistry are presented in order to demonstrate the feasibility of our approach. The focus is on the asymptotic behaviour of ladder diagrams, which provide the dominant contribution to short-range correlation in coupled cluster theory. Furthermore, we discuss possible consequences of our asymptotic analysis with respect to adaptive wavelet approximation.
Climate change and its impacts already pose considerable challenges for societies that will further increase with global warming (IPCC, 2014a, b). Uncertainties of the climatic response to greenhouse gas emissions include the potential passing of large-scale tipping points (e.g. Lenton et al., 2008; Levermann et al., 2012; Schellnhuber, 2010) and changes in extreme meteorological events (Field et al., 2012) with complex impacts on societies (Hallegatte et al., 2013). Thus climate change mitigation is considered a necessary societal response for avoiding uncontrollable impacts (Conference of the Parties, 2010). On the other hand, large-scale climate change mitigation itself implies fundamental changes in, for example, the global energy system. The associated challenges come on top of others that derive from equally important ethical imperatives like the fulfilment of increasing food demand that may draw on the same resources. For example, ensuring food security for a growing population may require an expansion of cropland, thereby reducing natural carbon sinks or the area available for bio-energy production. So far, available studies addressing this problem have relied on individual impact models, ignoring uncertainty in crop model and biome model projections. Here, we propose a probabilistic decision framework that allows for an evaluation of agricultural management and mitigation options in a multi-impact-model setting. Based on simulations generated within the Inter-Sectoral Impact Model Intercomparison Project (ISI-MIP), we outline how cross-sectorally consistent multi-model impact simulations could be used to generate the information required for robust decision making.
Using an illustrative future land use pattern, we discuss the trade-off between potential gains in crop production and associated losses in natural carbon sinks in the new multiple crop-and biome-model setting. In addition, crop and water model simulations are combined to explore irrigation increases as one possible measure of agricultural intensification that could limit the expansion of cropland required in response to climate change and growing food demand. This example shows that current impact model uncertainties pose an important challenge to long-term mitigation planning and must not be ignored in long-term strategic decision making.
The periglacial engine of mountain erosion - Part 2: Modelling large-scale landscape evolution
(2015)
There is growing recognition of strong periglacial control on bedrock erosion in mountain landscapes, including the shaping of low-relief surfaces at high elevations (summit flats). But, as yet, the hypothesis that frost action was crucial to the assumed Late Cenozoic rise in erosion rates remains compelling and untested. Here we present a landscape evolution model incorporating two key periglacial processes - regolith production via frost cracking and sediment transport via frost creep - which together are harnessed to variations in temperature and the evolving thickness of sediment cover. Our computational experiments time-integrate the contribution of frost action to shaping mountain topography over million-year timescales, with the primary and highly reproducible outcome being the development of flattish or gently convex summit flats. A simple scaling of temperature to marine delta O-18 records spanning the past 14 Myr indicates that the highest summit flats in mid-to high-latitude mountains may have formed via frost action prior to the Quaternary. We suggest that deep cooling in the Quaternary accelerated mechanical weathering globally by significantly expanding the area subject to frost. Further, the inclusion of subglacial erosion alongside periglacial processes in our computational experiments points to alpine glaciers increasing the long-term efficiency of frost-driven erosion by steepening hillslopes.
With accelerating climate cooling in the late Cenozoic, glacial and periglacial erosion became more widespread on the surface of the Earth. The resultant shift in erosion patterns significantly changed the large-scale morphology of many mountain ranges worldwide. Whereas the glacial fingerprint is easily distinguished by its characteristic fjords and U-shaped valleys, the periglacial fingerprint is more subtle but potentially prevails in some mid- to high-latitude landscapes. Previous models have advocated a frost-driven control on debris production at steep headwalls and glacial valley sides. Here we investigate the important role that periglacial processes also play in less steep parts of mountain landscapes. Understanding the influences of frost-driven processes in low-relief areas requires a focus on the consequences of an accreting soil mantle, which characterises such surfaces. We present a new model that quantifies two key physical processes: frost cracking and frost creep, as a function of both temperature and sediment thickness. Our results yield new insights into how climate and sediment transport properties combine to scale the intensity of periglacial processes. The thickness of the soil mantle strongly modulates the relation between climate and the intensity of mechanical weathering and sediment flux. Our results also point to an offset between the conditions that promote frost cracking and those that promote frost creep, indicating that a stable climate can provide optimal conditions for only one of those processes at a time. Finally, quantifying these relations also opens up the possibility of including periglacial processes in large-scale, long-term landscape evolution models, as demonstrated in a companion paper.
Models for estimating flood losses to infrastructure are rare and their reliability is seldom investigated although infrastructure losses might contribute considerably to the overall flood losses. In this paper, an empirical modelling approach for estimating direct structural flood damage to railway infrastructure and associated financial losses is presented. Via a combination of event data, i.e. photo-documented damage on the Northern Railway in Lower Austria caused by the March River flood in 2006, and simulated flood characteristics, i.e. water levels, flow velocities and combinations thereof, the correlations between physical flood impact parameters and damage occurred to the railway track were investigated and subsequently rendered into a damage model. After calibrating the loss estimation using recorded repair costs of the Austrian Federal Railways, the model was applied to three synthetic scenarios with return periods of 30, 100 and 300 years of March River flooding. Finally, the model results are compared to depth-damage-curve-based approaches for the infrastructure sector obtained from the Rhine Atlas damage model and the Damage Scanner model. The results of this case study indicate a good performance of our two-stage model approach. However, due to a lack of independent event and damage data, the model could not yet be validated. Future research in natural risk should focus on the development of event and damage documentation procedures to overcome this significant hurdle in flood damage modelling.
The electrophoretic deposition process was used to produce multi-layered ceramics consisting of alternating layers of fully stabilized cubic zirconia and partially stabilized tetragonal zirconia to make use of their different mechanical behaviour, investigating the possibility to deflect advancing cracks at the interfaces of the different layers. This crack deflection is apparently impacted by a toughening mechanism only found in the tetragonal stabilized zirconia polymorph and is characterized by the stress induced transformation of the metastable tetragonal phase into the monoclinic one, which is accompanied by a volume increase resulting in a closing mechanism for advancing cracks.
While improving the electrophoretic deposition process, we investigated the transformation toughening mechanism at the layer interfaces and their effect on crack propagation. Investigations involved a combination of different imaging methods, including light microscopy, white light interferometry, atomic force microscopy, scanning electron microscopy, energy dispersive X-ray spectroscopy and Raman spectroscopy.
Formalizing informal logic
(2015)
In this paper we investigate the extent to which formal argumentation models can handle ten basic characteristics of informal logic identified in the informal logic literature. By showing how almost all of these characteristics can be successfully modelled formally, we claim that good progress can be made toward the project of formalizing informal logic. Of the formal argumentation models available, we chose the Carneades Argumentation System (CAS), a formal, computational model of argument that uses argument graphs as its basis, structures of a kind very familiar to practitioners of informal logic through their use of argument diagrams.
We consider the signal detection problem in the Gaussian design trace regression model with low rank alternative hypotheses. We derive the precise (Ingster-type) detection boundary for the Frobenius and the nuclear norm. We then apply these results to show that honest confidence sets for the unknown matrix parameter that adapt to all low rank sub-models in nuclear norm do not exist. This shows that recently obtained positive results in [5] for confidence sets in low rank recovery problems are essentially optimal.
Botulinum toxin is a bacterial toxin that inhibits neurotransmitter release from neurons and thereby causes a flaccid paralysis. It is used as drug to treat a number of serious ailments and, more frequently, for aesthetic medical interventions. Botulinum toxin for pharmacological applications is isolated from bacterial cultures. Due to partial denaturation of the protein, the specific activity of these preparations shows large variations. Because of its extreme potential toxicity, pharmacological preparations must be carefully tested for their activity. For the current gold standard, the mouse lethality assay, several hundred thousand mice are killed per year. Alternative methods have been developed that suffer from one or more of the following deficits: In vitro enzyme assays test only the activity of the catalytic subunit of the toxin. Enzymatic and cell based immunological assays are specific for just one of the different serotypes. The current study takes a completely different approach that overcomes these limitations: Neuronal cell lines were stably transfected with plasmids coding for luciferases of different species, which were N-terminally tagged with leader sequences that redirect the luciferase into neuro-secretory vesicles. From these vesicles, luciferases were released upon depolarization of the cells. The depolarization-dependent release was efficiently inhibited by botulinum toxin in a concentration range (1 to 100 pM) that is used in pharmacological preparations. The new assay might thus be an alternative to the mouse lethality assay and the immunological assays already in use.
The present article is among the first reports on the effects of poly(ampholyte)s and poly(betaine) s on the biomimetic formation of calcium phosphate. We have synthesized a series of di- and triblock copolymers based on a non-ionic poly(ethylene oxide) block and several charged methacrylate monomers, 2-(trimethylammonium) ethyl methacrylate chloride, 2-((3-cyanopropyl)-dimethylammonium)ethyl methacrylate chloride, 3-sulfopropyl methacrylate potassium salt, and [2-(methacryloyloxy)ethyl]dimethyl-(3-sulfopropyl) ammonium hydroxide. The resulting copolymers are either positively charged, ampholytic, or betaine block copolymers. All the polymers have very high molecular weights of over 10(6) g mol(-1). All polymers are water-soluble and show a strong effect on the precipitation and dissolution of calcium phosphate. The strongest effects are observed with triblock copolymers based on a large poly(ethylene oxide) middle block (nominal M-n = 100 000 g mol(-1)). Surprisingly, the data show that there is a need for positive charges in the polymers to exert tight control over mineralization and dissolution, but that the exact position of the charge in the polymer is of minor importance for both calcium phosphate precipitation and dissolution.
BACKGROUND: Reproducible measurements of tendon structural properties are a prerequisite for accurate diagnosis of tendon disorders and for determination of their mechanical properties. Despite the widely used application of Ultrasonography (US) in musculoskeletal assessment, its operator dependency and lack of standardization influences the consistency of the measurement.
OBJECTIVE: To evaluate the intra-rater reproducibility of a standardized US method assessing the structural properties of the Achilles tendon (AT).
METHODS: Sixteen asymptomatic participants were positioned prone on an isokinetic dynamometer with the knee extended and ankle at 90. flexion. US was used to assess AT-length, cross-sectional area (CSA), and AT-elongation during isometric plantarflexion contraction. The intra-rater reproducibility was assessed by ICC (2.1), Test-Retest Variability (TRV, %), Bland-Altman analyses (Bias +/- LoA [1.96*SD]), and Standard-Error of Measurement (SEM).
RESULTS: Measurements of AT-length demonstrated an ICC of 0.93, TRV of 4.5 +/- 3.9%, Bias +/- LoA of -2.8 +/- 25.0 mm and SEM of 6.6 mm. AT-CSA showed an ICC of 0.79, TRV of 8.7 +/- 9.6%, Bias +/- LoA of 1.7 +/- 19.4 mm(2) and SEM of 5.3 mm(2). AT-elongation revealed an ICC of 0.92, TRV of 12.9 +/- 8.9%, Bias +/- LoA of 0.3 +/- 5.7 mm and SEM of 1.5 mm.
CONCLUSIONS: The presented methodology allows a reproducible assessment of Achilles tendon structural properties when performed by a single rater.
Had Hitler still managed to win at the End? Europe's Jews between Shoa Restructuring and new Dangers
(2015)
Maintaining quality
(2015)
Survey Research Methods has slightly revised its publication policies. Firstly, starting with the publication of this Editorial, SRM will accept - under specified conditions - manuscripts that discuss experiments in non-probability samples for peer-review. Secondly, SRM will require authors to publish replication materials of their study as Online supplement to their article. Finally, Survey Research Methods will publish replication studies of articles published in the journal. This Editorial gives reasons for these changes.
Background: Castilian-Spanish, Catalan, Galician, and European Portuguese are the most widely spoken languages of the Ibero-Romance group. An increasing number of authors have addressed the impact of aphasia on the morphosyntax of these varieties. However, accurate linguistic characterisations are scarce and the different sources of data have not been yet compiled.Aims: To stimulate state-of-the-art research, we provided a comprehensive summary of morphosyntactic aspects of Ibero-Romance and a review of how these are affected in non-fluent aphasia. The topics we dealt with are the use of verb argument structure and morphology, sentential negation and word order, definite articles, personal and reflexive pronouns, passives, topicalised constructions, questions, and relative clauses.Methods & Procedures: An exhaustive fieldwork and search of PubMed, Web of Science, and Medline records were performed to retrieve studies focused on morphosyntactic issues concerning the Ibero-Romance varieties. A total of 27 studies produced by 46 authors of varying background emerged. We did not review studies of category-specific deficits and aspects related to bilingual aphasia, although we assume that most speakers of Galician and Catalan are bilingual. Studies of spontaneous speech were included when no controlled experimental tasks were available.Outcomes & Results: The morphosyntactic commonalities of Ibero-Romance have been tackled from different theoretical perspectives. There exist asymmetries in findings which we explain with the use of different tasks (and task complexity) and individual differences between participants.Conclusions: Discourse-linking factors as well as deviations from the canonical pattern are recurrent answers to these asymmetries. A comprehensive theory of impairments in non-fluent aphasia integrating relevant aspects of both structural and processing accounts seems necessary.
This study presents a novel and easily applicable approach to recruit sulfhydryl-containing biomolecules to membranes by using a palmitic acid which is functionalized with a maleimide group. Notably, this strategy can also be employed with preformed (biological) membranes. The applicability of the assay is demonstrated by characterizing the binding of a Rhodamine-labeled peptide to lipid and cellular membranes using methods of fluorescence spectroscopy, lifetime measurement, and microscopy. Our approach offers new possibilities for preparing biologically active liposomes and manipulating living cells.
For an irreducible continuous time Markov chain, we derive the distribution of the first passage time from a given state i to another given state j and the reversed passage time from j to i, each under the condition of no return to the starting point. When these two distributions are identical, we say that i and j are in time duality. We introduce a new condition called permuted balance that generalizes the concept of reversibility and provides sufficient criteria, based on the structure of the transition graph of the Markov chain. Illustrative examples are provided.
In order to understand the timing of leaf wax synthesis in higher plants, we analysed the variability in leaf wax n-alkane concentration, composition (expressed as average chain length (ACL)), and delta H-2(wax) values as well as plant source water delta H-2 values (xylem and leaf water) in the evergreen tree Quercus agrifolia over a period of 9 months, beginning with leaf flush. We identified three distinct periods of leaf development with the first month following leaf flush being characterized by de novo synthesis and possibly removal of n-alkanes. During the following 3 months, n-alkane concentrations increased sevenfold and delta H-2(wax) and ACL values increased, suggesting this period was the major leaf wax n-alkane formation period. During the remaining 4 months of the experiment, stable values suggest cessation of leaf wax n-alkane formation. We find that n-alkane synthesis in Q. agrifolia takes place over 4 months, substantially longer than that observed for deciduous trees.
DNA origami nanostructures are a versatile tool that can be used to arrange functionalities with high local control to study molecular processes at a single-molecule level. Here, we demonstrate that DNA origami substrates can be used to suppress the formation of specific guanine (G) quadruplex structures from telomeric DNA. The folding of telomeres into G-quadruplex structures in the presence of monovalent cations (e.g. Na+ and K+) is currently used for the detection of K+ ions, however, with insufficient selectivity towards Na+. By means of FRET between two suitable dyes attached to the 3- and 5-ends of telomeric DNA we demonstrate that the formation of G-quadruplexes on DNA origami templates in the presence of sodium ions is suppressed due to steric hindrance. Hence, telomeric DNA attached to DNA origami structures represents a highly sensitive and selective detection tool for potassium ions even in the presence of high concentrations of sodium ions.
Land-use concepts provide decision support for the most efficient usage options according to sustainable development and multifunctionality requirements. However, developments in landscape-related, agricultural production schemes are primarily driven by economic benefits. Therefore, most agricultural land-use concepts tackle particular problems or interests and lack a systemic perspective. As a result, we discuss a conceptual model for future site-specific agricultural land-use with an inbuilt requirement for adequate experimental sites to enable monitoring systems for a new generation of ecosystem models and for new approaches to address science-stakeholder interactions.
We developed a new type of molecular rods consisting of two (or more) rigid units linked by a flexible joint. Consequently we called these constructs articulated rods (ARs). The syntheses of ARs were carried out by a flexible and modular approach providing access to a number of compounds with various functionalizations in terminal positions. First applications were presented with pyrene, cinnamoyl and anthracenyl labelled ARs.
Paging through history: parchment as a reservoir of ancient DNA for next generation sequencing
(2015)
Parchment represents an invaluable cultural reservoir. Retrieving an additional layer of information from these abundant, dated livestock-skins via the use of ancient DNA (aDNA) sequencing has been mooted by a number of researchers. However, prior PCR-based work has indicated that this may be challenged by cross-individual and cross-species contamination, perhaps from the bulk parchment preparation process. Here we apply next generation sequencing to two parchments of seventeenth and eighteenth century northern English provenance. Following alignment to the published sheep, goat, cow and human genomes, it is clear that the only genome displaying substantial unique homology is sheep and this species identification is confirmed by collagen peptide mass spectrometry. Only 4% of sequence reads align preferentially to a different species indicating low contamination across species. Moreover, mitochondrial DNA sequences suggest an upper bound of contamination at 5%. Over 45% of reads aligned to the sheep genome, and even this limited sequencing exercise yield 9 and 7% of each sampled sheep genome post filtering, allowing the mapping of genetic affinity to modern British sheep breeds. We conclude that parchment represents an excellent substrate for genomic analyses of historical livestock.
Leopard complex spotting is inherited by the incompletely dominant locus, LP, which also causes congenital stationary night blindness in homozygous horses. We investigated an associated single nucleotide polymorphism in the TRPM1 gene in 96 archaeological bones from 31 localities from Late Pleistocene (approx. 17 000 YBP) to medieval times. The first genetic evidence of LP spotting in Europe dates back to the Pleistocene. We tested for temporal changes in the LP associated allele frequency and estimated coefficients of selection by means of approximate Bayesian computation analyses. Our results show that at least some of the observed frequency changes are congruent with shifts in artificial selection pressure for the leopard complex spotting phenotype. In early domestic horses from Kirklareli-Kanligecit (Turkey) dating to 2700-2200 BC, a remarkably high number of leopard spotted horses (six of 10 individuals) was detected including one adult homozygote. However, LP seems to have largely disappeared during the late Bronze Age, suggesting selection against this phenotype in early domestic horses. During the Iron Age, LP reappeared, probably by reintroduction into the domestic gene pool from wild animals. This picture of alternating selective regimes might explain how genetic diversity was maintained in domestic animals despite selection for specific traits at different times.
In this work, gold nanostars (AuNSs) with size around 90 nm were prepared through an easy one-step method. They show excellent catalytic activity and large surface-enhanced Raman scattering (SERS) activity at the same time. Surprisingly, they exhibited different catalytic performance on the reduction of aromatic nitro compounds with different substituents on the para position. To understand such a difference, the SERS spectra were recorded, showing that the molecular orientation of reactants on the gold surface were different. We anticipate that this research will help to understand the relationship of the molecular orientation with the catalytic activity of gold nanoparticles.
We present the XMM-Newton discovery of X-ray emission from the planetary nebula (PN) A78, the second born-again PN detected in X-rays apart from A30. These two PNe share similar spectral and morphological characteristics: they harbor diffuse soft X-ray emission associated with the interaction between the H-poor ejecta and the current fast stellar wind and a point-like source at the position of the central star (CSPN). We present the spectral analysis of the CSPN, using for the first time an NLTE code for expanding atmospheres that takes line blanketing into account for the UV and optical spectra. The wind abundances are used for the X-ray spectral analysis of the CSPN and the diffuse emission. The X-ray emission from the CSPN in A78 can be modeled by a single C VI emission line, while the X-ray emission from its diffuse component is better described by an optically thin plasma emission model with a temperature of kT = 0.088 keV (T approximate to 1.0 x 10(6) K). We estimate X-ray luminosities in the 0.2-2.0 keV energy band of L-X,L-CSPN =(1.2 +/- 0.3) x 10(31) erg s(-1) and L-X,L-DIFF =(9.2 +/- 2.3) x 10(30) erg s(-1) for the CSPN and diffuse components, respectively.
We present the results of a broadband X-ray study of the enigmatic Be star Gamma Cassiopeiae (herein gamma Cas) based on observations made with both the Suzaku and INTEGRAL observatories.. Cas has long been recognized as the prototypical example of a small subclass of Be stars with moderately strong X-ray emission dominated by a hot thermal component in the 0.5-12 keV energy range (L-x approximate to 10(32)-10(33) erg s(-1)). This places them at the high end of the known luminosity distribution for stellar emission, but several orders of magnitude below typical accretion-powered Be X-ray binaries. The INTEGRAL observations spanned an eight-year baseline and represent the deepest measurement to date at energies above similar to 50 keV. We find that the INTEGRAL data are consistent within statistics to a constant intensity source above 20 keV, with emission extending up to similar to 100 keV, and that searches for all of the previously reported periodicities of the system at lower energies led to null results. We further find that our combined Suzaku and INTEGRAL spectrum, which we suggest is the most accurate broadband X-ray measurement of gamma Cas to date, is fitted extremely well with a thermal plasma emission model with a single absorption component. We found no compelling need for an additional non-thermal high-energy component. We discuss these results in the context of a currently favored models for gamma Cas and its analogs.
Magnetic reconnection in the partially ionized solar chromosphere is studied in 2.5 dimensional magnetohydrodynamic simulations including radiative cooling and ambipolar diffusion. A Harris current sheet with and without a guide field is considered. Characteristic values of the parameters in the middle chromosphere imply a high magnetic Reynolds number of similar to 10(6)-10(7) in the present simulations. Fast magnetic reconnection then develops as a consequence of the plasmoid instability without the need to invoke anomalous resistivity enhancements. Multiple levels of the instability are followed as it cascades to smaller scales, which approach the ion inertial length. The reconnection rate, normalized to the asymptotic values of magnetic field and Alfven velocity in the inflow region, reaches values in the range similar to 0.01-0.03 throughout the cascading plasmoid formation and for zero as well as for strong guide field. The outflow velocity reaches approximate to 40 km s(-1). Slow-mode shocks extend from the X-points, heating the plasmoids up to similar to 8 x 10(4) K. In the case of zero guide field, the inclusion of both ambipolar diffusion and radiative cooling causes a rapid thinning of the current sheet (down to similar to 30 m) and early formation of secondary islands. Both of these processes have very little effect on the plasmoid instability for a strong guide field. The reconnection rates, temperature enhancements, and upward outflow velocities from the vertical current sheet correspond well to their characteristic values in chromospheric jets.
We present results from VERITAS observations of the BL Lac object PG 1553+113 spanning the years 2010, 2011, and 2012. The time-averaged spectrum, measured between 160 and 560 GeV, is well described by a power law with a spectral index of 4.33 +/- 0.09. The time-averaged integral flux above 200 GeV measured for this period was (1.69 +/- 0.06) x 10(-11) photons cm(-2) s(-1), corresponding to 6.9% of the Crab Nebula flux. We also present the combined gamma-ray spectrum from the Fermi Large Area Telescope and VERITAS covering an energy range from 100 MeV to 560 GeV. The data are well fit by a power law with an exponential cutoff at 101.9 +/- 3.2 GeV. The origin of the cutoff could be intrinsic to PG 1553+113 or be due to the gamma-ray opacity of our universe through pair production off the extragalactic background light (EBL). Given lower limits to the redshift of z > 0.395 based on optical/UV observations of PG 1553+113, the cutoff would be dominated by EBL absorption. Conversely, the small statistical uncertainties of the VERITAS energy spectrum have allowed us to provide a robust upper limit on the redshift of PG 1553+113 of z <= 0.62. A strongly elevated mean flux of (2.50 +/- 0.14) x10(-11) photons cm(-2) s(-1) (10.3% of the Crab Nebula flux) was observed during 2012, with the daily flux reaching as high as (4.44 +/- 0.71) x10(-11) photons cm(-2) s(-1) (18.3% of the Crab Nebula flux) on MJD 56048. The light curve measured during the 2012 observing season is marginally inconsistent with a steady flux, giving a chi(2) probability for a steady flux of 0.03%.
We report on multifrequency observations performed during 2012 December-2013 August of the first narrow-line Seyfert 1 galaxy detected in gamma-rays, PMN J0948+0022 (z = 0.5846). A y -ray flare was observed by the Large Area Telescope on board Fermi during 2012 December-2013 January, reaching a daily peak flux in the 0.1-100 GeV energy range of (155 31) x 10 8 ph cm(-2) S-1 on 2013 January 1, corresponding to an apparent isotropic luminosity of similar to 1.5 x 1048 erg s(-1). The y -ray flaring period triggered Swift and Very Energetic Radiation Imaging Telescope Array System (VERITAS) observations in addition to radio and optical monitoring by Owens Valley Radio Observatory, Monitoring Of Jets in Active galactic nuclei with VLBA Experiments, and Catalina Real-time Transient Survey. A strong flare was observed in optical, UV, and X-rays on 2012 December 30, quasi-simultaneously to the y -ray flare, reaching a record flux for this source from optical to y gamma-rays. VERITAS observations at very high energy (E > 100 GeV) during 2013 January 6-17 resulted in an upper limit of F>0.2 Trev < 4.0 x 10(-12) ph cm(-2) s(-1). We compared the spectral energy distribution (SED) of the flaring state in 2013 January with that of an intermediate state observed in 2011. The two SEDs, modelled as synchrotron emission and an external Compton scattering of seed photons from a dust torus, can be modelled by changing both the electron distribution parameters and the magnetic field.
A series of three dialkyl phosphate resins with a Merrifield resin support was used to extract platinum from acidic media. In column operations total capacities of 85-130 mg/g were gained. The presence of palladium and rhodium results in the order: Pt(IV) > Pd(II) >> Rh(III). From a leach liquor gained from spent automotive catalysts metals forming anionic chloro complexes are co-extracted only to a small extent. However, in order to separate and enrich platinum a selective back-extraction can be done with a sodium thiocyanate solution. A second elution step with acidic thiourea leads to a mixed solution of palladium and rhodium.
While the influence of spatial-numerical associations in number categorization tasks has been well established, their role in mental arithmetic is less clear. It has been hypothesized that mental addition leads to rightward and upward shifts of spatial attention (along the "mental number line"), whereas subtraction leads to leftward and downward shifts. We addressed this hypothesis by analyzing spontaneous eye movements during mental arithmetic. Participants solved verbally presented arithmetic problems (e.g., 2 + 7, 8-3) aloud while looking at a blank screen. We found that eye movements reflected spatial biases in the ongoing mental operation: Gaze position shifted more upward when participants solved addition compared to subtraction problems, and the horizontal gaze position was partly determined by the magnitude of the operands. Interestingly, the difference between addition and subtraction trials was driven by the operator (plus vs. minus) but was not influenced by the computational process. Thus, our results do not support the idea of a mental movement toward the solution during arithmetic but indicate a semantic association between operation and space.
The Large Magellanic Cloud, a satellite galaxy of the Milky Way, has been observed with the High Energy Stereoscopic System (H.E.S.S.) above an energy of 100 billion electron volts for a deep exposure of 210 hours. Three sources of different types were detected: the pulsar wind nebula of the most energetic pulsar known, N 157B; the radio-loud supernova remnant N 132D; and the largest nonthermal x-ray shell, the superbubble 30 Dor C. The unique object SN 1987A is, unexpectedly, not detected, which constrains the theoretical framework of particle acceleration in very young supernova remnants. These detections reveal the most energetic tip of a g-ray source population in an external galaxy and provide via 30 Dor C the unambiguous detection of g-ray emission from a superbubble.
Background: The flowering plant Primula veris is a common spring blooming perennial that is widely cultivated throughout Europe. This species is an established model system in the study of the genetics, evolution, and ecology of heterostylous floral polymorphisms. Despite the long history of research focused on this and related species, the continued development of this system has been restricted due the absence of genomic and transcriptomic resources.
Results: We present here a de novo draft genome assembly of P. veris covering 301.8 Mb, or approximately 63% of the estimated 479.22 Mb genome, with an N50 contig size of 9.5 Kb, an N50 scaffold size of 164 Kb, and containing an estimated 19,507 genes. The results of a RADseq bulk segregant analysis allow for the confident identification of four genome scaffolds that are linked to the P. veris S-locus. RNAseq data from both P. veris and the closely related species P. vulgaris allow for the characterization of 113 candidate heterostyly genes that show significant floral morph-specific differential expression. One candidate gene of particular interest is a duplicated GLOBOSA homolog that may be unique to Primula (PveGLO2), and is completely silenced in L-morph flowers.
Conclusions: The P. veris genome represents the first genome assembled from a heterostylous species, and thus provides an immensely important resource for future studies focused on the evolution and genetic dissection of heterostyly. As the first genome assembled from the Primulaceae, the P. veris genome will also facilitate the expanded application of phylogenomic methods in this diverse family and the eudicots as a whole.
Mechanotransduction pathways are activated in response to biophysical stimuli during the development or homeostasis of organs and tissues. In zebrafish, the blood-flow-sensitive transcription factor Klf2a promotes VEGF-dependent angiogenesis. However, the means by which the Klf2a mechanotransduction pathway is regulated to prevent continuous angiogenesis remain unknown. Here we report that the upregulation of klf2 mRNA causes enhanced egfl7 expression and angiogenesis signaling, which underlies cardiovascular defects associated with the loss of cerebral cavernous malformation (CCM) proteins in the zebrafish embryo. Using CCM-protein-depleted human umbilical vein endothelial cells, we show that the misexpression of KLF2 mRNA requires the extracellular matrix-binding receptor beta 1 integrin and occurs in the absence of blood flow. Downregulation of beta 1 integrin rescues ccm mutant cardiovascular malformations in zebrafish. Our work reveals a beta 1 integrin-Klf2-Egfl7-signaling pathway that is tightly regulated by CCM proteins. This regulation prevents angiogenic overgrowth and ensures the quiescence of endothelial cells.
The structure of bulk liquid water was recently probed by x-ray scattering below the temperature limit of homogeneous nucleation (T-H) of similar to 232 K [J. A. Sellberg et al., Nature 510, 381-384 (2014)]. Here, we utilize a similar approach to study the structure of bulk liquid water below T-H using oxygen K-edge x-ray emission spectroscopy (XES). Based on previous XES experiments [T. Tokushima et al., Chem. Phys. Lett. 460, 387-400 (2008)] at higher temperatures, we expected the ratio of the 1b(1)' and 1b(1)" peaks associated with the lone-pair orbital in water to change strongly upon deep supercooling as the coordination of the hydrogen (H-) bonds becomes tetrahedral. In contrast, we observed only minor changes in the lone-pair spectral region, challenging an interpretation in terms of two interconverting species. A number of alternative hypotheses to explain the results are put forward and discussed. Although the spectra can be explained by various contributions from these hypotheses, we here emphasize the interpretation that the line shape of each component changes dramatically when approaching lower temperatures, where, in particular, the peak assigned to the proposed disordered component would become more symmetrical as vibrational interference becomes more important. (C) 2015 AIP Publishing LLC.
We study the linear and nonlinear acoustic response of SrTiO3 across its ferroelastic transition at T-a = 105 K by time domain Brillouin scattering. Above T-a we observe that for a strain amplitude of similar to 0.18% the sound velocity for compressive strain exceeds the tensile strain velocity by 3%. Below T-a we find a giant slowing down of the sound velocity by 12% and attribute this to the coupling of GHz phonons to ferroelastic twin domain walls. We propose a new mechanism for this coupling on the ultrafast time scale, providing an important new test ground for theories used to simulate atomic motion in domain forming crystals.