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Through space NMR shieldings of aromatic (benzene, mono-substituted and annelated benzenes, ferrocene, [14]- and [18]-annulenes, phenylenes and tetra- to heptahelicene) and anti-aromatic molecules (cyclobutadiene and pentalene) were assessed by ab initio molecular-orbital calculations. Employing the nucleus-independent chemical shifts (NICS) concept, these through space NMR shieldings were visualized as iso-chemical-shielding surfaces (ICSSs) and can be applied quantitatively to determine the stereochemistry of proximal nuclei. In addition, the distances in Å at ICSS values of ±0.1 ppm in-plane and perpendicular-to-center of the aromatic ring system were employed as a simple means to compare and estimate qualitatively the aromaticity of the systems at hand.
The trithiocarbonate 2-(benzylsulfanylthiocarbonylsulfanyl) propanoic acid is formed as minor by-product in the synthesis of the dithioester 2-((2-phenylthioacetyl)sulfanyl) propanoic acid via the Grignard route. The mechanism for this side reaction is not clear. The isolated trithiocarbonate may act as unsymmetrical but bifunctional RAFT agent in the aqueous polymerization of N,N-dimethyl acrylamide. Therefore, it is important to separate it completely from the dithioester before engaging the latter in controlled free radical polymerization to guarantee a maximum control.
The title compound, bis(5-methylthio-1,2-dithiole-3-thione)-disulfide, was yielded for the first time as by- product of the reaction of nickel(II) and cobalt(II) ions with 5-methylthio-1,2-dithiole-3-thione-4-thiolate. The compound can be obtained directly by oxidation of the ammonium salt of the ligand. C8H6S10 forms three polymorphs: (I), which crystallizes in the orthorhombic space group P212121, (II) and (III), which crystallize in the monoclinic space groups P21/c and P21/n, respectively. The crystal and molecular structures are presented here. The determination of the absolute configuration of (I) indicated the P-helical enantiomer. In contrast to this, the crystals of (II) und (III) are racemic, containing P- and M-helical enantiomers. The polymorphs differ in the kind of skewing around the disulfide bond and of the positions of the both dithiole rings to the S-S-moiety
Multinuclear dynamic NMR spectroscopy of 3,5-bis(trifluoromethylsulfonyl)-1,3,5-oxadiazinane (3) revealed the existence of two conformers with differently oriented CF3 groups with respect to the ring, and two dynamic processes: ring inversion and restricted rotation about the N-S bond. Two transition states connecting the two conformers and corresponding to clockwise and counterclockwise rotations about the N-S bond were found; the calculated activation barriers of about 12 kcal/mol are in excellent agreement with those measured experimentally for the related molecule 1,3,5-tris(trifluoromethylsulfonyl)-1,3,5-triazinane (1). X-ray analysis proved the existence of the symmetric isomer of 3, which is the minor isomer in solutions but the only one in the crystal due to packing effects. The normal Perlin effect (JCHax < JCHeq)observed for 2(6)-CH2 in 3, whereas the reversed Perlin effect was found for the 4-CH2 group in 3 as well as for all CH2 groups in 1 both experimentally and theoretically. The latter effect in compounds 1, 3, and 1- (methylsulfonyl)-3,5-bis(trifluoromethylsulfonyl)-1,3,5-triazinane (2) can be considered as a genuine reverse Perlin effect since larger values of 1JCH are observed for longer C-H bonds.
We study possible interrelations between the 300-year record of the yearly sunspot numbers and the solar inertial motion (SIM) using the recently developed technique of synchronization analysis. Phase synchronization of the sunspot cycle and the SIM is found and statistically confirmed in three epochs (1734-1790, 1855-1875 and 1907-1960) of the whole period 1700-2000. These results give quantitative support to the hypothesis that there is a weak interaction between the solar activity and the SIM.
The power of business
(2007)
The Pacific Solution meets Fortress Europe : Emerging Parallels in Transnational Refugee Regimes
(2007)
The mode of nutrition of mixotrophic flagellates determines the food quality for their consumers
(2007)
Fixation durations in reading are longer for within-word fixation positions close to word center than for positions near word boundaries. This counterintuitive result was termed the Inverted-Optimal Viewing Position (IOVP) effect. We proposed an explanation of the effect based on error-correction of mislocated fixations [Nuthmann, A., Engbert, R., & Kliegl, R. (2005). Mislocated fixations during reading and the inverted optimal viewing position effect. Vision Research, 45, 2201-2217], that suggests that the IOVP effect is not related to word processing. Here we demonstrate the existence of an IOVP effect in "mindless reading", a G-string scanning task. We compare the results from experimental data with results obtained from computer simulations of a simple model of the IOVP effect and discuss alternative accounts. We conclude that oculornotor errors, which often induce mislocalized fixations, represent the most important source of the IOVP effect. (c) 2006 Elsevier Ltd. All rights reserved.
The Focus Feature Revisited
(2007)
Spring algal development in deep temperate lakes is thought to be strongly influenced by surface irradiance, vertical mixing and temperature, all of which are expected to be altered by climate change. Based on long-term data from Lake Constance, we investigated the individual and combined effects of these variables on algal dynamics using descriptive statistics, multiple regression models and a processoriented dynamic simulation model. The latter considered edible and less-edible algae and was forced by observed or anticipated irradiance, temperature and vertical mixing intensity. Unexpectedly, irradiance often dominated algal net growth rather than vertical mixing for the following reason: algal dynamics depended on algal net losses from the euphotic layer to larger depth due to vertical mixing. These losses strongly depended on the vertical algal gradient which, in turn, was determined by the mixing intensity during the previous days, thereby introducing a memory effect. This observation implied that during intense mixing that had already reduced the vertical algal gradient, net losses due to mixing were small. Consequently, even in deep Lake Constance, the reduction in primary production due to low light was often more influential than the net losses due to mixing. In the regression model, the dynamics of small, fast-growing algae was best explained by vertical mixing intensity and global irradiance, whereas those of larger algae were best explained by their biomass 1 week earlier. The simulation model additionally revealed that even in late winter grazing may represent an important loss factor during calm periods when losses due to mixing are small. The importance of losses by mixing and grazing changed rapidly as it depended on the variable mixing intensity. Higher temperature, lower global irradiance and enhanced mixing generated lower algal biomass and primary production in the dynamic simulation model. This suggests that potential consequences of climate change may partly counteract each other.
Temperature dependent energy-dispersive X-ray diffraction and magnetic study of Fe/Al interface
(2007)
In situ temperature dependent energy-dispersive structural and magnetic study of electron beam evaporated Fe/Al multilayer sample (MLS) has been investigated. The structural studies show the formation of an intermixed FeAl transition layer of a few nanometers thick at the interface during deposition, which on annealing at 300 degrees C transforms to B2FeAl intermetallic phase. Magnetization decreases with increase in temperature and drops to minimum above 300 degrees C due to increase in anti-ferromagnetic interlayer coupling and formation of nonmagnetic FeAl phase at the interface. The Curie temperature (T-c) is found to be 288 degrees C and is much less than that of bulk bcc Fe.
Objective: Despite theoretical discrepancies between different concepts of temperament, some core dimensions are thought to be common to the various models. We compared temperamental traits derived from the New York Longitudinal Study (NYLS) model and the Cloninger dimensions in the developmental course and investigated the associations of temperament with sex as well as with obstetric risks or psychosocial risks present at birth. - Methods: Participants were 151 boys and 157 girls born at differing degrees of obstetric and psychosocial risk from a longitudinal study on a high-risk community sample. In infancy and childhood, NYLS-derived temperamental characteristics were assessed by a highly structured parent interview and standardized behavioral observations. At age 15 years, the Junior Temperament and Character Inventory/1218 was administered. - Results: Moderate correlations were found between Junior Temperament and Character Inventory scales in adolescence and NYLS-derived factors in childhood. The psychosocial risk load seemed to influence the expression of novelty seeking or corresponding NYLS-derived factors, whereas the obstetric risks did not contribute to variation in temperament. Our findings further support highly sex-specific gene x environment interactions on temperament in the developmental course. - Conclusion: The content of our NYLS-derived factors and the specific type of association across different temperament constructs fit into the increasing consensus regarding a small number of higher-order temperamental traits. (c) 2007 Elsevier Inc. All rights reserved.
Mono- and trans-1,4-dialkoxy substituted cyclohexanes (alkyl=Me, Et, i-Pr, t-Bu) were prepared using the solvomercuration-demercuration (SM-DM) procedure. The axialaxial and axial,axialequatorial, equatorial conformational equilibria of the products were studied by low temperature 1H and 13C NMR spectroscopy in CD2Cl2. The structures and relative energies of the participating conformers were calculated at both the B3LYP (6-311G*//6-311+G*) and MP2 (6-311+G*//6-311G*) levels of theory. In the case of DFT, good correlations of ;Gocalcd versus ;Goexptl were obtained. Both the structures and the energy differences of the conformers have been discussed with respect to established models of conformational analysis, viz. steric and hyperconjugative interactions. In addition, 1JH,C coupling constants were considered with respect to the hyperconjugation present.
We examined relations between eye movements (single-fixation durations) and RSVP-based event-related potentials (ERPs; N400s) recorded during reading the same sentences in two independent experiments. Longer fixation durations correlated with larger N400 amplitudes. Word frequency and predictability of the fixated word as well as the predictability of the upcoming word accounted for this covariance in a path-analytic model. Moreover, larger N400 amplitudes entailed longer fixation durations on the next word, a relation accounted for by word frequency. This pattern offers a neurophysiological correlate for the lag-word frequency effect on fixation durations: word processing is reliably expressed not only in fixation durations on currently fixated words, but also in those on subsequently fixated words.
Chlamydomonas acidophila faces high heavy-metal concentrations in acidic mining lakes, where it is a dominant phytoplankton species. To investigate the importance of metals to C. acidophila in these lakes, we examined the response of growth, photosynthesis, cell structure, heat-shock protein (Hsp) accumulation, and metal adsorption after incubation in metal-rich lake water and artificial growth medium enriched with metals (Fe, Zn). Incubation in both metal-rich lake water and medium caused large decreases in photosystem II function (though no differences among lakes), but no decrease in growth rate (except for medium + Fe). Concentrations of small Hsps were higher in algae incubated in metal-rich lake- water than in metal-enriched medium, whereas Hsp60 and Hsp70A were either less or equally expressed. Cellular Zn and Fe contents were lower, and metals adsorbed to the cell surface were higher, in lake-water-incubated algae than in medium- grown cells. The results indicate that high Zn or Fe levels are likely not the main or only contributor to the low primary production in mining lakes, and multiple adaptations of C. acidophila (e.g., high Hsp levels, decreased metal accumulation) increase its tolerance to metals and permit survival under such adverse environmental conditions. Supposedly, the main stress factor present in the lake water is an interaction between low P and high Fe concentrations.
Both the stoichiometry and complex stability constants of crown ether complexes with metal ions have been determined by examining gradual changes in their diffusional behavior in nonaqueous solution. Diffusion coefficients, D, were evaluated by pulsed field gradient (PFG) NMR titration experiments whilst complex stability constants were determined by nonlinear curve-fitting procedures, D versus csol., which also allow the treatment of multiple complexation equilibria (1:1 to 1:2 stoichiometries). Differences in the diffusion coefficients of the various free crown ethers with respect to their metal ion complexes indicate great sensitivity to both conformational changes and changes in molecular size upon complexation.
The paper presents a simulation and parameter-estimation approach for evaluating stochastic patterns of population growth and spread of an annual forest herb, Melampyrum pratense (Orobanchaceae). The survival of a species during large-scale changes in land use and climate will depend, to a considerable extent, on its dispersal and colonisation abilities. Predictions on species migration need a combination of field studies and modelling efforts. Our study on the ability of M. pratense to disperse into so far unoccupied areas is based on experiments in secondary woodland in NE Germany. Experiments started in 1997 at three sites where the species was not yet present, with 300 seeds sown within 1m2. Population development was then recorded until 2001 by mapping of individuals with a resolution of 5 cm. Additional observations considered density dependence of seed production. We designed a spatially explicit individual-based computer simulation model to explain the spatial patterns of population development and to predict future population spread. Besides primary drop of seeds (barochory) it assumed secondary seed transport by ants (myrmecochory) with an exponentially decreasing dispersal tail. An important feature of population-pattern explanation was the simultaneous estimation of both population-growth and dispersal parameters from consistent spatio-temporal data sets. As the simulation model produced stochastic time series and random spatially discrete distributions of individuals we estimated parameters by minimising the expectation of weighted sum of squares. These sums of squares criteria considered population sizes, radial population distributions around the area of origin and distributions of individuals within squares of 25cm×25 cm, the range of density action. Optimal parameter values, together with the precision of the estimates, were obtained from calculating sum of squares in regular grids of parameter values. Our modelling results showed that transport of fractions of seeds by ants over distances of 1-2m was indispensable for explaining the observed population spread that led to distances of at most 8mfrom population origin within 3 years. Projections of population development over four additional years gave a diffusion-like increase of population area without any "outposts". This prediction generated by the simulation model gave a hypothesis which should be revised by additional field observations. Some structural deviations between observations and model output already indicated that for full understanding of population spread the set of dispersal mechanisms assumed in the model may have to be extended by additional features of plant-animal mutualism.
Spectroscopic study of dielectric barrier discharges in cellular polypropylene ferroelectrets
(2007)
The transient light emission from the dielectric barrier discharges (DBDs) in cellular polypropylene ferroelectrets subjected to high electric poling fields was spectroscopically measured. The spectrum shows strong emission from the second positive system of molecular nitrogen, N-2(C (3)Pi(u))-> N-2(B (3)Pi(g)), and the first negative system of N-2(+), N-2(+)(B (2)Sigma(+)(u))-> N-2(+)(X (2)Sigma(+)(g)), consistent with a DBD in air. When a dc voltage is applied stepwise to the ferroelectret film, light emission starts above a threshold, coinciding with the threshold voltage in obtaining piezoelectricity. From selected vibronic band strength ratios, the electric field in the discharge was determined and found to agree with Townsend breakdown.
Investigations of spatial patterns in forest tree species composition are essential in the understanding of landscape dynamics, especially in areas of land-use change. The specific environmental factors controlling the present patterns, however, vary with the scale of observation. In this study we estimated abundance of adult trees and tree regeneration in a Southern Alpine valley in Ticino, Switzerland. We hypothesized that, at the present scale, spatial pattern of post-cultural tree species does not primarily depend on topographic features but responds instead to small- scale variation in historical land use. We used multivariate regression trees to relate species abundances to environmental variables. Species matrices were comprised of single tree species abundance as well as species groups. Groups were formed according to common ecological species requirements with respect to shade tolerance, soil moisture and soil nutrients. Though species variance could only be partially explained, a clear ranking in the relative importance of environmental variables emerged. Tree basal area of formerly cultivated Castanea sativa (Mill.) was the most important factor accounting for up to 50% of species' variation. Influence of topographic attributes was minor, restricted to profile curvature, and partly contradictory in response. Our results suggest the importance of biotic factors and soil properties for small-scale variation in tree species composition and need for further investigations in the study area on the ecological requirements of tree species in the early growing stage.
A novel electrochemical immunoassay based on the multiple affinity labeling of the indicator antibody with an electro-active tag is presented. The concept is illustrated for the determination of the glycated hemoglobin HbA1c in hemoglobin samples. Hemoglobin is adsorbed to the surfactant-modified surface of a piezoelectric quartz crystal. Whereas the quartz crystal nanobalance is used to validate the total Hb binding, the HbA1c on the sensor surface is recognized by an antibody and quantified electrochemically after the sugar moieties of the antibody have been labeled in-situ with ferroceneboronic acid. The sensitivity of this sensor is about threefold higher than the sensitivity of a hemoglobin sensor, where the ferroceneboronic acid is bound directly to HbA1c.
Bacteria play a key role in the world's oceans, supporting nutrient remineralisation and mediating carbon transfer. Little is known about annual changes in bacterial concentration, production and metabolism during the extreme seasonal changes in biological productivity in Antarctic waters. We measured rates of bacterial production, concentrations of viruses and bacteria and environmental parameters between February 2004 and January 2005 at an Antarctic coastal site. Concentrations of total bacteria and viruses were obtained using 4', 6-diamidino-2- phenylindole (DAPI) and SYBR Green I (Molecular Probes), respectively. Populations of bacteria in different metabolic states were estimated using vital stains. Concentrations of bacteria with intact or compromised plasma membranes were estimated using BacLight (Molecular Probes) and active cells estimated using 6-carboxyfluorescein diacetate (6CFDA). Our study showed 6CFDA and BacLight gave rapid and ecologically valuable insights into bacterial physiology, production and growth in natural Antarctic communities that were poorly represented by changes in total cell concentrations. Concentrations of total, active and intact bacteria declined rapidly at the end of summer probably owing to viral infection and microheterotrophic grazing. The decline continued over winter, likely owing to substrate limitation, and concentrations only increased after the phytoplankton bloom in spring and summer. Bacterial abundance was positively correlated with particulate organic carbon (POC) and nitrogen (PON), but not dissolved organic carbon (DOC), reflecting the refractory nature of the DOC pool. Only active and intact bacteria were significantly correlated with concentrations of chl a and rates of bacterial production. Furthermore, the obtained rates of [H-3]thymidine uptake suggest that bacterial growth rates can be sustained by the populations identified as intact or by active cells alone.