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Three furan-fused BODIPYs were synthesized with perfluorinated methyl, ethyl and n-propyl groups on the meso-carbon. They were obtained with high yields by reacting the furan-fused 2-carboxylpyrrole in corresponding perfluorinated acid and anhydride. With the increase in perfluorinated alkyl chain length, the molecular packing in the single crystal is influenced, showing increasing stacking distance and decreasing slope angle. All the BODIPYs were characterized as intense absorbers in near infrared region in solid state, peaking at similar to 800 nm with absorption coefficient of over 280 000 cm(-1). Facilitated by high thermal stability, the furan-fused BODIPYs were employed in vacuum-deposited organic solar cells as electron donors. All devices exhibit PCE over 6.0% with the EQE maximum reaching 70% at similar to 790 nm. The chemical modification of the BODIPY donors have certain influence on the active layer morphology, and the highest PCE of 6.4% was obtained with a notably high jsc of 13.6 mA cm(-2). Sensitive EQE and electroluminance studies indicated that the energy losses generated by the formation of a charge transfer state and the radiative recombination at the donor-acceptor interface were comparable in the range of 0.14-0.19 V, while non-radiative recombination energy loss of 0.38 V was the main energy loss route resulting in the moderate V-oc of 0.76 V.
Negatively charged flat gold nanotriangles, formed in a vesicular template phase and separated by an AOT-micelle-based depletion flocculation, were reloaded by adding a cationic polyelectrolyte, that is, a hyperbranched polyethylenimine (PEI). Heating the system to 100 degrees C in the presence of a gold chloride solution, the reduction process leads to the formation of gold nanoparticles inside the polymer shell surrounding the nanoplatelets. The gold nanoparticle formation is investigated by UV-vis spectroscopy, small-angle X-ray scattering, and dynamic light scattering measurements in combination with transmission electron microscopy. Spontaneously formed gold clusters in the hyperbranched PEI shell with an absorption maximum at 350 nm grow on the surface of the nanotriangles as hemispherical particles with diameters of similar to 6 nm. High-resolution micrographs show that the hemispherical gold particles are crystallized onto the {111} facets on the bottom and top of the platelet as well as on the edges without a grain boundary. Undulated gold nanoplatelet superstructures with special properties become available, which show a significantly modified performance in SERS-detected photocatalysis regarding both reactivity and enhancement factor.
Catanionic vesicles spontaneously formed by mixing the anionic surfactant bis(2-ethylhexyl)sulfosuccinate sodium salt with the cationic surfactant cetyltrimethylammonium bromide were used as a reducing medium to produce gold clusters, which are embedded and well-ordered into the template phase. The gold clusters can be used as seeds in the growth process that follows by adding ascorbic acid as a mild reducing component. When the ascorbic acid was added very slowly in an ice bath round-edged gold nanoflowers were produced. When the same experiments were performed at room temperature in the presence of Ag+ ions, sharp-edged nanoflowers could be synthesized. The mechanism of nanoparticle formation can be understood to be a non-diffusion-limited Ostwald ripening process of preordered gold nanoparticles embedded in catanionic vesicle fragments. Surface-enhanced Raman scattering experiments show an excellent enhancement factor of 1.7 . 10(5) for the nanoflowers deposited on a silicon wafer.
Negatively charged ultraflat gold nanotriangles (AuNTs) stabilized by the anionic surfactant dioctyl sodium sulfosuccinate (AOT) were reloaded with the cationic surfactant benzylhexadecyldimethylammonium chloride (BDAC). Because of the spontaneous formation of a catanionic AOT micelle/BDAC bilayer onto the surface of the reloaded AuNTs, a reduction of Ag+ ions leads to the formation of spherical silver nanoparticles (AgNPs). With increasing concentration of AgNPs on the AuNTs, the localized surface plasmon resonance (LSPR) is shifted stepwise from 1300 to 800 nm. The tunable LSPR enables to shift the extinction maximum to the wavelength of the excitation laser of the Raman microscope at 785 nm. Surface-enhanced Raman scattering (SERS) experiments performed under resonance conditions show an SERS enhancement factor of the analyte molecule rhodamine RG6 of 5.1 X 10(5), which can be related to the silver hot spots at the periphery of the undulated gold nanoplatelets.
Owing to their ability of concentrating electromagnetic fields to subwavelength mode volumes, plasmonic nanoparticles foster extremely high light-matter coupling strengths reaching far into the strong-coupling regime of light matter interaction. In this article, we present an experimental investigation on the dependence of coupling strength on the geometrical size of the nanoparticle. The coupling strength for differently sized hybrid plasmon-core exciton-shell nanorods was extracted from the typical resonance anticrossing of these systems, obtained by controlled modification of the environment permittivity using layer-by-layer deposition of polyelectrolytes. The observed size dependence of the coupling strength can be explained by a simple model approximating the electromagnetic mode volume by the geometrical volume of the particle. On the basis of this model, the coupling strength for particles of arbitrary size can be predicted, including the particle size necessary to support single-emitter strong coupling.
We trace the specific star formation rate (sSFR) of massive star-forming galaxies (greater than or similar to 10(10)M(circle dot)) from z similar to 2 to 7. Our method is substantially different from previous analyses, as it does not rely on direct estimates of star formation rate, but on the differential evolution of the galaxy stellar mass function (SMF). We show the reliability of this approach by means of semianalytical and hydrodynamical cosmological simulations. We then apply it to real data, using the SMFs derived in the COSMOS and CANDELS fields. We find that the sSFR is proportional to (1 + z)(1.1) (+/-) (0.2) at z > 2, in agreement with other observations but in tension with the steeper evolution predicted by simulations from z similar to 4 to 2. We investigate the impact of several sources of observational bias, which, however, cannot account for this discrepancy. Although the SMF of high-redshift galaxies is still affected by significant errors, we show that future large-area surveys will substantially reduce them, making our method an effective tool to probe the massive end of the main sequence of star-forming galaxies.
1-(Dimethylamino)-1-phenyl-1-silacyclohexane 1, was synthesized, and its molecular structure and conformational properties studied by gas-phase electron diffraction (GED), low temperature C-13 NMR spectroscopy and quantum-chemical calculations. The predominance of the 1-Ph-ax conformer (1-Ph-eq:1-Ph-ax ratio of 20:80%, Delta G degrees (317 K) = -0.87 kcal/mol) in the gas phase is close to the theoretically estimated conformational equilibrium. In solution, low temperature NMR spectroscopy showed analyzable decoalescence of C-ipso and C(1,5) carbon signals in C-13 NMR spectra at 103 K. Opposite to the gas state in the freon solution employed (CD2Cl2/CHFCl2/CHFCl2 = 1:1:3), which is still liquid at 100 K, the 1-Ph-eq conformer was found to be the preferred one [(1-Ph-eq: 1-Ph-ax = 77%: 23%, K = 77/23 = 2.8; -Delta G degrees = -RT In K (at 103 K) = 0.44 +/- 0.1 kcal/mol]. When comparing 1 with 1-phenyl-1-(X)silacylohexanes (X = H, Me, OMe, F, Cl), studied so far, the trend of predominance of the Ph-ax conformer in the gas phase and of the Ph-eq conformer in solution is confirmed.
The 3,3-disubstitued 3-silaheterocyclohexane with an electronegative substituent at silicon, 3-fluoro-3-methyl-3-silatetrahydropyran 1, was synthesized, and its molecular structure and conformational properties studied by gas-phase electron diffraction (GED) and low temperature C-13 and F-19 NMR spectroscopy. Quantum-chemical calculations were carried out both for the isolated species and Hcomplexes in gas and in polar medium. The predominance of the 1-FeqMeax conformer (1-F-eq:1-F-ax ratio of 65:35, Delta G degrees = 0.37 kcal/mol) determined from GED is close to the theoretically estimated conformational equilibrium, especially at the DFT level. In solution, low temperature NMR spectroscopy showed no decoalescence of the signals in C-13 (down to 95 K) and F-19 NMR spectra (down to 123 K). However, the calculated F-19 chemical shift of -173.6 ppm for the 1-FeqMeax conformer practically coincides with the experimentally observed value (-173 to -175 ppm) as distinct from that for the 1-FaxMeeq conformer (-188.8 ppm), suggesting compound 1 to be anancomeric in solution, in compliance with its theoretical and experimental preference in the gas phase.
The study investigated the incidence of Achilles and patellar tendinopathy in adolescent elite athletes and non-athletic controls. Furthermore, predictive and associated factors for tendinopathy development were analyzed. The prospective study consisted of two measurement days (M1/M2) with an interval of 3.2 +/- 0.9 years. 157 athletes (12.1 +/- 0.7 years) and 25 controls (13.3 +/- 0.6 years) without Achilles/patellar tendinopathy were included at Ml. Clinical and ultrasound examinations of both Achilles (AT) and patellar tendons (PT) were performed. Main outcome measures were incidence tendinopathy and structural intratendinous alterations (hypo-/hyperechogenicity, vascularization) at M2 [%]. Incidence of Achilles tendinopathy was 1% in athletes and 0% in controls. Patellar tendinopathy was more frequent in athletes (13 %)than in controls (4%). Incidence of intratendinous alterations in ATs was 1-2% in athletes and 0 % in controls, whereas in PTs it was 4-6 % in both groups (p >0.05). Intratendinous alterations at M2 were associated with patellar tendinopathy in athletes (p <= 0.01). Intratendinous alterations at M1, anthropometric data, training amount, sports or sex did not predict tendinopathy development (p>0.05). Incidence often dinopathy and intratendinous alterations in adolescent athletes is low in ATs and more common in PTs. Development of intratendinous alterations in PT is associated with tend in opathy. However, predictive factors could not be identified.
Understanding vegetation-modern pollen relationships is essential to provide confidence in fossil pollen reconstructions of long-term vegetation changes in savanna ecosystems. In this paper we compare the taxonomical composition and the diversity (Hill NO, N1, N2) of vegetation and modern pollen along precipitation and local grazing-intensity gradients in Namibian savannas. Modern pollen was extracted from surface soil samples collected from 5 x 5 m plots distributed along four 500 m gradients. Vegetation was surveyed in each plot. The results show a high correspondence between vegetation and pollen data in terms of composition. Precipitation and grazing explain a significant although low proportion of compositional change in the vegetation and pollen spectra. We identified pollen taxa as indicators of grazing pressure such as Limeum, Alternanthera, and particularly Tribulus. Correspondence between vegetation and pollen data in terms of taxa richness (NO) is limited, probably because of the influence of landscape heterogeneity and openness, as well as low pollen concentrations. In contrast, the effective numbers of common and dominant taxa (N1, N2) are consistent among the different datasets. We conclude that in spite of limitations, modern pollen assemblages can reflect changes in vegetation composition, richness and diversity patterns along precipitation and grazing gradients in savanna environments. (C) 2018 Elsevier B.V. All rights reserved.
Ring current effects on resonance-assisted and intramolecularly bridged hydrogen bond protons for 10-hydroxybenzo[h]quinoline 1 and a number of related compounds were calculated and the through-space NMR shieldings (TSNMRS) obtained hereby visualized as iso-chemical-shielding surfaces (ICSS) of various size and direction. These calculations revealed that this through-space effect is comparably large (up to 2 ppm) dependent on the position of the intramolecularly bridged OH proton, and therefore, contribute considerably to the chemical shift of the latter making it questionable to use delta(OH)/ppm in the estimation of intramolecular hydrogen bond strength without taking this into account. Furthermore, the anisotropy effects of additional groups on the aromatic moiety (e.g. the carbonyl group in salicylaldehyde or in o-hydroxyacetophenone of ca. 0.6 ppm deshielding) should also be considered. These through-space effects need to be taken into account when using OH chemical shifts to estimate hydrogen bond strength.
Understanding the molecular basis of morphological change remains a central challenge in evolutionary-developmental biology. The transition from outbreeding to selfing is often associated with a dramatic reduction in reproductive structures and functions, such as the loss of attractive pheromones in hermaphroditic Caenorhabditis elegans and a reduced flower size in plants. Here, we demonstrate that variation in the level of the brassinosteroid-biosynthesis enzyme CYP724A1 contributes to the reduced flower size of selfing Capsella rubella compared with its outbreeding ancestor Capsella grandiflora. The primary transcript of the C. rubella allele is spliced more efficiently than that of C. grandiflora, resulting in higher brassinosteroid levels. These restrict organ growth by limiting cell proliferation. More efficient splicing of the C. rubella allele results from two de novo mutations in the selfing lineage. Thus, our results highlight the potentially widespread importance of differential splicing efficiency and higher-than-optimal hormone levels in generating phenotypic variation.
Background: Core-specific sensorimotor exercises are proven to enhance neuromuscular activity of the trunk, improve athletic performance and prevent back pain. However, the dose-response relationship and, therefore, the dose required to improve trunk function is still under debate. The purpose of the present trial will be to compare four different intervention strategies of sensorimotor exercises that will result in improved trunk function.
Methods/design: A single-blind, four-armed, randomized controlled trial with a 3-week (home-based) intervention phase and two measurement days pre and post intervention (M1/M2) is designed. Experimental procedures on both measurement days will include evaluation of maximum isokinetic and isometric trunk strength (extension/flexion, rotation) including perturbations, as well as neuromuscular trunk activity while performing strength testing. The primary outcome is trunk strength (peak torque). Neuromuscular activity (amplitude, latencies as a response to perturbation) serves as secondary outcome. The control group will perform a standardized exercise program of four sensorimotor exercises (three sets of 10 repetitions) in each of six training sessions (30 min duration) over 3 weeks. The intervention groups’ programs differ in the number of exercises, sets per exercise and, therefore, overall training amount (group I: six sessions, three exercises, two sets; group II: six sessions, two exercises, two sets; group III: six sessions, one exercise, three sets). The intervention programs of groups I, II and III include additional perturbations for all exercises to increase both the difficulty and the efficacy of the exercises performed. Statistical analysis will be performed after examining the underlying assumptions for parametric and non-parametric testing.
Discussion: The results of the study will be clinically relevant, not only for researchers but also for (sports) therapists, physicians, coaches, athletes and the general population who have the aim of improving trunk function.
Long-distance race car drivers are classified as athletes. The sport is physically and mentally demanding, requiring long hours of practice. Therefore, optimal dietary intake is essential for health and performance of the athlete. The aim of the study was to evaluate dietary intake and to compare the data with dietary recommendations for athletes and for the general adult population according to the German Nutrition Society (DGE). A 24-h dietary recall during a competition preparation phase was obtained from 16 male race car drivers (28.3 ± 6.1 years, body mass index (BMI) of 22.9 ± 2.3 kg/m2). The mean intake of energy, nutrients, water and alcohol was recorded. The mean energy, vitamin B2, vitamin E, folate, fiber, calcium, water and alcohol intake were 2124 ± 814 kcal/day, 1.3 ± 0.5 mg/day, 12.5 ± 9.5 mg/day, 231.0 ± 90.9 ug/day, 21.4 ± 9.4 g/day, 1104 ± 764 mg/day, 3309 ± 1522 mL/day and 0.8 ± 2.5 mL/day respectively. Our study indicated that many of the nutrients studied, including energy and carbohydrate, were below the recommended dietary intake for both athletes and the DGE.
Static (one-legged stance) and dynamic (star excursion balance) postural control tests were performed by 14 adolescent athletes with and 17 without back pain to determine reproducibility. The total displacement, mediolateral and anterior-posterior displacements of the centre of pressure in mm for the static, and the normalized and composite reach distances for the dynamic tests were analysed. Intraclass correlation coefficients, 95% confidence intervals, and a Bland-Altman analysis were calculated for reproducibility. Intraclass correlation coefficients for subjects with (0.54 to 0.65), (0.61 to 0.69) and without (0.45 to 0.49), (0.52 to 0.60) back pain were obtained on the static test for right and left legs, respectively. Likewise, (0.79 to 0.88), (0.75 to 0.93) for subjects with and (0.61 to 0.82), (0.60 to 0.85) for those without back pain were obtained on the dynamic test for the right and left legs, respectively. Systematic bias was not observed between test and retest of subjects on both static and dynamic tests. The one-legged stance and star excursion balance tests have fair to excellent reliabilities on measures of postural control in adolescent athletes with and without back pain. They can be used as measures of postural control in adolescent athletes with and without back pain.
Agricultural land-use practices have intensified over the last decades, leading to population declines of various farmland species, including the European hare (Lepus europaeus). In many European countries, arable fields dominate agricultural landscapes. Compared to pastures, arable land is highly variable, resulting in a large spatial variation of food and cover for wildlife over the course of the year, which potentially affects habitat selection by hares. Here, we investigated within-home-range habitat selection by hares in arable areas in Denmark and Germany to identify habitat requirements for their conservation. We hypothesized that hare habitat selection would depend on local habitat structure, that is, vegetation height, but also on agricultural field size, vegetation type, and proximity to field edges. Active hares generally selected for short vegetation (1-25 cm) and avoided higher vegetation and bare ground, especially when fields were comparatively larger. Vegetation >50 cm potentially restricts hares from entering parts of their home range and does not provide good forage, the latter also being the case on bare ground. The vegetation type was important for habitat selection by inactive hares, with fabaceae, fallow, and maize being selected for, potentially providing both cover and forage. Our results indicate that patches of shorter vegetation could improve the forage quality and habitat accessibility for hares, especially in areas with large monocultures. Thus, policymakers should aim to increase areas with short vegetation throughout the year. Further, permanent set-asides, like fallow and wildflower areas, would provide year-round cover for inactive hares. Finally, the reduction in field sizes would increase the density of field margins, and farming different crop types within small areas could improve the habitat for hares and other farmland species.
We investigated whether a given landscape structure affects the level of home range size adaptation in response to resource variability. We tested whether increasing resource variability forces herbivorous mammals to increase their home ranges. In 2014 and 2015 we collared 40 European brown hares (Lepus europaeus) with GPS-tags to record hare movements in two regions in Germany with differing landscape structures. We examined hare home range sizes in relation to resource availability and variability by using the normalized difference vegetation index as a proxy. Hares in simple landscapes showed increasing home range sizes with increasing resource variability, whereas hares in complex landscapes did not enlarge their home range. Animals in complex landscapes have the possibility to include various landscape elements within their home ranges and are more resilient against resource variability. But animals in simple landscapes with few elements experience shortcomings when resource variability becomes high. The increase in home range size, the movement related increase in energy expenditure, and a decrease in hare abundances can have severe implications for conservation of mammals in anthropogenic landscapes. Hence, conservation management could benefit from a better knowledge about fine-scaled effects of resource variability on movement behaviour.
Stable Carbenes or Betaines?
(2018)
The anisotropy effect in H-1 NMR spectroscopy can be readily employed to indicate the position of carbene/betaine mesomeric equilibria. NR2 substituted carbene/betaines tend to adopt betaine structures, whereas in the absence of NR2 substituents, the betaine structures cannot stabilise the structure through both -donation effects of the NMe2 groups and the electronegativity of the nitrogen atoms, and the corresponding carbene-like structures are preferred. These conclusions are supported by calculated bond orders and (C-13)/ppm values. The spatial magnetic properties of isonitriles and carbon monoxide, which can be counted as stable carbenes or, at least, as carbene-analogues, also exist as stable betaine structures, which is again supported by structural and magnetic properties.
The aim of this study was to investigate the effect of a 6-week sensorimotor or resistance training on maximum trunk strength and response to sudden, high-intensity loading in athletes. Interventions showed no significant difference for maximum strength in concentric and eccentric testing (p>0.05). For perturbation compensation, higher peak torque response following SMT (Extension: +24Nm 95%CI +/- 19Nm; Rotation: + 19Nm 95%CI +/- 13Nm) and RT (Extension: +35Nm 95%CI +/- 16Nm; Rotation: +5Nm 95%CI +/- 4Nm) compared to CG (Extension: -4Nm 95%CI +/- 16Nm; Rotation: -2Nm 95%CI +/- 4Nm) was present (p<0.05).
Drunk decisions
(2018)
Background: Studies in humans and animals suggest a shift from goal-directed to habitual decision-making in addiction. We therefore tested whether acute alcohol administration reduces goal-directed and promotes habitual decision-making, and whether these effects are moderated by self-reported drinking problems. Methods: Fifty-three socially drinking males completed the two-step task in a randomised crossover design while receiving an intravenous infusion of ethanol (blood alcohol level=80 mg%), or placebo. To minimise potential bias by long-standing heavy drinking and subsequent neuropsychological impairment, we tested 18- to 19-year-old adolescents. Results: Alcohol administration consistently reduced habitual, model-free decisions, while its effects on goal-directed, model-based behaviour varied as a function of drinking problems measured with the Alcohol Use Disorders Identification Test. While adolescents with low risk for drinking problems (scoring <8) exhibited an alcohol-induced numerical reduction in goal-directed choices, intermediate-risk drinkers showed a shift away from habitual towards goal-directed decision-making, such that alcohol possibly even improved their performance. Conclusions: We assume that alcohol disrupted basic cognitive functions underlying habitual and goal-directed decisions in low-risk drinkers, thereby enhancing hasty choices. Further, we speculate that intermediate-risk drinkers benefited from alcohol as a negative reinforcer that reduced unpleasant emotional states, possibly displaying a novel risk factor for drinking in adolescence.