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Institute
- Institut für Geowissenschaften (325) (remove)
Large parts of the Earth’s interior are inaccessible to direct observation, yet global geodynamic processes are governed by the physical material properties under extreme pressure and temperature conditions. It is therefore essential to investigate the deep Earth’s physical properties through in-situ laboratory experiments. With this goal in mind, the optical properties of mantle minerals at high pressure offer a unique way to determine a variety of physical properties, in a straight-forward, reproducible, and time-effective manner, thus providing valuable insights into the physical processes of the deep Earth. This thesis focusses on the system Mg-Fe-O, specifically on the optical properties of periclase (MgO) and its iron-bearing variant ferropericlase ((Mg,Fe)O), forming a major planetary building block. The primary objective is to establish links between physical material properties and optical properties. In particular the spin transition in ferropericlase, the second-most abundant phase of the lower mantle, is known to change the physical material properties. Although the spin transition region likely extends down to the core-mantle boundary, the ef-fects of the mixed-spin state, where both high- and low-spin state are present, remains poorly constrained.
In the studies presented herein, we show how optical properties are linked to physical properties such as electrical conductivity, radiative thermal conductivity and viscosity. We also show how the optical properties reveal changes in the chemical bonding. Furthermore, we unveil how the chemical bonding, the optical and other physical properties are affected by the iron spin transition. We find opposing trends in the pres-sure dependence of the refractive index of MgO and (Mg,Fe)O. From 1 atm to ~140 GPa, the refractive index of MgO decreases by ~2.4% from 1.737 to 1.696 (±0.017). In contrast, the refractive index of (Mg0.87Fe0.13)O (Fp13) and (Mg0.76Fe0.24)O (Fp24) ferropericlase increases with pressure, likely because Fe Fe interactions between adjacent iron sites hinder a strong decrease of polarizability, as it is observed with increasing density in the case of pure MgO. An analysis of the index dispersion in MgO (decreasing by ~23% from 1 atm to ~103 GPa) reflects a widening of the band gap from ~7.4 eV at 1 atm to ~8.5 (±0.6) eV at ~103 GPa. The index dispersion (between 550 and 870 nm) of Fp13 reveals a decrease by a factor of ~3 over the spin transition range (~44–100 GPa). We show that the electrical band gap of ferropericlase significantly widens up to ~4.7 eV in the mixed spin region, equivalent to an increase by a factor of ~1.7. We propose that this is due to a lower electron mobility between adjacent Fe2+ sites of opposite spin, explaining the previously observed low electrical conductivity in the mixed spin region. From the study of absorbance spectra in Fp13, we show an increasing covalency of the Fe-O bond with pressure for high-spin ferropericlase, whereas in the low-spin state a trend to a more ionic nature of the Fe-O bond is observed, indicating a bond weakening effect of the spin transition. We found that the spin transition is ultimately caused by both an increase of the ligand field-splitting energy and a decreasing spin-pairing energy of high-spin Fe2+.
The Central Andean region is characterized by diverse climate zones with sharp transitions between them. In this work, the area of interest is the South-Central Andes in northwestern Argentina that borders with Bolivia and Chile. The focus is the observation of soil moisture and water vapour with Global Navigation Satellite System (GNSS) remote-sensing methodologies. Because of the rapid temporal and spatial variations of water vapour and moisture circulations, monitoring this part of the hydrological cycle is crucial for understanding the mechanisms that control the local climate. Moreover, GNSS-based techniques have previously shown high potential and are appropriate for further investigation. This study includes both logistic-organization effort and data analysis. As for the prior, three GNSS ground stations were installed in remote locations in northwestern Argentina to acquire observations, where there was no availability of third-party data.
The methodological development for the observation of the climate variables of soil moisture and water vapour is independent and relies on different approaches. The soil-moisture estimation with GNSS reflectometry is an approximation that has demonstrated promising results, but it has yet to be operationally employed. Thus, a more advanced algorithm that exploits more observations from multiple satellite constellations was developed using data from two pilot stations in Germany. Additionally, this algorithm was slightly modified and used in a sea-level measurement campaign. Although the objective of this application is not related to monitoring hydrological parameters, its methodology is based on the same principles and helps to evaluate the core algorithm. On the other hand, water-vapour monitoring with GNSS observations is a well-established technique that is utilized operationally. Hence, the scope of this study is conducting a meteorological analysis by examining the along-the-zenith air-moisture levels and introducing indices related to the azimuthal gradient.
The results of the experiments indicate higher-quality soil moisture observations with the new algorithm. Furthermore, the analysis using the stations in northwestern Argentina illustrates the limits of this technology because of varying soil conditions and shows future research directions. The water-vapour analysis points out the strong influence of the topography on atmospheric moisture circulation and rainfall generation. Moreover, the GNSS time series allows for the identification of seasonal signatures, and the azimuthal-gradient indices permit the detection of main circulation pathways.
With Arctic ground as a huge and temperature-sensitive carbon reservoir, maintaining low ground temperatures and frozen conditions to prevent further carbon emissions that contrib-ute to global climate warming is a key element in humankind’s fight to maintain habitable con-ditions on earth. Former studies showed that during the late Pleistocene, Arctic ground condi-tions were generally colder and more stable as the result of an ecosystem dominated by large herbivorous mammals and vast extents of graminoid vegetation – the mammoth steppe. Characterised by high plant productivity (grassland) and low ground insulation due to animal-caused compression and removal of snow, this ecosystem enabled deep permafrost aggrad-ation. Now, with tundra and shrub vegetation common in the terrestrial Arctic, these effects are not in place anymore. However, it appears to be possible to recreate this ecosystem local-ly by artificially increasing animal numbers, and hence keep Arctic ground cold to reduce or-ganic matter decomposition and carbon release into the atmosphere.
By measuring thaw depth, total organic carbon and total nitrogen content, stable carbon iso-tope ratio, radiocarbon age, n-alkane and alcohol characteristics and assessing dominant vegetation types along grazing intensity transects in two contrasting Arctic areas, it was found that recreating conditions locally, similar to the mammoth steppe, seems to be possible. For permafrost-affected soil, it was shown that intensive grazing in direct comparison to non-grazed areas reduces active layer depth and leads to higher TOC contents in the active layer soil. For soil only frozen on top in winter, an increase of TOC with grazing intensity could not be found, most likely because of confounding factors such as vertical water and carbon movement, which is not possible with an impermeable layer in permafrost. In both areas, high animal activity led to a vegetation transformation towards species-poor graminoid-dominated landscapes with less shrubs. Lipid biomarker analysis revealed that, even though the available organic material is different between the study areas, in both permafrost-affected and sea-sonally frozen soils the organic material in sites affected by high animal activity was less de-composed than under less intensive grazing pressure. In conclusion, high animal activity af-fects decomposition processes in Arctic soils and the ground thermal regime, visible from reduced active layer depth in permafrost areas. Therefore, grazing management might be utilised to locally stabilise permafrost and reduce Arctic carbon emissions in the future, but is likely not scalable to the entire permafrost region.
Volcanic hydrothermal systems are an integral part of most volcanoes and typically involve a heat source, adequate fluid supply, and fracture or pore systems through which the fluids can circulate within the volcanic edifice. Associated with this are subtle but powerful processes that can significantly influence the evolution of volcanic activity or the stability of the near-surface volcanic system through mechanical weakening, permeability reduction, and sealing of the affected volcanic rock. These processes are well constrained for rock samples by laboratory analyses but are still difficult to extrapolate and evaluate at the scale of an entire volcano. Advances in unmanned aircraft systems (UAS), sensor technology, and photogrammetric processing routines now allow us to image volcanic surfaces at the centimeter scale and thus study volcanic hydrothermal systems in great detail. This thesis aims to explore the potential of UAS approaches for studying the structures, processes, and dynamics of volcanic hydrothermal systems but also to develop methodological approaches to uncover secondary information hidden in the data, capable of indicating spatiotemporal dynamics or potentially critical developments associated with hydrothermal alteration. To accomplish this, the thesis describes the investigation of two near-surface volcanic hydrothermal systems, the El Tatio geyser field in Chile and the fumarole field of La Fossa di Vulcano (Italy), both of which are among the best-studied sites of their kind. Through image analysis, statistical, and spatial analyses we have been able to provide the most detailed structural images of both study sites to date, with new insights into the driving forces of such systems but also revealing new potential controls, which are summarized in conceptual site-specific models. Furthermore, the thesis explores methodological remote sensing approaches to detect, classify and constrain hydrothermal alteration and surface degassing from UAS-derived data, evaluated them by mineralogical and chemical ground-truthing, and compares the alteration pattern with the present-day degassing activity. A significant contribution of the often neglected diffuse degassing activity to the total amount of degassing is revealed and constrains secondary processes and dynamics associated with hydrothermal alteration that lead to potentially critical developments like surface sealing. The results and methods used provide new approaches for alteration research, for the monitoring of degassing and alteration effects, and for thermal monitoring of fumarole fields, with the potential to be incorporated into volcano monitoring routines.
Rapidly growing seismic and macroseismic databases and simplified access to advanced machine learning methods have in recent years opened up vast opportunities to address challenges in engineering and strong motion seismology from novel, datacentric perspectives. In this thesis, I explore the opportunities of such perspectives for the tasks of ground motion modeling and rapid earthquake impact assessment, tasks with major implications for long-term earthquake disaster mitigation.
In my first study, I utilize the rich strong motion database from the Kanto basin, Japan, and apply the U-Net artificial neural network architecture to develop a deep learning based ground motion model. The operational prototype provides statistical estimates of expected ground shaking, given descriptions of a specific earthquake source, wave propagation paths, and geophysical site conditions. The U-Net interprets ground motion data in its spatial context, potentially taking into account, for example, the geological properties in the vicinity of observation sites. Predictions of ground motion intensity are thereby calibrated to individual observation sites and earthquake locations.
The second study addresses the explicit incorporation of rupture forward directivity into ground motion modeling. Incorporation of this phenomenon, causing strong, pulse like ground shaking in the vicinity of earthquake sources, is usually associated with an intolerable increase in computational demand during probabilistic seismic hazard analysis (PSHA) calculations. I suggest an approach in which I utilize an artificial neural network to efficiently approximate the average, directivity-related adjustment to ground motion predictions for earthquake ruptures from the 2022 New Zealand National Seismic Hazard Model. The practical implementation in an actual PSHA calculation demonstrates the efficiency and operational readiness of my model. In a follow-up study, I present a proof of concept for an alternative strategy in which I target the generalizing applicability to ruptures other than those from the New Zealand National Seismic Hazard Model.
In the third study, I address the usability of pseudo-intensity reports obtained from macroseismic observations by non-expert citizens for rapid impact assessment. I demonstrate that the statistical properties of pseudo-intensity collections describing the intensity of shaking are correlated with the societal impact of earthquakes. In a second step, I develop a probabilistic model that, within minutes of an event, quantifies the probability of an earthquake to cause considerable societal impact. Under certain conditions, such a quick and preliminary method might be useful to support decision makers in their efforts to organize auxiliary measures for earthquake disaster response while results from more elaborate impact assessment frameworks are not yet available.
The application of machine learning methods to datasets that only partially reveal characteristics of Big Data, qualify the majority of results obtained in this thesis as explorative insights rather than ready-to-use solutions to real world problems. The practical usefulness of this work will be better assessed in the future by applying the approaches developed to growing and increasingly complex data sets.
The role of biogenic carbonate producers in the evolution of the geometries of carbonate systems has been the subject of numerous research projects. Attempts to classify modern and ancient carbonate systems by their biotic components have led to the discrimination of biogenic carbonate producers broadly into Photozoans, which are characterised by an affinity for warm tropical waters and high dependence on light penetration, and Heterozoans which are generally associated with both cool water environments and nutrient-rich settings with little to no light penetration. These broad categories of carbonate sediment producers have also been recognised to dominate in specific carbonate systems. Photozoans are commonly dominant in flat-topped platforms with steep margins, while Heterozoans generally dominate carbonate ramps. However, comparatively little is known on how these two main groups of carbonate producers interact in the same system and impact depositional geometries responding to changes in environmental conditions such as sea level fluctuation, antecedent slope, sediment transport processes, etc. This thesis presents numerical models to investigate the evolution of Miocene carbonate systems in the Mediterranean from two shallow marine domains: 1) a Miocene flat-topped platform dominated by Photozoans, with a significant component of Hetrozoans in the slope and 2) a Heterozoan distally steepened ramp, with seagrass-influenced (Photozoan) inner ramp. The overarching aim of the three articles comprising this cumulative thesis is to provide a numerical study of the role of Photozoans and Heterozoans in the evolution of carbonate system geometries and how these biotas respond to changes in environmental conditions. This aim was achieved using stratigraphic forward modelling, which provides an approach to quantitatively integrate multi-scale datasets to reconstruct sedimentary processes and products during the evolution of a sedimentary system.
In a Photozoan-dominated carbonate system, such as the Miocene Llucmajor platform in Western Mediterranean, stratigraphic forward modelling dovetailed with a robust set of sensitivity tests reveal how the geometry of the carbonate system is determined by the complex interaction of Heterozoan and Photozoan biotas in response to variable conditions of sea level fluctuation, substrate configuration, sediment transport processes and the dominance of Photozoan over Heterozoan production. This study provides an enhanced understanding of the different carbonate systems that are possible under different ecological and hydrodynamic conditions. The research also gives insight into the roles of different biotic associations in the evolution of carbonate geometries through time and space. The results further show that the main driver of platform progradation in a Llucmajor-type system is the lowstand production of Heterozoan sediments, which form the necessary substratum for Photozoan production.
In Heterozoan systems, sediment production is mainly characterised by high transport deposits, that are prone to redistribution by waves and gravity, thereby precluding the development of steep margins. However, in the Menorca ramp, the occurrence of sediment trapping by seagrass led to the evolution of distal slope steepening. We investigated, through numerical modelling, how such a seagrass-influenced ramp responds to the frequency and amplitude of sea level changes, variable carbonate production between the euphotic and oligophotic zone, and changes in the configuration of the paleoslope. The study reinforces some previous hypotheses and presents alternative scenarios to the established concepts of high-transport ramp evolution. The results of sensitivity experiments show that steep slopes are favoured in ramps that develop in high-frequency sea level fluctuation with amplitudes between 20 m and 40 m. We also show that ramp profiles are significantly impacted by the paleoslope inclination, such that an optimal antecedent slope of about 0.15 degrees is required for the Menorca distally steepened ramp to develop.
The third part presents an experimental case to argue for the existence of a Photozoan sediment threshold required for the development of steep margins in carbonate platforms. This was carried out by developing sensitivity tests on the forward models of the flat-topped (Llucmajor) platform and the distally steepened (Menorca) platform. The results show that models with Photozoan sediment proportion below a threshold of about 40% are incapable of forming steep slopes. The study also demonstrates that though it is possible to develop steep margins by seagrass sediment trapping, such slopes can only be stabilized by the appropriate sediment fabric and/or microbial binding. In the Photozoan-dominated system, the magnitude of slope steepness depends on the proportion of Photozoan sediments in the system. Therefore, this study presents a novel tool for characterizing carbonate systems based on their biogenic components.
The East African Rift System (EARS) is a significant example of active tectonics, which provides opportunities to examine the stages of continental faulting and landscape evolution. The southwest extension of the EARS is one of the most significant examples of active tectonics nowadays, however, seismotectonic research in the area has been scarce, despite the fundamental importance of neotectonics. Our first study area is located between the Northern Province of Zambia and the southeastern Katanga Province of the Democratic Republic of Congo. Lakes Mweru and Mweru Wantipa are part of the southwest extension of the EARS. Fault analysis reveals that, since the Miocene, movements along the active Mweru-Mweru Wantipa Fault System (MMFS) have been largely responsible for the reorganization of the landscape and the drainage patterns across the southwestern branch of the EARS. To investigate the spatial and temporal patterns of fluvial-lacustrine landscape development, we determined in-situ cosmogenic 10Be and 26Al in a total of twenty-six quartzitic bedrock samples that were collected from knickpoints across the Mporokoso Plateau (south of Lake Mweru) and the eastern part of the Kundelungu Plateau (north of Lake Mweru). Samples from the Mporokoso Plateau and close to the MMFS provide evidence of temporary burial. By contrast, surfaces located far from the MMFS appear to have remained uncovered since their initial exposure as they show consistent 10Be and 26Al exposure ages ranging up to ~830 ka. Reconciliation of the observed burial patterns with morphotectonic and stratigraphic analysis reveals the existence of an extensive paleo-lake during the Pleistocene. Through hypsometric analyses of the dated knickpoints, the potential maximum water level of the paleo-lake is constrained to ~1200 m asl (present lake lavel: 917 m asl). High denudation rates (up to ~40 mm ka-1) along the eastern Kundelungu Plateau suggest that footwall uplift, resulting from normal faulting, caused river incision, possibly controlling paleo-lake drainage. The lake level was reduced gradually reaching its current level at ~350 ka.
Parallel to the MMFS in the north, the Upemba Fault System (UFS) extends across the southeastern Katanga Province of the Democratic Republic of Congo. This part of our research is focused on the geomorphological behavior of the Kiubo Waterfalls. The waterfalls are the currently active knickpoint of the Lufira River, which flows into the Upemba Depression. Eleven bedrock samples along the Lufira River and its tributary stream, Luvilombo River, were collected. In-situ cosmogenic 10Be and 26Al were used in order to constrain the K constant of the Stream Power Law equation. Constraining the K constant allowed us to calculate the knickpoint retreat rate of the Kiubo Waterfalls at ~0.096 m a-1. Combining the calculated retreat rate of the knickpoint with DNA sequencing from fish populations, we managed to present extrapolation models and estimate the location of the onset of the Kiubo Waterfalls, revealing its connection to the seismicity of the UFS.
The shallow Earth’s layers are at the interplay of many physical processes: some being driven by atmospheric forcing (precipitation, temperature...) whereas others take their origins at depth, for instance ground shaking due to seismic activity. These forcings cause the subsurface to continuously change its mechanical properties, therefore modulating the strength of the surface geomaterials and hydrological fluxes. Because our societies settle and rely on the layers hosting these time-dependent properties, constraining the hydro-mechanical dynamics of the shallow subsurface is crucial for our future geographical development. One way to investigate the ever-changing physical changes occurring under our feet is through the inference of seismic velocity changes from ambient noise, a technique called seismic interferometry. In this dissertation, I use this method to monitor the evolution of groundwater storage and damage induced by earthquakes. Two research lines are investigated that comprise the key controls of groundwater recharge in steep landscapes and the predictability and duration of the transient physical properties due to earthquake ground shaking. These two types of dynamics modulate each other and influence the velocity changes in ways that are challenging to disentangle. A part of my doctoral research also addresses this interaction. Seismic data from a range of field settings spanning several climatic conditions (wet to arid climate) in various seismic-prone areas are considered. I constrain the obtained seismic velocity time-series using simple physical models, independent dataset, geophysical tools and nonlinear analysis. Additionally, a methodological development is proposed to improve the time-resolution of passive seismic monitoring.
Advances in hydrogravimetry
(2023)
The interest of the hydrological community in the gravimetric method has steadily increased within the last decade. This is reflected by numerous studies from many different groups with a broad range of approaches and foci. Many of those are traditionally rather hydrology-oriented groups who recognized gravimetry as a potential added value for their hydrological investigations. While this resulted in a variety of interesting and useful findings, contributing to extend the respective knowledge and confirming the methodological potential, on the other hand, many interesting and unresolved questions emerged.
This thesis manifests efforts, analyses and solutions carried out in this regard. Addressing and evaluating many of those unresolved questions, the research contributes to advancing hydrogravimetry, the combination of gravimetric and hydrological methods, in showing how gravimeters are a highly useful tool for applied hydrological field research.
In the first part of the thesis, traditional setups of stationary terrestrial superconducting gravimeters are addressed. They are commonly installed within a dedicated building, the impermeable structure of which shields the underlying soil from natural exchange of water masses (infiltration, evapotranspiration, groundwater recharge). As gravimeters are most sensitive to mass changes directly beneath the meter, this could impede their suitability for local hydrological process investigations, especially for near-surface water storage changes (WSC). By studying temporal local hydrological dynamics at a dedicated site equipped with traditional hydrological measurement devices, both below and next to the building, the impact of these absent natural dynamics on the gravity observations were quantified. A comprehensive analysis with both a data-based and model-based approach led to the development of an alternative method for dealing with this limitation. Based on determinable parameters, this approach can be transferred to a broad range of measurement sites where gravimeters are deployed in similar structures. Furthermore, the extensive considerations on this topic enabled a more profound understanding of this so called umbrella effect.
The second part of the thesis is a pilot study about the field deployment of a superconducting gravimeter. A newly developed field enclosure for this gravimeter was tested in an outdoor installation adjacent to the building used to investigate the umbrella effect. Analyzing and comparing the gravity observations from both indoor and outdoor gravimeters showed performance with respect to noise and stable environmental conditions was equivalent while the sensitivity to near-surface WSC was highly increased for the field deployed instrument. Furthermore it was demonstrated that the latter setup showed gravity changes independent of the depth where mass changes occurred, given their sufficiently wide horizontal extent. As a consequence, the field setup suits monitoring of WSC for both short and longer time periods much better. Based on a coupled data-modeling approach, its gravity time series was successfully used to infer and quantify local water budget components (evapotranspiration, lateral subsurface discharge) on the daily to annual time scale.
The third part of the thesis applies data from a gravimeter field deployment for applied hydrological process investigations. To this end, again at the same site, a sprinkling experiment was conducted in a 15 x 15 m area around the gravimeter. A simple hydro-gravimetric model was developed for calculating the gravity response resulting from water redistribution in the subsurface. It was found that, from a theoretical point of view, different subsurface water distribution processes (macro pore flow, preferential flow, wetting front advancement, bypass flow and perched water table rise) lead to a characteristic shape of their resulting gravity response curve. Although by using this approach it was possible to identify a dominating subsurface water distribution process for this site, some clear limitations stood out. Despite the advantage for field installations that gravimetry is a non-invasive and integral method, the problem of non-uniqueness could only be overcome by additional measurements (soil moisture, electric resistivity tomography) within a joint evaluation. Furthermore, the simple hydrological model was efficient for theoretical considerations but lacked the capability to resolve some heterogeneous spatial structures of water distribution up to a needed scale. Nevertheless, this unique setup for plot to small scale hydrological process research underlines the high potential of gravimetery and the benefit of a field deployment.
The fourth and last part is dedicated to the evaluation of potential uncertainties arising from the processing of gravity observations. The gravimeter senses all mass variations in an integral way, with the gravitational attraction being directly proportional to the magnitude of the change and inversely proportional to the square of the distance of the change. Consequently, all gravity effects (for example, tides, atmosphere, non-tidal ocean loading, polar motion, global hydrology and local hydrology) are included in an aggregated manner. To isolate the signal components of interest for a particular investigation, all non-desired effects have to be removed from the observations. This process is called reduction. The large-scale effects (tides, atmosphere, non-tidal ocean loading and global hydrology) cannot be measured directly and global model data is used to describe and quantify each effect. Within the reduction process, model errors and uncertainties propagate into the residual, the result of the reduction. The focus of this part of the thesis is quantifying the resulting, propagated uncertainty for each individual correction. Different superconducting gravimeter installations were evaluated with respect to their topography, distance to the ocean and the climate regime. Furthermore, different time periods of aggregated gravity observation data were assessed, ranging from 1 hour up to 12 months. It was found that uncertainties were highest for a frequency of 6 months and smallest for hourly frequencies. Distance to the ocean influences the uncertainty of the non-tidal ocean loading component, while geographical latitude affects uncertainties of the global hydrological component. It is important to highlight that the resulting correction-induced uncertainties in the residual have the potential to mask the signal of interest, depending on the signal magnitude and its frequency. These findings can be used to assess the value of gravity data across a range of applications and geographic settings.
In an overarching synthesis all results and findings are discussed with a general focus on their added value for bringing hydrogravimetric field research to a new level. The conceptual and applied methodological benefits for hydrological studies are highlighted. Within an outlook for future setups and study designs, it was once again shown what enormous potential is offered by gravimeters as hydrological field tools.
Carbonates carried in subducting slabs may play a major role in sourcing and storing carbon in the deep Earth’s interior. Current estimates indicate that between 40 to 66 million tons of carbon per year enter subduction zones, but it is uncertain how much of it reaches the lower mantle. It appears that most of this carbon might be extracted from subducting slabs at the mantle wedge and only a limited amount continues deeper and eventually reaches the deep mantle. However, estimations on deeply subducted carbon broadly range from 0.0001 to 52 million tons of carbon per year. This disparity is primarily due to the limited understanding of the survival of carbonate minerals during their transport to deep mantle conditions. Indeed, carbon has very low solubility in mantle silicates, therefore it is expected to be stored primarily in accessory phases such as carbonates. Among those carbonates, magnesite (MgCO3), as a single phase, is the most stable under all mantle conditions. However, experimental investigation on the stability of magnesite in contact with SiO2 at lower mantle conditions suggests that magnesite is stable only along a cold subducted slab geotherm. Furthermore, our understanding of magnesite’s stability when interacting with more complex mantle silicate phases remains incomplete. In the first part of this dissertation, laser-heated diamond anvil cells and multi-anvil apparatus experiments were performed to investigate the stability of magnesite in contact with iron-bearing mantle silicates. Sub-solidus reactions, melting, decarbonation and diamond formation were examined from shallow to mid-lower mantle conditions (25 to 68 GPa; 1300 to 2000 K). Multi-anvil experiments at 25 GPa show the formation of carbonate-rich melt, bridgmanite, and stishovite with melting occurring at a temperature corresponding to all geotherms except the coldest one. In situ X-ray diffraction, in laser-heating diamond anvil cells experiments, shows crystallization of bridgmanite and stishovite but no melt phase was detected in situ at high temperatures. To detect decarbonation phases such as diamond, Raman spectroscopy was used. Crystallization of diamonds is observed as a sub-solidus process even at temperatures relevant and lower than the coldest slab geotherm (1350 K at 33 GPa). Data obtained from this work suggest that magnesite is unstable in contact with the surrounding peridotite mantle in the upper-most lower mantle. The presence of magnesite instead induces melting under oxidized conditions and/or foster diamond formation under more reduced conditions, at depths ∼700 km. Consequently, carbonates will be removed from the carbonate-rich slabs at shallow lower mantle conditions, where subducted slabs can stagnate. Therefore, the transport of carbonate to deeper depths will be restricted, supporting the presence of a barrier for carbon subduction at the top of the lower mantle. Moreover, the reduction of magnesite, forming diamonds provides additional evidence that super-deep diamond crystallization is related to the reduction of carbonates or carbonated-rich melt.
The second part of this dissertation presents the development of a portable laser-heating system optimized for X-ray emission spectroscopy (XES) or nuclear inelastic scattering (NIS) spectroscopy with signal collection at near 90◦. The laser-heated diamond anvil cell is the only static pressure device that can replicate the pressure and temperatures of the Earth’s lower mantle and core. The high temperatures are reached by using high-powered lasers focused on the sample contained between the diamond anvils. Moreover, diamonds’ transparency to X-rays enables in situ X-ray spectroscopy measurements that can probe the sample under high-temperature and high-pressure conditions. Therefore, the development of portable laser-heating systems has linked high-pressure and temperature research with high-resolution X-ray spectroscopy techniques to synchrotron beamlines that do not have a dedicated, permanent, laser-heating system. A general description of the system is provided, as well as details on the use of a parabolic mirror as a reflective imaging objective for on-axis laser heating and radiospectrometric temperature measurements with zero attenuation of incoming X-rays. The parabolic mirror improves the accuracy of temperature measurements free from chromatic aberrations in a wide spectral range and its perforation permits in situ X-rays measurement at synchrotron facilities. The parabolic mirror is a well-suited alternative to refractive objectives in laser heating systems, which will facilitate future applications in the use of CO2 lasers.