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- climate change (95)
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- diffusion (47)
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- gamma rays: general (46)
- German (45)
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- Institut für Ernährungswissenschaft (723)
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Srivastava, S. ; Kehrig, C. ; Kantharia, N. G. ; Pérez-Montero, E. ; Vílchez, J. M. ; Iglesias-Páramo, J. ; Janardhan, P.
The main objective of this work is to investigate the evolution of massive stars, and the interplay between them and the ionized gas for a sample of local metal-poor Wolf-Rayet galaxies.
Optical integral field spectrocopy was used in combination with multi-wavelength radio data.
Combining optical and radio data, we locate Wolf-Rayet stars and supernova remnants across the Wolf-Rayet galaxies to study the spatial correlation between them. This study will shed light on the massive star formation and its feedback, and will help us to better understand
distant star-forming galaxies.
Wichura, Henry ; Jacobs, Louis L. ; Lin, Andrew ; Polcyn, Michael J. ; Manthi, Fredrick K. ; Winkler, Dale A. ; Strecker, Manfred ; Clemens, Matthew
Timing and magnitude of surface uplift are key to understanding the impact of crustal deformation and topographic growth on atmospheric circulation, environmental conditions, and surface processes. Uplift of the East African Plateau is linked to mantle processes, but paleoaltimetry data are too scarce to constrain plateau evolution and subsequent vertical motions associated with rifting. Here, we assess the paleotopographic implications of a beaked whale fossil (Ziphiidae) from the Turkana region of Kenya found 740 km inland from the present-day coastline of the Indian Ocean at an elevation of 620 m. The specimen is similar to 17 My old and represents the oldest derived beaked whale known, consistent with molecular estimates of the emergence of modern straptoothed whales (Mesoplodon). The whale traveled from the Indian Ocean inland along an eastward-directed drainage system controlled by the Cretaceous Anza Graben and was stranded slightly above sea level. Surface uplift from near sea level coincides with paleoclimatic change from a humid environment to highly variable and much drier conditions, which altered biotic communities and drove evolution in east Africa, including that of primates.
Formation or destruction of hyperbolic chaotic attractor under parameter variation is considered with an example represented by Smale-Williams solenoid in stroboscopic Poincare map of two alternately excited non-autonomous van der Pol oscillators. The transition occupies a narrow but finite parameter interval and progresses in such way that periodic orbits constituting a "skeleton" of the attractor undergo saddle-node bifurcation events involving partner orbits from the attractor and from a non-attracting invariant set, which forms together with its stable manifold a basin boundary of the attractor.
Gruden, Kristina ; Hren, Matjaz ; Herman, Ana ; Blejec, Andrej ; Albrecht, Tanja ; Selbig, Joachim ; Bauer, Christian G. ; Schuchardt, Johannes ; Or-Guil, Michal ; Zupancic, Klemen ; Svajger, Urban ; Stabuc, Borut ; Ihan, Alojz ; Kopitar, Andreja Natasa ; Ravnikar, Maja ; Knezevic, Miomir ; Rozman, Primoz ; Jeras, Matjaz
Background: Different immunotherapy approaches for the treatment of cancer and autoimmune diseases are being developed and tested in clinical studies worldwide. Their resulting complex experimental data should be properly evaluated, therefore reliable normal healthy control baseline values are indispensable.
Methodology/Principal Findings: To assess intra- and inter-individual variability of various biomarkers, peripheral blood of 16 age and gender equilibrated healthy volunteers was sampled on 3 different days within a period of one month. Complex "crossomics'' analyses of plasma metabolite profiles, antibody concentrations and lymphocyte subset counts as well as whole genome expression profiling in CD4(+)T and NK cells were performed. Some of the observed age, gender and BMI dependences are in agreement with the existing knowledge, like negative correlation between sex hormone levels and age or BMI related increase in lipids and soluble sugars. Thus we can assume that the distribution of all 39.743 analysed markers is well representing the normal Caucasoid population. All lymphocyte subsets, 20% of metabolites and less than 10% of genes, were identified as highly variable in our dataset.
Conclusions/Significance: Our study shows that the intra- individual variability was at least two-fold lower compared to the inter-individual one at all investigated levels, showing the importance of personalised medicine approach from yet another perspective.
Many Central Stars of Planetary Nebulae are very similar to massive Wolf-Rayet stars of the carbon sequence with respect to their spectra, chemical composition and wind properties. Therefore their study opens an additional way towards the understanding of the Wolf-Rayet phenomenon. While the study of Line Profile Variation will be difficult, espescially for the very compact early types, the comparision with other hydrogen-deficient Central Stars illuminates the driving mechanism of their winds. We speculate that at least two ingredients are needed. The ionization of their atmpospheres has to be stratified to enable multi-scattering processes and the amount of carbon and oxygen has to be high (more than a few percent by mass).
The compound [Nb6Cl14(pyrazine)(4)]center dot 2CH(2)Cl(2) (1) was investigated for its suitability as a starting compound for new ligand-supported hexanuclear niobium cluster compounds. The synthesis, stability to air and increased temperature, solubility and usability for subsequent reactions of 1, and purification and separation of the reaction products are discussed. The compounds with cluster units [Nb6Cl14L4], where L = iso-quinoline N-oxides (2), 1,1-dimethylethylenediamines (3), or thiazoles (4), and [Nb6Cl14(PEt3)(3.76)(Et3PO)(0.24)]-[Nb6Cl14(MeCN)(4)]center dot 4MeCN (5) are presented as follow-up products. The crystal structures of compounds 1-5 are analyzed, and the structures are discussed with respect to their intraand intermolecular bonding situations and crystal packing. In addition to hydrogen bonds and pi-pi interactions, the appearance of chalcogen and halogen bonds and lone pair-pi interactions between Nb-6 cluster units was observed for the first time.
An easy-to-do synthesis for the hexanuclear niobium cluster compound [Nb6Cl12(CH3OH)(4)(OCH3)(2)] . DABCO . 1.66 CH2Cl2 has been developed. An one-pot reaction between the cluster precursor [Nb6Cl14(H2O)(4)] . 4H(2)O and methanol with the addition of DABCO leads to the crystallization of the title compound in high yield within a few minutes. The single-crystal X-ray structure of this cluster compound has been determined. Very strong, nearly symmetric intercluster hydrogen bonds Nb-6-MeO...H...OMe-Nb-6 are present between the cluster units. A bridging co-crystalline DABCO molecule is also involved in a three-dimensional hydrogen-bonding network.
Zehm, Daniel ; Fudickar, Werner ; Hans, Melanie ; Schilde, Uwe ; Kelling, Alexandra ; Linker, Torsten
A series of 9,10-diarylanthracenes with various substituents at the ortho positions have been synthesised by palladium-catalysed cross-coupling reactions. Such compounds exhibit interesting physical properties and can be applied as molecular switches. Despite the high steric demand of the substituents, products were formed in moderate-to-good yields. In some cases, microwave conditions further improved yields. Bis-coupling afforded two isomers (syn and anti) that do not interconvert at room temperature. These products were easily separated and their relative stereochemistries were unequivocally assigned by NMR spectroscopy and X-ray analysis. The syn and anti isomers exhibit different physical properties (e.g., melting points and solubilities) and interconversion by rotation around the aryl-aryl axis commences at <100 °C for fluoro-substituted diarylanthracenes and at >300 °C for alkyl- or alkoxy-substituted diarylanthracenes. The reactions with singlet oxygen were studied separately and revealed different reactivities and reaction pathways. The yields and reactivities depend on the size and electronic nature of the substituents. The anti isomers form the same 9,10-endoperoxides as the syn species, occasionally accompanied by unexpected 1,4-endoperoxides as byproducts. Thermolysis of the endoperoxides exclusively yielded the syn isomers. The interesting rotation around the aryl-aryl axis allows the application of 9,10-diarylanthracenes as molecular switches, which are triggered by light and air under mild conditions. Finally, the oxygenation and thermolysis sequence provides a simple, synthetic access to a single stereoisomer (syn) from an unselective coupling step.
Prenylated flavanones were obtained from ortho-allyloxy chalcones through a one-pot sequence of Claisen rearrangement and 6-endo-trig cyclization, followed by olefin cross metathesis of the intermediate allyl flavanones with 2-methyl-2-butene. The synthetic utility of this route is illustrated for the synthesis of several naturally occurring prenyl flavanones.
Yenesew, Abiy ; Twinomuhwezi, Hannington ; Kiremire, Bernard T. ; Mbugua, Martin N. ; Gitu, Peter M. ; Heydenreich, Matthias ; Peter, Martin G.
A new pterocarpan (named 8-methoxyneorautenol) was isolated from the acetone ext. of the root bark of Erythrina abyssinica. In addn., the known isoflavonoid derivs. eryvarin L, erycristagallin and shinpterocarpin were identified for the first time from the roots of this plant. The structures were detd. on the basis of spectroscopic evidence. The new compd. showed selective antimicrobial activity against Trichophyton mentagrophytes. The acetone ext. of the root bark of E. abyssinica showed radical scavenging activity towards 2,2-diphenyl-1-picrylhydrazyl radical (DPPH). The pterocarpenes, 3-hydroxy-9-methoxy-10-(3,3-dimethylallyl)pterocarpene and erycristagallin, were the most active constituents of the roots of this plant and showing dose-dependent activities similar to that of the std. quercetin. [on SciFinder (R)]
7a-O-methyldeguelol, a modified rotenoid with an open ring-C, from the roots of Derris trifoloata
(2005)
Yenesew, Abiy ; Mushibe, E. K. ; Induli, M. ; Derese, Solomon ; Midiwo, Jacob O. ; Kabaru, Jacques M. ; Heydenreich, Matthias ; Koch, Andreas ; Peter, Martin G.
From the acetone extract of the roots of Derris trifoliata an isollavonoid derivative, named 7a-O- methyldeguelol, a modified rotenoid with an open ring-C, representing a new sub-class of isollavonoids (the sub-class is here named as rotenoloid), was isolated and characterised. In addition, the known rotenoids, rotenone, deguelin and alpha-toxicarol, were identified. The structures were determined on the basis of spectroscopic evidence. Rotenone and deguelin were identified as the larvicidal principles of the acetone extract of the roots of Derris trifoliata. (c) 2005 Elsevier Ltd. All rights reserved
Muiva-Mutisya, Lois ; Macharia, Bernard ; Heydenreich, Matthias ; Koch, Andreas ; Akala, Hoseah M. ; Derese, Solomon ; Omosa, Leonidah K. ; Yusuf, Amir O. ; Kamau, Edwin ; Yenesew, Abiy
The CH2Cl2/MeOH (1: 1) extract of the roots of Tephrosia villosa showed good antiplasmodial activity against the chloroquine-sensitive (D6) and chloroquine-resistant (W2) strains of Plasmodium falciparum with IC50 values of 3.1 +/- 0.4 and 1.3 +/- 0.3 mu g/mL, respectively. Chromatographic separation of the extract yielded a new rotenoid, 6 alpha-hydroxy-alpha-toxicarol, along with five known rotenoids, (rotenone, deguelin, sumatrol, 12 alpha-hydroxy-alpha-toxicarol and villosinol). Similar treatment of the extract of the stem of Tephrosia purpurea (IC50 = 4.1 +/- 0.4 and 1.9 +/- 0.2 mu g/mL against D6 and W2 strains of P. falciparum, respectively) yielded a new flavone having a unique substituent at C-7/C-8 [trivial name (+)-tephrodin], along with the known flavonoids tachrosin, obovatin methyl ether and derrone. The relative configuration and the most stable conformation in (+)-tephrodin was determined by NMR and theoretical energy calculations. The rotenoids and flavones tested showed good to moderate antiplasmodial activities (IC50 = 9 +/- 23 mu M). Whereas the cytotoxicity of rotenoids is known, the flavones (+)-tephrodin and tachrosin did not show significant cytotoxicity (IC50 > 100 mu M;) against mammalian African monkey kidney (vero) and human larynx carcinoma (HEp2) cell lines. (C) 2014 Phytochemical Society of Europe. Published by Elsevier B.V. All rights reserved.
Zhang, Yang ; Huang, Wentao ; Huang, Baochun ; van Hinsbergen, Douwe J. J. ; Yang, Tao ; Dupont-Nivet, Guillaume ; Guo, Zhaojie
The Gongjue basin from the eastern Qiangtang terrane is located in the transition region where the regional structural lineation curves from east-west-oriented in Tibet to north-south-oriented in Yunnan. In this study, we sampled the red beds in the basin from the lower Gongjue to upper Ranmugou formations for the first time covering the entire stratigraphic profile. The stratigraphic ages are bracketed within 53-43Ma by new detrital zircon U-Pb ages constraining the maximum deposition age to 52.51.5Ma. Rock magnetic and petrographic studies indicate that detrital magnetite and hematite are the magnetic carriers. Positive reversals and fold tests demonstrate that the characteristic remanent magnetization has a primary origin. The Gongjue and Ranmugou formations yield mean characteristic remanent magnetization directions of D-s/I-s=31.0 degrees/21.3 degrees and D-s/I-s=15.9 degrees/22.0 degrees, respectively. The magnetic inclination of these characteristic remanent magnetizations is significantly shallowed compared to the expected inclination for the locality. However, the elongation/inclination correction method does not provide a meaningful correction, likely because of syn-depositional rotation. Rotations relative to the Eurasian apparent polar wander path occurred in three stages: Stage I, 33.33.4 degrees clockwise rotation during the deposition of the Gongjue and lower Ranmugou formations; Stage II, 26.93.7 degrees counterclockwise rotation during deposition of the lower and middle Ranmugou formation; and Stage III, 17.73.3 degrees clockwise rotation after 43Ma. The complex rotation history recorded in the basin is possibly linked to sinistral shear along the Qiangtang block during India indentation into Asia and the early stage of the extrusion of the northwestern Indochina blocks away from eastern Tibet.
The prehistory of electrets is not known yet, but it is quite likely that the electrostatic charging behavior of amber (Greek: τò ηλεκτρoν, i.e., “electron”) already was familiar to people in ancient cultures (China, Egypt, Greece, etc.), before the Greek philosopher and scientist Thales of Miletus (6th century BCE)-or rather his disciples and followers-reported it in writing (cf. Figure 1). More than two millennia later, William Gilbert (1544–1603), the physician of Queen Elizabeth I, coined the term “electric” in his book De Magnete, Magneticisque Corporibus, et de Magno Magnete Tellure (1600) for dielectric materials that attract like amber and that included sulfur and glass [1]. The second half of the 18th century saw the invention of the electrophorus or electrophore [2], a capacitive electret device, in 1762 by Johan Carl Wilcke (1732–1796).
Current applications in porphyrin chemistry require the use of unsymmetrically substituted porphyrins. Many current industrial interests in optics and biomedicine require systems with either pushpull (electron-donating and -withdrawing groups) or amphiphilic systems (hydrophobic and hydrophilic groups). In this context we present the class of 5,10-A2B2-type porphyrins for which two different substituents are positioned in diagonally opposite meso positions. Thus, the intramolecular dipole moment in these tetrapyrroles is positioned along a beta-beta vector passing through two pyrrole rings. This is opposite to the situation of the frequently used 5,15-A2BC porphyrins for which the dipole moment is oriented along a mesomeso axis. We have elaborated syntheses of the 5,10-A2B2 porphyrins by using transition-metal-catalyzed transformations of 5,10-A2 porphyrins or direct substitutions reactions thereof; this gives the target molecules in 2277% overall yields. The compounds exhibit interesting structural, spectroscopic, and optical features and can serve as building blocks for new porphyrin arrays and applications.
The shape and the actuation capability of state of the art robotic devices typically relies on multimaterial systems from a combination of geometry determining materials and actuation components. Here, we present multifunctional 4D-actuators processable by 3D-printing, in which the actuator functionality is integrated into the shaped body. The materials are based on crosslinked poly(carbonate-urea-urethane) networks (PCUU), synthesized in an integrated process, applying reactive extrusion and subsequent water-based curing. Actuation capability could be added to the PCUU, prepared from aliphatic oligocarbonate diol, isophorone diisocyanate (IPDI) and water, in a thermomechanical programming process. When programmed with a strain of epsilon(prog) = 1400% the PCUU networks exhibited actuation apparent by reversible elongation epsilon'(rev) of up to 22%. In a gripper a reversible bending epsilon'(rev)((be)(nd)()) in the range of 37-60% was achieved when the actuation temperature (T-high) was varied between 45 degrees C and 49 degrees C. The integration of actuation and shape formation could be impressively demonstrated in two PCUU-based reversible fastening systems, which were able to hold weights of up to 1.1 kg. In this way, the multifunctional materials are interesting candidate materials for robotic applications where a freedom in shape design and actuation is required as well as for sustainable fastening systems.
Flow phenomena in the unsaturated zone are highly variable in time and space. Thus, it is challenging to measure and monitor such processes under field conditions. Here, we present a new setup and interpretation approach for combining a dye tracer experiment with a 4D ground-penetrating radar (GPR) survey. Therefore, we designed a rainfall experiment during which we measured three surface-based 3D GPR surveys using a pair of 500 MHz antennas. Such a survey setup requires accurate acquisition and processing techniquesto extract time-lapse information supporting the interpretation of selected cross-sections photographed after excavating the site. Our results reveal patterns of traveltime changes in the measured GPR data, which are associated with soil moisture changes. As distinct horizons are present at our site, such changes can be quantified and transferred into changes in total soil moisture content. Our soil moisture estimates are similar to the amount of infiltrated water, which confirms our experimental approach and makes us confident for further developing this strategy, especially, with respect to improving the temporal and spatial resolution. (C) 2015 Elsevier B.V. All rights reserved.
(40)A/Ar-39 step-heating of mica and amphibole megacrysts from hauyne-bearing olivine melilitite scoria/tephra from the Zelezna hurka yielded a 435 +/- 108 ka isotope correlation age for phlogopite and a more imprecise 1.55 Ma total gas age of the kaersutite megacryst. The amphibole megacrysts may constitute the first, and the younger phlogopite megacrysts the later phase of mafic, hydrous melilitic magma crystallization. It cannot be ruled out that the amphibole megacrysts are petrogenetically unrelated to tephra and phlogopite megacrysts and were derived from mantle xenoliths or disaggregated older, deep crustal pegmatites. This is in line both with the rarity of amphibole at Zelezna hurka and with the observed signs of magmatic resorption at the edges of amphibole crystals.
40Ar/39Ar dating of a hydrothermal pegmatitic buddingtonite–muscovite assemblage from Volyn, Ukraine
(2022)
We determined Ar-40/Ar-39 ages of buddingtonite, occurring together with muscovite, with the laser-ablation method. This is the first attempt to date the NH4-feldspar buddingtonite, which is typical for sedimentary-diagenetic environments of sediments, rich in organic matter, or in hydrothermal environments, associated with volcanic geyser systems. The sample is a hydrothermal breccia, coming from the Paleoproterozoic pegmatite field of the Korosten Plutonic Complex, Volyn, Ukraine. A detailed characterization by optical methods, electron microprobe analyses, backscattered electron imaging, and IR analyses showed that the buddingtonite consists of euhedral-appearing platy crystals of tens of micrometers wide, 100 or more micrometers in length, which consist of fine-grained fibers of <= 1 mu m thickness. The crystals are sector and growth zoned in terms of K-NH4-H3O content. The content of K allows for an age determination with the Ar-40/Ar-39 method, as well as in the accompanying muscovite, intimately intergrown with the buddingtonite. The determinations on muscovite yielded an age of 1491 +/- 9 Ma, interpreted as the hydrothermal event forming the breccia. However, buddingtonite apparent ages yielded a range of 563 +/- 14 Ma down to 383 +/- 12 Ma, which are interpreted as reset ages due to Ar loss of the fibrous buddingtonite crystals during later heating. We conclude that buddingtonite is suited for Ar-40/Ar-39 age determinations as a supplementary method, together with other methods and minerals; however, it requires a detailed mineralogical characterization, and the ages will likely represent minimum ages.
Schwarzer, Christian ; Huamani, Fatima Cßceres ; Cano, Asunción ; La Torre, María I. La ; Weigend, Maximilian
The Huaynaputina eruption (1600 AD, Moquegua, S Peru) in the northern Atacama Desert denuded the Ornate area of all vegetation and deposited deep pumice layers. Data on the flora, climate and soil characteristics of these slopes near Ornate at 1600-2600 m a.s.l. are provided. Fifty-nine angiosperm species established themselves on the pumice slopes in the past ca. 400 years, with the bulk of the small and herbaceous species and several species new records for Peru. Three Ornate sites were sampled in both a dry and a wet year and species numbers differed widely (14 versus 45 spp.). Among areas compared floristic composition is most similar to the Lomas de Tacna, and has less in common with geographically closer Lomas or Sierra formations. Nine species represent highly disjunct populations (200->700 km) from their nearest known living populations in central Peru, Chile, or Argentina/Bolivia and appear to have reached the area via long-distance dispersal. Abiotic conditions may have played an important role in limiting the establishment of species from the neighboring vegetation. Four taxa on the pumice slopes show clear morphological differences to populations elsewhere, two of them may represent neoendemics of the Ornate pumice, indicating rapid morphological divergence. (C) 2010 Elsevier Ltd. All rights reserved.
4-Alkyl-2,2,6,6-tetramethyl-1,4,2,6-oxaazadisilinanes RN[CH2Si(Me)2]2O [R = Me (1), i-Pr (2)] were synthesized by two methods which provided good yields up to 84%. Low temperature NMR study of compounds (1) and (2) revealed a frozen ring inversion with the energy barriers of 8.5 and 7.7 kcal/mol at 163 and 143 K, respectively, which is substantially lower than that for their carbon analog, N-methylmorpholine. DFT calculations performed on the example of molecule (1) showed that N-Meax conformer to exist in the sofa conformation with the coplanar fragment C-Si-O-Si-C, and its N-Meeq conformer in a flattened chair conformation.
4,4 '-Bis(tert-butyl)-2,2 '-bipyridinedichlorometal(II) - Synthesis, structure and EPR spectroscopy
(2011)
Due to the better solubility of the 4,4'-substituted bipyridine ligand a series of 4,4'0-bis(tert-butyl)-2,2'-bipyridinedichlorometal(II) complexes, [M(tbbpy)Cl(2)], with M = Cu, Ni, Zn, Pd, Pt was synthesised and characterised. The blue copper complex 4,4'-bis(tert-butyl)-2,2'-bipyridinedichlorocopper(II) was isolated in two different polymorphic forms, as prisms 1 with a solvent inclusion and solvent-free as needles 2. Both structures were determined by X-ray structure analysis. They crystallise in the monoclinic space group P2(1)/c with four molecules in the unit cell, but with different unit cells and packing motifs. Whereas in the prisms 1, with the unit cell parameters a = 12.1613(12), b = 10.6363(7), c = 16.3074(15) angstrom, eta = 94.446(8)degrees, the packing is dominated by intra-and intermolecular hydrogen bonds, in the needles 2, with a = 7.738(1), b = 18. 333(2), c = 13.291(3) angstrom, beta = 97.512(15)degrees, only intramolecular hydrogen bonds appear and the complex molecules are arranged in columns which are stabilised by p-p-stacking interactions. In both complexes the copper has a tetrahedrally distorted coordination sphere. These copper complexes were also studied by EPR spectroscopy in solution, as frozen glass and diamagnetically diluted powder with the analogue [Pd(tbbpy)Cl(2)] as host lattice.
Derese, Solomon ; Barasa, Leonard ; Akala, Hoseah M. ; Yusuf, Amir O. ; Kamau, Edwin ; Heydenreich, Matthias ; Yenesew, Abiy
The CH2Cl2/MeOH (1: 1) extract of the stem bark of Millettia oblata ssp. teitensis showed antiplasmodial activity (IC50 = 10-12 mu g/mL) against the chloroquine-sensitive (D6) and chloroquine-resistant (W2) strains of Plasmodium falciparum. Chromatographic separation of the extract led to the isolation of a new isoflavone, 4'-prenyloxyderrone (1), together with known isoflavones (8-O-methylretusin, durmillone, maximaisoflavone B, maximaisoflavone H and maximaisoflavone J), a rotenoid (tephrosin) and a triterpene (lupeol). Similar investigation of Millettia leucantha resulted in the identification of the isoflavones afrormosin and wistin, and the flavone chrysin. The identification of these compounds was based on their spectroscopic data. Five of the isoflavones isolated from these plants as well as 11 previously reported compounds from Millettia dura were tested and showed good to moderate antiplasmodial activities (IC50 = 13-53 mu M), with the new compound, 4'-prenyloxyderrone, being the most active (IC50 = 13-15 mu M).
Sarauli, David ; Peters, Kristina ; Xu, Chenggang ; Schulz, Burkhard ; Fattakhova-Rohlfing, Dina ; Lisdat, Fred
We report on the fabrication of a complex electrode architecture for efficient direct bioelectrocatalysis. In the developed procedure, the redox enzyme pyrroloquinoline quinone-dependent glucose dehydrogenase entrapped in a sulfonated polyaniline [poly(2-methoxyaniline-5-sulfonic acid)-co-aniline] was immobilized on macroporous indium tin oxide (macroITO) electrodes. The use of the 3D-conducting scaffold with a large surface area in combination with the conductive polymer enables immobilization of large amounts of enzyme and its efficient communication with the electrode, leading to enhanced direct bioelectrocatalysis. In the presence of glucose, the fabricated bioelectrodes show an exceptionally high direct bioelectrocatalytical response without any additional mediator. The catalytic current is increased more than 200-fold compared to planar ITO electrodes. Together with a high long-term stability (the current response is maintained for >90% of the initial value even after 2 weeks of storage), the transparent 3D macroITO structure with a conductive polymer represents a valuable basis for the construction of highly efficient bioelectronic units, which are useful as indicators for processes liberating glucose and allowing optical and electrochemical transduction.
A bright prominence associated with a coronal mass ejection (CME) was seen erupting from the Sun on 9 April 2008. This prominence was tracked by both the Solar Terrestrial Relations Observatory (STEREO) EUVI and COR1 telescopes, and was seen to rotate about the line of sight as it erupted; therefore, the event has been nicknamed the "Cartwheel CME." The threads of the prominence in the core of the CME quite clearly indicate the structure of a weakly to moderately twisted flux rope throughout the field of view, up to heliocentric heights of 4 solar radii. Although the STEREO separation was 48A degrees, it was possible to match some sharp features in the later part of the eruption as seen in the 304 line in EUVI and in the H alpha-sensitive bandpass of COR1 by both STEREO Ahead and Behind. These features could then be traced out in three-dimensional space, and reprojected into a view in which the eruption is directed toward the observer. The reconstructed view shows that the alignment of the prominence to the vertical axis rotates as it rises up to a leading-edge height of a parts per thousand aEuro parts per thousand 2.5 solar radii, and then remains approximately constant. The alignment at 2.5 solar radii differs by about 115A degrees from the original filament orientation inferred from H alpha and EUV data, and the height profile of the rotation, obtained here for the first time, shows that two thirds of the total rotation are reached within a parts per thousand aEuro parts per thousand 0.5 solar radii above the photosphere. These features are well reproduced by numerical simulations of an unstable moderately twisted flux rope embedded in external flux with a relatively strong shear field component.
We present 3D numerical simulations of the NGC6888 nebula considering the proper motion and the evolution of the star, from the red supergiant (RSG) to the Wolf-Rayet (WR) phase. Our simulations reproduce the limb-brightened morphology observed in [OIII] and X-ray emission maps. The synthetic maps computed by the numerical simulations show filamentary and clumpy structures produced by instabilities triggered in the interaction between the WR wind and the RSG shell.
Ground-penetrating radar (GPR) is an established geophysical tool to explore a wide range of near-surface environments. Today, the use of synthetic GPR data is largely limited to 2D because 3D modeling is computationally more expensive. In fact, only recent developments of modeling tools and powerful hardware allow for a time-efficient computation of extensive 3D data sets. Thus, 3D subsurface models and resulting GPR data sets, which are of great interest to develop and evaluate novel approaches in data analysis and interpretation, have not been made publicly available up to now. <br /> We use a published hydrofacies data set of an aquifer-analog study within fluvio-glacial deposits to infer a realistic 3D porosity model showing heterogeneities at multiple spatial scales. Assuming fresh-water saturated sediments, we generate synthetic 3D GPR data across this model using novel GPU-acceleration included in the open-source software gprMax. We present a numerical approach to examine 3D wave-propagation effects in modeled GPR data. Using the results of this examination study, we conduct a spatial model decomposition to enable a computationally efficient 3D simulation of a typical GPR reflection data set across the entire model surface. We process the resulting GPR data set using a standard 3D structural imaging sequence and compare the results to selected input data to demonstrate the feasibility and potential of the presented modeling studies. We conclude on conceivable applications of our 3D GPR reflection data set and the underlying porosity model, which are both publicly available and, thus, can support future methodological developments in GPR and other near-surface geophysical techniques.
Uhlig, Katja ; Madaboosi, Narayanan ; Schmidt, Stephan ; Jäger, Magnus S. ; Rose, Jürgen ; Duschl, Claus ; Volodkin, Dmitry V.
The interaction of diverse biomaterials with surfaces is more crucial than ever for biomedical applications to ensure efficiency and reproducibility. Very interesting surface materials are micrometer-thick polyelectrolyte multilayers. Not only their surface but also the bulk can be loaded with biomaterials like proteins or DNA for various purposes. Therefore, we established a method to analyze the lateral and vertical distribution of fluorescently labelled proteins of various size and charge in polyelectrolyte films composed of poly(L-lysine) and hyaluronic acid by confocal laser scanning microscopy. This approach enables us to measure the diffusion coefficients of the proteins via fluorescence recovery after photobleaching as a function of their vertical position in the film and facilitates the understanding of molecular interactions in the film with a high resolution in both space and time. As a result, we confirm that protein loading in the film is driven by electrostatic interactions - uncharged dextran molecules of 10 and 500 kDa do not diffuse into the film. Proteins of different sizes (3-11 nm) can diffuse relatively fast (D = 2-4 mm(2) s(-1)) independent of their net charge, indicating complex interpolymer interactions. This approach is a new powerful experimental tool to design the polyelectrolyte multilayers for bio-applications by finding a relationship between intermolecular interactions and mobility and availability of biomolecules to biological samples (e.g. cells) or detection units (e.g. biosensors).
Platz, Anna ; Weckmann, Ute ; Pek, Josef ; Kovacikova, Svetlana ; Klanica, Radek ; Mair, Johannes ; Aleid, Basel
The region of West Bohemia and Upper Palatinate belongs to the West Bohemian Massif. The study area is situated at the junction of three different Variscan tectonic units and hosts the ENE-WSW trending Ohre Rift as well as many different fault systems. The entire region is characterized by ongoing magmatic processes in the intra-continental lithospheric mantle expressed by a series of phenomena, including e.g. the occurrence of repeated earthquake swarms and massive degassing of mantle derived CO2 in form of mineral springs and mofettes. Ongoing active tectonics is mainly manifested by Cenozoic volcanism represented by different Quaternary volcanic structures. All these phenomena make the Ohre Rift a unique target area for European intra-continental geo-scientific research. With magnetotelluric (MT) measurements we image the subsurface distribution of the electrical resistivity and map possible fluid pathways. Two-dimensional (2D) inversion results by Munoz et al. (2018) reveal a conductive channel in the vicinity of the earthquake swarm region that extends from the lower crust to the surface forming a pathway for fluids into the region of the mofettes. A second conductive channel is present in the south of their model; however, their 2D inversions allow ambiguous interpretations of this feature. Therefore, we conducted a large 3D MT field experiment extending the study area towards the south. The 3D inversion result matches well with the known geology imaging different fluid/magma reservoirs at crust-mantle depth and mapping possible fluid pathways from the reservoirs to the surface feeding known mofettes and spas. A comparison of 3D and 2D inversion results suggests that the 2D inversion results are considerably characterized by 3D and off-profile structures. In this context, the new results advocate for the swarm earthquakes being located in the resistive host rock surrounding the conductive channels; a finding in line with observations e.g. at the San Andreas Fault, California.
Remote Sensing technologies allow to map biophysical, biochemical, and earth surface parameters of the land surface. Of especial interest for various applications in environmental and urban sciences is the combination of spectral and 3D elevation information. However, those two data streams are provided separately by different instruments, namely airborne laser scanner (ALS) for elevation and a hyperspectral imager (HSI) for high spectral resolution data. The fusion of ALS and HSI data can thus lead to a single data entity consistently featuring rich structural and spectral information. In this study, we present the application of fusing the first pulse return information from ALS data at a sub-decimeter spatial resolution with the lower-spatial resolution hyperspectral information available from the HSI into a hyperspectral point cloud (HSPC). During the processing, a plausible hyperspectral spectrum is assigned to every first-return ALS point. We show that the complementary implementation of spectral and 3D information at the point-cloud scale improves object-based classification and information extraction schemes. This improvements have great potential for numerous land cover mapping and environmental applications.
We present results of full 3D hydrodynamical and radiative transfer simulations of the colliding stellar winds in the massive binary system η Carinae. We accomplish this by applying the SimpleX algorithm for 3D radiative transfer on an unstructured Voronoi-Delaunay grid to recent 3D smoothed particle hydrodynamics (SPH) simulations of the binary colliding winds. We use SimpleX to obtain detailed ionization fractions of hydrogen and helium, in 3D, at the resolution of the original SPH simulations. We investigate several computational domain sizes and Luminous Blue Variable primary star mass-loss rates. We furthermore present new methods of visualizing and interacting with output from complex 3D numerical simulations, including 3D interactive graphics and 3D printing. While we initially focus on η Car, the methods employed can be applied to numerous other colliding wind (WR 140, WR 137, WR 19) and dusty `pinwheel' (WR 104, WR 98a) binary systems. Coupled with 3D hydrodynamical simulations, SimpleX simulations have the potential to help determine the regions where various observed time-variable emission and absorption lines form in these unique objects.
Pham, Cong Duc ; Petre, Anca ; Berquez, Laurent ; Flores Suárez, Rosaura ; Mellinger, Axel ; Wirges, Werner ; Gerhard, Reimund
In this paper, two non-destructive thermal methods are used in order to determine, with a high degree of accuracy, three-dimensional polarization distributions in thin films (12 mu m) of poly(vinylidenefluoride- trifluoroethylene) (PVDF-TrFE). The techniques are the frequency-domain Focused Laser Intensity Modulation Method (FLIMM) and time-domain Thermal-Pulse Tomography (TPT). Samples were first metalized with grid-shaped electrode and poled. 3D polarization mapping yielded profiles which reproduce the electrode-grid shape. The polarization is not uniform across the sample thickness. Significant polarization values are found only at depths beyond 0.5 mu m from the sample surface. Both methods provide similar results, TPT method being faster, whereas the FLIMM technique has a better lateral resolution.
Schennen, Stephan ; Tronicke, Jens ; Wetterich, Sebastian ; Allroggen, Niklas ; Schwamborn, Georg ; Schirrmeister, Lutz
Ice complex deposits are characteristic, ice-rich formations in northern East Siberia and represent an important part in the arctic carbon pool. Recently, these late Quaternary deposits are the objective of numerous investigations typically relying on outcrop and borehole data. Many of these studies can benefit from a 3D structural model of the subsurface for upscaling their observations or for constraining estimations of inventories, such as the local carbon stock. We have addressed this problem of structural imaging by 3D ground-penetrating radar (GPR), which, in permafrost studies, has been primarily used for 2D profiling. We have used a 3D kinematic GPR surveying strategy at a field site located in the New Siberian Archipelago on top of an ice complex. After applying a 3D GPR processing sequence, we were able to trace two horizons at depths below 20 m. Taking available borehole and outcrop data into account, we have interpreted these two features as interfaces of major lithologic units and derived a 3D cryostratigraphic model of the subsurface. Our data example demonstrated that a 3D surveying and processing strategy was crucial at our field site and showed the potential of 3D GPR to image geologic structures in complex ice-rich permafrost landscapes.
Ground-penetrating radar (GPR) is a standard geophysical technique used to image near-surface structures in sedimentary environments. In such environments, GPR data acquisition and processing are increasingly following 3D strategies. However, the processed GPR data volumes are typically still interpreted using selected 2D slices and manual concepts such as GPR facies analyses. In seismic volume interpretation, the application of (semi-)automated and reproducible approaches such as 3D attribute analyses as well as the production of attribute-based facies models are common practices today. In contrast, the field of 3D GPR attribute analyses and corresponding facies models is largely untapped. We have developed and applied a workflow to produce 3D attribute-based GPR facies models comprising the dominant sedimentary reflection patterns in a GPR volume, which images complex sandy structures on the dune island of Spiekeroog (Northern Germany). After presenting our field site and details regarding our data acquisition and processing, we calculate and filter 3D texture attributes to generate a database comprising the dominant texture features of our GPR data. Then, we perform a dimensionality reduction of this database to obtain meta texture attributes, which we analyze and integrate using composite imaging and (also considering additional geometric information) fuzzy c-means cluster analysis resulting in a classified GPR facies model. Considering our facies model and a corresponding GPR facies chart, we interpret our GPR data set in terms of near-surface sedimentary units, the corresponding depositional environments, and the recent formation history at our field site. Thus, we demonstrate the potential of our workflow, which represents a novel and clear strategy to perform a more objective and consistent interpretation of 3D GPR data collected across different sedimentary environments.
Ground-penetrating radar (GPR) is a method that can provide detailed information about the near subsurface in sedimentary and carbonate environments.
The classical interpretation of GPR data (e.g., based on manual feature selection) often is labor-intensive and limited by the experience of the intercally used for seismic interpretation, can provide faster, more repeatable, and less biased interpretations. We have recorded a 3D GPD data set collected across a paleokarst breccia pipe in the Billefjorden area on Spitsbergen, Svalbard. After performing advanced processing, we compare the results of a classical GPR interpretation to the results of an attribute-based classification.
Our attribute classification incorporates a selection of dip and textural attributes as the input for a k-means clustering approach. Similar to the results of the classical interpretation, the resulting classes differentiate between undisturbed strata and breccias or fault zones.
The classes also reveal details inside the breccia pipe that are not discerned in the classical fer that the intrapipe GPR facies result from subtle differences, such as breccia lithology, clast size, or pore-space filling.
Ibarra, Federico ; Liu, Sibiao ; Meeßen, Christian ; Prezzi, Claudia Beatriz ; Bott, Judith ; Scheck-Wenderoth, Magdalena ; Sobolev, Stephan Vladimir ; Strecker, Manfred
We present a new three-dimensional density model of the Central Andes characterizing the structure and composition of the lithosphere together with a geodynamic simulation subjected to continental intraplate shortening. The principal aim of this study is to assess the link between heterogeneities in the lithosphere and different deformation patterns and styles along the orogen-foreland system of the Central Andes. First, we performed a 3D integration of new geological and geophysical data with previous models through forward modelling of Bouguer anomalies. Subsequently, a geodynamic model was set-up and parametrized from the previously obtained 3D structure and composition. We do not find a unambigous correlation between the resulting density configuration and terrane boundaries proposed by other authors. Our models reproduce the observed Bouguer anomaly and deformation patterns in the foreland. We find that thin-skinned deformation in the Subandean fold-and thrust belt is controlled by a thick sedimentary layer and coeval underthrusting of thin crust of the foreland beneath the thick crust of the Andean Plateau. In the adjacent thick-skinned deformation province of the inverted Cretaceous extensional Santa Barbara System sedimentary strata are much thinner and crustal thickness transitions from greater values in the Andean to a more reduced thickness in the foreland. Our results show that deformation processes occur where the highest gradients of lithospheric strength are present between the orogen and the foreland, thus suggesting a spatial correlation between deformation and lithospheric strength.
Based on a numerical model of the Northeast German Basin (NEGB), we investigate the sensitivity of the calculated thermal field as resulting from heat conduction, forced and free convection in response to consecutive horizontal and vertical mesh refinements. Our results suggest that computational findings are more sensitive to consecutive horizontal mesh refinements than to changes in the vertical resolution. In addition, the degree of mesh sensitivity depends strongly on the type of the process being investigated, whether heat conduction, forced convection or free thermal convection represents the active heat driver. In this regard, heat conduction exhibits to be relative robust to imposed changes in the spatial discretization. A systematic mesh sensitivity is observed in areas where forced convection promotes an effective role in shorten the background conductive thermal field. In contrast, free thermal convection is to be regarded as the most sensitive heat transport process as demonstrated by non-systematic changes in the temperature field with respect to imposed changes in the model resolution.
Atilaw, Yoseph ; Heydenreich, Matthias ; Ndakala, Albert ; Akala, Hoseah M. ; Kamau, Edwin ; Yenesew, Abiy
The stem bark extract of Schizozygia coffaeoides (Apocynaceae) showed moderate antiplasmodial activity (IC50 = 8-12 mu g/mL) against the chloroquine-sensitive (D6) and chloroquine-resistant (W2) strains of Plasmodium falciparum. Chromatographic separation of the extract led to the isolation of a new schizozygane indoline alkaloid, named 3-oxo-14 alpha, 15 alpha-epoxyschizozygine. In addition, two dimeric anthraquinones, cassiamin A and cassiamin B, were identified for the first time in the family Apocynaceae. The structures of the isolated compounds were deduced on the basis of spectroscopic evidence. The schizozygane indole alkaloids showed good to moderate antiplasmodial activities (IC50 = 13-52 mu m). (C) 2014 Phytochemical Society of Europe. Published by Elsevier B.V. All rights reserved.
Mutai, Peggoty ; Heydenreich, Matthias ; Thoithi, Grace ; Mugumbate, Grace ; Chibale, Kelly ; Yenesew, Abiy
Two new 3-hydroxyisoflavanones, (S)-3,4',5-trihydroxy-2',7-dimethoxy-3'-prenylisoflavanone (trivial name kenusanone F 7-methyl ether) and (S)-3,5-dihydroxy-2',7-dimethoxy-2 '',2 ''-dimethylpyrano[5 '',6 '':3',4']isoflavanone (trivial name sophoronol-7-methyl ether) along with two known compounds (dalbergin and formononetin) were isolated from the stem bark of Dalbergia melanoxylon. The structures were elucidated using spectroscopic techniques. Kenusanone F 7-methyl ether showed activity against Mycobacterium tuberculosis, whereas both of the new compounds were inactive against the malaria parasite Plasmodium falciparum at 10 mu g/ml. Docking studies showed that the new compounds kenusanone F 7-methyl ether and sophoronol-7-methyl ether have high affinity for the M. tuberculosis drug target INHA.
Here, we study the 3-D subduction initiation process induced by the interaction between a hot thermochemical mantle plume and oceanic lithosphere using thermo-mechanical viscoplastic finite difference marker-in-cell models. Our numerical modeling results show that self-sustaining subduction is induced by plume-lithosphere interaction when the plume is sufficiently buoyant, the oceanic lithosphere is sufficiently old and the plate is weak enough to allow the buoyant plume to. pass through it. Subduction initiation occurs following penetration of the lithosphere by the hot plume and the downward displacement of broken, nearly circular segments of lithosphere (proto-slabs) as a result of partially molten plume rocks overriding the proto-slabs. Our experiments show four different deformation regimes in response to plume-lithosphere interaction: a) self-sustaining subduction initiation, in which subduction becomes self-sustaining; b) frozen subduction initiation, in which subduction stops at shallow depths; c) slab break-off, in which the subducting circular slab breaks off soon after formation; and d) plume underplating, in which the plume does not pass through the lithosphere and instead spreads beneath it (i.e., failed subduction initiation). These regimes depend on several parameters, such as the size, composition, and temperature of the plume, the brittle/plastic strength and age of the oceanic lithosphere, and the presence/absence of lithospheric heterogeneities. The results show that subduction initiates and becomes self-sustaining when the lithosphere is older than 10 Myr and the non dimensional ratio of the plume buoyancy force and lithospheric strength above the plume is higher than approximately 2. The outcomes of our numerical experiments are applicable for subduction initiation in the modern and Precambrian Earth and for the origin of plume-related corona structures on Venus. (C) 2016 Elsevier B.V. All rights reserved.
Gomez-Garcia, Angela Maria ; Meeßen, Christian ; Scheck-Wenderoth, Magdalena ; Monsalve, Gaspar ; Bott, Judith ; Bernhardt, Anne ; Bernal, Gladys
Geophysical data acquisition in oceanic domains is challenging, implying measurements with low and/or nonhomogeneous spatial resolution. The evolution of satellite gravimetry and altimetry techniques allows testing 3-D density models of the lithosphere, taking advantage of the high spatial resolution and homogeneous coverage of satellites. However, it is not trivial to discretise the source of the gravity field at different depths. Here, we propose a new method for inferring tectonic boundaries at the crustal level. As a novelty, instead of modeling the gravity anomalies and assuming a flat Earth approximation, we model the vertical gravity gradients (VGG) in spherical coordinates, which are especially sensitive to density contrasts in the upper layers of the Earth. To validate the methodology, the complex oceanic domain of the Caribbean region is studied, which includes different crustal domains with a tectonic history since Late Jurassic time. After defining a lithospheric starting model constrained by up-to-date geophysical data sets, we tested several a-priory density distributions and selected the model with the minimum misfits with respect to the VGG calculated from the EIGEN-6C4 data set. Additionally, the density of the crystalline crust was inferred by inverting the VGG field. Our methodology enabled us not only to refine, confirm, and/or propose tectonic boundaries in the study area but also to identify a new anomalous buoyant body, located in the South Lesser Antilles subduction zone, and high-density bodies along the Greater, Lesser, and Leeward Antilles forearcs.
Boldrighini, Carlo ; Frigio, Sandro ; Maponi, Pierluigi ; Pellegrinotti, Alessandro ; Sinai, Yakov G.
Guillemoteau, Julien ; Simon, Francois-Xavier ; Hulin, Guillaume ; Dousteyssier, Bertrand ; Dacko, Marion ; Tronicke, Jens
The in-phase response collected by portable loop-loop electromagnetic induction (EMI) sensors operating at low and moderate induction numbers (<= 1) is typically used for sensing the magnetic permeability (or susceptibility) of the subsurface. This is due to the fact that the in-phase response contains a small induction fraction and a preponderant induced magnetization fraction. The magnetization fraction follows the magneto-static equations similarly to the magnetic method but with an active magnetic source. The use of an active source offers the possibility to collect data with several loop-loop configurations, which illuminate the subsurface with different sensitivity patterns. Such multiconfiguration soundings thereby allows the imaging of subsurface magnetic permeability/susceptibility variations through an inversion procedure. This method is not affected by the remnant magnetization and theoretically overcomes the classical depth ambiguity generally encountered with passive geomagnetic data. To invert multiconfiguration in-phase data sets, we propose a novel methodology based on a full-grid 3-D multichannel deconvolution (MCD) procedure. This method allows us to invert large data sets (e.g. consisting of more than a hundred thousand of data points) for a dense voxel-based 3-D model of magnetic susceptibility subject to smoothness constraints. In this study, we first present and discuss synthetic examples of our imaging procedure, which aim at simulating realistic conditions. Finally, we demonstrate the applicability of our method to field data collected across an archaeological site in Auvergne (France) to image the foundations of a Gallo-Roman villa built with basalt rock material. Our synthetic and field data examples demonstrate the potential of the proposed inversion procedure offering new and complementary ways to interpret data sets collected with modern EMI instruments.
In the context of examining the potential usage of safe and sustainable geothermal energy in the Alberta Basin, whether in deep sediments or crystalline rock, the understanding of the in situ stress state is crucial. It is a key challenge to estimate the 3-D stress state at an arbitrarily chosen point in the crust, based on sparsely distributed in situ stress data.
To address this challenge, we present a large-scale 3-D geomechanical-numerical model (700 km x 1200 km x 80 km) from a large portion of the Alberta Basin, to provide a 3-D continuous quantification of the contemporary stress orientations and stress magnitudes. To calibrate the model, we use a large database of in situ stress orientation (321 S-Hmax) as well as stress magnitude data (981 S-V, 1720 S-hmin and 2 (+11) S-Hmax) from the Alberta Basin. To find the best-fit model, we vary the material properties and primarily the displacement boundary conditions of the model. This study focusses in detail on the statistical calibration procedure, because of the large amount of available data, the diversity of data types, and the importance of the order of data tests.
The best-fit model provides the total 3-D stress tensor for nearly the whole Alberta Basin, and allows estimation of stress orientation and stress magnitudes in advance of any well. First-order implications for the well design and configuration of enhanced geothermal systems are revealed. Systematic deviations of the modelled stress from the in situ data are found for stress orientations in the Peace River and the Bow Island Arch as well as for leak-off test magnitudes.
Gholamrezaie, Ershad ; Scheck-Wenderoth, Magdalena ; Bott, Judith ; Heidbach, Oliver ; Strecker, Manfred
Abstract. The Sea of Marmara, in northwestern Turkey, is a transition zone where the dextral North Anatolian Fault zone (NAFZ) propagates westward from the Anatolian Plate to the Aegean Sea Plate. The area is of interest in the context of seismic hazard of Istanbul, a metropolitan area with about 15 million inhabitants. Geophysical observations indicate that the crust is heterogeneous beneath the Marmara basin, but a detailed characterization of the crustal heterogeneities is still missing. To assess if and how crustal heterogeneities are related to the NAFZ segmentation below the Sea of Marmara, we develop new crustal-scale 3-D density models which integrate geological and seismological data and that are additionally constrained by 3-D gravity modeling. For the latter, we use two different gravity datasets including global satellite data and local marine gravity observation. Considering the two different datasets and the general non-uniqueness in potential field modeling, we suggest three possible “end-member” solutions that are all consistent with the observed gravity field and illustrate the spectrum of possible solutions. These models indicate that the observed gravitational anomalies originate from significant density heterogeneities within the crust. Two layers of sediments, one syn-kinematic and one pre-kinematic with respect to the Sea of Marmara formation are underlain by a heterogeneous crystalline crust. A felsic upper crystalline crust (average density of 2720 kgm⁻³) and an intermediate to mafic lower crystalline crust (average density of 2890 kgm⁻³) appear to be cross-cut by two large, dome-shaped mafic highdensity bodies (density of 2890 to 3150 kgm⁻³) of considerable thickness above a rather uniform lithospheric mantle (3300 kgm⁻³). The spatial correlation between two major bends of the main Marmara fault and the location of the highdensity bodies suggests that the distribution of lithological heterogeneities within the crust controls the rheological behavior along the NAFZ and, consequently, maybe influences fault segmentation and thus the seismic hazard assessment in the region.
Wiederkehr, Michael ; Bousquet, Romain ; Ziemann, Martin Andreas ; Berger, Alfons ; Schmid, Stefan M.
This study monitors regional changes in the crystallinity of carbonaceous matter (CM) by applying Micro-Raman spectroscopy to a total of 214 metasediment samples (largely so-called Bundnerschiefer) dominantly metamorphosed under blueschist- to amphibolite-facies conditions. They were collected within the northeastern margin of the Lepontine dome and easterly adjacent areas of the Swiss Central Alps. Three-dimensional mapping of isotemperature contours in map and profile views shows that the isotemperature contours associated with the Miocene Barrow-type Lepontine metamorphic event cut across refolded nappe contacts, both along and across strike within the northeastern margin of the Lepontine dome and adjacent areas. Further to the northeast, the isotemperature contours reflect temperatures reached during the Late Eocene subduction-related blueschist-facies event and/or during subsequent near-isothermal decompression; these contours appear folded by younger, large-scale post-nappe-stacking folds. A substantial jump in the recorded maximum temperatures across the tectonic contact between the frontal Adula nappe complex and surrounding metasediments indicates that this contact accommodated differential tectonic movement of the Adula nappe with respect to the enveloping Bundnerschiefer after maximum temperatures were reached within the northern Adula nappe, i.e. after Late Eocene time.
We present spectral classifications from optical spectroscopy of 263 massive stars in the north-eastern region of the Large Magellanic Cloud. The observed two-degree field includes the massive 30 Doradus star-forming region, the environs of SN1987A, and a number of star-forming complexes to the south of 30 Dor. These are the first classifications for the majority (203) of the stars and include eleven double-lined spectroscopic binaries. The sample also includes the first examples of early OC-type spectra (AA Omega 30 Dor 248 and 280), distinguished by the weakness of their nitrogen spectra and by C IV lambda 4658 emission. We propose that these stars have relatively unprocessed CNO abundances compared to morphologically normal O-type stars, indicative of an earlier evolutionary phase. From analysis of observations obtained on two consecutive nights, we present radial-velocity estimates for 233 stars, finding one apparent single-lined binary and nine (>3 sigma) outliers compared to the systemic velocity; the latter objects could be runaway stars or large-amplitude binary systems and further spectroscopy is required to investigate their nature.
Schulze, Patricia S. C. ; Bett, Alexander J. ; Bivour, Martin ; Caprioglio, Pietro ; Gerspacher, Fabian M. ; Kabaklı, Özde Ş. ; Richter, Armin ; Stolterfoht, Martin ; Zhang, Qinxin ; Neher, Dieter ; Hermle, Martin ; Hillebrecht, Harald ; Glunz, Stefan W. ; Goldschmidt, Jan Christoph
Monolithic perovskite silicon tandem solar cells can overcome the theoretical efficiency limit of silicon solar cells. This requires an optimum bandgap, high quantum efficiency, and high stability of the perovskite. Herein, a silicon heterojunction bottom cell is combined with a perovskite top cell, with an optimum bandgap of 1.68 eV in planar p-i-n tandem configuration. A methylammonium-free FA(0.75)Cs(0.25)Pb(I0.8Br0.2)(3) perovskite with high Cs content is investigated for improved stability. A 10% molarity increase to 1.1 m of the perovskite precursor solution results in approximate to 75 nm thicker absorber layers and 0.7 mA cm(-2) higher short-circuit current density. With the optimized absorber, tandem devices reach a high fill factor of 80% and up to 25.1% certified efficiency. The unencapsulated tandem device shows an efficiency improvement of 2.3% (absolute) over 5 months, showing the robustness of the absorber against degradation. Moreover, a photoluminescence quantum yield analysis reveals that with adapted charge transport materials and surface passivation, along with improved antireflection measures, the high bandgap perovskite absorber has the potential for 30% tandem efficiency in the near future.
Most 2.5D controlled-source electromagnetic (CSEM) modeling algorithms presented to date explicitly consider only sources that are point dipoles oriented parallel or perpendicular to the direction of constant conductivity. This makes simulations of complex source geometries expensive, requiring separate evaluations of many point dipole fields, and thus limits the practical applicability of such schemes for simulating and interpreting field data. We present a novel 2.5D CSEM modeling scheme that overcomes this limitation and permits efficient simulations of sources with general shape and orientation by evaluating fields for the entire source at once. We accommodate general sources by using a secondary field approach, in which primary fields are computed for the general source and a 1D background conductivity model. To carry out the required Fourier transforms between space and wavenumber domain using the same fast cosine and sine transform filters as in conventional algorithms, we split the primary and secondary fields into their symmetric and antisymmetric parts. For complex 3D source geometries, this approach is significantly more efficient than previous 2.5D algorithms. Our finite-difference algorithm also includes novel approaches for divergence correction at low frequencies and EM field interpolation across conductivity discontinuities. We describe the modeling scheme and demonstrate its accuracy and efficiency by comparisons of 2.5D-simulated data with 1D and 3D results.
The complete H-1 and C-13 NMR chemical shifts assignment for various 2-substituted and 2,2-disubstituted adamantane derivatives 1-38 in CDCl3 solution was realized on the basis of NMR experiments combined with chemical structure information and DFT-GIAO (B3LYP/6-31+G(d,p)-GIAO) calculations of chemical shifts in solution. Substituent-induced C-13 NMR chemical shifts (SCS) are discussed. C-H-ax center dot center dot center dot Y-ax contacts are a textbook prototype of steric hindrance in organic chemistry. The nature of these contacts will be further investigated in this work on basis of new adamantane derivatives, which are substituted at C-2 to provide models for 1,4-C-H-ax center dot center dot center dot Y-ax and 1,5-C-H-ax center dot center dot center dot Y-ax contacts. The B3LYP/6-31+G(d,p) calculations predicted the presence of NBO hyperconjugative attractive interactions between C-H-ax and Y-ax groups along C-H-ax center dot center dot center dot Y-ax contacts. The H-1 NMR signal separation, Delta delta(gamma-CH2), reflects the strength of the H-bonded C-H-ax center dot center dot center dot Y-ax contact. (C) 2015 Elsevier Ltd. All rights reserved.
A series of 5-unsubstituted and 5-substituted 2-alkylidene-4-oxothiazolidine-S-oxides were synthesized by the sulfur-oxidation with m-CPBA. The stereochemistry of 5-substituted sulfoxides was determined by means of NMR spectroscopy and DFT theoretical calculations. It was found that the thermodynamically less stable anti-isomer was initially formed in the course of the oxidation, but it underwent epimerization to the mixture enriched in the more stable syn-isomer, during the work-up process. The higher stability of syn-isomers is ascribed to the stronger hyperconjugative sigma(C-H)->sigma*(S-O) interaction versus the weaker sigma(C-C)->sigma*(S-O) delocalization in their anti-counterparts and to the existence of intramolecular 1,5-CH center dot center dot center dot C hydrogen bonds.
New spin probes bearing the 2,2,6,6-tetramethylpiperidine-1-yloxyl covalently bound to the imidazolium ion via a methylene spacer and an amide group are synthesized. If the anion is bis(trifluoromethylsulfonylimide) instead of iodide, the new spin probe has a similar structure as that of an ionic liquid. Nevertheless, the new spin probes are useful tools to investigate ionic liquids.
User-friendly protocols for the protecting group-free synthesis of 2,2'-biphenols via Suzuki-Miyaura coupling of o-halophenols and o-boronophenol are presented. The reactions proceed in water in the presence of simple additives such as K2CO3, KOH, KF, or TBAF and with commercially available Pd/C as precatalyst. Expensive or laboriously synthesized ligands or other additives are not required. In the case of bromophenols, efficient rate acceleration and short reaction times were accomplished by microwave irradiation.
Kammer, Stefan ; Kelling, Alexandra ; Baier, Heiko ; Mickler, Wulfhard ; Dosche, Carsten ; Rurack, Knut ; Kapp, Andreas ; Lisdat, Fred ; Holdt, Hans-Jürgen
2,11-Dialkylated 1,12-diazaperylenes (alkyl = Me, Et, iPr) dmedap, detdap and dipdap have been synthesized by reductive cyclization of 3,3-dialkylated 1,1-biisoquinolines 3a-c, resulting in the first copper(I) complexes of a large- surface ligand. The new copper(I) complexes show low-energy MLCT absorptions unprecedented for bis(-diimin)copper(I) complexes. The solid structures of the complexes[Cu(dipdap)2]BF4·CH2Cl2·1.5H2O, [Cu(dipdap)2]OTf·CH2Cl2, [Cu(dipdap)2]I·C2H4Cl2·THF·2H2O, [Cu(dmedap)2]OTf and [Cu(dipdap)2]AQSO3·H2O (AQSO3 = sodium 9,10-dihydro-9,10-dioxo-2- anthracenesulfonate) are reported. In [Cu(dipdap)2]BF4·CH2Cl2·1.5H2O, each copper(I) complex cation interacts with two others by - stacking interactions forming a novel supramolecular column structural motif running along the crystallographic c axis. In the crystalline compound [Cu(dipdap)2]AQSO3·H2O, aggregation between two complex cations and two additional anions by - stacking interactions is observed, leading to a tetrameric assembly. Furthermore, the three complex compounds [Cu(L)2]BF4 (L = dmedap, detdap, dipdap) were tested for sensory applications in aqueous buffer solutions in electrochemical studies of the complex immobilized on glassy carbon electrodes.
Block copolymers of 1H,1H,2H,2H-perfluorodecyl acrylate (AC8) were obtained from ARGET ATRP. To obtain block copolymers of low dispersity the PAC8 block was synthesized in anisole with a CuBr(2)/PMDETA catalyst in the presence of tin(II) 2-ethylhexanoate as a reducing agent. The PAC8 block was subsequently used as macroinitiator for copolymerization with butyl and tert-butyl acrylate carried out in scCO(2). To achieve catalyst solubility in CO(2) two fluorinated ligands were employed. The formation of block copolymers was confirmed by size exclusion chromatography and DSC.
1H, 13C, and 15N NMR study of the solution structure of metabridged bis(benzo-15-crown-5-ether)s
(1995)
1H NMR Lanthanideinduced Shift (LIS) investigations of highly flexible molecules : a new approach
(1993)
We present an algorithm that performs sequentially one-dimensional inversion of subsurface magnetic permeability and electrical conductivity by using multi-configuration electromagnetic induction sensor data. The presented method is based on the conversion of the in-phase and out-of-phase data into effective magnetic permeability and electrical conductivity of the equivalent homogeneous half-space. In the case of small-offset systems, such as portable electromagnetic induction sensors, for which in-phase and out-of-phase data are moderately coupled, the effective half-space magnetic permeability and electrical conductivity can be inverted sequentially within an iterative scheme. We test and evaluate the proposed inversion strategy using synthetic and field examples. First, we apply it to synthetic data for some highly magnetic environments. Then, the method is tested on real field data acquired in a basaltic environment to image a formation of archaeological interest. These examples demonstrate that a joint interpretation of in-phase and out-of-phase data leads to a better characterisation of the subsurface in magnetic environments such as volcanic areas.
Direct current systems employing a kinematic surveying strategy allow to analyze the electrical resistivity of the subsurface for large areas (i.e., several hectares). Typical applications are found in precision agriculture, archaeological prospecting and soil sciences. With the typical survey setting, the collected data sets are often characterized by a rather high level of noise and a rather coarse lateral sampling compared to data acquired with fixed electrodes. We therefore present an efficient one-dimensional inversion approach in which we put special attention on modeling the effects of noise. We apply this method to data recorded with a five-offset equatorial dipole-dipole system employing rolling electrodes. By performing several synthetic tests with realistic noise levels, we found that the considered five-configuration soundings allow for a reliable imaging of two-layer cases in the uppermost two meters of the subsurface, where the subsurface can be assumed to follow a horizontally layered geometry within 3 m around the system. By analyzing the corresponding sensitivity functions, we also show that the equatorial dipole-dipole array is relatively well suited for a 1D inversion approach compared to standard in-line electrode arrays. To illustrate this aspect, we show that our method can provide results similar to those obtained with a 2D Wenner imaging procedure for data recorded across a well-constrained 2D target. We finally apply our method to a large five-offset data set acquired in an agricultural study. The final pseudo-3D model of electrical resistivity is in accordance with borehole data available for the surveyed area. Our results demonstrate the applicability and the versatility of the presented inversion approach for large-scale data sets as they are typically collected with such rolling electrode systems. (C) 2017 Elsevier B.V. All rights reserved.
Selenides of the type R1Se-EMe3 (E = Si, Ge, Sn, Pb) react with xenon difluoride by cleavage of the Se-E bond to yield the R1Se-F intermediate and the fluorides Me3E-F, whereas the Se-C bond in PhSe-tBu (E = C) is stable against XeF2. The presence of R1Se-F intermediates is confirmed by addition to acetylenes (4-octyne, 3-hexyne). Thus, the fluoroselenenylation of acetylenes gives fluoro(organylseleno)olefins in preparative yields. In the cases of E = Si, Ge, Sn, and Pb, aryl and n-alkyl groups are suitable as the substituent R1. The X-ray crystal structural analysis of (E)-3- (p-carboxyphenylseleno)-4-fluorohex-3-ene - the first example of an uncharged fluoroselenoolefin synthesized from p- EtO2C-C6H4-Se-SnMe3, XeF2, and 3-hexyne followed by an ester hydrolysis - shows that the addition of the selenenylfluoride intermediate to the acetylene proceeds via a trans-addition, as is known for the R2Se2-XeF2 reagents.
13C NMR chemical shifts of unbranched 2-Alkyn-1-ols, w-Alkyn-1-ols and "internal" Alkyn-1-ols
(1995)
13 C NMR Chemical shift calculations for some substituted pyridines - a comparative consideration
(1997)
Calo, Camilla ; Henne, Paul D. ; Eugster, Patricia ; van Leeuwen, Jacqueline ; Gilli, Adrian ; Hamann, Yvonne ; La Mantia, Tommaso ; Pasta, Salvatore ; Vescovi, Elisa ; Tinner, Willy
A new sedimentary sequence from Lago di Venere on Pantelleria Island, located in the Strait of Sicily between Tunisia and Sicily was recovered. The lake is located in the coastal infra-Mediterranean vegetation belt at 2 m a.s.l. Pollen, charcoal and sedimentological analyses are used to explore linkages among vegetation, fire and climate at a decadal scale over the past 1200 years. A dry period from ad 800 to 1000 that corresponds to the Medieval Warm Period' (WMP) is inferred from sedimentological analysis. The high content of carbonate recorded in this period suggests a dry phase, when the ratio of evaporation/precipitation was high. During this period the island was dominated by thermophilous and drought-tolerant taxa, such as Quercus ilex, Olea, Pistacia and Juniperus. A marked shift in the sediment properties is recorded at ad 1000, when carbonate content became very low suggesting wetter conditions until ad 1850-1900. Broadly, this period coincides with the Little Ice Age' (LIA), which was characterized by wetter and colder conditions in Europe. During this time rather mesic conifers (i.e. Pinus pinaster), shrubs and herbs (e.g. Erica arborea and Selaginella denticulata) expanded, whereas more drought-adapted species (e.g. Q. ilex) declined. Charcoal data suggest enhanced fire activity during the LIA probably as a consequence of anthropogenic burning and/or more flammable fuel (e.g. resinous Pinus biomass). The last century was characterized by a shift to high carbonate content, indicating a change towards drier conditions, and re-expansion of Q. ilex and Olea. The post-LIA warming is in agreement with historical documents and meteorological time series. Vegetation dynamics were co-determined by agricultural activities on the island. Anthropogenic indicators (e.g. Cerealia-type, Sporormiella) reveal the importance of crops and grazing on the island. Our pollen data suggest that extensive logging caused the local extinction of deciduous Quercus pubescens around ad1750.
Sammoud, Senda ; Nevill, Alan Michael ; Negra, Yassine ; Bouguezzi, Raja ; Chaabene, Helmi ; Hachana, Younes
This study aimed to estimate the optimal body size, limb segment length, and girth or breadth ratios of 100-m breaststroke performance in youth swimmers. In total, 59 swimmers [male: n= 39, age = 11.5 (1.3) y; female: n= 20, age = 12.0 (1.0) y] participated in this study. To identify size/shape characteristics associated with 100-m breaststroke swimming performance, we computed a multiplicative allometric log-linear regression model, which was refined using backward elimination. Results showed that the 100-m breaststroke performance revealed a significant negative association with fat mass and a significant positive association with the segment length ratio (arm ratio = hand length/forearm length) and limb girth ratio (girth ratio = forearm girth/wrist girth). In addition, leg length, biacromial breadth, and biiliocristal breadth revealed significant positive associations with the 100-m breaststroke performance. However, height and body mass did not contribute to the model, suggesting that the advantage of longer levers was limb-specific rather than a general whole-body advantage. In fact, it is only by adopting multiplicative allometric models that the previously mentioned ratios could have been derived. These results highlighted the importance of considering anthropometric characteristics of youth breaststroke swimmers for talent identification and/or athlete monitoring purposes. In addition, these findings may assist orienting swimmers to the appropriate stroke based on their anthropometric characteristics.
This paper reports on the historical development of the Runge-Kutta methods beginning with the simple Euler method up to an embedded 13-stage method. Moreover, the design and the use of those methods under error order, stability and computation time conditions is edited for students of numerical analysis at undergraduate level. The second part presents applications in natural sciences, compares different methods and illustrates some of the difficulties of numerical solutions.
Tofelde, Stefanie ; Schildgen, Taylor F. ; Savi, Sara ; Pingel, Heiko ; Wickert, Andrew D. ; Bookhagen, Bodo ; Wittmann, Hella ; Alonso, Ricardo N. ; Cottle, John ; Strecker, Manfred
Fluvial fill terraces in intermontane basins are valuable geomorphic archives that can record tectonically and/or climatically driven changes of the Earth-surface process system. However, often the preservation of fill terrace sequences is incomplete and/or they may form far away from their source areas, complicating the identification of causal links between forcing mechanisms and landscape response, especially over multi-millennial timescales. The intermontane Toro Basin in the southern Central Andes exhibits at least five generations of fluvial terraces that have been sculpted into several-hundred-meter-thick Quaternary valley-fill conglomerates. New surface-exposure dating using nine cosmogenic Be-10 depth profiles reveals the successive abandonment of these terraces with a 100 kyr cyclicity between 75 +/- 7 and 487 +/- 34 ka. Depositional ages of the conglomerates, determined by four Al-26/Be-10 burial samples and U-Pb zircon ages of three intercalated volcanic ash beds, range from 18 +/- 141 to 936 +/- 170 ka, indicating that there were multiple cut-and-fill episodes. Although the initial onset of aggradation at similar to 1 Ma and the overall net incision since ca. 500 ka can be linked to tectonic processes at the narrow basin outlet, the superimposed 100 kyr cycles of aggradation and incision are best explained by eccentricity-driven climate change. Within these cycles, the onset of river incision can be correlated with global cold periods and enhanced humid phases recorded in paleoclimate archives on the adjacent Bolivian Altiplano, whereas deposition occurred mainly during more arid phases on the Altiplano and global interglacial periods. We suggest that enhanced runoff during global cold phases - due to increased regional precipitation rates, reduced evapotranspiration, or both - resulted in an increased sediment-transport capacity in the Toro Basin, which outweighed any possible increases in upstream sediment supply and thus triggered incision. Compared with two nearby basins that record precessional (21-kyr) and long-eccentricity (400-kyr) forcing within sedimentary and geomorphic archives, the recorded cyclicity scales with the square of the drainage basin length. (C) 2017 Elsevier B.V. All rights reserved.
1-Oxo-1,3-dithiolane (4) and its cis- andtrans-2-methyl (5,6), -4-methyl (7,8) and -5-methyl (9,10) derivatives were prepared by oxidizing the corresponding 1,3-dithiolanes (1-3) with NaIO4 in water. The oxides were purified and their isomers separated using thin layer chromatography. The structural characterization was carried out with 1H and 13C NMR spectroscopy and molecular modelling. The sulfoxides 4-6 and 8-10 attain two S(1) type envelopes (sometimes slightly distorted) the S=Oax envelope greatly dominating. Cis-4-methyl-1-oxo-1,3-dithiolane is a special case exhibiting both two closely related S=Oax (30 and 27%) as well as S=Oeq (21 and 22%) forms [S(1) and C(4) envelopes, respectively]. The relative energies of these conformations, the values of 1H-1H coupling constants and 1H and 13C chemical shifts were estimated by computational methods and they support well the conclusions based on the experimental data.
1-Oxo-1,3-dithiolane (4) and its cis- and trans-2-methyl (5,6), -4-methyl (7,8) and -5-methyl (9,10) derivatives were prepared by oxidizing the corresponding 1,3-dithiolanes (1-3) with NaIO(4) in water. The oxides were purified and their isomers separated using thin layer chromatography. The structural characterization was carried out with (1)H and (13)C NMR spectroscopy and molecular modelling. The sulfoxides 4-6 and 8-10 attain two S(1) type envelopes (sometimes slightly distorted) the S=O(ax) envelope greatly dominating. Cis-4-methyl-1-oxo-1,3-dithiolane is a special case exhibiting both two closely related S=O(ax) (30 and 27%) as well as S=O(eq) (21 and 22%) forms [S(1) and C(4) envelopes, respectively]. The relative energies of these conformations, the values of (1)H-(1)H coupling constants and (1)H and (13)C chemical shifts were estimated by computational methods and they support well the conclusions based on the experimental data.
Shainyan, Bagrat A. ; Suslova, Elena N. ; Tran Dinh Phien ; Shlykov, Sergey A. ; Heydenreich, Matthias ; Kleinpeter, Erich
1-Methylthio-1-phenyl-1-silacyclohexane 1, the first silacyclohexane with the sulfur atom at silicon, was synthesized and its molecular structure and conformational preferences studied by gas-phase electron diffraction (GED) and low temperature C-13 and Si-29 NMR spectroscopy (LT NMR). Quantum-chemical calculations were carried out both for the isolated species and solvate complexes in gas and in polar medium. The predominance of the 1-MeSaxPheq conformer in gas phase (1-Ph-eq :1-Ph-ax = 55:45, Delta G degrees = 0.13 kcal/mol) determined from GED is consistent with that measured in the freon solution by LT NMR (1-Ph-eq:1-Ph-ax = 65:35, Delta G degrees = 0.12 kcal/mol), the experimentally measured ratios being close to that estimated by quantum chemical calculations at both the DFT and MP2 levels of theory. (C) 2019 Elsevier Ltd. All rights reserved.
Wiesner-Reinhold, Melanie ; Barknowitz, Gitte ; Florian, Simone ; Mewis, Inga ; Schumacher, Fabian ; Schreiner, Monika ; Glatt, Hansruedi
We previously showed that purified 1-methoxy-3-indolylmethyl (1-MIM) glucosinolate, a secondary plant metabolite in Brassica species, is mutagenic in various in vitro systems and forms DNA and protein adducts in mouse models. In the present study, we administered 1-MIM glucosinolate in a natural matrix to mice, by feeding a diet containing pak choi powder and extract. Groups of animals were killed after 1, 2, 4 and 8 days of pak choi diet, directly or, in the case of the 8-day treatment, after 0, 8 and 16 days of recovery with pak choi-free diet. DNA adducts [N-2-(1-MIM)-dG, N-6-(1-MIM)-dA] in six tissues, as well as protein adducts [tau N-(1-MIM)-His] in serum albumin (SA) and hemoglobin (Hb) were determined using UPLC-MS/MS with isotopically labeled internal standards. None of the samples from the 12 control animals under standard diet contained any 1-MIM adducts. All groups receiving pak choi diet showed DNA adducts in all six tissues (exception: lung of mice treated for a single day) as well as SA and Hb adducts. During the feeding period, all adduct levels continuously increased until day 8 (in the jejunum until day 4). During the 14-day recovery period, N-2-(1-MIM)-dG in liver, kidney, lung, jejunum, cecum and colon decreased to 52, 41, 59, 11, 7 and 2%, respectively, of the peak level. The time course of N-6-(1-MIM)-dA was similar. Immunohistochemical analyses indicated that cell turnover is a major mechanism of DNA adduct elimination in the intestine. In the same recovery period, protein adducts decreased more rapidly in SA than in Hb, to 0.7 and 37%, respectively, of the peak level, consistent with the differential turnover of these proteins. In conclusion, the pak choi diet lead to the formation of high levels of adducts in mice. Cell and protein turnover was a major mechanism of adduct elimination, at least in gut and blood.
Shainyan, Bagrat A. ; Kirpichenko, Svetlana V. ; Kleinpeter, Erich ; Shlykov, Sergey A. ; Osadchiy, Dmitriy Yu ; Chipanina, Nina N. ; Oznobikhina, Larisa P.
The first Si-H-containing azasilaheterocycle, 1,3-dimethyl-3-silapiperidine 1, was synthesized, and its molecular structure and conformational properties were studied by gas-phase electron diffraction (GED), low temperature NMR, IR and Raman spectroscopy and quantum chemical calculations. The compound exists as a mixture of two conformers possessing the chair conformation with the equatorial NMe group and differing by axial or equatorial position of the SiMe group. In the gas phase, the SiMeax conformer predominates (GED: ax/eq = 65(7):35(7)%,Delta G = 0.36(18) kcal/mol; IR: ax/eq = 62(5):38(5)%,Delta G = 0.16(7) kcal/mol). In solution, at 143 k the SiMeeq conformer predominates' in the frozen equilibrium (NMR: ax/eq = 31.5(1.5):68.5(1.5)%, Delta G = -0.22(2) kcal/mol). Thermodynamic parameters of the ring inversion are determined (Delta G(double dagger) = 8.9-9.0 kcal/mol, Delta H-double dagger = 9.6 kcal/mol, Delta S-double dagger = 2.1 eu). High-level quantum chemical calculations :(MP2, G2, CCSD(T)) nicely reproduce the experimental geometry and the predominance of the axial conformer in the gas phase.
Mikat, Jürgen E. R. ; Franco, Olga ; Regenstein, Wolfgang ; Reck, Günter ; Knochenhauer, Gerald ; Schulz, Burkhard ; Orgzall, Ingo
Zebger-Gong, Hong ; Mueller, Dominik ; Diercke, Michaela ; Haffner, Dieter ; Hocher, Berthold ; Verberckmoes, Steven ; Schmidt, Sven ; D'Haese, Patrick C. ; Querfeld, Uwe
Background and objective Whether treatment with vitamin D receptor activators contributes to cardiovascular disease in patients with chronic kidney disease is a matter of debate. We studied mechanisms involved in vitamin D-related vascular calcifications in vivo and in vitro.
Methods Aortic calcifications were induced in subtotally nephrectomized (SNX) rats by treatment with a high dose (0.25 mu g/kg per day) of 1,25-dihydroxyvitamin D-3 (calcitriol) given for 6 weeks. Likewise, primary rat vascular smooth muscle cells (VSMCs) were incubated with calcitriol at concentrations ranging from 10(-11) to 10(-7) mol/l. Immunohistochemistry revealed that the aortic expression of osteopontin, osteocalcin and bone sialoprotein was significantly increased in calcitriol-treated SNX rats compared to untreated SNX controls. In addition, aortic expression of the transient receptor potential vanilloid calcium channel 6 (TRPV6) and calbindin D9k was significantly up-regulated by treatment with calcitriol. Furthermore, calcitriol significantly increased expression of the osteogenic transcription factor osterix. In-vitro studies showed similar results, confirming that these effects could be attributed to treatment with calcitriol.
Conclusions High-dose calcitriol treatment induces an osteoblastic phenotype in VSMC both in SNX rats and in vitro, associated with up-regulation of proteins regulating mineralization and calcium transport, and of the osteogenic transcription factor osterix.
Herein, we represent cation-responsive fluorescent probes for the divalent cations Zn2+, Mg2+ and Ca2+, which show cation-induced fluorescence enhancements (FE) in water. The Zn2+-responsive probes Zn1, Zn2, Zn3 and Zn4 are based on o-aminoanisole-N,N-diacetic acid (AADA) derivatives and show in the presence of Zn2+ FE factors of 11.4, 13.9, 6.1 and 8.2, respectively. Most of all, Zn1 and Zn2 show higher Zn2+ induced FE than the regioisomeric triazole linked fluorescent probes Zn3 and Zn4, respectively. In this set, ZN2 is the most suitable probe to detect extracellular Zn2+ levels. For the Mg2+-responsive fluorescent probes Mg1, Mg2 and Mg3 based on o-aminophenol-N,N,O-triacetic acid (APTRA) derivatives, we also found that the regioisomeric linkage influences the fluorescence responds towards Mg2+ (Mg1+100 mM Mg2+ (FEF=13.2) and Mg3+100 mM Mg2+ (FEF=2.1)). Mg2 shows the highest Mg2+-induced FE by a factor of 25.7 and an appropriate K-d value of 3 mM to measure intracellular Mg2+ levels. Further, the Ca2+-responsive fluorescent probes Ca1 and Ca2 equipped with a 1,2-bis(o-aminophenoxy)ethane-N,N,N',N'-tetraacetic acid (BAPTA) derivative show high Ca2+-induced FEs (Ca1 (FEF=22.1) and Ca2 (FEF=23.0)). Herein, only Ca1 (K-d=313 nM) is a suitable Ca2+ fluorescent indicator to determine intracellular Ca2+ levels.
Kammer, Stefan ; Starke, Ines ; Pietrucha, Andreas ; Kelling, Alexandra ; Mickler, Wulfhard ; Schilde, Uwe ; Dosche, Carsten ; Kleinpeter, Erich ; Holdt, Hans-Jürgen
A series of new monocationic iridium(III) complexes [Ir((CN)-N-boolean AND)(2)((NN)-N-boolean AND)]PF6 with "large-surface" alpha,alpha'-diimin ligands (NN)-N-boolean AND (dap = 1,12-diazaperylene, dmedap = 2,11-dimethyl-1,12-diazaperylene, dipdap = 2,11-diisopropyl-1,12-diazaperylene) and different cyclometalating ligands (CN)-N-boolean AND (piq = 1-phenylisoquinoline, bzq = benzo[h]quinoline, ppz = 1-phenylpyrazole, thpy = 2-(2-thienyl)pyridine, ppy = 2-phenylpyridine, meppy = 2-(4-methylphenyl)pyridine, dfppy = 2-(2,4-difluorophenyl)pyridine) were synthesized. The solid structures of the complexes [Ir(piq)(2)(dap)]PF6, [Ir(bzq)(2)(dap)]PF6, [Ir(ppy)(2)(dipdap)]PF6, [Ir(piq)(2)(dmedap)]PF6, [Ir(ppy)(2)(dap)]PF6 and [Ir(ppz)(2)(dap)]PF6 are reported. In [Ir(piq)(2)(dap)]PF6, the dap ligand and one of the piq ligands of each cationic complex are involved in pi-pi stacking interactions forming supramolecular channels running along the crystallographic c axis. In the crystalline [Ir(bzq)(2)(dap)]PF6 pi-pi stacking interactions between the metal complexes lead to the formation of a 2D layer structure. In addition, CH-pi interactions were found in all compounds, which are what stabilizes the solid structure. In particular, a significant number of them were found in [Ir(piq)(2)(dap)]PF6 and [Ir(bzq)(2)(dap)]PF6. The crystal structures of [Ir(ppy)(2)(dipdap)]PF6 and [Ir(ppy)(2)(dmedap)]PF6 are also presented, being the first examples of bis-cyclometalated iridium(III) complexes with phenanthroline-type alpha,alpha'-diimin ligands bearing bulky alkyl groups in the neighbourhood of the N-donor atoms. These ligands implicate a distorted octahedral coordination geometry that in turn destabilized the Ir-N-N boolean AND N bonds. The new iridium (III) complexes are not luminescent. All compounds show an electrochemically irreversible anodic peak between 1.15 and 1.58 V, which is influenced by the different cyclometalated ligands. All of the new complexes show two reversible successive one-electron "large-surface" ligand-centred reductions around -0.70 V and -1.30 V. Electrospray ionisation mass spectrometry (ESI-MS) and collision induced decomposition (CID) measurements were used to investigate the stability of the new complexes. Thereby, the stability agreed well with the order of the Ir-N-N boolean AND N bond lengths.
Awad, Duha Jawad ; Conrad, Franziska ; Koch, Andreas ; Schilde, Uwe ; Poeppl, Andreas ; Strauch, Peter
A series of new N2S2 mixed ligand transition metal complexes, where N-2 is phenanthroline and S-2 is 1,2- dithiooxalate (dto) or 1,2-dithiosquarate (dtsq), has been synthesized and characterized. IR spectra reveal that the 1,2- dithiolate ligands are coordinated via the sulfur atoms forming a N2S2 coordination sphere. The copper(II) complex [Cu(phen)(dto)] was studied by EPR spectroscopy as a diamagnetically diluted powder. The diamagnetic dilution resulted from doping of the copper complex into the isostructural host lattice of the nickel complex [Ni(phen)(dto)]. The electronic situation in the frontier orbitals of the copper complex calculated from the experimental data is compared to the results of EHT and DFT calculations. Furthermore, one side product, chlorobis(1,10-phenanthroline)copper(I) ethanol solvate hydrate [(phen)(2)CuCl]center dot C2H5OH center dot H2O, was formed by a reduction process and characterized by X-ray diffraction. In the crystal packing one-dimensional columns of dimers are formed, stabilized by significant pi-pi interactions.
1 + 2 is more than 2 + 1: Violations of commutativity and identity axioms in mental arithmetic
(2015)
Over the past decade or so, a large number of studies have revealed that conceptual meaning is sensitive to situational context. More recently, similar contextual influences have been documented in the domain of number knowledge. Here we show such context dependency in a length production task. Adult participants saw single digit addition problems of the form n1 + n2 and produced the sum by changing bi-directionally the length of a horizontally extended line, using radially arranged buttons. We found that longer lines were produced when n1 < n2 compared to n1 > n2 and that unit size increased with result size. Thus, the mathematical axioms of commutativity and identity do not seem to hold in mental addition. We discuss implications of these observations for our understanding of cognitive mechanisms involved in mental arithmetic and for situated cognition generally.
We dissect the sources of error leading to inaccuracies in the description of the geometry and optical excitation energies of pi-conjugated polymers. While the ground-state bond length alternation is shown to be badly reproduced by standard functionals, the recently adapted functionals PBEh* and omega PBE* as well as the double hybrid functional XYGJ-OS manage to replicate results obtained at the CCSD(T) level. By analysis of the bond length alternation in the excited state, a sensitive dependence of the exciton localization on the long-range behavior of the functional and the amount of Hartree-Fock exchange present is shown. Introducing thermal disorder through molecular dynamics simulations allows the consideration of a range of thermally accessible configurations of each oligomer, including trans to cis rotations, which break the conjugation of the backbone. Thermal disorder has a considerable effect when combined with functionals that overestimate the delocalization of the excitation, such as B3LYP. For functionals with a larger amount of exact exchange such as our PBEh* and omega PBE*, however, the effect is small, as excitations are often localized enough to fit between twists in the chain.