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Macrocycles based on L-cystine were synthesized by ring-closing metathesis (RCM) and subsequently polymerized by entropy-driven ring-opening metathesis polymerization (ED-ROMP). Monomer conversion reached similar to 80% in equilibrium and the produced poly (ester-amine-disulfide-alkene)s exhibited apparent molar masses (M-w(app)) of up to 80 kDa and dispersities (D) of similar to 2. The polymers can be further functionalized with acid anhydrides and degraded by reductive cleavage of the main-chain disulfide.
I can see clearly now
(2017)
Past research has revealed that narcissists lack forgiveness. However, little is known about factors that might either buffer or, more critically, enhance the link between narcissism and lack of forgiveness. To address this gap in the literature, the present studies focused on the moderating role of clarity of transgression-related motivations. In an original and a replication study (Ns = 509 and 532, respectively), participants rated their levels of narcissistic admiration and rivalry and recalled a personal episode in which someone had hurt them. Subsequently, participants reported on their lack of forgiveness toward their transgressor. Response speed to these ratings served as an indirect clarity measure, with faster responses indicating greater clarity. In both studies, narcissistic rivalry (but not admiration) was positively related to lack of forgiveness and this relationship was stronger among individuals who were clear about their transgression-related motivations. Results inform our understanding of socio-emotional factors that contribute to narcissists' lack of forgiveness following interpersonal hurt.
Fragmentation of landscapes creates a transition zone in between natural habitats or different kinds of land use. In forested and agricultural landscapes with transition zones, microclimate and matter cycling are markedly altered. This probably accelerates and is intensified by global warming. However, there is no consensus on defining transition zones and quantifying relevant variables for microclimate and matter cycling across disciplines. This article is an attempt to a) revise definitions and offer a framework for quantitative ecologists, b) review the literature on microclimate and matter cycling in transition zones and c) summarise this information using meta-analysis to better understand bio-geochemical and bio-geophysical processes and their spatial extent in transition zones. We expect altered conditions in soils of transition zones to be 10-20 m with a maximum of 50 m, and 25-50 m for above-ground space with a maximum of 125 m.
Near edge X-ray absorption fine structure (NEXAFS) simulations based on the conventional configuration interaction singles (CIS) lead to excitation energies, which are systematically blue shifted. Using a (restricted) open shell core hole reference instead of the Hartree Fock (HF) ground state orbitals improves (Decleva et al., Chem. Phys., 1992, 168, 51) excitation energies and the shape of the spectra significantly. In this work, we systematically vary the underlying SCF approaches, that is, based on HF or density functional theory, to identify best suited reference orbitals using a series of small test molecules. We compare the energies of the K edges and NEXAFS spectra to experimental data. The main improvement compared to conventional CIS, that is, using HF ground state orbitals, is due to the electrostatic influence of the core hole. Different SCF approaches, density functionals, or the use of fractional occupations lead only to comparably small changes. Furthermore, to account for bigger systems, we adapt the core-valence separation for our approach. We demonstrate that the good quality of the spectrum is not influenced by this approximation when used together with the non-separated ground state wave function. Simultaneously, the computational demands are reduced remarkably. (C) 2016 Wiley Periodicals, Inc.
Complexation with dissolved humic matter can be crucial in controlling the mobility of toxic or radioactive contaminant metals. For speciation and transport modelling, a dynamic equilibrium process is commonly assumed, where association and dissociation run permanently. This is, however, questionable in view of reported observations of a growing resistance to dissociation over time. In this study, the isotope exchange principle was employed to gain direct insight into the dynamics of the complexation equilibrium, including kinetic inertisation phenomena. Terbium(III), an analogue of trivalent actinides, was used as a representative of higher-valent metals. Isotherms of binding to (flocculated) humic acid, determined by means of Tb-160 as a radiotracer, were found to be identical regardless of whether the radioisotope was introduced together with the bulk of stable Tb-159 or subsequently after pre-equilibration for up to 3 months. Consequently, there is a permanent exchange of free and humic-bound Tb since all available binding sites are occupied in the plateau region of the isotherm. The existence of a dynamic equilibrium was thus evidenced. There was no indication of an inertisation under these experimental conditions. If the small amount of Tb-160 was introduced prior to saturation with Tb-159, the expected partial desorption of Tb-160 occurred at much lower rates than observed for the equilibration process in the reverse procedure. In addition, the rates decreased with time of pre-equilibration. Inertisation phenomena are thus confined to the stronger sites of humic molecules (occupied at low metal concentrations). Analysing the time-dependent course of isotope exchange according to first-order kinetics indicated that up to 3 years are needed to attain equilibrium. Since, however, metal-humic interaction remains reversible, exchange of metals between humic carriers and mineral surfaces cannot be neglected on the long time scale to be considered in predictive transport models.
We present a high-resolution study of the upper mantle structure of Central Europe, including the western part of the East European Platform, based on S-receiver functions of 345 stations. A distinct contrast is found between Phanerozoic Europe and the East European Craton across the Trans-European Suture Zone. To the west, a pronounced velocity reduction with depth interpreted as lithosphere-asthenosphere boundary (LAB) is found at an average depth of 90 km. Beneath the craton, no strong and continuous LAB conversion is observed. Instead we find a distinct velocity reduction within the lithosphere, at 80-120 km depth. This mid-lithospheric discontinuity (MLD) is attributed to a compositional boundary between depleted and more fertile lithosphere created by late Proterozoic metasomatism. A potential LAB phase beneath the craton is very weak and varies in depth between 180 and 250 km, consistent with a reduced velocity contrast between the lower lithosphere and the asthenosphere. Within the Trans-European Suture Zone, lithospheric structure is characterized by strong heterogeneity. A dipping or step-wise increase to LAB depth of 150 km is imaged from Phanerozoic Europe to 20-22 degrees E, whereas no direct connection to the cratonic LAB or MLD to the east is apparent. At larger depths, a positive conversion associated with the lower boundary of the asthenosphere is imaged at 210-250 km depth beneath Phanerozoic Europe, continuing down to 300 km depth beneath the craton. Conversions from both 410 km and 660 km discontinuities are found at their nominal depth beneath Phanerozoic Europe, and the discontinuity at 410 km depth can also be traced into the craton. A potential negative conversion on top of the 410 km discontinuity found in migrated images is analyzed by modeling and attributed to interference with other converted phases.
The Kenya rift revisited
(2017)
We present three-dimensional (3-D) models that describe the present-day thermal and rheological state of the lithosphere of the greater Kenya rift region aiming at a better understanding of the rift evolution, with a particular focus on plume-lithosphere interactions. The key methodology applied is the 3-D integration of diverse geological and geophysical observations using gravity modelling. Accordingly, the resulting lithospheric-scale 3-D density model is consistent with (i) reviewed descriptions of lithological variations in the sedimentary and volcanic cover, (ii) known trends in crust and mantle seismic velocities as revealed by seismic and seismological data and (iii) the observed gravity field. This data-based model is the first to image a 3-D density configuration of the crystalline crust for the entire region of Kenya and northern Tanzania. An upper and a basal crustal layer are differentiated, each composed of several domains of different average densities. We interpret these domains to trace back to the Precambrian terrane amalgamation associated with the East African Orogeny and to magmatic processes during Mesozoic and Cenozoic rifting phases. In combination with seismic velocities, the densities of these crustal domains indicate compositional differences. The derived lithological trends have been used to parameterise steady-state thermal and rheological models. These models indicate that crustal and mantle temperatures decrease from the Kenya rift in the west to eastern Kenya, while the integrated strength of the lithosphere increases. Thereby, the detailed strength configuration appears strongly controlled by the complex inherited crustal structure, which may have been decisive for the onset, localisation and propagation of rifting.
Moderate to large earthquakes can increase the amount of water feeding stream flows, mobilizing excess water from deep groundwater, shallow groundwater, or the vadose zone. Here we examine the regional pattern of streamflow response to the Maule M8.8 earthquake across Chile's diverse topographic and hydro-climatic gradients. We combine streamflow analyses with groundwater flow modeling and a random forest classifier, and find that, after the earthquake, at least 85 streams had a change in flow. Discharge mostly increased () shortly after the earthquake, liberating an excess water volume of >1.1 km3, which is the largest ever reported following an earthquake. Several catchments had increased discharge of >50 mm, locally exceeding seasonal streamflow discharge under undisturbed conditions. Our modeling results favor enhanced vertical permeability induced by dynamic strain as the most probable process explaining the observed changes at the regional scale. Supporting this interpretation, our random forest classification identifies peak ground velocity and elevation extremes as most important for predicting streamflow response. Given the mean recurrence interval of ∼25 yr for >M8.0 earthquakes along the Peru–Chile Trench, our observations highlight the role of earthquakes in the regional water cycle, especially in arid environments.
Temporal and spatial stability of the vegetation climate relationship is a basic ecological assumption for pollen-based quantitative inferences of past climate change and for predicting future vegetation. We explore this assumption for the Holocene in eastern continental Asia (China, Mongolia). Boosted regression trees (BRT) between fossil pollen taxa percentages (Abies, Artemisia, Betula, Chenopodiaceae, Cyperaceae, Ephedra, Picea, Pinus, Poaceae and Quercus) and climate model outputs of mean annual precipitation (P-ann) and mean temperature of the warmest month (Mt(wa)) for 9 and 6 ka (ka = thousand years before present) were set up and results compared to those obtained from relating modern pollen to modern climate. Overall, our results reveal only slight temporal differences in the pollen climate relationships. Our analyses suggest that the importance of P-ann compared with Mt(wa) for taxa distribution is higher today than it was at 6 ka and 9 ka. In particular, the relevance of P-ann for Picea and Pinus increases and has become the main determinant. This change in the climate tree pollen relationship parallels a widespread tree pollen decrease in north-central China and the eastern Tibetan Plateau. We assume that this is at least partly related to vegetation climate disequilibrium originating from human impact. Increased atmospheric CO2 concentration may have permitted the expansion of moisture-loving herb taxa (Cyperaceae and Poaceae) during the late Holocene into arid/semi-arid areas. We furthermore find that the pollen climate relationship between north-central China and the eastern Tibetan Plateau is generally similar, but that regional differences are larger than temporal differences. In summary, vegetation climate relationships in China are generally stable in space and time, and pollen-based climate reconstructions can be applied to the Holocene. Regional differences imply the calibration-set should be restricted spatially.
Intensive land use is a major cause of biodiversity loss, but most studies comparing the response of multiple taxa rely on simple diversity measures while analyses of other community attributes are only recently gaining attention. Species-abundance distributions (SADs) are a community attribute that can be used to study changes in the overall abundance structure of species groups, and whether these changes are driven by abundant or rare species. We evaluated the effect of grassland management intensity for three land-use modes (fertilization, mowing, grazing) and their combination on species richness and SADs for three belowground (arbuscular mycorrhizal fungi, prokaryotes and insect larvae) and seven aboveground groups (vascular plants, bryophytes and lichens; arthropod herbivores; arthropod pollinators; bats and birds). Three descriptors of SADs were evaluated: general shape (abundance decay rate), proportion of rare species (rarity) and proportional abundance of the commonest species (dominance). Across groups, taxonomic richness was largely unaffected by land-use intensity and only decreased with increasing mowing intensity. Of the three SAD descriptors, abundance decay rate became steeper with increasing combined land-use intensity across groups. This reflected a decrease in rarity among plants, herbivores and vertebrates. Effects of fertilization on the three descriptors were similar to the combined land-use intensity effects. Mowing intensity only affected the SAD descriptors of insect larvae and vertebrates, while grazing intensity produced a range of effects on different descriptors in distinct groups. Overall, belowground groups had more even abundance distribtitions than aboveground groups. Strong differences among aboveground groups and between above- and belowground groups indicate that no single taxonomic group can serve as an indicator for effects in other groups. In the past, the use of SADs has been hampered by concerns over theoretical models underlying specific forms of SADs. Our study shows that SAD descriptors that are not connected to a particular model are suitable to assess the effect of land use on community structure.