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In order to gain further insights into early solar system aggregation processes, we carried out an experiment on board the International Space Station, which allowed us to study the behavior of dust particles exposed to electric arc discharges under long-term microgravity. The experiment led to the formation of robust, elongated, fluffy aggregates, which were studied by scanning electron microscopy, electron backscatter diffraction, and synchrotron micro-computed tomography. The morphologies of these aggregates strongly resemble the typical shapes of fractal fluffy-type calcium-aluminum-rich inclusions (CAIs). We conclude that a small amount of melting could have supplied the required stability for such fractal structures to have survived transportation and aggregation to and compaction within planetesimals. Other aggregates produced in our experiment have a massy morphology and contain relict grains, likely resulting from the collision of grains with different degrees of melting, also observed in some natural CAIs. Some particles are surrounded by igneous rims, which remind in thickness and crystal orientation of Wark–Lovering rims; another aggregate shows similarities to disk-shaped CAIs. These results imply that a (flash-)heating event with subsequent aggregation could have been involved in the formation of different morphological CAI characteristics.
Convective rain cell properties and the resulting precipitation scaling in a warm-temperate climate
(2022)
Convective precipitation events have been shown to intensify at rates exceeding the Clausius–Clapeyron rate (CC rate) of ca. 7% K−1 under current climate conditions. In this study, we relate atmospheric variables (low-level dew point temperature, convective available potential energy, and vertical wind shear), which are regarded as ingredients for severe deep convection, to properties of convective rain cells (cell area, maximum precipitation intensity, lifetime, precipitation sum, and cell speed). The rain cell properties are obtained from a rain gauge-adjusted radar dataset in a mid-latitude region, which is characterized by a temperate climate with warm summers (Germany). Different Lagrangian cell properties scale with dew point temperature at varying rates. While the maximum precipitation intensity of cells scales consistently at the CC rate, the area and precipitation sum per cell scale at varying rates above the CC rate. We show that this super-CC scaling is caused by a covarying increase of convective available potential energy with dew point temperature. Wind shear increases the precipitation sum per cell mainly by increasing the spatial cell extent. From a Eulerian point of view, this increase is partly compensated by a higher cell velocity, which leads to Eulerian precipitation scaling rates close to and slightly above the CC rate. Thus, Eulerian scaling rates of convective precipitation are modulated by convective available potential energy and vertical wind shear, making it unlikely that present scaling rates can be applied to future climate conditions. Furthermore, we show that cells that cause heavy precipitation at fixed locations occur at low vertical wind shear and, thus, move relatively slowly compared to typical cells.
Moisture sources of heavy precipitation in Central Europe in synoptic situations with Vb-cyclones
(2022)
During the past century, several extreme summer floods in Central Europe were associated with so-called Vb-cyclones propagating from the Mediterranean Sea north-eastward to Central Europe. The processes intensifying the precipitation in synoptic situations with Vb-cyclones in the Danube, Elbe, and Odra catchments are only partially understood. Our study aims to investigate these processes with Lagrangian moisture-source diagnostics for 16 selected Vb-events. Moreover, we analyse the characteristics of typical moisture source regions during 1107 Vb-events from 1901 to 2010 based on ERA-20C reanalysis dynamically downscaled with COSMO-CLM+NEMO. We observe moisture contributions by various source regions highlighting the complex dynamical interplay of different air masses leading to moisture convergence in synoptic situations with Vb-cyclones. Overall, up to 80% of the precipitation originates from the European continent, indicating the importance of continental moisture recycling, especially within the respective river catchment. Other major moisture uptake regions are the North Sea, the Baltic Sea, the North Atlantic, and for a few events the Black Sea. Remarkably, anomalies in these oceanic source regions show no connection to precipitation amounts in synoptic situations with Vb-cyclones. In contrast, the Vb-cyclones with the highest precipitation are associated with anomalously high evaporation in the Mediterranean Sea, even though the Mediterranean Sea is only a minor moisture source region on average. Interestingly, the evaporation anomalies are not connected with sea-surface temperature but with wind-speed anomalies (Spearman’s rank correlation coefficient R≈0.7, significant with p<0.01) indicating mainly dynamically driven evaporation. The particular role of the Mediterranean Sea hints towards possible importance of Mediterranean moisture for the early-stage intensification of Vb-cyclones and the pre-moistening of the continental uptake regions upstream of the target catchments.
The Yacoraite Formation (Salta rift, Argentina) consists of Maastrichtian–Danian lacustrine carbonate and siliciclastic deposits with interbedded volcanic ash layers, organized in four third-order stratigraphic sequences. It offers the exceptional opportunity to jointly apply in situ zircon and carbonate U-Pb geochronology that resulted in two distinct depositional age depth models. Ages of the youngest zircon population from ash layers were linearly interpolated to derive a zircon depositional age depth model. A carbonate depositional age depth model was instead obtained from dated carbonate phases including microbialites, ooids, oncoids of calcitic and dolomitic mineralogy as well as early lacustrine calcite cements. Mean ages were defined from different carbonate phases belonging to the same layer and then linearly interpolated. Sedimentation rates were calculated from both depth models between pairs of dated samples and used to estimate the age of sequence boundaries, as well as the duration of the four stratigraphic sequences. The zircon and carbonate depositional age depth models agree with biostratigraphic constraints and exhibit excellent consistency. The onset and end of sedimentation were estimated at 68.2 ± 0.9 Ma and 62.3 ± 0.6 Ma (duration ca 5.7 Ma) via zircon geochronology and at 67.9 ± 1.7 Ma and 61.9 ± 1.3 Ma (duration ca 6.0 Ma) via carbonate geochronology. Results from this study show that with suitable samples and a newly implemented working strategy, in situ U-Pb dating of depositional and early diagenetic carbonates represent a valuable chronostratigraphic tool for estimating sedimentation rate and duration in poorly time-framed depositional systems.
Atmospheric particles play an important role in the radiative balance of the Earth, as well as they affect human health and air quality. Hence, the chemical characterization constitutes a crucial task to determinate their properties, sources and fate. Particularly, the analysis of nanoparticles (d<100 nm) represents an analytical challenge, since these particles are abundant in number but have very little mass.
This accumulative thesis focuses on the chemical characterization of nanoparticles, performed in both laboratory and field studies. Here, I present four manuscripts, two of which are my main project as a lead author.
The first manuscript (Caudillo et al., 2021) focuses on the gas and the particle phase originated from biogenic precursor gases (α-pinene and isoprene). The experiments were performed in the CLOUD chamber at CERN to simulate pure biogenic new particle formation. Both gas and particle phases are measured with a nitrate CI-APi-TOF mass spectrometer, while the TD-DMA is coupled to it for particle-phase measurements, this setup allows a direct comparison as both measurements use the identical chemical ionization and detector. This study demonstrates the suitability of the TD-DMA for measuring newly formed nanoparticles and it confirms that isoprene suppresses new particle formation but contributes to the growth of newly formed particles.
The second manuscript (Caudillo et al., 2022) presents an intercomparison of four different techniques (including the TD-DMA) for measuring the chemical composition of SOA nanoparticles. The measurements were conducted in the CLOUD chamber. The intercomparison was done by contrasting the observed chemical composition, the calculated volatility, and the thermal desorption behavior (for the thermal desorption techniques). The methods generally agreed on the most important compounds that are found in the nanoparticles. However, they did see different parts of the organic spectrum. Potential explanations for these differences are suggested.
The third manuscript (Ungeheuer al., 2022) presents both laboratory and ambient measurements to investigate the ability of lubricant oil to form new particles. These new particles are an important source of ultrafine particles in the areas nearby large airports. The ambient measurements were performed downwind of Frankfurt International Airport, and it was found that the fraction of lubricant oil is largest in the smallest particles. In the laboratory, the main finding was that evaporated lubricant oil nucleates and forms new particles rapidly. The results suggest that nucleation of lubricant oil and subsequent particle growth can occur in the cooling exhaust plumes of aircraft-turbofans.
The fourth manuscript (Wang et al., 2022) is a new particle formation study in the CLOUD chamber at CERN. This study shows that nitric acid, sulfuric acid, and ammonia interact synergistically and rapidly form particles under upper free tropospheric conditions. These particles can grow by condensation (driven by the availability of ammonia) up to CCN sizes and INP particles. The ability of these particles to act as a CCN and INP was also investigated and it was found to be as efficient as for desert dust. This mechanism constitutes an important finding and it can account for previous observations of high concentrations of ammonia and ammonium nitrate over the Asia monsoon region.
Diamonds growing in the Earth’s mantle often trap inclusions of fluids that are highly saline in composition. These fluids are thought to emerge from deep in subduction zones and may also be involved in the generation of some of the kimberlite magmas. However, the source of these fluids and the mechanism of their transport into the mantle lithosphere are unresolved. Here, we present experimental results showing that alkali chlorides are stable solid phases in the mantle lithosphere below 110 km. These alkali chlorides are formed by the reaction of subducted marine sediments with peridotite and show identical K/Na ratios to fluid inclusions in diamond. At temperatures >1100°C and low pressures, the chlorides are unstable; here, potassium is accommodated in mica and melt. The reaction of subducted sediments with peridotite explains the occurrence of Mg carbonates and the highly saline fluids found in diamonds and in chlorine-enriched kimberlite magmas.
Metasomatic reaction zones between mafic and ultramafic rocks exhumed from subduction zones provide a window into mass-transfer processes at high pressure. However, accurate interpretation of the rock record requires distinguishing high-pressure metasomatic processes from inherited oceanic signatures prior to subduction. We integrated constraints from bulk-rock geochemical compositions and petrophysical properties, mineral chemistry, and thermodynamic modeling to understand the formation of reaction zones between juxtaposed metagabbro and serpentinite as exemplified by the Voltri Massif (Ligurian Alps, Italy). Distinct zones of variably metasomatized metagabbro are dominated by chlorite, amphibole, clinopyroxene, epidote, rutile, ilmenite, and titanite between serpentinite and eclogitic metagabbro. Whereas the precursor serpentinite and oxide gabbro formed and were likely already in contact in an oceanic setting, the reaction zones formed by diffusional Mg-metasomatism between the two rocks from prograde to peak, to retrograde conditions in a subduction zone. Metasomatism of mafic rocks by Mg-rich fluids that previously equilibrated with serpentinite could be widespread along the subduction interface, within the subducted slab, and the mantle wedge. Furthermore, the models predict that talc formation by Si-metasomatism of serpentinite in subduction zones is limited by pressure-dependent increase in the silica activity buffered by the serpentine-talc equilibrium. Elevated activities of aqueous Ca and Al species would also favor the formation of chlorite and garnet. Accordingly, unusual conditions or processes would be required to stabilize abundant talc at high P-T conditions. Alternatively, a different set of mineral assemblages, such as serpentine- or chlorite-rich rocks, may be controlling the coupling-decoupling transition of the plate interface.
Talc formation via silica-metasomatism of ultramafic rocks is believed to play key roles in subduction zone processes. Yet, the conditions of talc formation remain poorly constrained. We used thermodynamic reaction-path models to assess the formation of talc at the slab-mantle interface and show that it is restricted to a limited set of pressure–temperature conditions, protolith, and fluid compositions. In contrast, our models predict that chlorite formation is ubiquitous at conditions relevant to the slab-mantle interface of subduction zones. The scarcity of talc and abundance of chlorite is evident in the rock record of exhumed subduction zone terranes. Talc formation during Si-metasomatism may thus play a more limited role in volatile cycling, strain localization, and in controlling the decoupling-coupling transition of the plate interface. Conversely, the observed and predicted ubiquity of chlorite corroborates its prominent role in slab-mantle interface processes that previous studies attributed to talc.
Key Points:
Limited talc formation by Si-metasomatism of ultramafic rocks in subduction zones
Chlorite formation is likely pervasive at the slab-mantle interface
Preferential formation of chlorite has wide-ranging chemical and physical implications for subduction zone processes
Plain Language Summary: In subduction zones, talc can form during chemical reactions of mantle rocks with silica-enriched fluids at the interface between descending oceanic plates and the overriding mantle. Its formation and distribution in subduction zones are believed to affect the volatile budget, rheological properties, and the down-dip limit of the decoupling of the slab-mantle interface. Therefore, illuminating the conditions that facilitate talc formation at high pressure-temperature conditions is key in assessing its roles in fundamental subduction zone processes. Using thermodynamic reaction-path models, we show that the formation of talc at the slab-mantle interface is restricted to a limited set of environmental conditions, because its formation is highly sensitive to the compositions of the mantle rocks and reactant fluids. Contrary to common belief, talc is unlikely to form in high abundance in ultramafic rocks metasomatized by Si-rich slab-derived fluids. Rather, our models predict the ubiquitous formation of chlorite along with other silicate minerals during Si-metasomatism due to the competing effects from other dissolved components that favor their formation over talc. This study calls into question the importance of talc during Si-metasomatism in subduction zones but highlights the more predominant role of chlorite.
Garnet xenocrysts from kimberlites provide unique insights into the composition, structure and evolution of the subcontinental lithospheric mantle (SCLM). For example, different metasomatic events in the SCLM are reflected in compositional differences between garnet xenocrysts. As mantle metasomatism largely controls the physical and chemical properties of the SCLM, it exerts first order control over the genesis of kimberlitic magmas and diamond formation. However, dating mantle lithologies and processes is complicated by high ambient temperatures that allow the equilibration of most isotopic systems up to the time of kimberlite eruption. As a consequence, the temporal connection between metasomatic events in the mantle and kimberlite genesis is commonly ambiguous.
In this study, we applied LA-ICPMS U-Pb dating to 43 harzburgitic, lherzolithic and megacrystic garnet xenocrysts from the ~376 Ma diamondiferous V. Grib kimberlite, Russia, in order to investigate the link between different types of mantle metasomatism and kimberlite genesis.
Our results indicate that, with two possible exceptions, only harzburgitic garnet overlaps in age with the kimberlite eruption, whereas lherzolitic and megacrystic garnet crystals are ~20 to 130 million years older. Furthermore, garnet U-Pb ages and Ni-in-garnet temperatures of ~820 to 1200 °C do not correlate. This, and the high closure temperature of U-Pb in garnet (≥900 °C) suggests that the garnet U-Pb ages indeed reflect metasomatic events in the SCLM. However, the U-Pb ages could also reflect cooling ages. In this case, the metasomatic events recorded in the garnet crystals must still have occurred up to ~130 million years prior to the eruption of the V. Grib kimberlite.
These findings have far-reaching implications for the genesis of (diamondiferous) kimberlites, as they clearly show that the time lag between metasomatic events in the SCLM, as recorded in kimberlitic garnet xenocrysts, and kimberlite eruption may extend to tens of millions of years.
Fossil records of early solar irradiation and cosmolocation of the CAI factory: a reappraisal
(2021)
Calcium-aluminum–rich inclusions (CAIs) in meteorites carry crucial information about the environmental conditions of the nascent Solar System prior to planet formation. Based on models of 50V–10Be co-production by in-situ irradiation, CAIs are considered to have formed within ~0.1 AU from the proto-Sun. Here, we present vanadium (V) and strontium (Sr) isotopic co-variations in fine- and coarse-grained CAIs and demonstrate that kinetic isotope effects during partial condensation and evaporation best explain V isotope anomalies previously attributed to solar particle irradiation. We also report initial excesses of 10Be and argue that CV CAIs possess essentially a homogeneous level of 10Be, inherited during their formation. Based on numerical modeling of 50V–10Be co-production by irradiation, we show that CAI formation during protoplanetary disk build-up likely occurred at greater heliocentric distances than previously considered, up to planet-forming regions (~1AU), where solar particle fluxes were sufficiently low to avoid substantial in-situ irradiation of CAIs.