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A comprehensive molecular analysis of a simple aqueous complexing system. U(VI) acetate. selected to be independently investigated by various spectroscopic (vibrational, luminescence, X-ray absorption, and nuclear magnetic resonance spectroscopy) and quantum chemical methods was achieved by an international round-robin test (RRT). Twenty laboratories from six different countries with a focus on actinide or geochemical research participated and contributed to this scientific endeavor. The outcomes of this RRT were considered on two levels of complexity: first, within each technical discipline, conformities as well as discrepancies of the results and their sources were evaluated. The raw data from the different experimental approaches were found to be generally consistent. In particular, for complex setups such as accelerator-based X-ray absorption spectroscopy, the agreement between the raw data was high. By contrast, luminescence spectroscopic data turned out to be strongly related to the chosen acquisition parameters. Second, the potentials and limitations of coupling various spectroscopic and theoretical approaches for the comprehensive study of actinide molecular complexes were assessed. Previous spectroscopic data from the literature were revised and the benchmark data on the U(VI) acetate system provided an unambiguous molecular interpretation based on the correlation of spectroscopic and theoretical results. The multimethodologic approach and the conclusions drawn address not only important aspects of actinide spectroscopy but particularly general aspects of modern molecular analytical chemistry.
A well-preserved sequence, by Archean standards, of mantle-derived metabasalts and metakomatiites forms large parts of the lower Onverwacht Group of the Barberton Greenstone Belt (South Africa). To elucidate the origin of mafic and ultramafic rocks from this 3.55 to 3.45 Ga sequence, we present a comprehensive geochemical dataset including major and trace elements as well as Lu-Hf and Sm-Nd isotope compositions for a variety of metavolcanic rocks. These include metabasalts of the amphibolite-facies Sandspruit and Theespruit Formations as well as metabasalts and metakomatiites of the lower greenschist-facies Komati Formation. Based on their incompatible trace element patterns, the basalts of the Sandspruit and Theespruit Formations can be subdivided into a light rare earth element (LREE) depleted group, a LREE-undepleted group, and a LREE-enriched group. Positive epsilon Hf-(t) and epsilon Nd-(t) values of ca. +3 to +4 and 0 to +2, respectively, together with depletions in Th and La-CN/Yb-CN indicate derivation of the LREE-depleted basalts from a depleted mantle source. However, chondritic epsilon Hf-(t) and epsilon Nd-(t) values combined with positive Th and La-CN/Yb-CN of the LREE-enriched samples indicate a contribution from older granitoid crust in the petrogenesis of these samples. Trace element patterns of komatiites and basalts of the Komati Formation are generally flat relative to primitive mantle with slight depletions in heavy rare earth elements and Th and overall positive epsilon Hf-(t) of + 2.5 +/- 3.5 (2 s.d.) and epsilon Nd-(t) of + 0.5 +/- 2.2 (2 s. d.). The coherence in trace element characteristics suggests a common magmatic origin for basalts and komatiites. This study reveals that the two lavas were derived from the same mantle plume, i. e. komatiites were formed by high degrees of melting of a depleted mantle source containing residual garnet and the basalts were formed by moderate degrees of partial melting in shallower regions of the mantle. Based on the current dataset, combined with published data, we propose a geodynamic model for the oldest units of the Barberton Greenstone Belt that describes the development from a submerged continental setting (for the Sandspruit and Theespruit Formations) to a submarine plateau setting (for the Komati Formation) as a consequence of continental rifting.
Objectives: The objectives of this study were to determine the interrater reliability (IRR) of assessment of multiple systematic reviews (AMSTAR) 2 for reviews of pharmacological or psychological interventions for the treatment of major depression, to compare it to that of AMSTAR and risk of bias in systematic reviews (ROBIS), and to assess the convergent validity between the appraisal tools. Results: The median kappa values as a measure of IRR indicated a moderate agreement for AMSTAR 2 (median = 0.51), a substantial agreement for AMSTAR (median = 0.62), and a fair agreement for ROBIS (median = 0.27). Validity results showed a positive association for AMSTAR and AMSTAR 2 (r = 0.91) as well as ROBIS and AMSTAR 2 (r = 0.84). For the overall rating, AMSTAR 2 showed a high concordance with ROBIS and a lower concordance with AMSTAR. Conclusion: The IRR of AMSTAR 2 was found to be slightly lower than the IRR of AMSTAR and higher than the IRR of ROBIS. Validity measurements indicate that AMSTAR 2 is closely related to both ROBIS and AMSTAR. (C) 2019 Elsevier Inc. All rights reserved.
Nitrate or ammonium
(2019)
In freshwaters, algal species are exposed to different inorganic nitrogen (Ni) sources whose incorporation varies in biochemical energy demand. We hypothesized that due to the lesser energy requirement of ammonium (NH4+)-use, in contrast to nitrate (NO3-)-use, more energy remains for other metabolic processes, especially under CO2-and phosphorus (Pi) limiting conditions. Therefore, we tested differences in cell characteristics of the green alga Chlamydomonas acidophila grown on NH4+ or NO3- under covariation of CO2 and Pi-supply in order to determine limitations, in a full-factorial design. As expected, results revealed higher carbon fixation rates for NH4+ grown cells compared to growth with NO3- under low CO2 conditions. NO3- -grown cells accumulated more of the nine analyzed amino acids, especially under Pi-limited conditions, compared to cells provided with NH4+. This is probably due to a slower protein synthesis in cells provided with NO3-. In contrast to our expectations, compared to NH4+ -grown cells NO3- -grown cells had higher photosynthetic efficiency under Pi-limitation. In conclusion, growth on the Ni-source NH4+ did not result in a clearly enhanced Ci-assimilation, as it was highly dependent on Pi and CO2 conditions (replete or limited). Results are potentially connected to the fact that C. acidophila is able to use only CO2 as its inorganic carbon (Ci) source.
Distinct cellular roles for PDCD10 define a gut-brain axis in cerebral cavernous malformation
(2019)
Cerebral cavernous malformation (CCM) is a genetic, cerebrovascular disease. Familial CCM is caused by genetic mutations in KRIT1, CCM2, or PDCD10. Disease onset is earlier and more severe in individuals with PDCD10 mutations. Recent studies have shown that lesions arise from excess mitogen-activated protein kinase kinase kinase 3 (MEKK3) signaling downstream of Toll-like receptor 4 (TLR4) stimulation by lipopolysaccharide derived from the gut microbiome. These findings suggest a gut-brain CCM disease axis but fail to define it or explain the poor prognosis of patients with PDCD10 mutations. Here, we demonstrate that the gut barrier is a primary determinant of CCM disease course, independent of microbiome configuration, that explains the increased severity of CCM disease associated with PDCD10 deficiency. Chemical disruption of the gut barrier with dextran sulfate sodium augments CCM formation in a mouse model, as does genetic loss of Pdcd10, but not Krit1, in gut epithelial cells. Loss of gut epithelial Pdcd10 results in disruption of the colonic mucosal barrier. Accordingly, loss of Mucin-2 or exposure to dietary emulsifiers that reduce the mucus barrier increases CCM burden analogous to loss of Pdcd10 in the gut epithelium. Last, we show that treatment with dexamethasone potently inhibits CCM formation in mice because of the combined effect of action at both brain endothelial cells and gut epithelial cells. These studies define a gut-brain disease axis in an experimental model of CCM in which a single gene is required for two critical components: gut epithelial function and brain endothelial signaling.
We present follow-up observations of the K2-133 multiplanet system. Previously, we announced that K2-133 contained three super-Earths orbiting an M1.5V host star – with tentative evidence of a fourth outer-planet orbiting at the edge of the temperate zone. Here, we report on the validation of the presence of the fourth planet, determining a radius of 1.73+0.14−0.13 R⊕. The four planets span the radius gap of the exoplanet population, meaning further follow-up would be worthwhile to obtain masses and test theories of the origin of the gap. In particular, the trend of increasing planetary radius with decreasing incident flux in the K2-133 system supports the claim that the gap is caused by photo-evaporation of exoplanet atmospheres. Finally, we note that K2-133 e orbits on the edge of the star's temperate zone, and that our radius measurement allows for the possibility that this is a rocky world. Additional mass measurements are required to confirm or refute this scenario.
3-Bromopyruvic acid (3BP) is a potential anticancer drug, the action of which on cellular metabolism is not yet entirely clear. The presence of a bromine atom suggests that it is also reactive towards low-energy electrons, which are produced in large quantities during tumour radiation therapy. Detailed knowledge of the interaction of 3BP with secondary electrons is a prerequisite to gain a complete picture of the effects of 3BP in different forms of cancer therapy. Herein, dissociative electron attachment (DEA) to 3BP in the gas phase has been studied both experimentally by using a crossed-beam setup and theoretically through scattering and quantum chemical calculations. These results are complemented by a vacuum ultraviolet absorption spectrum. The main fragmentation channel is the formation of Br- close to 0 eV and within several resonant features at 1.9 and 3-8 eV. At low electron energies, Br- formation proceeds through sigma* and pi* shape resonances, and at higher energies through core-excited resonances. It is found that the electron-capture cross-section is clearly increased compared with that of non-brominated pyruvic acid, but, at the same time, fragmentation reactions through DEA are significantly altered as well. The 3BP transient negative ion is subject to a lower number of fragmentation reactions than those of pyruvic acid, which indicates that 3BP could indeed act by modifying the electron-transport chains within oxidative phosphorylation. It could also act as a radio-sensitiser.
Fibrous membranes capable of dynamically responding to external stimuli are highly desirable in textiles and biomedical materials, where adaptive behavior is required to accommodate complex environmental changes. For example, the creation of fabrics with temperature-dependent moisture permeability or self-regulating membranes for air filtration is dependent on the development of materials that exhibit a reversible stimuli-responsive pore size change. Here, by imbuing covalently crosslinked poly(ε-caprolactone) (cPCL) fibrous meshes with a reversible bidirectional shape-memory polymer actuation (rbSMPA) we create a material capable of temperature-controlled changes in porosity. Cyclic thermomechanical testing was used to characterize the mechanical properties of the meshes, which were composed of randomly arranged microfibers with diameters of 2.3 ± 0.6 μm giving an average pore size of approx. 10 μm. When subjected to programming strains of εm = 300% and 100% reversible strain changes of εʹrev = 22% ± 1% and 6% ± 1% were measured, with switching temperature ranges of 10 °C–30 °C and 45 °C–60 °C for heating and cooling, respectively. The rbSMPA of cPCL fibrous meshes generated a microscale reversible pore size change of 11% ± 3% (an average of 1.5 ± 0.6 μm), as measured by scanning electron microscopy. The incorporation of a two-way shape-memory actuation capability into fibrous meshes is anticipated to advance the development and application of smart membrane materials, creating commercially viable textiles and devices with enhanced performance and novel functionality.
Context. Metal-poor massive stars are assumed to be progenitors of certain supernovae, gamma-ray bursts, and compact object mergers that might contribute to the early epochs of the Universe with their strong ionizing radiation. However, this assumption remains mainly theoretical because individual spectroscopic observations of such objects have rarely been carried out below the metallicity of the Small Magellanic Cloud. Aims. Here we explore the predictions of the state-of-the-art theories of stellar evolution combined with those of stellar atmospheres about a certain type of metal-poor (0.02 Z(circle dot)) hot massive stars, the chemically homogeneously evolving stars that we call Transparent Wind Ultraviolet INtense (TWUIN) stars. Methods. We computed synthetic spectra corresponding to a broad range in masses (20 130 M-circle dot) and covering several evolutionary phases from the zero-age main-sequence up to the core helium-burning stage. We investigated the influence of mass loss and wind clumping on spectral appearance and classified the spectra according to the Morgan-Keenan (MK) system. Results. We find that TWUIN stars show almost no emission lines during most of their core hydrogen-burning lifetimes. Most metal lines are completely absent, including nitrogen. During their core helium-burning stage, lines switch to emission, and even some metal lines (oxygen and carbon, but still almost no nitrogen) are detected. Mass loss and clumping play a significant role in line formation in later evolutionary phases, particularly during core helium-burning. Most of our spectra are classified as an early-O type giant or supergiant, and we find Wolf-Rayet stars of type WO in the core helium-burning phase. Conclusions. An extremely hot, early-O type star observed in a low-metallicity galaxy could be the result of chemically homogeneous evolution and might therefore be the progenitor of a long-duration gamma-ray burst or a type Ic supernova. TWUIN stars may play an important role in reionizing the Universe because they are hot without showing prominent emission lines during most of their lifetime.
Background Small-sided games have been suggested as a viable alternative to conventional endurance training to enhance endurance performance in youth soccer players. This has important implications for long-term athlete development because it suggests that players can increase aerobic endurance through activities that closely resemble their sport of choice. Data Sources The data sources utilised were Google Scholar, PubMed and Microsoft Academic. Study Eligibility Criteria Studies were eligible for inclusion if interventions were carried out in male soccer players (aged < 18years) and compared the effects of small-sided games and conventional endurance training on aerobic endurance performance. We defined small-sided games as modified [soccer] games played on reduced pitch areas, often using adapted rules and involving a smaller number of players than traditional games. We defined conventional endurance training as continuous running or extensive interval training consisting of work durations>3min. Study Appraisal and Synthesis Methods The inverse-variance random-effects model for meta-analyses was used because it allocates a proportionate weight to trials based on the size of their individual standard errors and facilitates analysis whilst accounting for heterogeneity across studies. Effect sizes were represented by the standardised mean difference and presented alongside 95% confidence intervals. Results Seven studies were included in this meta-analysis. Both modes of training were effective in increasing endurance performance. Within-mode effect sizes were both of moderate magnitude [small-sided games: 0.82 (95% confidence interval 0.05, 1.60), Z=2.07 (p=0.04); conventional endurance training: 0.89 (95% confidence interval 0.06, 1.72), Z=2.10 (p=0.04)]. There were only trivial differences [0.04 (95% confidence interval -0.36, 0.43), Z=0.18 (p=0.86)] between the effects on aerobic endurance performance of small-sided games and conventional endurance training. Subgroup analyses showed mostly trivial differences between the training methods across key programming variables such as set duration (>= or < 4 min) and recovery period between sets (>= or< 3min). Programmes that were longer than 8 weeks favoured small-sided games [effect size=0.45 (95% confidence interval -0.12, 1.02), Z=1.54 (p=0.12)], with the opposite being true for conventional endurance training [effect size=-0.33 (95% confidence interval -0.79, 0.14), Z=1.39 (p=0.16)]. Programmes with more than 4 sets per session favoured small-sided games [effect size=0.53 (95% confidence interval -0.52, 1.58), Z=0.98 (p=0.33)] with only a trivial difference between those with 4, or fewer, sets [effect size=-0.13 (95% confidence interval -0.52, 0.26), Z=0.65 (p=0.52)]. Conclusions Small-sided games are as effective as conventional endurance training for increasing aerobic endurance performance in male youth soccer players. This is important for practitioners as it means that small-sided games can allow both endurance and skills training to be carried out simultaneously, thus providing a more efficient training stimulus. Small-sided games offer the same benefits as conventional endurance training with two sessions per week, with4 sets of 4 min of activity, interspersed with recovery periods of 3min, recommended in this population.
We explore the production and escape of ionizing photons in young galaxies by investigating the ultraviolet and optical emission-line properties of models of ionization-bounded and density-bounded H II regions, active-galactic-nucleus (AGN) narrow-line regions, and radiative shocks computed all using the same physically consistent description of element abundances and depletion on to dust grains down to very low metallicities. We compare these models with a reference sample of metal-poor star-forming galaxies and Lyman-continuum (LyC) leakers at various redshifts, which allows the simultaneous exploration of more spectral diagnostics than typically available at once for individual subsamples. We confirm that current single- and binary-star population synthesis models do not produce hard-enough radiation to account for the high-ionization emission of the most metal-poor galaxies. Introducing either an AGN or radiative-shock component brings models into agreement with observations. A published model including X-ray binaries is an attractive alternative to reproduce the observed rise in He II lambda 4686/H beta ratio with decreasing oxygen abundance in metal-poor star-forming galaxies, but not the high observed He II lambda 4686/H beta ratios of galaxies with large EW(H beta). A source of harder ionizing radiation appears to be required in these extreme objects, such as an AGN or radiative-shock component, perhaps linked to an initial-mass-function bias towards massive stars at low metallicity. This would also account for the surprisingly high [O I]/[O III] ratios of confirmed LyC leakers relative to ionization-bounded models. We find no simple by-eye diagnostic of the nature of ionizing sources and the escape of LyC photon, which require proper simultaneous fits of several lines to be discriminated against.
Biochar is being discussed as a soil amendment to improve soil fertility and mitigate climate change. While biochar interactions with soil microbial biota have been frequently studied, interactions with soil mesofauna are understudied. We here present an experiment in which we tested if the collembolan Folsomia candida I) can transport biochar particles, II) if yes, how far the particles are distributed within 10 days, and III) if it shows a preference among biochars made from different feedstocks, i.e. pine wood, pine bark and spelt husks. In general, biochar particles based on pine bark and pine wood were consistently distributed significantly more than those made of spelt husks, but all types were transported more than 4cm within 10 days. Additionally, we provide evidence that biochar particles can become readily attached to the cuticle of collembolans and hence be transported, potentially even over large distances. Our study shows that the soil mesofauna can indeed act as a vector for the transport of biochar particles and show clear preferences depending on the respective feedstock, which would need to be studied in more detail in the future.
Biochar is being discussed as a soil amendment to improve soil fertility and mitigate climate change. While biochar interactions with soil microbial biota have been frequently studied, interactions with soil mesofauna are understudied. We here present an experiment in which we tested if the collembolan Folsomia candida I) can transport biochar particles, II) if yes, how far the particles are distributed within 10 days, and III) if it shows a preference among biochars made from different feedstocks, i.e. pine wood, pine bark and spelt husks. In general, biochar particles based on pine bark and pine wood were consistently distributed significantly more than those made of spelt husks, but all types were transported more than 4cm within 10 days. Additionally, we provide evidence that biochar particles can become readily attached to the cuticle of collembolans and hence be transported, potentially even over large distances. Our study shows that the soil mesofauna can indeed act as a vector for the transport of biochar particles and show clear preferences depending on the respective feedstock, which would need to be studied in more detail in the future.
Obligate human pathogenic Neisseria gonorrhoeae are the second most frequent bacterial cause of sexually transmitted diseases. These bacteria invade different mucosal tissues and occasionally disseminate into the bloodstream. Invasion into epithelial cells requires the activation of host cell receptors by the formation of ceramide-rich platforms. Here, we investigated the role of sphingosine in the invasion and intracellular survival of gonococci. Sphingosine exhibited an anti-gonococcal activity in vitro. We used specific sphingosine analogs and click chemistry to visualize sphingosine in infected cells. Sphingosine localized to the membrane of intracellular gonococci. Inhibitor studies and the application of a sphingosine derivative indicated that increased sphingosine levels reduced the intracellular survival of gonococci. We demonstrate here, that sphingosine can target intracellular bacteria and may therefore exert a direct bactericidal effect inside cells.
Time-resolved crystallography reveals allosteric communication aligned with molecular breathing
(2019)
A comprehensive understanding of protein function demands correlating structure and dynamic changes. Using time-resolved serial synchrotron crystallography, we visualized half-of-the-sites reactivity and correlated molecular-breathing motions in the enzyme fluoroacetate dehalogenase. Eighteen time points from 30 milliseconds to 30 seconds cover four turnover cycles of the irreversible reaction. They reveal sequential substrate binding, covalent-intermediate formation, setup of a hydrolytic water molecule, and product release. Small structural changes of the protein mold and variations in the number and placement of water molecules accompany the various chemical steps of catalysis. Triggered by enzyme-ligand interactions, these repetitive changes in the protein framework’s dynamics and entropy constitute crucial components of the catalytic machinery.
Nowadays, structural health monitoring of critical infrastructures is considered as of primal importance especially for managing transport infrastructure however most current SHM methodologies are based on point-sensors that show various limitations relating to their spatial positioning capabilities, cost of development and measurement range. This publication describes the progress in the SENSKIN EC co-funded research project that is developing a dielectric-elastomer sensor, formed from a large highly extensible capacitance sensing membrane and is supported by an advanced micro-electronic circuitry, for monitoring transport infrastructure bridges. The sensor under development provides spatial measurements of strain in excess of 10%, while the sensing system is being designed to be easy to install, require low power in operation concepts, require simple signal processing, and have the ability to self-monitor and report. An appropriate wireless sensor network is also being designed and developed supported by local gateways for the required data collection and exploitation. SENSKIN also develops a Decision-Support-System (DSS) for proactive condition-based structural interventions under normal operating conditions and reactive emergency intervention following an extreme event. The latter is supported by a life-cycle-costing (LCC) and life-cycle-assessment (LCA) module responsible for the total internal and external costs for the identified bridge rehabilitation, analysis of options, yielding figures for the assessment of the economic implications of the bridge rehabilitation work and the environmental impacts of the bridge rehabilitation options and of the associated secondary effects respectively. The overall monitoring system will be evaluated and benchmarked on actual bridges of Egnatia Highway (Greece) and Bosporus Bridge (Turkey).
Background: The pathophysiology behind the subacute but persistent hypercoagulable state after traumatic brain injury (TBI) is poorly understood but contributes to morbidity induced by venous thromboembolism. Because platelets and their microvesicles have been hypothesized to play a role in post-traumatic hypercoagulability, administration of commonly used agents may ameliorate this coagulability. We hypothesized that utilization of aspirin, ketorolac, amitriptyline, unfractionated heparin, or enoxaparin would modulate the platelet aggregation response after TBI. Methods: Concussive TBI was induced by weight drop. Mice were then randomized to receive aspirin, ketorolac, amitriptyline, heparin, enoxaparin, or saline control at 2 and 8 h after TBI. Mice were sacrificed at 6 or 24 h after injury to determine coagulability by rotational thromboelastometry (ROTEM), platelet function testing with impedance aggregometry, and microvesicle enumeration. Platelet sphingolipid metabolites were analyzed by mass spectrometry. Results: ROTEM demonstrated increased platelet contribution to maximum clot firmness at 6 h after TBI in mice that received aspirin or amitriptyline, but this did not persist at 24 h. By contrast, adenosine diphosphate- and arachidonic acid-induced platelet aggregation at 6 h was significantly lower in mice receiving ketorolac, aspirin, and amitriptyline compared with mice receiving saline at 6 h after injury and only arachidonic acid-initiated platelet aggregation was decreased by aspirin at 24 h. There were no differences in microvesicle production at either time point. Platelet sphingosine-1-phosphate levels were decreased at 6 h in the group receiving amitriptyline and increased at 24 h along with platelet ceramide levels at 24 h in the amitriptyline group. Conclusion: After TBI, amitriptyline decreased platelet aggregability and increased contribution to clot in a manner similar to aspirin. The amitriptyline effects on platelet function and sphingolipid metabolites may represent a possible role of the acid sphingomyelinase in the hypercoagulability observed after injury. In addition, inhibition of platelet reactivity may be an underappreciated benefit of low molecular weight heparins, such as enoxaparin. (C) 2019 Elsevier Inc. All rights reserved.
Ventilator-associated pneumonia (VAP) is a major cause of morbidity and mortality in critically ill patients. Here, we employed the broad antibacterial effects of sphingosine to prevent VAP by developing a novel method of coating surfaces of endotracheal tubes with sphingosine and sphingosine analogs. Sphingosine and phytosphingosine coatings of endotracheal tubes prevent adherence and mediate killing of Pseudomonas aeruginosa, Acinetobacter baumannii, and Staphylococcus aureus, even in biofilms. Most importantly, sphingosine-coating of endotracheal tubes also prevented P. aeruginosa and S. aureus pneumonia in vivo. Coating of the tubes with sphingosine was stable, without obvious side effects on tracheal epithelial cells and did not induce inflammation. In summary, we describe a novel method to coat plastic surfaces and provide evidence for the application of sphingosine and phytosphingosine as novel antimicrobial coatings to prevent bacterial adherence and induce killing of pathogens on the surface of endotracheal tubes with potential to prevent biofilm formation and VAP.Key messagesNovel dip-coating method to coat plastic surfaces with lipids.Sphingosine and phytosphingosine as novel antimicrobial coatings on plastic surface.Sphingosine coatings of endotracheal tubes prevent bacterial adherence and biofilms.Sphingosine coatings of endotracheal tubes induce killing of pathogens.Sphingosine coatings of endotracheal tubes ventilator-associated pneumonia.
Local probes of the electronic ground state are essential for understanding hydrogen bonding in aqueous environments. When tuned to the dissociative core-excited state at the O1s pre-edge of water, resonant inelastic X-ray scattering back to the electronic ground state exhibits a long vibrational progression due to ultrafast nuclear dynamics. We show how the coherent evolution of the OH bonds around the core-excited oxygen provides access to high vibrational levels in liquid water. The OH bonds stretch into the long-range part of the potential energy curve, which makes the X-ray probe more sensitive than infra-red spectroscopy to the local environment. We exploit this property to effectively probe hydrogen bond strength via the distribution of intramolecular OH potentials derived from measurements. In contrast, the dynamical splitting in the spectral feature of the lowest valence-excited state arises from the short-range part of the OH potential curve and is rather insensitive to hydrogen bonding.
Biological responses to climate change have been widely documented across taxa and regions, but it remains unclear whether species are maintaining a good match between phenotype and environment, i.e. whether observed trait changes are adaptive. Here we reviewed 10,090 abstracts and extracted data from 71 studies reported in 58 relevant publications, to assess quantitatively whether phenotypic trait changes associated with climate change are adaptive in animals. A meta-analysis focussing on birds, the taxon best represented in our dataset, suggests that global warming has not systematically affected morphological traits, but has advanced phenological traits. We demonstrate that these advances are adaptive for some species, but imperfect as evidenced by the observed consistent selection for earlier timing. Application of a theoretical model indicates that the evolutionary load imposed by incomplete adaptive responses to ongoing climate change may already be threatening the persistence of species.
Background: Population-specificity of exploratory dietary patterns limits their generalizability in investigations with type 2 diabetes incidence.
Objective: The aim of this study was to derive country-specific exploratory dietary patterns, investigate their association with type 2 diabetes incidence, and replicate diabetes-associated dietary patterns in other countries.
Methods: Dietary intake data were used, assessed by country-specific questionnaires at baseline of 11,183 incident diabetes cases and 14,694 subcohort members (mean age 52.9 y) from 8 countries, nested within the European Prospective Investigation into Cancer and Nutrition study (mean follow-up time 6.9 y). Exploratory dietary patterns were derived by principal component analysis. HRs for incident type 2 diabetes were calculated by Prentice-weighted Cox proportional hazard regression models. Diabetes-associated dietary patterns were simplified or replicated to be applicable in other countries. A meta-analysis across all countries evaluated the generalizability of the diabetes-association.
Results: Two dietary patterns per country/UK-center, of which overall 3 dietary patterns were diabetes-associated, were identified. A risk-lowering French dietary pattern was not confirmed across other countries: pooled HRFrance per 1 SD: 1.00; 95% CI: 0.90, 1.10. Risk-increasing dietary patterns, derived in Spain and UK-Norfolk, were confirmed, but only the latter statistically significantly: HRSpain: 1.09; 95% CI: 0.97, 1.22 and HRUK-Norfolk: 1.12; 95% CI: 1.04, 1.20. Respectively, this dietary pattern was characterized by relatively high intakes of potatoes, processed meat, vegetable oils, sugar, cake and cookies, and tea. Conclusions: Only few country/center-specific dietary patterns (3 of 18) were statistically significantly associated with diabetes incidence in this multicountry European study population. One pattern, whose association with diabetes was confirmed across other countries, showed overlaps in the food groups potatoes and processed meat with identified diabetes-associated dietary patterns from other studies. The study demonstrates that replication of associations of exploratory patterns with health outcomes is feasible and a necessary step to overcome population-specificity in associations from such analyses.
Permafrost thaw subjects previously frozen organic carbon (OC) to microbial decomposition, generating the greenhouse gases (GHG) carbon dioxide (CO2) and methane (CH4) and fueling a positive climate feedback. Over one quarter of permafrost OC is stored in deep, ice-rich Pleistocene-aged yedoma permafrost deposits. We used a combination of anaerobic incubations, microbial sequencing, and ultrahigh-resolution mass spectrometry to show yedoma OC biolability increases with depth along a 12-m yedoma profile. In incubations at 3 degrees C and 13 degrees C, GHG production per unit OC at 12-versus 1.3-m depth was 4.6 and 20.5 times greater, respectively. Bacterial diversity decreased with depth and we detected methanogens at all our sampled depths, suggesting that in situ microbial communities are equipped to metabolize thawed OC into CH4. We concurrently observed an increase in the relative abundance of reduced, saturated OC compounds, which corresponded to high proportions of C mineralization and positively correlated with anaerobic GHG production potentials and higher proportions of OC being mineralized as CH4. Taking into account the higher global warming potential (GWP) of CH4 compared to CO2, thawed yedoma sediments in our study had 2 times higher GWP at 12-versus 9.0-m depth at 3 degrees C and 15 times higher GWP at 13 degrees C. Considering that yedoma is vulnerable to processes that thaw deep OC, our findings imply that it is important to account for this increasing GHG production and GWP with depth to better understand the disproportionate impact of yedoma on the magnitude of the permafrost carbon feedback.
Large earthquakes initiate chains of surface processes that last much longer than the brief moments of strong shaking. Most moderate‐ and large‐magnitude earthquakes trigger landslides, ranging from small failures in the soil cover to massive, devastating rock avalanches. Some landslides dam rivers and impound lakes, which can collapse days to centuries later, and flood mountain valleys for hundreds of kilometers downstream. Landslide deposits on slopes can remobilize during heavy rainfall and evolve into debris flows. Cracks and fractures can form and widen on mountain crests and flanks, promoting increased frequency of landslides that lasts for decades. More gradual impacts involve the flushing of excess debris downstream by rivers, which can generate bank erosion and floodplain accretion as well as channel avulsions that affect flooding frequency, settlements, ecosystems, and infrastructure. Ultimately, earthquake sequences and their geomorphic consequences alter mountain landscapes over both human and geologic time scales. Two recent events have attracted intense research into earthquake‐induced landslides and their consequences: the magnitude M 7.6 Chi‐Chi, Taiwan earthquake of 1999, and the M 7.9 Wenchuan, China earthquake of 2008. Using data and insights from these and several other earthquakes, we analyze how such events initiate processes that change mountain landscapes, highlight research gaps, and suggest pathways toward a more complete understanding of the seismic effects on the Earth's surface.
All-in-One "Schizophrenic" self-assembly of orthogonally tuned thermoresponsive diblock copolymers
(2019)
Smart, fully orthogonal switching was realized in a highly biocompatible diblock copolymer system with variable trigger-induced aqueous self-assembly. The polymers are composed of nonionic and zwitterionic blocks featuring lower and upper critical solution temperatures (LCSTs and UCSTs). In the system investigated, diblock copolymers from poly(N-isopropyl methacrylamide) (PNIPMAM) and a poly(sulfobetaine methacrylamide), systematic variation of the molar mass of the latter block allowed for shifting the UCST of the latter above the LCST of the PNIPMAM block in a salt-free condition. Thus, successive thermal switching results in "schizophrenic" micellization, in which the roles of the hydrophobic core block and the hydrophilic shell block are interchanged depending on the temperature. Furthermore, by virtue of the strong electrolyte-sensitivity of the zwitterionic polysulfobetaine block, we succeeded to shift its UCST below the LCST of the PNIPMAM block by adding small amounts of an electrolyte, thus inverting the pathway of switching. This superimposed orthogonal switching by electrolyte addition enabled us to control the switching scenarios between the two types of micelles (i) via an insoluble state, if the LCST-type cloud point is below the UCST-type cloud point, which is the case at low salt concentrations or (ii) via a molecularly dissolved state, if the LCST-type cloud point is above the UCST-type cloud point, which is the case at high salt concentrations. Systematic variation of the block lengths allowed for verifying the anticipated behavior and identifying the molecular architecture needed. The versatile and tunable self-assembly offers manifold opportunities, for example, for smart emulsifiers or for sophisticated carrier systems.
An understanding of the factors limiting the open-circuit voltage (V-oc) and related photon energy loss mechanisms is critical to increase the power conversion efficiency (PCE) of small-molecule organic solar cells (OSCs), especially those with near-infrared (NIR) absorbers. In this work, two NIR boron dipyrromethene (BODIPY) molecules are characterized for application in planar (PHJ) and bulk (BHJ) heterojunction OSCs. When two H atoms are substituted by F atoms on the peripheral phenyl rings of the molecules, the molecular aggregation type in the thin film changes from the H-type to J-type. For PHJ devices, the nonradiative voltage loss of 0.35 V in the J-aggregated BODIPY is lower than that of 0.49 V in the H-aggregated device. In BHJ devices with a nonradiative voltage loss of 0.35 V, a PCE of 5.5% is achieved with an external quantum efficiency (EQE) maximum of 68% at 700 nm.
Intermolecular charge-transfer states at the interface between electron donating (D) and accepting (A) materials are crucial for the operation of organic solar cells but can also be exploited for organic light-emitting diodes(1,2). Non-radiative charge-transfer state decay is dominant in state-of-the-art D-A-based organic solar cells and is responsible for large voltage losses and relatively low power-conversion efficiencies as well as electroluminescence external quantum yields in the 0.01-0.0001% range(3,4). In contrast, the electroluminescence external quantum yield reaches up to 16% in D-A-based organic light-emitting diodes(5-7). Here, we show that proper control of charge-transfer state properties allows simultaneous occurrence of a high photovoltaic and emission quantum yield within a single, visible-light-emitting D-A system. This leads to ultralow-emission turn-on voltages as well as significantly reduced voltage losses upon solar illumination. These results unify the description of the electro-optical properties of charge-transfer states in organic optoelectronic devices and foster the use of organic D-A blends in energy conversion applications involving visible and ultraviolet photons(8-11).
Purpose: Postoperative cognitive dysfunction (POCD) appears in up to 30% of patients suffering from postoperative delirium (POD). Both are associated with higher mortality and postoperative complications, prolonged hospital stays, and increased costs. Multi-modal models with pre-admission risk reduction counselling, perioperative monitoring, and training of multidisciplinary patient care providers have been shown to decrease the prevalence of both. The aim of our study is to understand how far those measures are known and implemented in routine care and to detect potential gaps in the current practice regarding risk communication and information flow between involved caregivers for patients at risk for POD/POCD. Patients and Methods: As part of a multicenter study, seven semi-structured focus group (FG) discussions with nurses and physicians from tertiary care hospitals (surgery, anesthesiology, and orthopedics, n=31) and general practitioners (GPs) in private practice (n=7) were performed. Transcribed discussions were analyzed using qualitative content analysis. Results: POD is present above all in the daily work of nurses, whereas physicians do not perceive it as a relevant problem. Physicians report that no regular risk assessment or risk communication was performed prior to elective surgery. Information about POD often gets lost during hand-offs and is not regularly reported in discharge letters. Thus, persisting cognitive dysfunction is often missed. The importance of standardized documentation and continuous education concerning risks, screening, and treatment was emphasized. The often-suggested pre-OP medication adjustment was seen as less important; in contrast, avoiding withdrawal was regarded as far more important. Conclusion: Altogether, it seems that standards and available best practice concepts are rarely implemented. In contrast to physicians, nurses are highly aware of delirium and ask for standardized procedures and more responsibility. Therefore, raising awareness regarding risks, screening tools, and effective preventive measures for POD/POCD seems an urgent goal. Nurses should have a central role in coordination and care of POD to prevent the risk for POCD.
Fungi are an important component of microbial communities and are well known for their ability to decompose refractory, highly polymeric organic matter. In soils and aquatic systems, fungi play an important role in carbon processing, however, their diversity, community structure and function as well as ecological role, particularly in groundwater, are poorly studied. The aim of this study was to examine the fungal community composition, diversity and function in groundwater from 16 boreholes located in the vicinity of two lakes in NE Germany that are characterized by contrasting trophic status. The analysis of 28S rRNA gene sequences amplified from the groundwater revealed high fungal diversity arid clear differences in community structure between the aquifers. Most sequences were assigned to Ascomycota and Basidiomycota, but members of Chytridiomycota, Cryptomycota, Zygomycota, Blastocladiomycota, Glomeromycota and Neocallimastigomycota were also detected. In addition, 27 species of fungi were successfully isolated from the groundwater samples and tested for their ability to decompose complex organic polymers - the predominant carbon source in the groundwater. Most isolates showed positive activities for at least one of the tested polymer types, with three strains, belonging to the genera Gibberella, Isaria and Cadophora, able to decompose all tested substrates. Our results highlight the high diversity of fungi in groundwater, and point to their important ecological role in breaking down highly polymeric organic matter in these isolated microbial habitats. (C) 2019 Elsevier Ltd and British Mycological Society. All rights reserved.
Global change has complex eco-evolutionary consequences for organisms and ecosystems, but related concepts (e.g., novel ecosystems) do not cover their full range. Here we propose an umbrella concept of "ecological novelty" comprising (1) a site-specific and (2) an organism-centered, eco-evolutionary perspective. Under this umbrella, complementary options for studying and communicating effects of global change on organisms, ecosystems, and landscapes can be included in a toolbox. This allows researchers to address ecological novelty from different perspectives, e.g., by defining it based on (a) categorical or continuous measures, (b) reference conditions related to sites or organisms, and (c) types of human activities. We suggest striving for a descriptive, non-normative usage of the term "ecological novelty" in science. Normative evaluations and decisions about conservation policies or management are important, but require additional societal processes and engagement with multiple stakeholders.
Objectives
The aims of this study were to investigate the effects of a six-week in-season period of soccer training and games (congested period) on plasma volume variations (PV), hematological parameters, and physical fitness in elite players. In addition, we analyzed relationships between training load, hematological parameters and players’ physical fitness.
Methods
Eighteen elite players were evaluated before (T1) and after (T2) a six-week in-season period interspersed with 10 soccer matches. At T1 and T2, players performed the Yo-Yo intermittent recovery test level 1 (YYIR1), the repeated shuttle sprint ability test (RSSA), the countermovement jump test (CMJ), and the squat jump test (SJ). In addition, PV and hematological parameters (erythrocytes [M/mm3], hematocrit [%], hemoglobin [g/dl], mean corpuscular volume [fl], mean corpuscular hemoglobin content [pg], and mean hemoglobin concentration [%]) were assessed. Daily ratings of perceived exertion (RPE) were monitored in order to quantify the internal training load.
Results
From T1 to T2, significant performance declines were found for the YYIR1 (p<0.001, effect size [ES] = 0.5), RSSA (p<0.01, ES = 0.6) and SJ tests (p< 0.046, ES = 0.7). However, no significant changes were found for the CMJ (p = 0.86, ES = 0.1). Post-exercise, RSSA blood lactate (p<0.012, ES = 0.2) and PV (p<0.01, ES = 0.7) increased significantly from T1 to T2. A significant decrease was found from T1 to T2 for the erythrocyte value (p<0.002, ES = 0.5) and the hemoglobin concentration (p<0.018, ES = 0.8). The hematocrit percentage rate was also significantly lower (p<0.001, ES = 0.6) at T2. The mean corpuscular volume, mean corpuscular hemoglobin content and the mean hemoglobin content values were not statistically different from T1 to T2. No significant relationships were detected between training load parameters and percentage changes of hematological parameters. However, a significant relationship was observed between training load and changes in RSSA performance (r = -0.60; p<0.003).
Conclusions
An intensive period of “congested match play” over 6 weeks significantly compromised players’ physical fitness. These changes were not related to hematological parameters, even though significant alterations were detected for selected measures.
Objectives
The aims of this study were to investigate the effects of a six-week in-season period of soccer training and games (congested period) on plasma volume variations (PV), hematological parameters, and physical fitness in elite players. In addition, we analyzed relationships between training load, hematological parameters and players’ physical fitness.
Methods
Eighteen elite players were evaluated before (T1) and after (T2) a six-week in-season period interspersed with 10 soccer matches. At T1 and T2, players performed the Yo-Yo intermittent recovery test level 1 (YYIR1), the repeated shuttle sprint ability test (RSSA), the countermovement jump test (CMJ), and the squat jump test (SJ). In addition, PV and hematological parameters (erythrocytes [M/mm3], hematocrit [%], hemoglobin [g/dl], mean corpuscular volume [fl], mean corpuscular hemoglobin content [pg], and mean hemoglobin concentration [%]) were assessed. Daily ratings of perceived exertion (RPE) were monitored in order to quantify the internal training load.
Results
From T1 to T2, significant performance declines were found for the YYIR1 (p<0.001, effect size [ES] = 0.5), RSSA (p<0.01, ES = 0.6) and SJ tests (p< 0.046, ES = 0.7). However, no significant changes were found for the CMJ (p = 0.86, ES = 0.1). Post-exercise, RSSA blood lactate (p<0.012, ES = 0.2) and PV (p<0.01, ES = 0.7) increased significantly from T1 to T2. A significant decrease was found from T1 to T2 for the erythrocyte value (p<0.002, ES = 0.5) and the hemoglobin concentration (p<0.018, ES = 0.8). The hematocrit percentage rate was also significantly lower (p<0.001, ES = 0.6) at T2. The mean corpuscular volume, mean corpuscular hemoglobin content and the mean hemoglobin content values were not statistically different from T1 to T2. No significant relationships were detected between training load parameters and percentage changes of hematological parameters. However, a significant relationship was observed between training load and changes in RSSA performance (r = -0.60; p<0.003).
Conclusions
An intensive period of “congested match play” over 6 weeks significantly compromised players’ physical fitness. These changes were not related to hematological parameters, even though significant alterations were detected for selected measures.
The fall into the Oligocene icehouse is marked by a steady decline in global temperature with punctuated cooling at the Eocene-Oligocene transition, both of which are well documented in the marine realm. However, the chronology and mechanisms of cooling on land remain unclear. Here, we use clumped isotope thermometry on northeastern Tibetan continental carbonates to reconstruct a detailed Paleogene surface temperature record for the Asian continental interior, and correlate this to an enhanced pollen data set. Our results show two successive dramatic (>9 degrees C) temperature drops, at 37 Ma and at 33.5 Ma. These large-magnitude decreases in continental temperatures can only be explained by a combination of both regional cooling and shifts of the rainy season to cooler months, which we interpret to reflect a decline of monsoonal intensity. Our results suggest that the response of Asian surface temperatures and monsoonal rainfall to the steady decline of atmospheric CO2 and global temperature through the late Eocene was nonlinear and occurred in two steps separated by a period of climatic instability. Our results support the onset of the Antarctic Circumpolar Current coeval to the Oligocene isotope event 1 (Oi-1) glaciation at 33.5 Ma, reshaping the distribution of surface heat worldwide; however, the origin of the 37 Ma cooling event remains less clear.
Ring current electrons (1–100 keV) have received significant attention in recent decades, but many questions regarding their major transport and loss mechanisms remain open. In this study, we use the four‐dimensional Versatile Electron Radiation Belt code to model the enhancement of phase space density that occurred during the 17 March 2013 storm. Our model includes global convection, radial diffusion, and scattering into the Earth's atmosphere driven by whistler‐mode hiss and chorus waves. We study the sensitivity of the model to the boundary conditions, global electric field, the electric field associated with subauroral polarization streams, electron loss rates, and radial diffusion coefficients. The results of the code are almost insensitive to the model parameters above 4.5 RERE, which indicates that the general dynamics of the electrons between 4.5 RE and the geostationary orbit can be explained by global convection. We found that the major discrepancies between the model and data can stem from the inaccurate electric field model and uncertainties in lifetimes. We show that additional mechanisms that are responsible for radial transport are required to explain the dynamics of ≥40‐keV electrons, and the inclusion of the radial diffusion rates that are typically assumed in radiation belt studies leads to a better agreement with the data. The overall effect of subauroral polarization streams on the electron phase space density profiles seems to be smaller than the uncertainties in other input parameters. This study is an initial step toward understanding the dynamics of these particles inside the geostationary orbit.
Plain Language Summary Radiation belts of the Earth, which are the zones of charged energetic particles trapped by the geomagnetic field, comprise enormous and dynamic systems. While the inner radiation belt, composed mainly of high-energy protons, is relatively stable, the outer belt, filled with energetic electrons, is highly variable and depends substantially on solar activity. Hence, extended reliable observations and the improved models of the electron intensities in the outer belt depending on solar wind parameters are necessary for prediction of their dynamics. The Cluster mission has been measuring electron flux intensities in the radiation belts since its launch in 2000, thus providing a huge dataset that can be used for radiation belts analysis. Using 16 years of electron measurements by the Cluster mission corrected for background contamination, we derived a uniform linear-logarithmic dependence of electron fluxes in the outer belt on the solar wind dynamic pressure.
Marine snow aggregates represent heterogeneous agglomerates of dead and living organic matter. Composition is decisive for their sinking rates, and thereby for carbon flux to the deep sea. For oligotrophic oceans, information on aggregate composition is particularly sparse. To address this, the taxonomic composition of aggregates collected from the subtropical and oligotrophic Sargasso Sea (Atlantic Ocean) was characterized by 16S and 18S rRNA gene sequencing. Taxonomy assignment was aided by a collection of the contemporary plankton community consisting of 75 morphologically and genetically identified plankton specimens. The diverse rRNA gene reads of marine snow aggregates, not considering Trichodesmium puffs, were dominated by copepods (52%), cnidarians (21%), radiolarians (11%), and alveolates (8%), with sporadic contributions by cyanobacteria, suggesting a different aggregate composition than in eutrophic regions. Composition linked significantly with sampling location but not to any measured environmental parameters or plankton biomass composition. Nevertheless, indicator and network analyses identified key roles of a few rare taxa. This points to complex regulation of aggregate composition, conceivably affected by the environment and plankton characteristics. The extent to which this has implications for particle densities, and consequently for sinking rates and carbon sequestration in oligotrophic waters, needs further interrogation.