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Syntheses and conformational analyses of new naphth[1,2-e][1,3]oxazino[3,2-c]quinazolin-13-ones
(2012)
The syntheses of naphth[1,2-e][1,3]oxazino[3,2-c]quinazolin-13-one derivatives (3a-f) were achieved by the solvent-free heating of benzyloxycarbonyl-protected intermediates (2a-f) with MeONa. For intermediates 2a-f, prepared by the reactions of substituted aminonaphthols with benzyl N-(2-formylphenyl)carbamate, not only the expected trans ring form B and chain form A1, but also the rearranged chain form A2 as a new tautomer were detected in DMSO at room temperature. The quantity of A2 in the tautomeric mixture was changed with time. Conformational analyses of the target heterocycles 3a-f by NMR spectroscopy and accompanying theoretical calculations at the DFT level of theory revealed that the oxazine ring preferred a twisted chair conformation and the quinazolone ring was planar. Besides the conformations, both the configurations at C-7a and C-15 and the preferred rotamers of the 1-naphthyl substituent at C-15 were assigned, which allowed evaluation of the aryl substituent-dependent steric hindrance in this part of the molecules. Configurational assignments were corroborated by quantifying the ring current effect of 15-aryl in terms of spatial NICS.
The esters of 4-hydroxy-cyclohexanone and a series of carboxylic acids R-COOH with R of different electronic and steric influence (R=Me, Et, n-Pr, i-Pr, n-Bu, i-Bu, sec-Bu, t-Bu, CF3, CH2Cl, CHCl2, CCl3, CH2Br, CHBr2, and CBr3) were synthesized and the conformational equilibria studied by 1H and 13C NMR spectroscopy at 103 K and at 295 K, respectively. The geometry of optimized structures of the axial/equatorial chair conformers was computed at the ab initio MO and DFT levels of theory. Only one preferred conformation was obtained for the axial and the equatorial conformer as well. When comparing the conformational equilibria of the cyclohexanone esters with those of the corresponding cyclohexyl esters a certain polarity contribution of the cyclohexanone framework was revealed, which is independent of the substituent effects and increases the stability of the axial conformers by a constant amount.
The conformational equilibria of 1-phenyl-1-silacyclohexane 1, 3-phenyl-1,3-thiasilacyclohexane 2, 1-methyl-1- phenyl-1-silacyclohexane 3, and 3-methyl-3-phenyl-1,3-thiasilacyclohexane 4 have been studied for the first time by low temperature C-13 NMR spectroscopy at 103 K. Predominance of the equatorial conformer of compound 1 (Ph-eq/Ph-ax=78%:22%) is much less than in its carbon analog, phenylcyclohexane (nearly 100% of Ph-eq). And in contrast to 1-methyl-1- phenylcyclohexane, the conformers with the equatorial Ph group are predominant for compounds 3 and 4: at 103 K, Ph-eq/Ph- ax ratios are 63%:37% (3) and 68%:32% (4). As the Si-C bonds are elongated with respect to C-C bonds, the barriers to ring inversion are only between 5.2-6.0 (ax -> eq) and 5.4-6.0 (eq -> ax) kcal mol(-1). Parallel calculations at the DFT and MP2 level of theory (as well as the G2 calculations for compound 1) show qualitative agreement with the experiment. The additivity/nonadditivity of conformational energies of substituents on cyclohexane and silacyclohexane derivatives is analyzed. The geminally disubstituted cyclohexanes containing a phenyl group show large deviations from additivity, whereas in 1-methyl-1-phenyl-1-silacyclohexane and 3-methyl-3-phenyl-1,3-thiasilacyclohexane the effects of the methyl and phenyl groups are almost additive. The reasons for the different conformational preferences in carbocyclic and heterocyclic compounds are analyzed using the homodesmotic reactions approach.
4,4-Dimethyl-1-(trifluoromethylsulfonyl)-1,4-azasilinane 1 and 2,2,6,6-tetramethyl-4-(trifluoromethylsulfonyl)- 1,4,2,6-oxazadisilinane 2 were studied by variable temperature dynamic 1H, 13C, 19F NMR spectroscopy and theoretical calculations at the DFT (density functional theory) and MP2 (Moller-Plesset 2) levels of theory. Both kinetic (barriers to ring inversion) and thermodynamic data (frozen conformational equilibria) could be obtained for the two compounds. The computations revealed two minima on the potential energy surface for molecules 1 and 2 corresponding to the rotamers with the CF3SO2 group directed inward and outward the ring, the latter being 0.20.4 kcal/mol (for 1) and 1.1 kcal/mol (for 2) more stable than the former. The vibrational calculations at the DFT and MP2 levels of theory give the values of the free energy difference Delta G degrees for the 'inward' reversible arrow 'outward' equilibrium consistent with those determined from the experimentally measured ratio of the rotamers. The structure of crystalline compound 2 was ascertained by X-ray diffraction analysis.
The CH2Cl2-MeOH (1:1) extract of the aerial parts of Sphaeranthus bullatus, an annual herb native to tropical East Africa, showed activity against chloroquine sensitive D6 (IC50 9.7 mu g/mL) and chloroquine resistant W2 (IC50 15.0 mu g/mL) strains of Plasmodium falciparum. Seventeen secondary metabolites were isolated from the extract through conventional chromatographic techniques and identified using various spectroscopic methods. The compounds were evaluated for their in vitro antiplasmodial, antileishmanial and anticancer activities revealing activity of four carvotacetone derivatives, namely 3-acetoxy-7-hydroxy-5-tigloyloxycarvotacetone (1) 3,7-dihydroxy-5-tigloyloxycarvotacetone (2), 3-acetoxy-5,7-dihydroxycarvotacetone (3) and 3,5,7-trihydroxycarvotacetone (4); with antiplasmodial IC50 values of 1.40, 0.79, 0.60 and 3.40 mu g/mL, respectively, against chloroquine sensitive D6 strains of P. falciparum; antiplasmodial activity of IC50 2.00, 0.90, 0.68 and 2.80 mu g/mL respectively, against chloroquine resistant W2 strains of P. falciparum, antileishmanial IC50, values of 0.70, 3.00, 0.70 and 17.00 mu g/mL, respectively, against the parasite L. donovanii promastigotes, and anticancer activity against human SK-MEL, KB, BT-549 and SK-OV-3 tumor cells, with IC50 values between <1.1 - 5.3 mu g/mL, for 1-3. In addition, cytotoxic effects of the active compounds were evaluated against monkey kidney fibroblasts (VERO) and pig kidney epithelial cells (LLC-PK11). The structures of carvotacetone derivatives were determined by ID and 2D NMR spectroscopy; the absolute stereochemical configuration of 3-acetoxy-7-hydroxy-5-tigloyloxycarvotacetone (I) was determined as 3R, 4R, 5S by circular dichroism, specific rotation, H-1 NMR and 2D NMR ROESY and NOESY experiments.
The study was conducted to investigate the quantity and the main food sources of carbohydrate (CHO) intake of junior elite triathletes during a short-term moderate (MOD; 12 km swimming, 100 km cycling, 30 km running per wk) and intensive training period (INT; 23 km swimming, 200 km cycling, 45 km running per wk). Self-reported dietary-intake data accompanied by training protocols of 7 male triathletes (18.1 +/- 2.4 yr, 20.9 +/- 1.4 kg/m(2)) were collected on 7 consecutive days during both training periods in the same competitive season. Total energy and CHO intake were calculated based on the German Food Database. A paired t test was applied to test for differences between the training phases (alpha = .05). CHO intake was slightly higher in INT than in MOD (9.0 +/- 1.6 g . kg(-1) . d(-1) vs. 7.8 +/- 1.6 g . kg(-1) . d(-1); p = .041). Additional CHO in INT was mainly ingested during breakfast (115 +/- 37 g in MOD vs. 175 +/- 23 g in INT; p = .002) and provided by beverages (280.5 +/- 97.3 g/d vs. 174.0 +/- 58.3 g/d CHO; p = .112). Altogether, main meals provided approximately two thirds of the total CHO intake. Pre- and postexercise snacks additionally supplied remarkable amounts of CHO (198.3 +/- 84.3 g/d in INT vs. 185.9 +/- 112 g/d CHO in MOD; p = .231). In conclusion, male German junior triathletes consume CHO in amounts currently recommended for endurance athletes during moderate to intensive training periods. Main meals provide the majority of CHO and should therefore not be skipped. CHO-containing beverages, as well as pre- and postexercise snacks, may provide a substantial amount of CHO intake in training periods with high CHO requirements.
Novel piperidine-fused benzoxazino- and
quinazolinonaphthoxazines-synthesis and conformational study
(2012)
The reactions of 1-(amino(2-hydroxyphenyl)methyl)-2-naphthol (3) and 1-(amino(2-aminophenyl) methyl)-2-naphthol (6) with glutardialdehyde resulted in the formation of piperidine-fused benzox-azinonaphthoxazine 4 and quinazolinonaphthoxazine 7, respectively, both in diastereopure form. The full conformational search protocols of 4 and 7 were successfully carried out by NMR spectroscopy and accompanying molecular modelling; the global minimum-energy conformers of all diastereomers were computed, and the assignments of the most stable stereoisomers, G(tct)(1) for 4 and G(tct)(1) for 7, were corroborated by spatial NOE information relating to the H-7a-H-10a-H-15b and H,H coupling patterns of the protons in the flexible part of the piperidine moiety. Additionally, mass spectrometric fragmentation was investigated in collision-induced dissociation experiments. The elemental compositions of the ions were determined by accurate mass measurements. (C) 2012 Elsevier Ltd. All rights reserved.
Dietary records are often biased, especially those of overweight individuals. The purpose of the study was to investigate underreporting among persons of normal weight with a very high energy intake (El).
The total energy expenditure (TEE) of 16 elite athletes (BMI 24 +/- 2 kg/m(2)) and 17 controls (BMI 23 3 kg/m2) was measured using the doubly-labeled water technique (DLW, 14d). El was estimated using 2 x 3-day dietary records. Underreporters were identified by BLACK'S cut-off (El:TEE < 0.76). 44% of athletes (El: 3584 824 kcal/d; TEE: 4621 1460 kcal/d) and 29% of controls (El: 2552 680 kcal/d; TEE: 3151 822 kcal/d) were identified as underreporters. TEE explains 52% of underreporting. In summary, a high energy intake seems to strongly predict underreporting. Prevalence and magnitude of underreporting increase with increasing energy intake.
A simple and efficient method for the conversion of alcohols and phenols to primary O-thiocarbamates and S-thiocarbamates in the absence of solvent (solvent-free condition) using silica sulfuric acid (equivalent to SiO2-OSO3H) as a solid acid is described. The products are easily distinguished by IR, NMR and X-ray data. X-ray data of the compounds reveal a planar trigonal orientation of the NH2 nitrogen atom with the partial C,N double-bond character and the C=S or C=O groups in synperiplanar position with C-aryl-O and C-alkyl-S moieties, respectively. Moreover, the -O-CS-NH2 group which is perpendicular to the plane of the benzene ring in 1c and the central thiocarbamate -S-CO-NH2 group in 2b are essentially planar.
The conformational analysis of the first representative of the Si-alkoxy substituted six-membered Si,N-heterocycles, 1,3-dimethyl-3-isopropoxy-3-silapiperidine, was performed by low-temperature 1H and 13C NMR spectroscopy and DFT theoretical calculations. In contrast to the expectations from the conformational energies of methyl and alkoxy substituents, the Meaxi-PrOeq conformer was found to predominate in the conformational equilibrium in the ratio Meaxi-PrOeq : Meeqi-PrOax of ca. 2 : 1 as from the 1H and 13C NMR study. The thermodynamic parameters obtained by the complete line shape analysis showed that the main contribution to the barrier to ring inversion originates from the entropy term of the free energy of activation.
Density Functional Calculations of the Anisotropic Effects of Borazine and 1,3,2,4-Diazadiboretidine
(2012)
On the basis of the nucleus-independent chemical shift (NICS) concept, the anisotropic effects of two inorganic rings, namely, borazine and planar 1,3,2,4-diazadiboretidine, are quantitatively calculated and visualized as isochemical shielding surfaces (ICSSs). Dissection of magnetic shielding values along the three Cartesian axes into contributions from s and p bonds by the natural chemical shieldingnatural bond orbital (NCSNBO) method revealed that their appearance is not a simple reflection of the extent of (anti)aromaticity.
1-Isopropyl-3-methyl-3-phenyl-1,3-azasilinane 1 and 1-isopropyl-3,3-dimethyl-1,3-azasilinane 2 were synthesized and a detailed analysis of their NMR spectra, conformational equilibria and ring inversion processes is presented. Low temperature H-1/C-13 NMR spectroscopy, iteration of the H-1 NMR spectra and quantum chemical calculations showed slight predominance of the PheqMeax over the PhaxMeeq conformer of 1 at low temperature. The barrier for the chair to chair interconversion of both compounds was measured to be 8.25 kcal/mol.
1. The complex, nonlinear response of dryland systems to grazing and climatic variations is a challenge to management of these lands. Predicted climatic changes will impact the desertification of drylands under domestic livestock production. Consequently, there is an urgent need to understand the response of drylands to grazing under climate change. 2. We enhanced and parameterized an ecohydrological savanna model to assess the impacts of a range of climate change scenarios on the response of a semi-arid African savanna to grazing. We focused on the effects of temperature and CO2 level increase in combination with changes in inter- and intra-annual precipitation patterns on the long-term dynamics of three major plant functional types. 3. We found that the capacity of the savanna to sustain livestock grazing was strongly influenced by climate change. Increased mean annual precipitation and changes in intra-annual precipitation pattern have the potential to slightly increase carrying capacities of the system. In contrast, decreased precipitation, higher interannual variation and temperature increase are leading to a severe decline of carrying capacities owing to losses of the perennial grass biomass. 4. Semi-arid rangelands will be at lower risk of shrub encroachment and encroachment will be less intense under future climatic conditions. This finding holds in spite of elevated levels of atmospheric CO2 and irrespective of changes in precipitation pattern, because of the drought sensitivity of germination and establishment of encroaching species. 5. Synthesis and applications. Changes in livestock carrying capacities, both positive and negative, mainly depend on the highly uncertain future rainfall conditions. However, independent of the specific changes, shrub encroachment becomes less likely and in many cases less severe. Thus, managers of semi-arid rangelands should shift their focus from woody vegetation towards perennial grass species as indicators for rangeland degradation. Furthermore, the resulting reduced competition from woody vegetation has the potential to facilitate ecosystem restoration measures such as re-introduction of desirable plant species that are only little promising or infeasible under current climatic conditions. On a global scale, the reductions in standing biomass resulting from altered degradation dynamics of semi-arid rangelands can have negative impacts on carbon sequestration.
In fragmented landscapes, the survival of species and the maintenance of populations with healthy genetic structures will largely depend on movement/dispersal of organisms across matrix areas. In this article, we highlight that effects of fragmentation and climate change occur simultaneously and may enhance or mitigate each other. We systematically analyzed the effect of increasing interannual variation in rainfall on the genetic structure of two neighbouring small mammal subpopulations in a fragmented savanna landscape. The effect of interannual rainfall variation is analyzed for two contrasting scenarios that differ in mean annual rainfall and are both close to a dispersal threshold. Scenario 1 (low mean annual rainfall) lies slightly below this threshold and scenario 2 (high mean annual rainfall) slightly above, i.e. the amount of rainfall in an average rainfall year prevents dispersal in scenario 1, but promotes gene flow in scenario 2. We show that the temporal dynamics of the matrix was crucial for gene flow and the genetic structure of the neighbouring small mammal subpopulations. The most important result is that the increase in rainfall variability could both increase and decrease the genetic difference between the subpopulations in a complex pattern, depending on the scenario and on the amount of variation in rainfall. Finally, we discuss that the relevance of the matrix as temporarily suitable habitat may become a key aspect for biodiversity conservation. We conclude to incorporate temporal changes in matrix suitability in metapopulation theory since local extinctions, gene flow and re-colonization are likely to be affected in fragmented landscapes with such dynamic matrix areas.
The spatial magnetic properties (through-space NMR shieldings, or TSNMRSs) of the antiaromatic 9-oxaanthracene anion 12(-) and of the corresponding 9-dimeric dianion 11(2-) have been calculated by the gauge-invariant atomic orbitals (GIAO) perturbation method employing the nucleus independent chemical shift (NICS) concept and visualized as iso-chemical-shielding surfaces (ICSSs) of various size and direction. The TSNMRS values, thus obtained, can be employed to indicate antiaromaticity by paratropic ring currents of the anionic compounds of 11(2-) and 12(-) studied and other neutral and ionic antiaromatic molecules from previous studies because anisotropic effects of functional groups in H-1 NMR spectra have quantitatively proven to be the molecular response property of theoretical spatial nucleus independent chemical shieldings (NICS).
A comprehensive numerical device simulation of the electrical and optical characteristics accompanied with experimental measurements of a new highly efficient system for polymer-based light-emitting diodes doped with phosphorescent dyes is presented. The system under investigation comprises an electron transporter attached to a polymer backbone blended with an electronically inert small molecule and an iridium-based green phosphorescent dye which serves as both emitter and hole transporter. The device simulation combines an electrical and an optical model. Based on the known highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) levels of all components as well as the measured electrical and optical characteristics of the devices, we model the emissive layer as an effective medium using the dye's HOMO as hole transport level and the polymer LUMO as electron transport level. By fine-tuning the injection barriers at the electron and hole-injecting contact, respectively, in simulated devices, unipolar device characteristics were fitted to the experimental data. Simulations using the so-obtained set of parameters yielded very good agreement to the measured currentvoltage, luminancevoltage characteristics, and the emission profile of entire bipolar light-emitting diodes, without additional fitting parameters. The simulation was used to gain insight into the physical processes and the mechanisms governing the efficiency of the organic light-emitting diode, including the position and extent of the recombination zone, carrier concentration profiles, and field distribution inside the device. The simulations show that the device is severely limited by hole injection, and that a reduction of the hole-injection barrier would improve the device efficiency by almost 50%.
We measured the ultrafast optical response of metal-dielectric superlattices by broadband all-optical pump-probe spectroscopy. The observed phase of the superlattice mode depends on the probe wavelength, making assignments of the excitation mechanism difficult. Ultrafast x-ray diffraction data reveal the true oscillation phase of the lattice which changes as a function of the excitation fluence. This result is confirmed by the fluence dependence of optical transients. We set up a linear chain model of the lattice dynamics and successfully simulated the broadband optical reflection by unit-cell resolved calculation of the strain-dependent dielectric functions of the constituting materials.
Inhalt: Historische Stationen: Ruediger Liwak -- "In Gottes Namen fahren wir.". Zur Bedeutung von Wallfahrtstraditionen im Alten Israel -- Dalia Marx, Der fehlende Tempel - Der Stellenwert des zerstoerten Tempels in der Kultur des Volkes Israels -- Johann Ev. Hafner, Pilgern in der Spaetantike. Motive und Strukturen in Egerias "Itinerarium" -- Marie-Luise Heckmann, Ein Heiliger mit vielen Gesichtern. Jakobus von Compostela im 12. Jahrhundert -- Heinz-Dieter Heimann, ". in grosser eil gen der Wilssnagk gelaufen". Gezaehlte Froemmigkeit, Kultwerbung und kulturelle Polarisation ueber die Wilsnacker Wallfahrten -- Daniel Vorpahl, "Wozu in die Ferne schweifen ?". Zur Geschichte der Pilgerkritik, ihrer Argumentation und Wirkung -- Aktuelle Formen: Susanne Talabardon, Ans Ende der Welt - zu den eigenen Wurzeln. Geschichte(n) chassidischen Pilgerns -- Hans-Michael Haussig, hagg, 'umra und ziyara. Formen des freiwilligen und verpflichtenden Pilgerns im Islam -- Jenny Vorpahl, Pilgerberichte im Wandel der Zeit. Jakobspilger zwischen Neuzeit und Moderne -- Christina Toelkes, Moderner Pilgertourismus in Rom. Eine empirische, motivorientierte Studie -- Stefan Gatzhammer, Aspekte des religioes motivierten Tourismus in Europa heute. Motivation, Ziele, Trends -- Ulrich Knefelkamp, Wege der Jakobspilger in Brandenburg. Ein Projektbericht.
A number of N-substituted 2,2-dimethyl-1,4,2-oxazasilinanes 1 were synthesized and studied by variable temperature dynamic H-1 and C-13 NMR spectroscopy, room temperature N-15 NMR spectroscopy and theoretical calculations at the DFT and MP2 levels of theory. Both the preferred conformers were assigned and the barrier to the ring inversion of the saturated six-membered ring determined. From 1 the corresponding methyl iodide salts were produced, their structure studied by X-ray analysis and found to be in excellent agreement with the results of the theoretical calculations.
A silicon analog of quinolizidine 3,3,7,7-tetramethylhexahydro-1H-[1,4,2]oxazasilino[4,5-d][1,4,2]oxazasilin-9a-yl)methanol 3 was synthesized. X-ray diffraction analysis confirmed the trans configuration and low temperature NMR spectroscopy both the flexibility (barrier of interconversion 5.8 kcal mol(-1)) and the conformational equilibrium (chair-chair and chair-twist conformers) of the compound. The relative stability of the different isomers/conformers of 3 was calculated also at the MP2/6-311G(d,p) level of theory. Intra- and intermolecular hydrogen bonding in 3 and the appropriate equilibrium between free and self-associated molecules was studied in solvents of different polarity. Both the N-methyl quaternary ammonium salt and the O-trimethylsilyl derivative of 3 could be obtained and their structure determined.
The esters of 4-hydroxy-cyclohexanone and a series of carboxylic acids R-COOH with R of different electronic and steric influence (R=Me, Et, n-Pr, i-Pr, n-Bu, i-Bu, sec-Bu, t-Bu, CF3, CH2Cl, CHCl2, CCl3, CH2Br, CHBr2, and CBr3) were synthesized and the conformational equilibria studied by H-1 and C-13 NMR spectroscopy at 103 K and at 295 K, respectively. The geometry of optimized structures of the axial 'equatorial chair conformers was computed at the ab initio MO and DFT levels of theory. Only one preferred conformation was obtained for the axial and the equatorial conformer as well. When comparing the conformational equilibria of the cyclohexanone esters with those of the corresponding cyclohexyl esters a certain polarity contribution of the cyclohexanone framework was revealed, which is independent of the substituent effects and increases the stability of the axial conformers by a constant amount.
The validity of the Taft equation: log(k(R)/k(CH3)) = rho*sigma* + delta E-S was studied with the aid of NBO computational results concerning cyclohexyl esters RCOOC6H11 [R = Methyl, Ethyl, n-Propyl, Isopropyl, n-Butyl, Isobutyl, sec-Butyl, tert-Butyl, Neopentyl, CH(CH2CH3)(2), CH(CH3)C(CH3)(3), C(CH3)(2)CH2CH3, C(CH3)(2)C(CH3)(3), CH(CH3)(Np), CH(iPr)(tBu), C(Me)(Et)(iPr), C(Et)(2)(tBu) or C(Et)(iPr)(tBu)]. It was proved that the sigma*(alkyl) value is a composite substitutent constant including the polar and steric contributions. A novel computational sigma(q)* substituent constant scale is presented based on the NBO atomic charges of the alpha-carbon and the computational total steric exchange energies E(ster) of the cyclohexyl esters specified above. The method used offers a useful way to calculate sigma*(alkyl) values for alkyl groups for which experimental Taft's polar sigma* parameters are not available.
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.
The conformational equilibria of 1-phenyl-1-silacyclohexane 1, 3-phenyl-1,3-thiasilacyclohexane 2, 1-methyl-1-phenyl-1-silacyclohexane 3, and 3-methyl-3-phenyl-1,3-thiasilacyclohexane 4 have been studied for the first time by low temperature C-13 NMR spectroscopy at 103 K. Predominance of the equatorial conformer of compound 1 (Ph-eq/Ph-ax=78%:22%) is much less than in its carbon analog, phenylcyclohexane (nearly 100% of Ph-eq). And in contrast to 1-methyl-1-phenylcyclohexane, the conformers with the equatorial Ph group are predominant for compounds 3 and 4: at 103 K, Ph-eq/Ph-ax ratios are 63%:37% (3) and 68%:32% (4). As the Si-C bonds are elongated with respect to C-C bonds, the barriers to ring inversion are only between 5.2-6.0 (ax -> eq) and 5.4-6.0 (eq -> ax) kcal mol(-1). Parallel calculations at the DFT and MP2 level of theory (as well as the G2 calculations for compound 1) show qualitative agreement with the experiment. The additivity/nonadditivity of conformational energies of substituents on cyclohexane and silacyclohexane derivatives is analyzed. The geminally disubstituted cyclohexanes containing a phenyl group show large deviations from additivity, whereas in 1-methyl-1-phenyl-1-silacyclohexane and 3-methyl-3-phenyl-1,3-thiasilacyclohexane the effects of the methyl and phenyl groups are almost additive. The reasons for the different conformational preferences in carbocyclic and heterocyclic compounds are analyzed using the homodesmotic reactions approach.
The minima on the potential energy surface of 1,2-bis(o-carboxyphenoxy)ethane (CPE) molecule in its electronic ground state were searched by a molecular dynamics simulation performed with MM2 force field. For each of the found minimum-energy conformers, the corresponding equilibrium geometry, charge distribution, HOMO-LUMO energy gap, force field, vibrational normal modes and associated IR and Raman spectral data were determined by means of the density functional theory (DFT) based electronic structure calculations carried out by using B3LYP method and various Pople-style basis sets. The obtained theoretical data confirmed the significant effects of the intra- and inter-molecular hydrogen bonding interactions on the conformational structure, force field, and group vibrations of the molecule. The same data have also revealed that two of the determined stable conformers, both of which exhibit pseudo-crown structure, are considerably more favorable in energy to the others and accordingly provide the major contribution to the experimental spectra of CPE. In the light of the improved vibrational spectral data obtained within the "SQM FF" methodology and "Dual Scale Factors" approach for the monomer and dimer forms of these two conformers, a reliable assignment of the fundamental bands observed in the experimental room-temperature IR and Raman spectra of the molecule was given, and the sensitivities of its group vibrations to conformation, substitution and dimerization were discussed.
4,4-Dimethyl-1-(trifluoromethylsulfonyl)-1,4-azasilinane 1 and 2,2,6,6-tetramethyl-4-(trifluoromethylsulfonyl)-1,4,2,6-oxazadisilinane 2 were studied by variable temperature dynamic 1H, 13C, 19F NMR spectroscopy and theoretical calculations at the DFT (density functional theory) and MP2 (Moller-Plesset 2) levels of theory. Both kinetic (barriers to ring inversion) and thermodynamic data (frozen conformational equilibria) could be obtained for the two compounds. The computations revealed two minima on the potential energy surface for molecules 1 and 2 corresponding to the rotamers with the CF3SO2 group directed inward and outward the ring, the latter being 0.20.4 kcal/mol (for 1) and 1.1 kcal/mol (for 2) more stable than the former. The vibrational calculations at the DFT and MP2 levels of theory give the values of the free energy difference Delta G degrees for the 'inward' reversible arrow 'outward' equilibrium consistent with those determined from the experimentally measured ratio of the rotamers. The structure of crystalline compound 2 was ascertained by X-ray diffraction analysis.
Based on the nucleus-independent chemical shift (NICS) concept, isotropic magnetic shielding values have been computed along the three Cartesian axes for ethene, cyclobutadiene, benzene, naphthalene, and benzocyclobutadiene, starting from the molecular/ring center up to 10 angstrom away. These through-space NMR spectroscopic shielding (TSNMRS) values, which reflect the anisotropic effects, have been broken down into contributions from localized- and canonical molecular orbitals (LMOs and CMOs); these contributions revealed that the proton NMR spectroscopic chemical shifts of nuclei that are spatially close to the C?C double bond or the aromatic ring should not be explained in terms of the conventionally accepted p-electron shielding/deshielding effects. In fact, these effects followed the predictions only for the antiaromatic cyclobutadiene ring.
In this field experiment we investigate the impact of land use induced savanna degradation on movement behaviour of the spotted sand lizard (Pedioplanis l. lineoocellata) in the southern Kalahari. Foraging behaviour of lizards was tested in a factorial design (low vs. high prey availability) in degraded and non-degraded habitats.
An interaction between habitat structure and prey availability affected movement behaviour. In degraded habitats with low prey availability and in non-degraded habitats with high prey availability the spotted sand lizard moved more like an active forager. In contrast, in degraded habitats with high prey availability and in non-degraded habitats with low prey availability lizards moved like sit-and-wait foragers. Interestingly, the behavioural flexibility of the spotted sand lizard seems to buffer extreme conditions and negative effects of land use impacts.
1,3-Dimethyl-3-phenyl-1,3-azasilinane was synthesized and its conformational behavior was studied by the low temperature NMR spectroscopy and quantum chemical calculations. The compound was shown to exist as an equilibrium mixture of the PhaxMeeq and PheqMeax chair conformers with the N-methyl substituent in equatorial position. The barrier to ring inversion was also determined.
Syntheses of thiazolidine-fused heterocycles via exo-mode cyclizations of vinylogous N-acyliminium ions incorporating heteroatom-based nucleophiles have been examined and discussed. The formation of (5,6)-membered systems was feasible with all nucleophiles tried (O, S and N), while the closing of the five-membered ring was restricted to O- and S-nucleophiles. The closure of a four-membered ring failed. Instead, the bicyclic (5,6)-membered acetal derivative and the tricyclic system with an eight-membered central ring were obtained from the substrates containing O and S nucleophilic moieties, respectively. The reaction outcome and stereochemistry are rationalized using quantum chemical calculations at B3LYP/6-31G(d) level. The exclusive cis-stereoselectivity in the formation of (5,6)- and (5,5)-membered systems results from thermodynamic control, whereas the formation of the eight-membered ring was kinetically controlled.
HIRSCHMULLER, A., V. FREY, L. KONSTANTINIDIS, H. BAUR, H-H. DICKHUTH, N. P. SUDKAMP, and P. HELWIG. Prognostic Value of Achilles Tendon Doppler Sonography in Asymptomatic Runners. Med. Sci. Sports Exerc., Vol. 44, No. 2, pp. 199-205, 2012. Introduction: Midportion Achilles tendinopathy (MPT) is a common problem in running athletes. Nevertheless, its etiology is not fully understood, and no valid prognostic criterion to predict the development of MPT could be identified to date. The purpose of the present study, therefore, was to evaluate whether power Doppler ultrasonography (PDU) is a suitable method to identify a predisposition to MPT in yet asymptomatic runners. Methods: At 23 major running events, 634 asymptomatic long-distance runners were tested for Achilles tendon thickness, vascularization, and structural abnormalities using a high-resolution PDU device (Toshiba Aplio SSA-770A/80, 12 MHz). In addition, their medical history and anthropometric data were documented. All subjects were contacted 6 and 12 months later and asked about any new symptoms. The collected anamnestic, anthropometric, and ultrasonographic data were subjected to regression analysis to determine their predictive value concerning the manifestation of midportion Achilles tendon complaints (P < 0.05). Results: The highest odds ratio (OR) for manifestation of MPT within 1 yr was found for intratendinous blood flow ("neovascularization,'' OR = 6.9, P < 0.001). An increased risk was also identified for subjects with a positive history of Achilles tendon complaints (OR = 3.8, P < 0.001). A third relevant parameter, just above the level of significance, was a spindle-shaped thickening of the tendon on PDU (Wald chi(2) = 3.42). Conclusions: PDU detection of intratendinous microvessels in the Achilles tendons of healthy runners seems to be a prognostically relevant factor concerning the manifestation of symptomatic MPT. This finding lays the foundation for an early identification of a predisposition to MPT as well as prophylactic intervention in as yet asymptomatic runners.
Cell-level kinetic models for therapeutically relevant processes increasingly benefit the early stages of drug development. Later stages of the drug development processes, however, rely on pharmacokinetic compartment models while cell-level dynamics are typically neglected. We here present a systematic approach to integrate cell-level kinetic models and pharmacokinetic compartment models. Incorporating target dynamics into pharmacokinetic models is especially useful for the development of therapeutic antibodies because their effect and pharmacokinetics are inherently interdependent. The approach is illustrated by analysing the F(ab)-mediated inhibitory effect of therapeutic antibodies targeting the epidermal growth factor receptor. We build a multi-level model for anti-EGFR antibodies by combining a systems biology model with in vitro determined parameters and a pharmacokinetic model based on in vivo pharmacokinetic data. Using this model, we investigated in silico the impact of biochemical properties of anti-EGFR antibodies on their F(ab)-mediated inhibitory effect. The multi-level model suggests that the F(ab)-mediated inhibitory effect saturates with increasing drug-receptor affinity, thereby limiting the impact of increasing antibody affinity on improving the effect. This indicates that observed differences in the therapeutic effects of high affinity antibodies in the market and in clinical development may result mainly from Fc-mediated indirect mechanisms such as antibody-dependent cell cytotoxicity.
The chemical master equation (CME) is the fundamental evolution equation of the stochastic description of biochemical reaction kinetics. In most applications it is impossible to solve the CME directly due to its high dimensionality. Instead, indirect approaches based on realizations of the underlying Markov jump process are used, such as the stochastic simulation algorithm (SSA). In the SSA, however, every reaction event has to be resolved explicitly such that it becomes numerically inefficient when the system's dynamics include fast reaction processes or species with high population levels. In many hybrid approaches, such fast reactions are approximated as continuous processes or replaced by quasi-stationary distributions in either a stochastic or a deterministic context. Current hybrid approaches, however, almost exclusively rely on the computation of ensembles of stochastic realizations. We present a novel hybrid stochastic-deterministic approach to solve the CME directly. Our starting point is a partitioning of the molecular species into discrete and continuous species that induces a partitioning of the reactions into discrete-stochastic and continuous-deterministic processes. The approach is based on a WKB (Wentzel-Kramers-Brillouin) ansatz for the conditional probability distribution function (PDF) of the continuous species (given a discrete state) in combination with Laplace's method of integral approximation. The resulting hybrid stochastic-deterministic evolution equations comprise a CME with averaged propensities for the PDF of the discrete species that is coupled to an evolution equation of the related expected levels of the continuous species for each discrete state. In contrast to indirect hybrid methods, the impact of the evolution of discrete species on the dynamics of the continuous species has to be taken into account explicitly. The proposed approach is efficient whenever the number of discrete molecular species is small. We illustrate the performance of the new hybrid stochastic-deterministic approach in an application to model systems of biological interest.
Beringian climate and environmental history are poorly characterized at its easternmost edge. Lake sediments from the northern Yukon Territory have recorded sedimentation, vegetation, summer temperature and precipitation changes since similar to 16 cal ka BP. Herb-dominated tundra persisted until similar to 14.7 cal ka BP with mean July air temperatures <= 5 degrees C colder and annual precipitation 50 to 120 mm lower than today. Temperatures rapidly increased during the Bolling/Allerod interstadial towards modern conditions, favoring establishment of Betula-Salix shrub tundra. Pollen-inferred temperature reconstructions recorded a pronounced Younger Dryas stadial in east Beringia with a temperature drop of similar to 1.5 degrees C (similar to 2.5 to 3.0 degrees C below modern conditions) and low net precipitation (90 to 170 mm) but show little evidence of an early Holocene thermal maximum in the pollen record. Sustained low net precipitation and increased evaporation during early Holocene warming suggest a moisture-limited spread of vegetation and an obscured summer temperature maximum. Northern Yukon Holocene moisture availability increased in response to a retreating Laurentide Ice Sheet, postglacial sea level rise, and decreasing summer insolation that in turn led to establishment of Alnus-Berula shrub tundra from similar to 5 cal ka BP until present, and conversion of a continental climate into a coastal-maritime climate near the Beaufort Sea.
Sediments of Lake Donggi Cona on the northeastern Tibetan Plateau were studied to infer changes in the lacustrine depositional environment, related to climatic and non-climatic changes during the last 19 kyr. The lake today fills a 30x8 km big and 95 m deep tectonic basin, associated with the Kunlun Fault. The study was conducted on a sediment-core transect through the lake basin, in order to gain a complete picture of spatio-temporal environmental change. The recovered sediments are partly finely laminated and are composed of calcareous muds with variable amounts of carbonate micrite, organic matter, detrital silt and clay. On the basis of sedimentological, geochemical, and mineralogical data up to five lithological units (LU) can be distinguished that document distinct stages in the development of the lake system.
The onset of the lowermost LU with lacustrine muds above basal sands indicates that lake level was at least 39 m below the present level and started to rise after 19 ka, possibly in response to regional deglaciation. At this time, the lacustrine environment was characterized by detrital sediment influx and the deposition of siliciclastic sediment. In two sediment cores, upward grain-size coarsening documents a lake-level fall after 13 cal ka BP, possibly associated with the late-glacial Younger Dryas stadial. From 11.5 to 4.3 cal ka BP, grain-size fining in sediment cores from the profundal coring sites and the onset of lacustrine deposition at a litoral core site (2 m water depth) in a recent marginal bay of Donggi Cona document lake-level rise during the early to mid-Holocene to at least modern level. In addition, high biological productivity and pronounced precipitation of carbonate micrites are consistent with warm and moist climate conditions related to an enhanced influence of summer monsoon. At 4.3 cal ka BP the lake system shifted from an aragonite- to a calcite-dominated system, indicating a change towards a fully open hydrological lake system. The younger clay-rich sediments are moreover non-laminated and lack any diagenetic sulphides, pointing to fully ventilated conditions, and the prevailing absence of lake stratification. This turning point in lake history could imply either a threshold response to insolation-forced climate cooling or a response to a non-climatic trigger, such as an erosional event or a tectonic pulse that induced a strong earthquake, which is difficult to decide from our data base.
Ostracodes (Ostracoda, Crustacea) are aquatic micro-crustaceans with a significant representation in the fossil record. If the environmental influence on the species composition of their communities is robustly quantified, past changes in ostracode communities reflected in fossil assemblages can be used for paleo-environmental reconstruction. We analyzed ostracode assemblages in recently deposited surface sediments from 56 lakes in western and central Mongolia, and simultaneously recorded local water chemistry and solute concentration in order to elucidate the distribution of individual ostracode species in relation to these broad environmental gradients. Multivariate analysis indicated that the species variation in ostracode assemblages could be mainly attributed to variations in percent calcium (%Ca) relative to total cation content, mean annual precipitation, calcium concentration, alkalinity, percent bicarbonate relative to total anion content, and mean July temperature. This matches well with the results of a similar analysis on presence/absence data of living ostracodes in nearshore samples, even though some differences exist between the faunal composition of both datasets. The documented response of ostracode species to environmental variation tracks the typical solute evolutionary pathway for surface waters in this region, characterized by calcite precipitation and consequent depletion in dissolved calcium. Hence, the best quantitative inference model (WA-PLS model with R-jack(2) = 0.70, RMSEP = 0.40) for paleolimnological application was obtained for %Ca. Comparison between this model and a specific conductance (SC) inference model based on the same dataset, and based on ostracode datasets from different regions, indicated that the %Ca inference model suffers less than the SC inference model from a step-change in reconstructed values. The statistical power of different inference models based on Mongolian ostracodes are variously affected by the common dominance of a single euryhaline species (Limnocythere inopinata), limited faunal turnover in the freshwater portion of the salinity gradient, and the bimodal frequency distribution of SC among regional lakes. The latter probably represents true scarcity of lakes with intermediate salinity rather than a biased representation in our dataset. In a broader context of ostracode ecology, and with respect to regional paleolimnological applications, we highlight the potential of fossil Mongolian ostracode assemblages to trace past hydrological shifts associated with changes in groundwater inflow.
Thermokarst lakes are assumed to develop cyclically, driven by processes that are triggered by climate and maintained by internal feedbacks that may trigger lake drainage. However, the duration of these cycles remains uncertain, as well as whether or not they affect the stabilization of lake ecosystems in permafrost regions over millennial time scales. Our research has combined investigations into modern lake-to-lake variability with a study of the long-term development of individual lakes. We have investigated the physico-chemical and diatom compositions of a set of 101 lakes with a variety of different origins in central Yakutia (Eastern Siberia), including thermokarst lakes, fluvial-erosion thermokarst lakes, fluvial-erosion lakes, and dune lakes. We found a significant relationship between lake genesis and the present-day variability in environmental and diatom characteristics, as revealed by multi-response permutation procedures, indicator species analyses, and redundancy analyses. Environmental parameters also exhibit a significant correlation with variations in the diatom data, for which they may have been to a substantial extent responsible. Mg and SO4 concentrations, together with pH and water depth, were identified as the most important parameters, influencing the variations in the diatom data almost as much as the entire environmental parameter set. We were therefore able to establish a robust Mg-diatom transfer function, which was then applied to three Holocene lake records. From these reconstructions, together with a general interpretation of the diatom record (including, e.g., the ratio between benthic/epiphytic and planktonic taxa), we have been able to infer that all three of these lakes show (1) a continuous record with no desiccation events, (2) high lake water-levels during the early Holocene, (3) centennial to millennial scale variability, and (4) high levels of variability during the early Holocene but rather stable conditions during the late Holocene (a feature that is also known from other sites around the world). We therefore concluded that the development of these three lakes was mainly driven directly by the climate, rather than by thaw lake cycling.
The first 1400-year floating varve chronology for north-eastern Germany covering the late Allered to the early Holocene has been established by microscopic varve counts from the Rehwiese palaeolake sediment record. The Laacher See Tephra (LST), at the base of the studied interval, forms the tephrochronological anchor point. The fine laminations were examined using a combination of micro-facies and mu XRF analyses and are typical of calcite varves, which in this case provide mainly a warm season signal. Two varve types with different sub-layer structures have been distinguished: (I) complex varves consisting of up to four seasonal sub-layers formed during the Allered and early Holocene periods, and, (II) simple two sub-layer type varves only occurring during the Younger Dryas. The precision of the chronology has been improved by varve-to-varve comparison of two independently analyzed sediment profiles based on well-defined micro-marker layers. This has enabled both (1) the precise location of single missing varies in one of the sediment profiles, and, (2) the verification of varve interpolation in disturbed varve intervals in the parallel core. Inter-annual and decadal-scale variability in sediment deposition processes were traced by multi-proxy data series including seasonal layer thickness, high-resolution element scans and total organic and inorganic carbon data at a five-varve resolution. These data support the idea of a two-phase Younger Dryas, with the first interval (12,675-12,275 varve years BP) characterised by a still significant but gradually decreasing warm-season calcite precipitation and a second phase (12,275-11,690 varve years BP) with only weak calcite precipitation. Detailed correlation of these two phases with the Meerfelder Maar record based on the LST isochrone and independent varve counts provides clues about regional differences and seasonal aspects of YD climate change along a transect from a location proximal to the North Atlantic in the west to a more continental site in the east
Temporally changing drivers for late-Holocene vegetation changes on the northern Tibetan Plateau
(2012)
Fossil pollen records have been widely used as indicators of past changes in vegetation and variations in climate. The driving mechanisms behind these vegetation changes have, however, remained unclear. In order to evaluate vegetation changes that have occurred in the northern part of the Tibetan Plateau and the possible drivers behind these changes, we have applied a moving-window Redundancy Analysis (RDA) to high resolution (10-15 years) pollen and sedimentary data from Lake Kusai covering the last 3770 years. Our analyses reveal frequent fluctuations in the relative abundances of alpine steppe and alpine desert components. The sedimentary proxies (including total organic carbon content, total inorganic carbon content, and "end-member" indices from grain-size analyses) that explain statistically some of the changes in the pollen assemblage vary significantly with time, most probably reflecting multiple underlying driving processes. Climate appears to have had an important influence on vegetation changes when conditions were relatively wet and stable. However, a gradual decrease in vegetation cover was identified after 1500 cal a BP, after which the vegetation appears to have been affected more by extreme events such as dust-storms or fluvial erosion than by general climatic trends. Furthermore, pollen spectra over the last 600 years are shown by Procrustes analysis to be statistically different from those recovered from older samples, which we attribute to increased human impact that resulted in unprecedented changes to the vegetation composition. Overall, changes in vegetation and climate on the northern part of the Tibetan Plateau appear to have roughly followed the evolution of the Asian Summer Monsoon. After taking into account the highly significant millennial (1512 years) periodicity revealed by time-series analysis, the regional vegetation and climate changes also show variations that appear to match variations in the mid-latitude westerlies.
Inorganic minerals form a major component of lacustrine sediments and have the potential to reveal detailed information on previous climatic and hydrological conditions. The ability to extract such information however, has been restricted by a limited understanding of the relationships between minerals and the environment. In an attempt to fill in this gap in our knowledge, 146 surface sediment samples have been investigated from 146 lakes on the Tibetan Plateau. The mineral compositions derived from these samples by X-Ray Diffraction (XRD) were used to examine the relationships between mineral compositions and the environmental variables determined for each site. Statistical techniques including Multivariate regression trees (MRT) and Redundancy Analysis (RDA), based on the mineral spectra and environmental variables, reveal that the electrical conductivity (EC) and Mg/Ca ratios of lake water are the most important controls on the composition of endogenic minerals. No endogenic minerals precipitate under hyper-fresh water conditions (EC lower than 0.13 mS/cm), with calcite commonly forming in water with EC values above 0.13 mS/cm. Between EC values of 0.13 and 26 mS/cm the mineral composition of lake sediments can be explained in terms of variations in the Mg/Ca ratio: calcite dominates at Mg/Ca ratios of less than 33, whereas aragonite commonly forms when the ratio is greater than 33. Where EC values are between 26 and 39 mS/cm, monohydrocalcite precipitates together with calcite and aragonite; above 39 mS/cm, gypsum and halite commonly form. Information on the local geological strata indicates that allogenic (detrital) mineral compositions are primarily influenced by the bedrock compositions within the catchment area. By applying these relationships to the late glacial and Holocene mineral record from Chaka Salt Lake, five lake stages have been identified and their associated EC conditions inferred. The lake evolved from a freshwater lake during the late glacial (before 11.4 cal. ka BP) represented by the lowest EC values (< 0.13 mS/cm), to a saline lake with EC values slightly higher than 39 mS/cm during the early and mid Holocene (ca. 11.4-5.3 cal. ka BP), and finally to a salt lake (after 5.3 cal. ka BP). These results illustrate the utility of our mineral-environmental model for the quantitative reconstruction of past environmental conditions from lake sediment records.
Organic geochemical proxy data from surface sediment samples and a sediment core from Lake Donggi Cona were used to infer environmental changes on the northeastern Tibetan Plateau spanning the last 18.4 kyr. Long-chain n-alkanes dominate the aliphatic hydrocarbon fraction of the sediment extract from most surface sediment samples and the sediment core. Unsaturated mid-chain n-alkanes (nC(23:1) and nC(25:1)) have high abundances in some samples, especially in core samples from the late glacial and early Holocene. TOC contents, organic biomarker and non-pollen-palynomorph concentrations and results from organic petrologic analysis on selected samples suggest three major episodes in the history of Lake Donggi Cona. Before ca. 12.6 cal ka BP samples contain low amounts of organic matter due to cold and arid conditions during the late glacial. After 12.6 cal ka BP, relatively high contents of TOC and concentrations of Botryococcus fossils, as well as enhanced concentrations of mid-chain n-alkanes and n-alkenes suggest a higher primary and macrophyte productivity than at present This is supported by high contents of palynomorphs derived from higher plants and algae and was possibly triggered by a decrease of salinity and amelioration of climate during the early Holocene. Since 6.8 cal ka BP Lake Donggi Cona has been an oligotrophic freshwater lake. Proxy data suggest that variations in insolation drive ecological changes in the lake, with increased aquatic productivity during the early Holocene summer insolation maximum. Short-term drops of TOC contents or biomarker concentrations (at 9.9 cal ka BP, after 8.0 and between 3.5 and 1.7 cal ka BP) can possibly be related to relatively cool and dry episodes reported from other sites on the north-eastern Tibetan Plateau, which are hypothesized to occur in phase with Northern Hemisphere cooling events.
Ciliate epibionts associated with crustacean zooplankton are widespread in aquatic systems, but their ecological roles are little known. We studied the occurrence of ciliate epibionts on crustacean zooplankton in nine German lakes with different limnological features during the summer of 2011. We also measured the detachment and re-attachment rates of the ciliates, changes in their motility, and the feeding rates of attached vs. detached ciliate epibionts. Epibionts were found in all lakes sampled except an acidic lake with large humic inputs. Epibiont prevalence was as high as 80.96% on the cladoceran Daphnia cucullata, 67.17% on the cladoceran Diaphanosoma brachyurum, and 46.67% on the calanoid copepod Eudiaptomus gracilis. Both cladoceran groups typically had less than 10 epibionts per individual, while the epibiont load on E. gracilis ranged from 1 to >30 epibionts per individual. After the death of the zooplankton host, the peritrich ciliate epibiont Epistylis sp. detached in an exponential fashion with a half-life of 5 min, and 98% detached within 30 min, leaving behind the stalks used for attachment. Immediately after detachment, the ciliates were immotile, but 62% became motile within 60 min. When a new host was present, only 27% reattached after 120 min. The average measured ingestion rate and clearance rate of Epistylis were 11,745 bacteria ciliate(-1) h(-1) and 24.33 mu l ciliate(-1) h(-1), respectively. Despite their high feeding rates, relatively low epibiont abundances were observed in the field, which suggests either diversion of energy to stalk formation, high metabolic loss by the epibionts, or high mortality among the epibiont populations.
Using the carcass sinking rate and density determined in laboratory for several freshwater zooplankton species, we developed a model of zooplankton carcass sinking as affected by turbulence and stratification. The model was subsequently used to estimate the residence time of zooplankton carcasses in the water column of Lake Stechlin, a typical temperate dimictic lake in northeastern Germany. The residence time varied among the different species and was strongly affected by thermal stratification. At the peak of summer stratification, the carcasses stayed up to 5 d in the 70 m-deep water column before reaching the lake bottom. Residence time was long enough that zooplankton carcasses could serve as an important matter and energy source for bacteria in the lake's pelagic zone and hence have the potential to significantly affect aquatic carbon and nutrient cycling. The proposed model of sinking rates, based on physically sound relationships, can be easily applied to other passively sinking particles, and be integrated into large ecosystem models.
Intra- and interrater variability of sonographic investigations of patella and achilles tendons
(2012)
Background: Clinical examinations of tendon disorders routinely include ultrasound examinations, despite the fact that availability of data concerning validity criteria of these measurements are limited. The present study therefore aims to evaluate the reliability of measurements of Achilles- and Patella tendon diameter and in the detection of structural adaptations.
Materials and Methods: In 14 healthy, recreationally active subjects both asymptomatic Achilles (AT) and patella tendons (PT) were measured twice by two examiners in a test-retest design. Besides the detection of anteroposterior (a.p.-) and mediolateral (m.l.-) diameters, areas of hypoechogenicity and neovascularisation were registered. Data were analysed descriptively with calculation of test-retest variability (TRV), intraclass-correlation coefficient (ICC) and Bland and Altman's plots with bias and 95% limits of agreement (LOA).
Results: Intra- and interrater differences of AT- and PT-a.p.-diameter varied from 0.2 - 1.2 mm, those of AT- and PT-m.l-diameter from 0.7-5.1 mm. Areas of hypoechogenicity were visible in 24% of the tendons, while 15% showed neovascularisations. Intrarater AT-a.p.-diameters showed sparse deviations (TRV 4.5-7.4%; ICC 0.60-0.84; bias -0.05-0.07 mm; LOA-0.6-0.5 to -1.1 - 1.0 mm), while interrater AT- and PT-m.l.-diameters were highly variable (TRV 13.7-19.7%; ICC 0.11-0.20; bias -1.4-4.3 mm; LOA-5.5-2.7 to -10.5 - 1.9 mm).
Conclusion: Our results suggest that the measurement of AT- and PT-a.p.-diameters is a reliable parameter. In contrast, reproducibility of AT- and PT-m.l.-diameters is questionable. The study corroborates the presence of hypoechogenicity and neovascularisation in asymptomatic tendons.
Parameters of a formal working-memory model were estimated for verbal and spatial memory updating of children. The model proposes interference though feature overwriting and through confusion of whole elements as the primary cause of working-memory capacity limits. We tested 2 age groups each containing 1 group of normal intelligence and I deficit group. For young children the deficit was developmental dyslexia; for older children it was a general learning difficulty. The interference model predicts less interference through overwriting but more through confusion of whole elements for the dyslexic children than for their age-matched controls. Older children exhibited less interference through confusion of whole elements and a higher processing rate than young children, but general learning difficulty was associated with slower processing than in the age-matched control group. Furthermore, the difference between verbal and spatial updating mapped onto several meaningful dissociations of model parameters.
Inhalt: Introduction Developments in creating corpora dlexDB, subtitles, and tabloid newspapers Rating corpus emotionality Current study Method Materials Corpora Results Type-token ratio Validity: Effects of task difficulty Emotionality of a corpus Validity: Effects of emotionality Discussion Outlook References
Background Preparticipation examinations (PPE) are frequently used to evaluate eligibility for competitive sports in adolescent athletes. Nevertheless, the effectiveness of these examinations is under debate since costs are high and its validity is discussed controversial.
Purpose To analyse medical findings and consequences in adolescent athletes prior to admission to a sports school.
Methods In 733 adolescent athletes (318 girls, 415 boys, age 12.3+/-0.4, 16 sports disciplines), history and clinical examination (musculoskeletal, cardiovascular, general medicine) was performed to evaluate eligibility. PPE was completed by determination of blood parameters, ECG at rest and during ergometry, echocardiography and x-rays and ultrasonography if indicated. Eligibility was either approved or rated with restriction. Recommendations for therapy and/or prevention were given to the athletes and their parents.
Results Historical (h) and clinical (c) findings (eg, pain, verified pathologies) were more frequent regarding the musculoskeletal system (h: 120, 16.4%; c: 247, 33.7%) compared to cardiovascular (h: 9, 1.2%; c: 23, 3.1%) or general medicine findings (h: 116, 15.8%; c: 71, 9.7%). ECG at rest was moderately abnormal in 46 (6.3%) and severely abnormal in 25 athletes (3.4%). Exercise ECG was suspicious in 25 athletes (3.4%). Relevant echocardiographic abnormalities were found in 17 athletes (2.3%). In 52 of 358 cases (14.5%), x-rays led to diagnosis (eg, Spondylolisthesis). Eligibility was temporarily restricted in 41 athletes (5.6%). Three athletes (0.4%) had to be excluded from competitive sports. Therapy (eg, physiotherapy, medication) and/or prevention (sensorimotor training, vaccination) recommendations were deduced due to musculoskeletal (t:n = 76,10.3%; p:n = 71,9.8%) and general medicine findings (t:n = 80, 10.9%; p:n = 104, 14.1%).
Conclusion Eligibility for competitive sports is restricted in only 5.5% of adolescent athletes at age 12. Eligibility refusals are rare. However, recommendations for therapy and prevention are frequent, mainly regarding the musculoskeletal system. In spite of time and cost consumption, adolescent preparticipation before entering a career in high-performance sports is supported.
Neuromuscular activity of the lower leg is dependent on the task performed, speed of movement and gender. Whether training volume influences neuromuscular activity is not known. The EMG of physically active persons differing in running mileage was analysed to investigate this. 55 volunteers were allocated to a low (LM: < 30 km), intermediate (IM: > 30 km & < 45 km) or high mileage (HM: > 45 km) group according to their weekly running volume. Neuromuscular activity of the lower leg was measured during running (3.33 m.s(-1)). Mean amplitude values for preactivation, weight acceptance and push-off were calculated and normalised to the mean activity of the entire gait cycle. Higher activity in the gastrocnemius group was observed in weight acceptance in LM compared to IM (+30%) and HM (+25%) but lower activity was present in the push-off for LM compared to IM and HM. For the peroneal muscle, differences were present in the push-off where HM showed increased activity compared to IM (+24%) and LM (+60%). The tibial muscle revealed slightly lower activity during preactivation for the high mileage runners. Neuromuscular activity differs during stance between the high and intermediate group compared to low mileage runners. Slight adaptations in neuromuscular activation indicate a more target-oriented activation strategy possibly due to repetitive training in runners with higher weekly mileage.
The aim of this study was to acquire static and dynamic foot geometry and loading in childhood, and to establish data for age groups of a population of 1-13 year old infants and children.
A total of 10,382 children were recruited and 7788 children (48% males and 52% females) were finally included into the data analysis. For static foot geometry foot length and foot width were quantified in a standing position. Dynamic foot geometry and loading were assessed during walking on a walkway with self selected speed (Novel Emed X, 100 Hz, 4 sensors/cm(2)). Contact area (CA), peak pressure (PP), force time integral (FTI) and the arch index were calculated for the total, fore-, mid- and hindfoot.
Results show that most static and dynamic foot characteristics change continuously during growth and maturation. Static foot length and width increased with age from 13.1 +/- 0.8 cm (length) and 5.7 +/- 0.4 cm (width) in the youngest to 24.4 +/- 1.5 cm (length) and 8.9 +/- 0.6 cm (width) in the oldest. A mean walking velocity of 0.94 +/- 0.25 m/s was observed. Arch-index ranged from 0.32 +/- 0.04 [a.u.] in the one-year old to 0.21 +/- 0.13 [a.u.] in the 5-year olds and remains constant afterwards.
This study provides data for static and dynamic foot characteristics in children based on a cohort of 7788 subjects. Static and dynamic foot measures change differently during growth and maturation. Dynamic foot measurements provide additional information about the children's foot compared to static measures.
We present ultrafast x-ray diffraction (UXRD) experiments on different photoexcited oxide superlattices. All data are successfully simulated by dynamical x-ray diffraction calculations based on a microscopic model, that accounts for the linear response of phonons to the excitation laser pulse. Some Bragg reflections display a highly nonlinear strain dependence. The origin of linear and two distinct nonlinear response phenomena is discussed in a conceptually simpler model using the interference of envelope functions that describe the diffraction efficiency of the average constituent nanolayers. The combination of both models facilitates rapid and accurate simulations of UXRD experiments.
Normalization schemes for ultrafast x-ray diffraction using a table-top laser-driven plasma source
(2012)
We present an experimental setup of a laser-driven x-ray plasma source for femtosecond x-ray diffraction. Different normalization schemes accounting for x-ray source intensity fluctuations are discussed in detail. We apply these schemes to measure the temporal evolution of Bragg peak intensities of perovskite superlattices after ultrafast laser excitation.
Epitaxially grown metallic oxide transducers support the generation of ultrashort strain pulses in SrTiO3 (STO) with high amplitudes up to 0.5%. The strain amplitudes are calibrated by real-time measurements of the lattice deformation using ultrafast x-ray diffraction. We determine the speed at which the strain fronts propagate by broadband picosecond ultrasonics and conclude that, above a strain level of approx. 0.2%, the compressive and tensile strain components travel at considerably different sound velocities, indicating nonlinear wave behavior. Simulations based on an anharmonic linear-chain model are in excellent accord with the experimental findings and show how the spectrum of coherent phonon modes changes with time.
When gold nanoparticles are covered with nanometric layers of transparent polyelectrolytes, the plasmon absorption spectrum A(lambda) increases by a factor of approximately three and shifts to the red. These modifications of dissipative experimental observables stop when the cover layer thickness approaches the particle diameter. Spectral modifications of dispersive parameters like the reflection R, however, keep changing with increasing cover layer thickness. The shift of the plasmon resonance caused by two interacting particle layers is studied as a function of the separating distance between the two layers. We discuss these observations in the context of an effective medium theory and conclude that it can only be applied for a layer thickness on the order of the particle diameter.
During reading information is acquired from word(s) beyond the word that is currently looked at. It is still an open question whether such parafoveal information can influence the current viewing of a word, and if so, whether such parafoveal-on-foveal effects are attributable to distributed processing or to mislocated fixations which occur when the eyes are directed at a parafoveal word but land on another word instead. In two display-change experiments, we orthogonally manipulated the preview and target difficulty of word n+2 to investigate the role of mislocated fixations on the previous word n+1. When the eyes left word n, an easy or difficult word n+2 preview was replaced by an easy or difficult n+2 target word. In Experiment 1, n+2 processing difficulty was manipulated by means of word frequency (i.e., easy high-frequency vs. difficult low-frequency word n+2). In Experiment 2, we varied the visual familiarity of word n+2 (i.e., easy lower-case vs. difficult alternating-case writing). Fixations on the short word n+1, which were likely to be mislocated, were nevertheless not influenced by the difficulty of the adjacent word n+2, the hypothesized target of the mislocated fixation. Instead word n+1 was influenced by the preview difficulty of word n+2, representing a delayed parafoveal-on-foveal effect. The results challenge the mislocated-fixation hypothesis as an explanation of parafoveal-on-foveal effects and provide new insight into the complex spatial and temporal effect structure of processing inside the perceptual span during reading.
Parameters of a formal working-memory model were estimated for verbal and spatial memory updating of children. The model proposes interference though feature overwriting and through confusion of whole elements as the primary cause of working-memory capacity limits. We tested 2 age groups each containing 1 group of normal intelligence and 1 deficit group. For young children the deficit was developmental dyslexia; for older children it was a general learning difficulty. The interference model predicts less interference through overwriting but more through confusion of whole elements for the dyslexic children than for their age-matched controls. Older children exhibited less interference through confusion of whole elements and a higher processing rate than young children, but general learning difficulty was associated with slower processing than in the age-matched control group. Furthermore, the difference between verbal and spatial updating mapped onto several meaningful dissociations of model parameters.
Three ERP experiments examined the effect of word presentation rate (i.e., stimulus onset asynchrony, SOA) on the time course of word frequency and predictability effects in sentence reading. In Experiments 1 and 2, sentences were presented word-by-word in the screen center at an SOA of 700 and 490 ms, respectively. While these rates are typical for psycholinguistic ERP research, natural reading happens at a considerably faster pace. Accordingly. Experiment 3 employed a near-normal SOA of 280 ms, which approximated the rate of normal reading. Main results can be summarized as follows: (1) The onset latency of early frequency effects decreases gradually with increasing presentation rates. (2) An early interaction between top-down and bottom-up processing is observed only under a near-normal SOA. (3) N400 predictability effects occur later and are smaller at a near-normal (i.e., high) presentation rate than at the lower rates commonly used in ERP experiments. (4) ERP morphology is different at the shortest compared to longer SOAs. Together, the results point to a special role of a near-normal presentation rate for visual word recognition and therefore suggest that SOA should be taken into account in research of natural reading.
Preview fixation duration modulates identical and semantic preview benefit in Chinese reading
(2012)
Semantic preview benefit from parafoveal words is critical for proposals of distributed lexical processing during reading. Semantic preview benefit has been demonstrated for Chinese reading with the boundary paradigm in which unrelated or semantically related previews of a target word N + 1 are replaced by the target word once the eyes cross an invisible boundary located after word N (Yan et al., 2009); for the target word in position N + 2, only identical compared to unrelated-word preview led to shorter fixation times on the target word (Yan et al., in press). A reanalysis of these data reveals that identical and semantic preview benefits depend on preview duration (i.e., the fixation duration on the preboundary word). Identical preview benefit from word N + 1 increased with preview duration. The identical preview benefit was also significant for N + 2, but did not significantly interact with preview duration. The previously reported semantic preview benefit from word N + 1 was mainly due to single- or first-fixation durations following short previews. We discuss implications for notions of serial attention shifts and parallel distributed processing of words during reading.
Semantic information extraction from the parafovea has been reported only in simplified Chinese for a special subset of characters and its generalizability has been questioned. This study uses traditional Chinese, which differs from simplified Chinese in visual complexity and in mapping semantic forms, to demonstrate access to parafoveal semantic information during reading of this script. Preview duration modulates various types (identical, phonological, and unrelated) of parafoveal information extraction. Parafoveal semantic extraction is more elusive in English; therefore, we conclude that such effects in Chinese are presumably caused by substantial cross-language differences from alphabetic scripts. The property of Chinese characters carrying rich lexical information in a small region provides the possibility of semantic extraction in the parafovea.
Semantic processing from parafoveal words is an elusive phenomenon in alphabetic languages, but it has been demonstrated only for a restricted set of noncompound Chinese characters. Using the gaze-contingent boundary paradigm, this experiment examined whether parafoveal lexical and sublexical semantic information was extracted from compound preview characters. Results generalized parafoveal semantic processing to this representative set of Chinese characters and extended the parafoveal processing to radical (sublexical) level semantic information extraction. Implications for notions of parafoveal information extraction during Chinese reading are discussed.
The vesicle-inducing protein in plastids (VIPP1) was suggested to play a role in thylakoid membrane formation via membrane vesicles. As this functional assignment is under debate, we investigated the function of VIPP1 in Chlamydomonas reinhardtii. Using immunofluorescence, we localized VIPP1 to distinct spots within the chloroplast. In VIPP1-RNA interference/artificial microRNA cells, we consistently observed aberrant, prolamellar body-like structures at the origin of multiple thylakoid membrane layers, which appear to coincide with the immunofluorescent VIPP1 spots and suggest a defect in thylakoid membrane biogenesis. Accordingly, using quantitative shotgun proteomics, we found that unstressed vipp1 mutant cells accumulate 14 to 20% less photosystems, cytochrome b(6)f complex, and ATP synthase but 30% more light-harvesting complex II than control cells, while complex assembly, thylakoid membrane ultrastructure, and bulk lipid composition appeared unaltered. Photosystems in vipp1 mutants are sensitive to high light, which coincides with a lowered midpoint potential of the Q(A)/Q(A)(-) redox couple and increased thermosensitivity of photosystem II (PSII), suggesting structural defects in PSII. Moreover, swollen thylakoids, despite reduced membrane energization, in vipp1 mutants grown on ammonium suggest defects in the supermolecular organization of thylakoid membrane complexes. Overall, our data suggest a role of VIPP1 in the biogenesis/assembly of thylakoid membrane core complexes, most likely by supplying structural lipids.
During natural reading, a parafoveal preview of the upcoming word facilitates its subsequent recognition (e.g., shorter fixation durations compared to masked preview) but nothing is known about the neural correlates of this so-called preview benefit. Furthermore, while the evidence is strong that readers preprocess orthographic features of upcoming words, it is controversial whether word meaning can also be accessed parafoveally. We investigated the timing, scope, and electrophysiological correlates of parafoveal information use in reading by simultaneously recording eye movements and fixation-related brain potentials (FRPs) while participants read word lists fluently from left to right. For one word the target (e.g., "blade") parafoveal information was manipulated by showing an identical ("blade"), semantically related ("knife"), or unrelated ("sugar") word as preview. In boundary trials, the preview was shown parafoveally but changed to the correct target word during the incoming saccade. Replicating classic findings, target words were fixated shorter after identical previews. In the EEG, this benefit was reflected in an occipitotemporal preview positivity between 200 and 280 ms. In contrast, there was no facilitation from related previews. In parafoveal-on-foveal trials, preview and target were embedded at neighboring list positions without a display change. Consecutive fixation of two related words produced N400 priming effects, but only shortly (160 ms) after the second word was directly fixated. Results demonstrate that neural responses to words are substantially altered by parafoveal preprocessing under normal reading conditions. We found no evidence that word meaning contributes to these effects. Saccade-contingent display manipulations can be combined with EEG recordings to study extrafoveal perception in vision.
The development of theories and computational models of reading requires an understanding of processing constraints, in particular of timelines related to word recognition and oculomotor control. Timelines of word recognition are usually determined with event-related potentials (ERPs) recorded under conditions of serial visual presentation (SVP) of words; timelines of oculomotor control are derived from parameters of eye movements (EMs) during natural reading. We describe two strategies to integrate these approaches. One is to collect ERPs and EMs in separate SVP and natural reading experiments for the same experimental material (but different subjects). The other strategy is to co-register EMs and ERPs during natural reading from the same subjects. Both strategies yield data that allow us to determine how lexical properties influence ERPs (e.g., the N400 component) and EMs (e.g., fixation durations) across neighboring words. We review our recent research on the effects of frequency and predictability of words on both EM and ERP measures with reference to current models of eye-movement control during reading. Results are in support of the proposition that lexical access is distributed across several fixations and across brain-electric potentials measured on neighboring words.
In many near-surface geophysical studies it is now common practice to collect co-located disparate geophysical data sets to explore subsurface structures. Reconstruction of physical parameter distributions underlying the available geophysical data sets usually requires the use of tomographic reconstruction techniques. To improve the quality of the obtained models, the information content of all data sets should be considered during the model generation process, e.g., by employing joint or cooperative inversion approaches. Here, we extend the zonal cooperative inversion methodology based on fuzzy c-means cluster analysis and conventional single-input data set inversion algorithms for the cooperative inversion of data sets with partially co-located model areas. This is done by considering recent developments in fuzzy c-means cluster analysis. Additionally, we show how supplementary a priori information can be incorporated in an automated fashion into the zonal cooperative inversion approach to further constrain the inversion. The only requirement is that this a priori information can be expressed numerically; e.g., by physical parameters or indicator variables. We demonstrate the applicability of the modified zonal cooperative inversion approach using synthetic and field data examples. In these examples, we cooperatively invert S- and P-wave traveltime data sets with partially co-located model areas using water saturation information expressed by indicator variables as additional a priori information. The approach results in a zoned multi-parameter model, which is consistent with all available information given to the zonal cooperative inversion and outlines the major subsurface units. In our field example, we further compare the obtained zonal model to sparsely available borehole and direct-push logs. This comparison provides further confidence in our zonal cooperative inversion model because the borehole and direct-push logs indicate a similar zonation.
Mapping hydrological parameter distributions in high resolution is essential to understand and simulate groundwater flow and contaminant transport. Of particular interest is surface-based ground-penetrating radar (GPR) reflection imaging in electrically resistive sediments because of the expected close link between the subsurface water content and the dielectric permittivity, which controls GPR wave velocity and reflectivity. Conventional tools like common midpoint (CMP) velocity analysis provide physical parameter models of limited resolution only. We present a novel reflection amplitude inversion workflow for surface-based GPR data capable of resolving the subsurface dielectric permittivity and related water content distribution with markedly improved resolution. Our scheme is an adaptation of a seismic reflection impedance inversion scheme to surface-based GPR data. Key is relative-amplitude-preserving data preconditioning including GPR deconvolution, which results in traces with the source-wavelet distortions and propagation effects largely removed. The subsequent inversion for the underlying dielectric permittivity and water content structure is constrained by in situ dielectric permittivity data obtained by direct-push logging. After demonstrating the potential of our novel scheme on a realistic synthetic data set, we apply it to two 2-D 100 MHz GPR profiles acquired over a shallow sedimentary aquifer resulting in water content images of the shallow (3-7 m depth) saturated zone having decimeter resolution.
Assessing the human and economic threat introduced by sliding or creeping masses is of major importance in landslide hazard assessment and mitigation. Especially, in the densely populated alpine region unstable hillslopes represent a major hazard to men and infrastructure. Detailed knowledge, especially, of the dominant site-specific controlling factors such as subsurface architecture and geology is thereby key in assessing slope vulnerability. In order to quantify the geological variations at a creeping hillslope in the Austrian Alps, we have collected six 2D refraction seismic profiles. We propose using a layer-based inversion strategy to reconstruct P-wave velocity models from first arrival times. Considering the geological complexity at such sites, the selected inversion approach eases the interpretability of geological structures given intrinsic optimization for only a discrete, user-defined, number of layers. As the applied layer-based inversion approach fits our travel time data equally well as traditional smooth inversion approaches, it represents a feasible mean to summarize the structural complexity often present at such sites. Analysis of the inversion results illustrates that bedrock topography clearly deviates from a previously assumed planar surface and exhibits distinct variations across the slope extension. Bedrock topography additionally impacts the intermediate geological units and, thus, this information is critical for further analyses such as geomechanical modeling. (C) 2012 Elsevier B.V. All rights reserved.
Crosshole traveltime tomography using particle swarm optimization a near-surface field example
(2012)
Particle swarm optimization (PSO) is a relatively new global optimization approach inspired by the social behavior of bird flocking and fish schooling. Although this approach has proven to provide excellent convergence rates in different optimization problems, it has seldom been applied to inverse geophysical problems. Until today, published geophysical applications mainly focus on finding an optimum solution for simple, 1D inverse problems. We have applied PSO-based optimization strategies to reconstruct 2D P-wave velocity fields from crosshole traveltime data sets. Our inversion strategy also includes generating and analyzing a representative ensemble of acceptable models, which allows us to appraise uncertainty and nonuniqueness issues. The potential of our strategy was tested on field data collected at a well-constrained test site in Horstwalde, Germany. At this field site, the shallow subsurface mainly consists of sand- and gravel-dominated glaciofluvial sediments, which, as known from several boreholes and other geophysical experiments, exhibit some well-defined layering at the scale of our crosshole seismic data. Thus, we have implemented a flexible, layer-based model parameterization, which, compared with standard cell-based parameterizations, allows for significantly reducing the number of unknown model parameters and for efficiently implementing a priori model constraints. Comparing the 2D velocity fields resulting from our PSO strategy to independent borehole and direct-push data illustrated the benefits of choosing an efficient global optimization approach. These include a straightforward and understandable appraisal of nonuniqueness issues as well as the possibility of an improved and also more objective interpretation.
Polarization of the electromagnetic wavefield has significant implications for the acquisition and interpretation of ground-penetrating radar (GPR) data. Based on the geometrical and physical properties of the subsurface scatterer and the physical properties of its surrounding material, strong polarization phenomena might occur. Here, we develop an attribute-based analysis approach to extract and characterize buried utility pipes using two broadside antenna configurations. First, we enhance and extract the utilities by making use of their distinct symmetric nature through the application of a symmetry-enhancing image-processing algorithm known as phase symmetry. Second, we assess the polarization characteristics by calculating two attributes (polarization angle and linearity) using principal component analysis. Combination of attributes derived from these steps into a novel depolarization attribute allows one to efficiently detect and distinguish different utilities present within 3-D GPR data. The performance of our analysis approach is illustrated using synthetic examples and evaluated using field examples (including a dual-configuration 3-D data set) collected across a field site, where detailed ground-truth information is available. Our results demonstrate that the proposed approach allows for a more detailed extraction and combination of utility relevant information compared to approaches relying on single-component data and, thus, eases the interpretation of multicomponent GPR data sets.
Decomposition of geophysical signals (e.g., seismic and ground-penetrating radar data) into the time-frequency domain can provide valuable information for advanced interpretation (e.g., tuning effects) and processing (e.g., inverse Q-filtering). The quality of these subsequent processing steps is strongly related to the resolution of the selected time-frequency representation (TFR). In this study, we introduce a high-resolution spectral decomposition approach representing an extension of the recently proposed Tree-Based Pursuit (TBP) method. TBP significantly reduces the computational cost compared to the well known Matching Pursuit (MP) technique by introducing a tree structure prior to the actual matching procedure. Following the original implementation of TBP, we additionally incorporate waveforms commonly used in geophysical data processing and present an alternative approach to take phase shifts into account. Application of the proposed method to synthetic data and comparison of the results with other typically used decomposition approaches, illustrate the ability of our approach to provide decomposition results highly localized in both time and frequency. Applying our procedure to field GPR data illustrates its applicability to real data and provides examples for potential applications such as analyzing thin-bed responses and modulating the data frequency content.
The transition from juvenility through maturation to senescence is a complex process that involves the regulation of longevity. Here, we identify JUNGBRUNNEN1 (JUB1), a hydrogen peroxide (H2O2)-induced NAC transcription factor, as a central longevity regulator in Arabidopsis thaliana. JUB1 overexpression strongly delays senescence, dampens intracellular H2O2 levels, and enhances tolerance to various abiotic stresses, whereas in jub1-1 knockdown plants, precocious senescence and lowered abiotic stress tolerance are observed. A JUB1 binding site containing a RRYGCCGT core sequence is present in the promoter of DREB2A, which plays an important role in abiotic stress responses. JUB1 transactivates DREB2A expression in mesophyll cell protoplasts and transgenic plants and binds directly to the DREB2A promoter. Transcriptome profiling of JUB1 overexpressors revealed elevated expression of several reactive oxygen species-responsive genes, including heat shock protein and glutathione S-transferase genes, whose expression is further induced by H2O2 treatment. Metabolite profiling identified elevated Pro and trehalose levels in JUB1 overexpressors, in accordance with their enhanced abiotic stress tolerance. We suggest that JUB1 constitutes a central regulator of a finely tuned control system that modulates cellular H2O2 level and primes the plants for upcoming stress through a gene regulatory network that involves DREB2A.
Although the positive effect of elevated CO2 concentration [CO2] on plant growth is well known, it remains unclear whether global climate change will positively or negatively affect crop yields. In particular, relatively little is known about the role of hormone pathways in controlling the growth responses to elevated [CO2]. Here, we studied the impact of elevated [CO2] on plant biomass and metabolism in Arabidopsis (Arabidopsis thaliana) in relation to the availability of gibberellins (GAs). Inhibition of growth by the GA biosynthesis inhibitor paclobutrazol (PAC) at ambient [CO2] (350 mu mol CO2 mol(-1)) was reverted by elevated [CO2] (750 mu mol CO2 mol(-1)). Thus, we investigated the metabolic adjustment and modulation of gene expression in response to changes in growth of plants imposed by varying the GA regime in ambient and elevated [CO2]. In the presence of PAC (low-GA regime), the activities of enzymes involved in photosynthesis and inorganic nitrogen assimilation were markedly increased at elevated [CO2], whereas the activities of enzymes of organic acid metabolism were decreased. Under ambient [CO2], nitrate, amino acids, and protein accumulated upon PAC treatment; however, this was not the case when plants were grown at elevated [CO2]. These results suggest that only under ambient [CO2] is GA required for the integration of carbohydrate and nitrogen metabolism underlying optimal biomass determination. Our results have implications concerning the action of the Green Revolution genes in future environmental conditions.
The tricarboxylic acid (TCA) cycle is a crucial component of respiratory metabolism in both photosynthetic and heterotrophic plant organs. All of the major genes of the tomato TCA cycle have been cloned recently, allowing the generation of a suite of transgenic plants in which the majority of the enzymes in the pathway are progressively decreased. Investigations of these plants have provided an almost complete view of the distribution of control in this important pathway. Our studies suggest that citrate synthase, aconitase, isocitrate dehydrogenase, succinyl CoA ligase, succinate dehydrogenase, fumarase and malate dehydrogenase have control coefficients flux for respiration of -0.4, 0.964, -0.123, 0.0008, 0.289, 0.601 and 1.76, respectively; while 2-oxoglutarate dehydrogenase is estimated to have a control coefficient of 0.786 in potato tubers. These results thus indicate that the control of this pathway is distributed among malate dehydrogenase, aconitase, fumarase, succinate dehydrogenase and 2-oxoglutarate dehydrogenase. The unusual distribution of control estimated here is consistent with specific non-cyclic flux mode and cytosolic bypasses that operate in illuminated leaves. These observations are discussed in the context of known regulatory properties of the enzymes and some illustrative examples of how the pathway responds to environmental change are given.
Translatome and metabolome effects triggered by gibberellins during rosette growth in Arabidopsis
(2012)
Although gibberellins (GAs) are well known for their growth control function, little is known about their effects on primary metabolism. Here the modulation of gene expression and metabolic adjustment in response to changes in plant (Arabidopsis thaliana) growth imposed on varying the gibberellin regime were evaluated. Polysomal mRNA populations were profiled following treatment of plants with paclobutrazol (PAC), an inhibitor of GA biosynthesis, and gibberellic acid (GA(3)) to monitor translational regulation of mRNAs globally. Gibberellin levels did not affect levels of carbohydrates in plants treated with PAC and/or GA(3). However, the tricarboxylic acid cycle intermediates malate and fumarate, two alternative carbon storage molecules, accumulated upon PAC treatment. Moreover, an increase in nitrate and in the levels of the amino acids was observed in plants grown under a low GA regime. Only minor changes in amino acid levels were detected in plants treated with GA(3) alone, or PAC plus GA(3). Comparison of the molecular changes at the transcript and metabolite levels demonstrated that a low GA level mainly affects growth by uncoupling growth from carbon availability. These observations, together with the translatome changes, reveal an interaction between energy metabolism and GA-mediated control of growth to coordinate cell wall extension, secondary metabolism, and lipid metabolism.
Background: There are alternative substrates to the mitochondrial respiration.
Results: Data-driven model-based analysis renders predictions of alternative substrates to the mitochondrial respiration.
Conclusion: Metabolomics data in conjunction with flux-based models can discriminate among hypotheses based on enzymology alone.
Significance: This analysis provides a basic framework for in silico studies of alternative pathways in metabolism.