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Carbonates play a key role in the chemistry and dynamics of our planet. They are directly connected to the CO2 budget of our atmosphere and have a great impact on the deep carbon cycle. Moreover, recent studies have shown that carbonates are stable along the geothermal gradient down to Earth's lower mantle conditions, changing their crystal structure and related properties. Subducted carbonates may also react with silicates to form new phases. These reactions will redistribute elements, such as calcium (Ca), magnesium (Mg), iron (Fe) and carbon in the form of carbon dioxide (CO2), but also trace elements, that are carried by the carbonates. The trace elements of most interest are strontium (Sr) and rare earth elements (REE) which have been found to be important constituents in the composition of the primitive lower mantle and in mineral inclusions found in super-deep diamonds. However, the stability of carbonates in presence of mantle silicates at relevant temperatures is far from being well understood. Related to this, very little is known about distribution processes of trace elements between carbonates and mantle silicates. To shed light on these processes, we studied reactions between Sr- and REE-containing CaCO3 and Mg/Fe-bearing silicates of the system (Mg,Fe)2SiO4 - (Mg,Fe)SiO3 at high pressure and high temperature using synchrotron radiation based μ-X-ray diffraction (μ-XRD) and μ-X-ray fluorescence (μ-XRF) with μm-resolution in a laser-heated diamond anvil cell. X-ray diffraction is used to derive the structural changes of the phase reactions whereas X-ray fluorescence gives information on the chemical changes in the sample. In-situ experiments at high pressure and high temperature were performed at beamline P02.2 at PETRA III (Hamburg, Germany) and at beamline ID27 at ESRF (Grenoble, France). In addition to μ-XRD and μ-XRF, ex-situ measurements were made on the recovered sample material using transmission electron microscopy (TEM) and provided further insights into the reaction kinetics of carbonate-silicate reactions.
Our investigations show that CaCO3 is unstable in presence of mantle silicates above 1700 K and a reaction takes place in which magnesite plus CaSiO3-perovskite are formed. In addition, we observed that a high content of iron in the carbonate-silicate system favours dolomite formation during the reaction. The subduction of natural carbonates with significant amounts of Sr leads to a comprehensive investigation of the stability not only of CaCO3 phases in contact with mantle silicates but also of SrCO3 (and of Sr-bearing CaCO3). We found that SrCO3 reacts with (Mg,Fe)SiO3-perovskite to form magnesite and gained evidence for the formation of SrSiO3-perovskite.
To complement our study on the stability of SrCO3 at conditions of the Earth's lower mantle, we performed powder X-ray diffraction and single crystal X-ray diffraction experiments at ambient temperature and up to 49 GPa. We observed a transformation from SrCO3-I into a new high-pressure phase SrCO3-II at around 26 GPa with Pmmn crystal structure and a bulk modulus of 103(10) GPa. This information is essential to fully understand the phase behaviour and stability of carbonates in the Earth's lower mantle and to elucidate the possibility of introducing Sr into mantle silicates by carbonate-silicate reactions.
Simultaneous recording of μ-XRD and μ-XRF in the μm-range over the heated areas provides spatial information not only about phase reactions but also on the elemental redistribution during the reactions. A comparison of the spatial intensity distribution of the XRF signal before and after heating indicates a change in the elemental distribution of Sr and an increase in Sr-concentration was found around the newly formed SrSiO3-perovskite. With the help of additional TEM analyses on the quenched sample material the elemental redistribution was studied at a sub-micrometer scale. Contrary to expectations from combined μ-XRD and μ-XRF measurements, we found that La and Eu were not incorporated into the silicate phases, instead they tend to form either isolated oxide phases (e.g. Eu2O3, La2O3) or hydroxyl-bastnäsite (La(CO3)(OH)). In addition, we observed the transformation from (Mg,Fe)SiO3-perovskite to low-pressure clinoenstatite during pressure release. The monoclinic structure (P21/c) of this phase allows the incorporation of Ca as shown by additional EDX analyses and, to a minor extent, Sr too.
Based on our experiments, we can conclude that a detection of the trace elements in-situ at high pressure and high temperature remains challenging. However, our first findings imply that silicates may incorporate the trace elements provided by the carbonates and indicate that carbonates may have a major effect on the trace element contents of mantle phases.
Orogenic peridotites represent portions of upper subcontinental mantle now incorporated in mountain belts. They often contain layers, lenses and irregular bodies of pyroxenite and eclogite. The origin of this heterogeneity and the nature of these layers is still debated but it is likely to involve processes such as transient melts coming from the crust or the mantle and segregating in magma conduits, crust-mantle interaction, upwelling of the asthenosphere and metasomatism. All these processes occur in the lithospheric mantle and are often related with the subduction of crustal rocks to mantle depths. In fact, during subduction, fluids and melts are released from the slab and can interact with the overlying mantle, making the study of deep melts in this environment crucial to understand mantle heterogeneity and crust-mantle interaction. The aim of this thesis is precisely to better constrain how such processes take place studying directly the melt trapped as primary inclusions in pyroxenites and eclogites. The Bohemian Massif, crystalline core of the Variscan belt, is targeted for these purposes because it contains orogenic peridotites with layers of pyroxenite and eclogite and other mafic rocks enclosed in felsic high pressure and ultra-high pressure crustal rocks. Within this Massif mafic rocks from two areas have been selected: the garnet clinopyroxenite in orogenic peridotite of the Granulitgebirge and the ultra-high pressure eclogite in the diamond-bearing gneisses of the Erzgebirge. In both areas primary melt inclusions were recognized in the garnet, ranging in size between 2-25 µm and with different degrees of crystallization, from glassy to polycrystalline. They have been investigated with Micro Raman spectroscopy and EDS mapping and the mineral assemblage is kumdykolite, phlogopite, quartz, kokchetavite, phase with a main Raman peak at 430 cm-1, phase with a main Raman peak at 412 cm-1, white mica and calcite with some variability in relative abundance depending on the case study. In the Granulitgebirge osumilite and pyroxene are also present, whereas calcite is one of the main phases in the Erzgebirge. The presence of glass and the mineral assemblage in the nanogranitoids suggest that they were former droplets of melt trapped in the garnet while it was growing. Glassy inclusions and re-homogenized nanogranitoids show a silicate melt that is granitic, hydrous, high in alkalis and weakly peraluminous. The melt is also enriched in both case studies in Cs, Pb, Rb, U, Th, Li and B suggesting the involvement of crustal component, i.e. white mica (main carrier of Cs, Pb, Rb, Li and B), and a fluid (Cs, Th and U) in the melt producing reaction. The whole rock in both cases mainly consists of garnet and clinopyroxene with, in Erzgebirge samples, the additional presence of quartz both in the matrix and as a polycrystalline inclusion in the garnet. The latter is interpreted as a quartz pseudomorph after coesite and occurs in the same microstructural position as the melt inclusions. Both rock types show a crustal and subduction zone signature with garnet and clinopyroxene in equilibrium. Melt was likely present during the metamorphic peak of the rock, as it occurs in garnet.
Our data suggest that the processes most likely responsible for the formation of the investigated rocks in both areas is a metasomatic reaction between a melt produced in the crust and mafic layers formerly located in the mantle wedge for the Granulitgebirge and in the subducted continental crust itself in the Erzgebirge. Thus metasomatism in the first case took place in the mantle overlying the slab, whereas in the second case metasomatism took place in the continental crust that already contained, before subduction, mafic layers. Moreover, the presence of former coesite in the same microstructural position of the melt inclusions in the Erzgebirge garnets suggest that metasomatism took place at ultra-high pressure conditions.
Summarizing, in this thesis we provide new insights into the geodynamic evolution of the Bohemian Massif based on the study of melt inclusions in garnet in two different mafic rock types, combining the direct microstructural and geochemical investigation of the inclusions with the whole-rock and mineral geochemistry. We report for the first time data, directly extracted from natural rocks, on the metasomatic melt responsible for the metasomatism of several areas of the Bohemian Massif. Besides the two locations here investigated, belonging to the Saxothuringian Zone, a signature similar to the investigated melt is clearly visible in pyroxenite and peridotite of the T-7 borehole (again Saxothuringian Zone) and the durbachite suite located in the Moldanubian Zone.
Compound natural hazards likeEl Ninoevents cause high damage to society, which to manage requires reliable risk assessments. Damage modelling is a prerequisite for quantitative risk estimations, yet many procedures still rely on expert knowledge, and empirical studies investigating damage from compound natural hazards hardly exist. A nationwide building survey in Peru after theEl Ninoevent 2017 - which caused intense rainfall, ponding water, flash floods and landslides - enables us to apply data-mining methods for statistical groundwork, using explanatory features generated from remote sensing products and open data. We separate regions of different dominant characteristics through unsupervised clustering, and investigate feature importance rankings for classifying damage via supervised machine learning. Besides the expected effect of precipitation, the classification algorithms select the topographic wetness index as most important feature, especially in low elevation areas. The slope length and steepness factor ranks high for mountains and canyons. Partial dependence plots further hint at amplified vulnerability in rural areas. An example of an empirical damage probability map, developed with a random forest model, is provided to demonstrate the technical feasibility.
A local and flexible definition of the monsoon season based on hydrological evidence is important for the understanding and management of Himalayan water resources. Here, we present an objective statistical method to retrieve seasonal hydrometeorological transitions. Applied to daily rainfall data (1951-2015), this method shows an average longitudinal delay of similar to 15 days, with later monsoon onset and earlier withdrawal in the western Himalaya, consistent with the continental progression of wet air masses. This delay leads to seasons of different length along the Himalaya and biased precipitation amounts when using uniform calendric monsoon boundaries. In the Central Himalaya annual precipitation has increased, due primarily to an increase of premonsoon precipitation. These findings highlight issues associated with a static definition of monsoon boundaries and call for a deeper understanding of nonmonsoonal precipitation over the Himalayan water tower. <br /> Plain Language Summary Precipitation in the Himalayas determines water availability for the Indian foreland with large socioeconomic implications. Despite its importance, spatial and temporal patterns of precipitation are poorly understood. Here, we estimate the long-term average and trends of seasonal precipitation at the scale of individual catchments draining the Himalayas. We apply a statistical method to detect the timing of hydrometeorological seasons from local precipitation measurements, focusing on monsoon onset and withdrawal. We identify longitudinal and latitudinal delays, resulting in seasons of different length along and across the Himalayas. These spatial patterns and the annual variability of the monsoon boundaries mean that oft-used, fixed calendric dates, for example, 1 June to 30 September, may be inadequate for retrieving monsoon rainfall totals. Moreover, we find that, despite its prominent contribution to annual rainfall totals, the Indian summer monsoon cannot explain the increase of the annual precipitation over the Central Himalayas. Instead, this appears to be mostly driven by changes in premonsoon and winter rainfall. So far, little attention has been paid to premonsoon precipitation, but governed by evaporative processes and surface water availability, it may be enhanced by irrigation and changed land use in the Gangetic foreland.
Forested areas are assumed not to be influenced by erosion processes. However, forest soils of Northern Germany in a hummocky ground moraine landscape can sometimes exhibit a very shallow thickness on crest positions and buried soils on slope positions. The question consequently is: Are these on-going or ancient erosional and depositional processes? Plutonium isotopes act as soil erosion/deposition tracers for recent (last few decades) processes. Here, we quantified the 239+240PU inventories in a small, forested catchment (ancient forest "Melzower Forst", deciduous trees), which is characterised by a hummocky terrain including a kettle hole. Soil development depths (depth to C horizon) and 239+240PU inventories along a catena of sixteen different profiles were determined and correlated to relief parameters. Moreover, we compared different modelling approaches to derive erosion rates from Pu data. <br /> We find a strong relationship between soil development depths, distance-to-sink and topography along the catena. Fully developed Retisols (thicknesses > 1 m) in the colluvium overlay old land surfaces as documented by fossil Ah horizons. However, we found no relationship of Pu-based erosion rates to any relief parameter. Instead, 239+240PU inventories showed a very high local, spatial variability (36-70 Bq m(-2)). Low annual rainfall, spatially distributed interception and stem flow might explain the high variability of the 239+240PU inventories, giving rise to a patchy input pattern. Different models resulted in quite similar erosion and deposition rates (max: -5 t ha(-1) yr(-1) to +7.3 t ha(-1) yr(-1)). Although some rates are rather high, the magnitude of soil erosion and deposition - in terms of soil thickness change - is negligible during the last 55 years. The partially high values are an effect of the patchy Pu deposition on the forest floor. This forest has been protected for at least 240 years. Therefore rather natural events and anthropogenic activities during medieval times or even earlier must have caused the observed soil pattern, which documents strong erosion and deposition processes.
Atmospheric dynamics of extreme discharge events from 1979 to 2016 in the southern Central Andes
(2020)
During the South-American Monsoon season, deep convective systems occur at the eastern flank of the Central Andes leading to heavy rainfall and flooding. We investigate the large- and meso-scale atmospheric dynamics associated with extreme discharge events (> 99.9th percentile) observed in two major river catchments meridionally stretching from humid to semi-arid conditions in the southern Central Andes. Based on daily gauge time series and ERA-Interim reanalysis, we made the following three key observations: (1) for the period 1940-2016 daily discharge exhibits more pronounced variability in the southern, semi-arid than in the northern, humid catchments. This is due to a smaller ratio of discharge magnitudes between intermediate (0.2 year return period) and rare events (20 year return period) in the semi-arid compared to the humid areas; (2) The climatological composites of the 40 largest discharge events showed characteristic atmospheric features of cold surges based on 5-day time-lagged sequences of geopotential height at different levels in the troposphere; (3) A subjective classification revealed that 80% of the 40 largest discharge events are mainly associated with the north-northeastward migration of frontal systems and 2/3 of these are cold fronts, i.e. cold surges. This work highlights the importance of cold surges and their related atmospheric processes for the generation of heavy rainfall events and floods in the southern Central Andes.
Temperature changes and variations in pore fluid salinity may negatively affect the permeability of clay-bearing sandstones with implications for natural fluid flow and geotechnical applications alike. In this study these factors are investigated for a sandstone dominated by illite as the clay phase. Systematic long-term flow-through experiments were conducted and complemented with comprehensive microstructural investigations and the application of Derjaguin-Landau-Verwey-Overbeek (DLVO) theory to explain mechanistically the observed permeability changes. Initially, sample permeability was not affected by low pore fluid salinity indicating strong attraction of the illite particles to the pore walls as supported by electron microprobe analysis (EMPA). Increasing temperature up to 145 degrees C resulted in an irreversible permeability decrease by 1.5 orders of magnitude regardless of the pore fluid composition (i.e., deionized water and 2 M NaCl solution). Subsequently diluting the high salinity pore fluid to below 0.5 M yielded an additional permeability decline by 1.5 orders of magnitude, both at 145 degrees C and after cooling to room temperature. By applying scanning electron microscopy (SEM) and mercury intrusion porosimetry (MIP) thermo-mechanical pore throat closure and illite particle migration were identified as independently operating mechanisms responsible for observed permeability changes during heating and dilution, respectively. These observations indicate that permeability of illite-bearing sandstones will be impaired by heating and exposure to low salinity pore fluids. In addition, chemically induced permeability variations proved to be path dependent with respect to the applied succession of fluid salinity changes.
Fractures efficiently affect fluid flow in geological formations, and thereby determine mass and energy transport in reservoirs, which are not least exploited for economic resources. In this context, their response to mechanical and thermal changes, as well as fluid-rock interactions, is of paramount importance. In this study, a two-stage flow-through experiment was conducted on a pure quartz sandstone core of low matrix permeability, containing one single macroscopic tensile fracture. In the first short-term stage, the effects of mechanical and hydraulic aperture on pressure and temperature cycles were investigated. The purpose of the subsequent intermittent-flow long-term (140 days) stage was to constrain the evolution of the geometrical and hydraulic fracture properties resulting from pressure solution. Deionized water was used as the pore fluid, and permeability, as well as the effluent Si concentrations, were systematically measured. Overall, hydraulic aperture was shown to be significantly less affected by pressure, temperature and time, in comparison to mechanical aperture. During the long-term part of the experiment at 140 degrees C, the effluent Si concentrations likely reached a chemical equilibrium state within less than 8 days of stagnant flow, and exceeded the corresponding hydrostatic quartz solubility at this temperature. This implies that the pressure solution was active at the contacting fracture asperities, both at 140 degrees C and after cooling to 33 degrees C. The higher temperature yielded a higher dissolution rate and, consequently, a faster attainment of chemical equilibrium within the contact fluid. X-ray mu CT observations evidenced a noticeable increase in fracture contact area ratio, which, in combination with theoretical considerations, implies a significant decrease in mechanical aperture. In contrast, the sample permeability, and thus the hydraulic fracture aperture, virtually did not vary. In conclusion, pressure solution-induced fracture aperture changes are affected by the degree of time-dependent variations in pore fluid composition. In contrast to the present case of a quasi-closed system with mostly stagnant flow, in an open system with continuous once-through fluid flow, the activity of the pressure solution may be amplified due to the persistent fluid-chemical nonequilibrium state, thus possibly enhancing aperture and fracture permeability changes.
Temporal variation of natural light sources such as airglow limits the ability of night light sensors to detect changes in small sources of artificial light (such as villages). This study presents a method for correcting for this effect globally, using the satellite radiance detected from regions without artificial light emissions. We developed a routine to define an approximate grid of locations worldwide that do not have regular light emission. We apply this method with a 5 degree equally spaced global grid (total of 2016 individual locations), using data from the Visible Infrared Imaging Radiometer Suite (VIIRS) Day-Night Band (DNB). This code could easily be adapted for other future global sensors. The correction reduces the standard deviation of data in the Earth Observation Group monthly DNB composites by almost a factor of two. The code and datasets presented here are available under an open license by GFZ Data Services, and are implemented in the Radiance Light Trends web application.