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Institute
- Institut für Geowissenschaften (314) (remove)
The effects of varying LiPF6 salt concentration and the presence of lithium bis(oxalate)borate additive on the electronic structure of commonly used lithium-ion battery electrolyte solvents (ethylene carbonate-dimethyl carbonate and propylene carbonate) have been investigated. X-ray Raman scattering spectroscopy (a non-resonant inelastic X-ray scattering method) was utilized together with a closed-circle flow cell. Carbon and oxygen K-edges provide characteristic information on the electronic structure of the electrolyte solutions, which are sensitive to local chemistry. Higher Li+ ion concentration in the solvent manifests itself as a blue-shift of both the pi* feature in the carbon edge and the carbonyl pi* feature in the oxygen edge. While these oxygen K-edge results agree with previous soft X-ray absorption studies on LiBF4 salt concentration in propylene carbonate, carbon K-edge spectra reveal a shift in energy, which can be explained with differing ionic conductivities of the electrolyte solutions.
An overview is given on the current state of X-ray absorption measurements on silicate melts and glasses. The challenges, limitations, and achievements of analyzing X-ray absorption spectra measured in liquids to determine structural properties of major and minor elements in magmas are described, with particular focus on describing non-Gaussian pair distribution functions in highly disordered glasses and melts, measured at in situ conditions. This includes a discussion on the progress of combining experiments with data from molecular dynamics simulations. For the measurements at conditions of the deep Earth, various experimental approaches and necessities are discussed and two examples are described in more detail. Finally, the achievements and prospects are presented for measuring X-ray absorption spectra indirectly by X-ray Raman scattering.
Woodlands and steppes
(2018)
Based on fossil organism remains including plant macrofossils, charcoal, pollen, and invertebrates preserved in syngenetic deposits of the Batagay permafrost sequence in the Siberian Yana Highlands, we reconstructed the environmental history during marine isotope stages (MIS) 6 to 2. Two fossil assemblages, exceptionally rich in plant remains, allowed for a detailed description of the palaeo-vegetation during two climate extremes of the Late Pleistocene, the onset of the last glacial maximum (LGM) and the last interglacial. In addition, altogether 41 assemblages were used to outline the vegetation history since the penultimate cold stage of MIS 6. Accordingly, meadow steppes analogue to modern communities of the phytosociological order Festucetalia lenensis formed the primary vegetation during the Saalian and Weichselian cold stages. Cold-resistant tundra-steppe communities (Carici rupestris-Kobresietea bellardii) as they occur above the treeline today were, in contrast to more northern locations, mostly lacking. During the last interglacial, open coniferous woodland similar to modern larch taiga was the primary vegetation at the site. Abundant charcoal indicates wildfire events during the last interglacial. Zoogenic disturbances of the local vegetation were indicated by the presence of ruderal plants, especially by abundant Urtica dioica, suggesting that the area was an interglacial refugium for large herbivores. Meadow steppes, which formed the primary vegetation during cold stages and provided potentially suitable pastures for herbivores, were a significant constituent of the plant cover in the Yana Highlands also under the full warm stage conditions of the last interglacial. Consequently, meadow steppes occurred in the Yana Highlands during the entire investigated timespan from MIS 6 to MIS 2 documenting a remarkable environmental stability. Thus, the proportion of meadow steppe vegetation merely shifted in response to the respectively prevailing climatic conditions. Their persistence indicates low precipitation and a relatively warm growing season throughout and beyond the late Pleistocene. The studied fossil record also proves that modern steppe occurrences in the Yana Highlands did not establish as late as in the Holocene but instead are relicts of a formerly continuous steppe belt extending from Central Siberia to Northeast Yakutia during the Pleistocene. The persistence of plants and invertebrates characteristic of meadow steppe vegetation in interior Yakutia throughout the late Quaternary indicates climatic continuity and documents the suitability of this region as a refugium also for other organisms of the Pleistocene mammoth steppe including the iconic large herbivores. (C)2018 Elsevier Ltd. All rights reserved.
Modelers can improve a model by addressing the causes for the model errors (data errors and structural errors). This leads to implementing model enhancements (MEs), for example, meteorological data based on more monitoring stations, improved calibration data, and/or modifications in process formulations. However, deciding on which MEs to implement remains a matter of expert knowledge. After implementing multiple MEs, any improvement in model performance is not easily attributed, especially when considering different objectives or aspects of this improvement (e.g., better dynamics vs. reduced bias). We present an approach for comparing the effect of multiple MEs based on real observations and considering multiple objectives (MMEMO). A stepwise selection approach and structured plots help to address the multidimensionality of the problem. Tailored analyses allow a differentiated view on the effect of MEs and their interactions. MMEMO is applied to a case study employing the mesoscale hydro-sedimentological model WASA-SED for the Mediterranean-mountainous Isabena catchment, northeast Spain. The investigated seven MEs show diverse effects: some MEs (e.g., rainfall data) cause improvements for most objectives, while other MEs (e.g., land use data) only affect a few objectives or even decrease model performance. Interaction of MEs was observed for roughly half of the MEs, confirming the need to address them in the analysis. Calibration and increasing the temporal resolution showed by far stronger impact than any of the other MEs. The proposed framework can be adopted in other studies to analyze the effect of MEs and, thus, facilitate the identification and implementation of the most promising MEs for comparable cases.
This study analyzes the influence of local and regional climatic factors on the stable isotopic composition of rainfall in the Vietnamese Mekong Delta (VMD) as part of the Asian monsoon region. It is based on 1.5 years of weekly rainfall samples. In the first step, the isotopic composition of the samples is analyzed by local meteoric water lines (LMWLs) and single-factor linear correlations. Additionally, the contribution of several regional and local factors is quantified by multiple linear regression (MLR) of all possible factor combinations and by relative importance analysis. This approach is novel for the interpretation of isotopic records and enables an objective quantification of the explained variance in isotopic records for individual factors. In this study, the local factors are extracted from local climate records, while the regional factors are derived from atmospheric backward trajectories of water particles. The regional factors, i.e., precipitation, temperature, relative humidity and the length of backward trajectories, are combined with equivalent local climatic parameters to explain the response variables delta O-18, delta H-2, and d-excess of precipitation at the station of measurement. The results indicate that (i) MLR can better explain the isotopic variation in precipitation (R-2 = 0.8) compared to single-factor linear regression (R-2 = 0.3); (ii) the isotopic variation in precipitation is controlled dominantly by regional moisture regimes (similar to 70 %) compared to local climatic conditions (similar to 30 %); (iii) the most important climatic parameter during the rainy season is the precipitation amount along the trajectories of air mass movement; (iv) the influence of local precipitation amount and temperature is not sig-nificant during the rainy season, unlike the regional precipitation amount effect; (v) secondary fractionation processes (e.g., sub-cloud evaporation) can be identified through the d-excess and take place mainly in the dry season, either locally for delta O-18 and delta H-2, or along the air mass trajectories for d-excess. The analysis shows that regional and local factors vary in importance over the seasons and that the source regions and transport pathways, and particularly the climatic conditions along the pathways, have a large influence on the isotopic composition of rainfall. Although the general results have been reported qualitatively in previous studies (proving the validity of the approach), the proposed method provides quantitative estimates of the controlling factors, both for the whole data set and for distinct seasons. Therefore, it is argued that the approach constitutes an advancement in the statistical analysis of isotopic records in rainfall that can supplement or precede more complex studies utilizing atmospheric models. Due to its relative simplicity, the method can be easily transferred to other regions, or extended with other factors. The results illustrate that the interpretation of the isotopic composition of precipitation as a recorder of local climatic conditions, as for example performed for paleorecords of water isotopes, may not be adequate in the southern part of the Indochinese Peninsula, and likely neither in other regions affected by monsoon processes. However, the presented approach could open a pathway towards better and seasonally differentiated reconstruction of paleoclimates based on isotopic records.
Bedrock landsliding in mountain belts can elevate overall chemical weathering rates through rapid dissolution of exhumed reactive mineral phases in transiently stored deposits. This link between a key process of erosion and the resultant weathering affects the sequestering of carbon dioxide through weathering of silicate minerals and broader links between erosion in active orogens and climate change. Here we address the effect on the carbon cycle of weathering induced by bedrock landsliding in Taiwan and the Western Southern Alps of New Zealand. Using solute chemistry data from samples of seepage from landslide deposits and river discharge from catchments with variable proportions of landsliding, we model the proportion of silicate and carbonate weathering and the balance of sulfuric and carbonic acids that act as weathering agents. We correct for secondary precipitation, geothermal, and cyclic input, to find a closer approximation of the weathering explicitly occurring within landslide deposits. We find highly variable proportions of sulfuric and carbonic acids driving weathering in landslides and stable hillslopes. Despite this variability, the predominance of rapid carbonate weathering within landslides and catchments where mass wasting is prevalent results at best in limited sequestration of carbon dioxide by this process of rapid erosion. In many cases where sulfuric acid is a key weathering agent, a net release of CO2 to the atmosphere occurs. This suggests that a causal link between erosion in mountain belts and climate change through the sequestration of CO2, if it exists, must operate through a process other than chemical weathering driven by landsliding. Plain Language Summary There is a long-standing debate surrounding the link between erosion and climate. It is often suggested that as temperatures increase, rainier and stormier weather could increase erosion of rock; as that rock is exposed, silicate minerals within could break down, which, on long time scales, can remove CO2 from the atmosphere, lowering global temperatures and acting as a negative feedback. Recent studies have shown that landslide deposits are key locations for the link between chemical weathering and physical erosion in some mountain belts. To test how landslides affect the erosion-climate link, we used samples of water seeping through landslides in Taiwan and New Zealand to calculate the amount of carbon dioxide that is either absorbed or released through this chemical reaction. We find that the large amount of freshly exposed rock in Taiwanese landslide deposits contains significant carbonate rock and sulfide minerals; the net result of the weathering of these minerals is a release of carbon dioxide, which inverts the traditional perspective on the role erosion plays in controlling carbon dioxide release. In some mountain belts, it seems that increased erosion and resulting landsliding may act to increase carbon dioxide in the air, opening further questions into the nature of erosional-climatic links.
A comprehensive hydro-sedimentological dataset for the Isabena catchment, northeastern (NE) Spain, for the period 2010-2018 is presented to analyse water and sediment fluxes in a Mediterranean mesoscale catchment. The dataset includes rainfall data from 12 rain gauges distributed within the study area complemented by meteorological data of 12 official meteo-stations. It comprises discharge data derived from water stage measurements as well as suspended sediment concentrations (SSCs) at six gauging stations of the River Isabena and its sub-catchments. Soil spectroscopic data from 351 suspended sediment samples and 152 soil samples were collected to characterize sediment source regions and sediment properties via fingerprinting analyses. The Isabena catchment (445 km(2)) is located in the southern central Pyrenees ranging from 450 m to 2720 m a.s.l.; together with a pronounced topography, this leads to distinct temperature and precipitation gradients. The River Isabena shows marked discharge variations and high sediment yields causing severe siltation problems in the downstream Barasona Reservoir. The main sediment source is badland areas located on Eocene marls that are well connected to the river network. The dataset features a comprehensive set of variables in a high spatial and temporal resolution suitable for the advanced process understanding of water and sediment fluxes, their origin and connectivity and sediment budgeting and for the evaluation and further development of hydro-sedimentological models in Mediterranean mesoscale mountainous catchments.
Volcanic activities triggered or inhibited by resonance of volcanic edifices to large earthquakes
(2018)
The existence of a causal link between large earthquakes and volcanic unrest is widely accepted. Recent observations have also revealed counterintuitive negative responses of volcanoes to large earthquakes, including decreased gas emissions and subsidence in volcanic areas. In order to explore the mechanisms that could simultaneously explain both the positive and negative responses of volcanic activity to earthquakes, we here focus on the role played by topography. In the laboratory, we shook a volcanic edifice analogue, made of gel, previously injected with a buoyant fluid. We find that shaking triggers rapid migration of the buoyant fluid upward, downward, or laterally, depending on the fluid’s buoyancy and storage depth; bubbly fluids stored at shallow depth ascend, while low-buoyancy fluids descend or migrate laterally. The migration of fluids induced by shaking is two orders of magnitude faster than without shaking. Downward or lateral fluid migration may decrease volcanic gas emissions and cause subsidence as a negative response, while upward migration is consistent both with an increase in volcanic activity and immediate unrest (deformation and seismicity) after large earthquakes. The fluid migration is more efficient when the oscillation frequency is close to the resonance frequency of the edifice. The resonance frequency for a 30-km-wide volcanic mountain range, such as those where subsidence was observed, is ∼0.07 Hz. Only large earthquakes are able to cause oscillation at such low frequencies.
With the growing size and use of night light time series from the Visible Infrared Imaging Radiometer Suite Day/Night Band (DNB), it is important to understand the stability of the dataset. All satellites observe differences in pixel values during repeat observations. In the case of night light data, these changes can be due to both environmental effects and changes in light emission. Here we examine the stability of individual locations of particular large scale light sources (e.g., airports and prisons) in the monthly composites of DNB data from April 2012 to September 2017. The radiances for individual pixels of most large light emitters are approximately normally distributed, with a standard deviation of typically 15-20% of the mean. Greenhouses and flares, however, are not stable sources. We observe geospatial autocorrelation in the monthly variations for nearby sites, while the correlation for sites separated by large distances is small. This suggests that local factors contribute most to the variation in the pixel radiances and furthermore that averaging radiances over large areas will reduce the total variation. A better understanding of the causes of temporal variation would improve the sensitivity of DNB to lighting changes.
Abstract. The aim of this study is to investigate the shallow thermal field differences for two differently aged passive continental margins by analyzing regional variations in geothermal gradient and exploring the controlling factors for these variations. Hence, we analyzed two previously published 3-D conductive and lithospheric-scale thermal models of the Southwest African and the Norwegian passive margins. These 3-D models differentiate various sedimentary, crustal, and mantle units and integrate different geophysical data such as seismic observations and the gravity field. We extracted the temperature–depth distributions in 1 km intervals down to 6 km below the upper thermal boundary condition. The geothermal gradient was then calculated for these intervals between the upper thermal boundary condition and the respective depth levels (1, 2, 3, 4, 5, and 6 km below the upper thermal boundary condition). According to our results, the geothermal gradient decreases with increasing depth and shows varying lateral trends and values for these two different margins. We compare the 3-D geological structural models and the geothermal gradient variations for both thermal models and show how radiogenic heat production, sediment insulating effect, and thermal lithosphere–asthenosphere boundary (LAB) depth influence the shallow thermal field pattern. The results indicate an ongoing process of oceanic mantle cooling at the young Norwegian margin compared with the old SW African passive margin that seems to be thermally equilibrated in the present day.