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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.
Low thermal conductivity boulder with high porosity identified on C-type asteroid (162173) Ryugu
(2019)
C-type asteroids are among the most pristine objects in the Solar System, but little is known about their interior structure and surface properties. Telescopic thermal infrared observations have so far been interpreted in terms of a regolith-covered surface with low thermal conductivity and particle sizes in the centimetre range. This includes observations of C-type asteroid (162173) Ryugu1,2,3. However, on arrival of the Hayabusa2 spacecraft at Ryugu, a regolith cover of sand- to pebble-sized particles was found to be absent4,5 (R.J. et al., manuscript in preparation). Rather, the surface is largely covered by cobbles and boulders, seemingly incompatible with the remote-sensing infrared observations. Here we report on in situ thermal infrared observations of a boulder on the C-type asteroid Ryugu. We found that the boulder’s thermal inertia was much lower than anticipated based on laboratory measurements of meteorites, and that a surface covered by such low-conductivity boulders would be consistent with remote-sensing observations. Our results furthermore indicate high boulder porosities as well as a low tensile strength in the few hundred kilopascal range. The predicted low tensile strength confirms the suspected observational bias6 in our meteorite collections, as such asteroidal material would be too frail to survive atmospheric entry7
Low thermal conductivity boulder with high porosity identified on C-type asteroid (162173) Ryugu
(2019)
C-type asteroids are among the most pristine objects in the Solar System, but little is known about their interior structure and surface properties. Telescopic thermal infrared observations have so far been interpreted in terms of a regolith-covered surface with low thermal conductivity and particle sizes in the centimetre range. This includes observations of C-type asteroid (162173) Ryugu1,2,3. However, on arrival of the Hayabusa2 spacecraft at Ryugu, a regolith cover of sand- to pebble-sized particles was found to be absent4,5 (R.J. et al., manuscript in preparation). Rather, the surface is largely covered by cobbles and boulders, seemingly incompatible with the remote-sensing infrared observations. Here we report on in situ thermal infrared observations of a boulder on the C-type asteroid Ryugu. We found that the boulder’s thermal inertia was much lower than anticipated based on laboratory measurements of meteorites, and that a surface covered by such low-conductivity boulders would be consistent with remote-sensing observations. Our results furthermore indicate high boulder porosities as well as a low tensile strength in the few hundred kilopascal range. The predicted low tensile strength confirms the suspected observational bias6 in our meteorite collections, as such asteroidal material would be too frail to survive atmospheric entry7.
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.
Being at the western fringe of Europe, Iberia had a peculiar prehistory and a complex pattern of Neolithization. A few studies, all based on modern populations, reported the presence of DNA of likely African origin in this region, generally concluding it was the result of recent gene flow, probably during the Islamic period. Here, we provide evidence of much older gene flow from Africa to Iberia by sequencing whole genomes from four human remains from northern Portugal and southern Spain dated around 4000 years BP (from the Middle Neolithic to the Bronze Age). We found one of them to carry an unequivocal sub-Saharan mitogenome of most probably West or West-Central African origin, to our knowledge never reported before in prehistoric remains outside Africa. Our analyses of ancient nuclear genomes show small but significant levels of sub-Saharan African affinity in several ancient Iberian samples, which indicates that what we detected was not an occasional individual phenomenon, but an admixture event recognizable at the population level. We interpret this result as evidence of an early migration process from Africa into the Iberian Peninsula through a western route, possibly across the Strait of Gibraltar.
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.
The early Cretaceous Koegel Fontein intrusive complex is situated near the Atlantic coast in South Africa, about 350 km northwest of Cape Town. The complex comprises felsic units of granite and syenite with compositionally related dykes, and a single intrusive plug of diorite. Existing zircon U-Pb ages of 144 +/- 2 Ma for the syenite and 133.9 +/- 1.3 Ma for the granite suggest that the emplacement of the complex took place over a period of about 10 My. This study provides additional and independent ages of the Koegel Fontein complex by Ar-40/Ar-39 dating to confirm the onset and duration of magmatism and better define the sequence of igneous units that comprise it. New laser step-heating Ar-40/Ar-3(9) ages on plagioclase and biotite from the main intrusive units in the complex are presented here, including samples previously dated by U-Pb dating. The Ar-40/Ar-39 ages for the granite and syenite units (131.1 +/- 0.9 Ma and 143.3 +/- 0.9, respectively) are in good agreement with the zircon U-Pb ages. Other units not previously dated include the Rooivleitjie alkaline granite (150.7 +/- 0.6 Ma), two quartz-porphyry dykes (143.0 +/- 0.9 and 139.4 +/- 1.7 Ma) and the Zout Rivier diorite plug (133.0 +/- 1.0 Ma). The new results confirm an early onset of magmatism at Koegel Fontein relative to that of the Etendeka Province some 1000 km to the north, which is consistent with the regional south-to-north propagation of South Atlantic rifting. The youngest Ar-40/Ar-3(9) ages at Koegel Fontein (134 to 131 Ma, Rietpoort Granite and 133 Ma, Zout Rivier diorite) correspond to the age of the first magnetic seafloor-spreading anomaly offshore, and we suggest that the longevity of Koegel Fontein magmatism relates to a superposition of pre-drift magmatism onshore and spreading-related magmatism as continental separation began.
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.