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Partial melting is a first order process for the chemical differentiation of the crust (Vielzeuf et al., 1990). Redistribution of chemical elements during melt generation crucially influences the composition of the lower and upper crust and provides a mechanism to concentrate and transport chemical elements that may also be of economic interest. Understanding of the diverse processes and their controlling factors is therefore not only of scientific interest but also of high economic importance to cover the demand for rare metals.
The redistribution of major and trace elements during partial melting represents a central step for the understanding how granite-bound mineralization develops (Hedenquist and Lowenstern, 1994). The partial melt generation and mobilization of ore elements (e.g. Sn, W, Nb, Ta) into the melt depends on the composition of the sedimentary source and melting conditions. Distinct source rocks have different compositions reflecting their deposition and alteration histories. This specific chemical “memory” results in different mineral assemblages and melting reactions for different protolith compositions during prograde metamorphism (Brown and Fyfe, 1970; Thompson, 1982; Vielzeuf and Holloway, 1988). These factors do not only exert an important influence on the distribution of chemical elements during melt generation, they also influence the volume of melt that is produced, extraction of the melt from its source, and its ascent through the crust (Le Breton and Thompson, 1988). On a larger scale, protolith distribution and chemical alteration (weathering), prograde metamorphism with partial melting, melt extraction, and granite emplacement are ultimately depending on a (plate-)tectonic control (Romer and Kroner, 2016). Comprehension of the individual stages and their interaction is crucial in understanding how granite-related mineralization forms, thereby allowing estimation of the mineralization potential of certain areas. Partial melting also influences the isotope systematics of melt and restite. Radiogenic and stable isotopes of magmatic rocks are commonly used to trace back the source of intrusions or to quantify mixing of magmas from different sources with distinct isotopic signatures (DePaolo and Wasserburg, 1979; Lesher, 1990; Chappell, 1996). These applications are based on the fundamental requirement that the isotopic signature in the melt reflects that of the bulk source from which it is derived. Different minerals in a protolith may have isotopic compositions of radiogenic isotopes that deviate from their whole rock signature (Ayres and Harris, 1997; Knesel and Davidson, 2002). In particular, old minerals with a distinct parent-to-daughter (P/D) ratio are expected to have a specific radiogenic isotope signature. As the partial melting reaction only involves selective phases in a protolith, the isotopic signature of the melt reflects that of the minerals involved in the melting reaction and, therefore, should be different from the bulk source signature. Similar considerations hold true for stable isotopes.
In this pilot study, we describe a high-pressure incubation system allowing multiple subsampling of a pressurized culture without decompression. The system was tested using one piezophilic (Photobacterium profundum), one piezotolerant (Colwellia maris) bacterial strain and a decompressed sample from the Mediterranean deep sea (3044 m) determining bacterial community composition, protein production (BPP) and cell multiplication rates (BCM) up to 27 MPa. The results showed elevation of BPP at high pressure was by a factor of 1.5 +/- 1.4 and 3.9 +/- 2.3 for P. profundum and C. maris, respectively, compared to ambient-pressure treatments and by a factor of 6.9 +/- 3.8 fold in the field samples. In P. profundum and C. maris, BCM at high pressure was elevated (3.1 +/- 1.5 and 2.9 +/- 1.7 fold, respectively) compared to the ambient-pressure treatments. After 3 days of incubation at 27 MPa, the natural bacterial deep-sea community was dominated by one phylum of the genus Exiguobacterium, indicating the rapid selection of piezotolerant bacteria. In future studies, our novel incubation system could be part of an isopiestic pressure chain, allowing more accurate measurement of bacterial activity rates which is important both for modeling and for predicting the efficiency of the oceanic carbon pump.
Variation of deuterium excess in surface waters across a 5000-m elevation gradient in eastern Nepal
(2020)
The strong elevation gradient of the Himalaya allows for investigation of altitude and orographic impacts on surface water delta O-18 and delta D stable isotope values. This study differentiates the time- and altitude-variable contributions of source waters to the Arun River in eastern Nepal. It provides isotope data along a 5000-m gradient collected from tributaries as well as groundwater, snow, and glacial-sourced surface waters and time-series data from April to October 2016. We find nonlinear trends in delta O-18 and delta D lapse rates with high-elevation lapse rates (4000-6000 masl) 5-7 times more negative than low-elevation lapse rates (1000-3000 masl). A distinct seasonal signal in delta O-18 and delta D lapse rates indicates time-variable source-water contributions from glacial and snow meltwater as well as precipitation transitions between the Indian Summer Monsoon and Winter Westerly Disturbances. Deuterium excess correlates with the extent of snowpack and tracks melt events during the Indian Summer Monsoon season. Our analysis identifies the influence of snow and glacial melt waters on river composition during low-flow conditions before the monsoon (April/May 2016) followed by a 5-week transition to the Indian Summer Monsoon-sourced rainfall around mid-June 2016. In the post-monsoon season, we find continued influence from glacial melt waters as well as ISM-sourced groundwater.
Lithium and boron are trace components of magmas, released during exsolution of a gas phase during volcanic activity.
In this study, we determine the diffusivity and isotopic fractionation of Li and B in hydrous silicate melts.
Two glasses were synthesized with the same rhyolitic composition (4.2 wt% water), having different Li and B contents; these were studied in diffusion-couple experiments that were performed using an internally heated pressure vessel, operated at 300 MPa in the temperature range 700-1250 degrees C for durations from 0 s to 24 h. From this we determined activation energies for Li and B diffusion of 57 +/- 4 kJ/mol and 152 +/- 15 kJ/mol with pre-exponential factors of 1.53 x 10(-7) m(2)/s and 3.80 x 10(-8) m(2)/s, respectively.
Lithium isotopic fractionation during diffusion gave beta values between 0.15 and 0.20, whereas B showed no clear isotopic fractionation.
Our Li diffusivities and isotopic fractionation results differ somewhat from earlier published values, but overall confirm that Li diffusivity increases with water content. Our results on B diffusion show that similarly to Li, B mobility increases in the presence of water.
By applying the Eyring relation, we confirm that B diffusivity is limited by viscous flow in silicate melts.
Our results on Li and B diffusion present a new tool for understanding degassing-related processes, offering a potential geospeedometer to measure volcanic ascent rates.
Li and B in ascending magmas: an experimental study on their mobility and isotopic fractionation
(2022)
This research study focuses on the behaviour of Li and B during magmatic ascent, and decompression-driven degassing related to volcanic systems. The main objective of this dissertation is to determine whether it is possible to use the diffusion properties of the two trace elements as a tool to trace magmatic ascent rate. With this objective, diffusion-couple and decompression experiments have been performed in order to study Li and B mobility in intra-melt conditions first, and then in an evolving system during decompression-driven degassing.
Synthetic glasses were prepared with rhyolitic composition and an initial water content of 4.2 wt%, and all the experiments were performed using an internally heated pressure vessel, in order to ensure a precise control on the experimental parameters such as temperature and pressure.
Diffusion-couple experiments were performed with a fix pressure 300 MPa. The temperature was varied in the range of 700-1250 °C with durations between 0 seconds and 24 hours. The diffusion-couple results show that Li diffusivity is very fast and starts already at very low temperature. Significant isotopic fractionation occurs due to the faster mobility of 6Li compared to 7Li. Boron diffusion is also accelerated by the presence of water, but the results of the isotopic ratios are unclear, and further investigation would be necessary to well constrain the isotopic fractionation process of boron in hydrous silicate melts. The isotopic ratios results show that boron isotopic fractionation might be affected by the speciation of boron in the silicate melt structure, as 10B and 11B tend to have tetrahedral and trigonal coordination, respectively.
Several decompression experiments were performed at 900 °C and 1000 °C, with pressures going from 300 MPa to 71-77 MPa and durations of 30 minutes, two, five and ten hours, in order to trigger water exsolution and the formation of vesicles in the sample. Textural observations and the calculation of the bubble number density confirmed that the bubble size and distribution after decompression is directly proportional to the decompression rate.
The overall SIMS results of Li and B show that the two trace elements tend to progressively decrease their concentration with decreasing decompression rates. This is explained because for longer decompression times, the diffusion of Li and B into the bubbles has more time to progress and the melt continuously loses volatiles as the bubbles expand their volumes.
For fast decompression, Li and B results show a concentration increase with a δ7Li and δ11B decrease close to the bubble interface, related to the sudden formation of the gas bubble, and the occurrence of a diffusion process in the opposite direction, from the bubble meniscus to the unaltered melt. When the bubble growth becomes dominant and Li and B start to exsolve into the gas phase, the silicate melt close to the bubble gets depleted in Li and B, because of a stronger diffusion of the trace elements into the bubble.
Our data are being applied to different models, aiming to combine the dynamics of bubble nucleation and growth with the evolution of trace elements concentration and isotopic ratios. Here, first considerations on these models will be presented, giving concluding remarks on this research study. All in all, the final remarks constitute a good starting point for further investigations. These results are a promising base to continue to study this process, and Li and B can indeed show clear dependences on decompression-related magma ascent rates in volcanic systems.
Changes in topography on Earth, particularly the growth of major mountain belts like the Central Andes, have a fundamental impact on regional and global atmospheric circulation patterns. These patterns, in turn, affect processes such as precipitation, erosion, and sedimentation. Over the last two decades, various geochemical, geomorphologic, and geologic approaches have helped identify when, where, and how quickly topography has risen in the past. The current spatio-temporal picture of Central Andean growth is now providing insight into which deep-Earth processes have left their imprint on the shape of the Earth's surface.
Two of the most controversial issues concerning the late Cenozoic evolution of the Andean orogen are the timing of uplift of the intraorogenic Puna plateau and its eastern border, the Eastern Cordillera, and ensuing changes in climatic and surface-process conditions in the intermontane basins of the NW-Argentine Andes. The Eastern Cordillera separates the internally drained, arid Puna from semi-arid intermontane basins and the humid sectors of the Andean broken foreland and the Subandean fold-and-thrust belt to the east. With elevations between 4,000 and 6,000 m the eastern flanks of the Andes form an efficient orographic barrier with westward-increasing elevation and asymmetric rainfall distribution and amount with respect to easterly moisture-bearing winds. This is mirrored by pronounced gradients in the efficiency of surface processes that erode and re-distribute sediment from the uplifting ranges. Although the overall pattern of deformation and uplift in this sector of the southern central Andes shows an eastward migration of deformation, a well-developed deformation front does not exist and uplift and associated erosion and sedimentary processes are highly disparate in space and time. In addition, periodic deformation within intermontane basins, and continued diachronous foreland uplifts associated with the reactivation of inherited basement structures furthermore make a rigorous assessment of the spatiotemporal uplift patterns difficult.
This thesis focuses on the tectonic evolution of the Eastern Cordillera of NW Argentina, the depositional history of its intermontane sedimentary basins, and the regional topographic evolution of the eastern flank of the Puna Plateau. The intermontane basins of the Eastern Cordillera and the adjacent morphotectonic provinces of the Sierras Pampeanas and the Santa Bárbara System are akin to reverse fault bounded, filled, and partly coalesced sedimentary basins of the Puna Plateau. In contrast to the Puna basins, however, which still form intact morphologic entities, repeated deformation, erosion, and re-filling have impacted the basins in the Eastern Cordillera. This has resulted in a rich stratigraphy of repeated basin fills, but many of these basins have retained vestiges of their early depositional history that may reach back in time when these areas were still part of a contiguous and undeformed foreland basin. Fortunately, these strata also contain abundant volcanic ashes that are not only important horizons to decipher tectono-sedimentary events through U-Pb geochronology and geochemical correlation, but they also represent terrestrial recorders of the hydrogen-isotope composition of ancient meteoric waters that can be compared to the isotopic composition of modern meteoric water. The ash horizons are thus unique recorders of past environmental conditions and lend themselves to tracking the development of rainfall barriers and tectonically forced climate and environmental change through time.
U-Pb zircon geochronology and paleocurrent reconstructions of conglomerate sequences in the Humahuaca Basin of the Eastern Cordillera at 23.5° S suggest that the basin was an integral part of a largely unrestricted depositional system until 4.2 Ma, which subsequently became progressively decoupled from the foreland by range uplifts to the east that forced easterly moisture-bearing winds to precipitate in increasingly eastward locations. Multiple cycles of severed hydrological conditions and drainage re-capture are identified together with these processes that were associated with basin filling and sediment evacuation, respectively. Moreover, systematic relationships among faults, regional unconformities and deformed landforms reveal a general pattern of intra-basin deformation that appears to be linked with basin-internal deformation during or subsequent to episodes of large-scale sediment removal. Some of these observations are supported by variations in the hydrogen stable isotope composition of volcanic glass from the Neogene to Quaternary sedimentary record, which can be related to spatiotemporal changes in topography and associated orographic effects. δDg values in the basin strata reveal two main trends associated with surface uplift in the catchment area between 6.0 and 3.5 Ma and the onset of semiarid conditions in the basin following the attainment of threshold elevations for effective orographic barriers to the east after 3.5 Ma. The disruption of sediment supply from western sources after 4.2 Ma and subsequent hinterland aridification, moreover, emphasize the possibility that these processes were related to lateral orogenic growth of the adjacent Puna Plateau. As a result of the hinterland aridification the regions in the orogen interior have been characterized by an inefficient fluvial system, which in turn has helped maintaining internal drainage conditions, sediment storage, and relief reduction within high-elevation basins.
The diachronous nature of basin formation and impacts on the fluvial system in the adjacent broken foreland is underscored by the results of detailed sediment provenance and paleocurrent analyses, as well as U-Pb zircon geochronology in the Lerma and Metán basins at ca. 25° S. This is particularly demonstrated by the isolated uplift of the Metán range at ~10 Ma, which is more than 50 km away from the presently active orogenic front along the eastern Puna margin and the Eastern Cordillera to the west. At about 5 Ma, Puna-sourced sediments disappear from the foreland record, documenting further range uplifts in the Eastern Cordillera and hydrological isolation of the neighboring Angastaco Basin from the foreland. Finally, during the late Pliocene and Quaternary, deformation has been accommodated across the entire foreland and is still active. To elucidate the interactions between tectonically controlled changes in elevation and their impact on atmospheric circulation processes in this region, this thesis provides additional, temporally well-constrained hydrogen stable isotope results of volcanic glass samples from the broken foreland, including the Angastaco Basin, and other intermontane basins farther south. The results suggest similar elevations of intermontane basins and the foreland sectors prior to ca. 7 Ma. In case of the Angastaco Basin the region was affected by km-scale surface uplift of the basin. A comparison with coeval isotope data collected from sedimentary sequences in the Puna plateau explains rapid shifts in the intermontane δDg record and supports the notion of recurring phases of enhanced deep convection during the Pliocene, and thus climatic conditions during the middle to late Pliocene similar to the present day.
Combined, field-based and isotope geochemical methods used in this study of the NW-Argentine Andes have thus helped to gain insight into the systematics, rate changes, interactions, and temporal characteristics among tectonically controlled deformation patterns, the build-up of topography impacting atmospheric processes, the distribution of rainfall, and resulting surface processes in a tectonically active mountain belt. Ultimately, this information is essential for a better understanding of the style and the rates at which non-collisional mountain belts evolve, including the development orogenic plateaus and their bordering flanks. The results presented in this study emphasize the importance of stable isotope records for paleoaltimetric and paleoenvironmental studies in mountain belts and furnishes important data for a rigorous interpretation of such records.
Groundwater transit time is an essential hydrologic metric for groundwater resources management. However, especially in tropical environments, studies on the transit time distribution (TTD) of groundwater infiltration and its corresponding mean transit time (mTT) have been extremely limited due to data sparsity. In this study, we primarily use stable isotopes to examine the TTDs and their mTTs of both vertical and horizontal infiltration at a riverbank infiltration area in the Vietnamese Mekong Delta (VMD), representative of the tropical climate in Asian monsoon regions. Precipitation, river water, groundwater, and local ponding surface water were sampled for 3 to 9 years and analysed for stable isotopes (delta O-18 and delta H-2), providing a unique data set of stable isotope records for a tropical region. We quantified the contribution that the two sources contributed to the local shallow groundwater by a novel concept of two-component lumped parameter models (LPMs) that are solved using delta O-18 records. The study illustrates that two-component LPMs, in conjunction with hydrological and isotopic measurements, are able to identify subsurface flow conditions and water mixing at riverbank infiltration systems. However, the predictive skill and the reliability of the models decrease for locations farther from the river, where recharge by precipitation dominates, and a low-permeable aquitard layer above the highly permeable aquifer is present. This specific setting impairs the identifiability of model parameters. For river infiltration, short mTTs (<40 weeks) were determined for sites closer to the river (<200 m), whereas for the precipitation infiltration, the mTTs were longer (>80 weeks) and independent of the distance to the river. The results not only enhance the understanding of the groundwater recharge dynamics in the VMD but also suggest that the highly complex mechanisms of surface-groundwater interaction can be conceptualized by exploiting two-component LPMs in general. The model concept could thus be a powerful tool for better understanding both the hydrological functioning of mixing processes and the movement of different water components in riverbank infiltration systems.
The isotopic composition of water in ice sheets is extensively used to infer past climate changes. In low-accumulation regions their interpretation is, however, challenged by poorly constrained effects that may influence the initial isotope signal during and after deposition of the snow. This is reflected in snow-pit isotope data from Kohnen Station, Antarctica, which exhibit a seasonal cycle but also strong interannual variations that contradict local temperature observations. These inconsistencies persist even after averaging many profiles and are thus not explained by local stratigraphic noise. Previous studies have suggested that post-depositional processes may significantly influence the isotopic composition of East Antarctic firn. Here, we investigate the importance of post-depositional processes within the open-porous firn (greater than or similar to 10 cm depth) at Kohnen Station by separating spatial from temporal variability. To this end, we analyse 22 isotope profiles obtained from two snow trenches and examine the temporal isotope modifications by comparing the new data with published trench data extracted 2 years earlier. The initial isotope profiles undergo changes over time due to downward advection, firn diffusion and densification in magnitudes consistent with independent estimates. Beyond that, we find further modifications of the original isotope record to be unlikely or small in magnitude (<< 1 parts per thousand RMSD). These results show that the discrepancy between local temperatures and isotopes most likely originates from spatially coherent processes prior to or during deposition, such as precipitation intermittency or systematic isotope modifications acting on drifting or loose surface snow.