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Tectonics and geothermal gradients from subduction to collision in the NW Variscan Iberian Massif
(2022)
The earliest tectonometamorphic record of tectonic slices incorporated to the base of an orogen holds the key to understand how an orogen is built. The tectonic pile of the NW Iberian section of the Variscan Orogen includes tectonic slices separated by crustal-scale thrusts. The earliest tectonometamorphic record in the uppermost parautochthon is calculated at 11–14 kbar and 450–500°C (P-T gradient about 13°C/km), suggesting a subduction-related metamorphic recrystallization at lower pressure than the overlying Lower Allochthon. Early conditions calculated in the autochthon (9–10 kbar and 425–450°C; 16°C/km) point to a relatively ‘cold’ collisional setting. Higher thermal gradients obtained from some sections of the autochthon (11–12 kbar and 700–725°C; 21°C/km) and the Lower Parautochthon (7.5 kbar and 550–700°C; 24–31°C/km), correspond to more advanced and ‘hot’ stages of collision. New U–Pb monazite geochronology indicates a 318–311 Ma age for the final formation of HT domes in the region. We propose the rapid decrease in P-T gradient (from <10 to 16°C/km) documents a fail to sustain further burial along a regular subduction zone. We consider the subsequent increase in the geothermal gradient (from 16 to 31°C/km) as the culmination of previous crustal accretion and the onset of crustal underthrusting and later processes in a collisional stage. We propose these switches in the early tectonometamorphic record of individual tectonic slices as potential markers to track the transition from subduction to collision in collisional orogens.
While high-quality climate reconstructions of some past warm periods in the Cenozoic era now exist, the geological processes responsible for driving the observed longterm changes in atmospheric CO2 are not sufficiently well understood. The long-term change in atmospheric CO2 across the Cenozoic has been proposed to be driven by processes such as terrestrial weathering, organic carbon production and burial, reverse weathering, and volcanic degassing. One way of constraining the relative importance of the various driving forces proposed so far is to better understand the degree to which ocean chemistry has changed because the chemistry of seawater responds to geologic processes that drive atmospheric CO2. In addition, knowledge of the concentration of the major elements in seawater is crucial for accurately applying proxies such as those based on the boron isotopic composition and Mg/Ca of marine carbonates (a proxy for palaeo pH/CO2 and palaeotemperature, respectively). Previously reported records of seawater composition are primarily derived from fluid inclusions in marine evaporites; however, the results are sparse due to the limited availability of such deposits. In this thesis, changes in the Eocene seawater chemistry were reconstructed using trace element (elements/Ca) and isotopic (δ26Mg) proxies in a Larger Benthic Foraminifera (LBFs), i.e., Nummulites sp., to constrain the driving processes of long-term changes in seawater chemistry.
To achieve the objective of this thesis, first, a measurement protocol was established using LA-ICPMS to measure the K/Ca ratio simultaneously with other element/calcium ratios, which is challenging due to the interference of ArH+ on K+. Utilising this newly established measurement protocol, laboratory-cultured Operculina ammonoides grown at different seawater calcium concentrations ([Ca2+]), repeated at different temperatures, as well as modern O. ammonoides collected from different regions exhibiting a range of seawater parameters, were investigated. A significant correlation was observed between K/Casw and K/CaLBF, allowing K/CaLBF to potentially be used as a proxy for seawater major ion reconstructions. In addition, modern O. ammonoides demonstrated no significant influence of most seawater parameters (temperature, salinity, pH, or [CO32-]) on K/CaLBF. Modern O.
ammonoides were also assessed for their Mg isotopic composition (δ26Mg), revealing no significant effect of temperature or salinity on δ26MgLBF. Furthermore, the Mg isotopic fractionation in O. ammonoides was found to be close to that of inorganic calcite, indicating minimal vital effects in these large benthic foraminifera.
Operculina ammonoides is the nearest living relative of the abundant Eocene genus Nummulites, enabling the reconstruction of seawater chemistry using the calibration based on O. ammonoides. The trace elemental/calcium proxies, including Na/Ca, K/Ca, and Mg/Ca, as well as the δ26Mg proxy, were investigated in Eocene Nummulites. The result showed that during the Eocene, [Ca2+]sw was 1.6-2 times higher, while [K+]sw was ~2 times lower than the modern seawater composition. Furthermore, [Mg2+]sw decreased from the early Eocene (54.3− +9 7..69 mmol kg-1 at ~55 Ma) to Late Eocene (37.8− +4 4..3 4 mmol kg-1 at ~31 Ma), followed by
an increase toward modern seawater [Mg]. In contrast, the variability in δ26Mgsw values remained within a narrow range of ~0.3 ‰ throughout the Cenozoic. The reconstructed [Ca2+]sw agrees with the suggestion that Cenozoic seawater chemistry changes can be explained via a change in the seafloor spreading rate. When combined with existing records, the observed minimal change in δ26Mgsw with an increase in [Mg2+]sw suggests an additional possible role of a decrease in the formation of authigenic clay minerals coincident with the Cenozoic decline in deep ocean temperature, which is also supported by the increase in the [K+]sw reconstructed here for the first time. This finding highlights that the reduction in seafloor-spreading rate and decline in reverse weathering during the Cenozoic era has played a significant role in the evolution of seawater chemistry, emphasizing the importance of these processes in driving long-term changes in the carbon cycle.
Upper mantle shear zones are complex systems where deformation is commonly closely interacting with metamorphic (solid-solid) and/or melt/fluid-rock reactions. Here, feedback processes between deformation, reactions, grain size reduction and phase mixing result in strain weakening and the localization of deformation. The expression of these interlinked processes is portrayed by the microfabrics of strained peridotites and pyroxenites. The present thesis is focusing on these processes and their impact on the deformation in three upper mantle shear zones situated in the peridotite massifs of Lanzo (Italian Alps), Erro-Tobbio (Italian Alps) and Ronda (Betic Cordillera, Spain). In all three shear zones, the presence of melt led to phase mixing either by interstitial crystallization of pyroxenes from a Si-saturated and partially also highly evolved melt or by melt-rock reactions of pyroxene porphyroclasts with a Si-undersaturated melt. The effect of melt on the localization of strain is twofold and variable. Enhanced deformation by melt-wetted boundaries is assumed for all shear zones. Additionally, phase mixing by crystallization of interstitial pyroxenes or melt-rock reactions reduce or maintain the grain size by the formation of fine grained neoblasts and secondary phase boundary pinning. In this regard, pre- to early syn-kinematic, map-scale percolation of OH-bearing, evolved melts in the NW Ronda peridotite massif and the associated crystallization of interstitial pyroxenes result in the activation of grain size sensitive deformation mechanisms in the entire melt-effected area. In the rocks collected at Erro-Tobbio, syn-kinematic melt-rock reactions of pyroxene porphyroclasts and Si-undersaturated melt led to the formation of ultramylonitic neoblast tails (grain size ~10 μm). Compared to the adjacent coarser-grained olivine-dominated matrix, the activation of diffusion creep led to an increase in the strain rate by an order of magnitude within interconnected ultramylonitic layers. Strain localization and softening in ultramylonitic layers are also documented in the Lanzo samples. Neoblast tails of pyroxene porphyroclasts were likewise identified as their precursor. The phase assemblage of the tails, including ortho- and clinopyroxene, olivine, plagioclase, and spinel (± amphibole), and their geochemical trends suggest, unlike in Erro-Tobbio, a formation by continuous net-transfer reactions enhanced by the spinel lherzolite to plagioclase lherzolite transition.
The new results obtained from the three studied shear zones underscore the importance of reactions for the interlinked processes of grain size reduction, phase mixing, strain localization and strain softening in upper mantle shear zones. Concerning strain localization, the nature of the reaction (solid-solid, melt/fluid-rock) seems to play a subordinate role compared to its timing. Pre- to early syn-kinematic melt-triggered reactions result in strain localization along map-scale shear zones. Late stage syn-kinematic melt-rock or metamorphic reactions under high stress conditions are capable of localizing the deformation along discrete, sub-centimeter thick ultramylonites.
The metasomatised continental mantle may play a key role in the generation of some ore deposits, in particular mineral systems enriched in platinum-group elements (PGE) and Au. The cratonic lithosphere is the longest-lived potential source for these elements, but the processes that facilitate their pre-concentration in the mantle and their later remobilisation to the crust are not yet well-established. Here, we report new results on the petrography, major-element, and siderophile- and chalcophile-element composition of native Ni, base metal sulphides (BMS), and spinels in a suite of well-characterised, highly metasomatised and weakly serpentinised peridotite xenoliths from the Bultfontein kimberlite in the Kaapvaal Craton, and integrate these data with published analyses. Pentlandite in polymict breccias (failed kimberlite intrusions at mantle depth) has lower trace-element contents (e.g., median total PGE 0.72 ppm) than pentlandite in phlogopite peridotites and Mica-Amphibole-Rutile-Ilmenite-Diopside (MARID) rocks (median 1.6 ppm). Spinel is an insignificant host for all elements except Zn, and BMS and native Ni account for typically <25% of the bulk-rock PGE and Au. High bulk-rock Te/S suggest a role for PGE-bearing tellurides, which, along with other compounds of metasomatic origin, may host the missing As, Ag, Cd, Sb, Te and, in part, Bi that are unaccounted for by the main assemblage.
The close spatial relationship between BMS and metasomatic minerals (e.g., phlogopite, ilmenite) indicates that the lithospheric mantle beneath Bultfontein was resulphidised by metasomatism after initial melt depletion during stabilisation of the cratonic lithosphere. Newly-formed BMS are markedly PGE-poor, as total PGE contents are <4.2 ppm in pentlandite from seven samples, compared to >26 ppm in BMS in other peridotite xenoliths from the Kaapvaal craton. This represents a strong dilution of the original PGE abundances at the mineral scale, perhaps starting from precursor PGE alloy and small volumes of residual BMS. The latter may have been the precursor to native Ni, which occurs in an unusual Ni-enriched zone in a harzburgite and displays strongly variable, but overall high PGE abundances (up to 81 ppm). In strongly metasomatised peridotites, Au is enriched relative to Pd, and was probably added along with S. A combination of net introduction of S, Au +/− PGE from the asthenosphere and intra-lithospheric redistribution, in part sourced from subducted materials, during metasomatic events may have led to sulphide precipitation at ~80–120 km beneath Bultfontein. This process locally enhanced the metallogenic fertility of this lithospheric reservoir. Further mobilisation of the metal budget stored in these S-rich domains and upwards transport into the crust may require interaction with sulphide-undersaturated melts that can dissolve sulphides along with the metals they store.
Vor rund 60 Jahren ist das Buch Mensch und Raum von Otto Friedrich Bollnow erstmals erschienen. Der folgende Beitrag geht der Frage nach, inwieweit die Überlegungen des Philosophen (unter bestimmten Aspekten) noch heute aktuell sind. Bollnows Raum-Verständnis weicht in seiner phänomenologischen Orientierung geradezu grundlegend vom heute vorherrschenden sozialwissenschaftlichen Raumdenken ab. Umso mehr regt Bollnow dazu an, die Lehren des wissenschaftlichen Mainstream kritisch gegen den Strich zu lesen. Ins Zentrum der Suche nach heute möglicherweise bedeutsamen Themen und Methoden des Denkens rückt das Wohnen. Wie denkt Bollnow das Wohnen, und was sagt uns dies in einer Zeit, in der die Menschen ganz anders wohnen als in den 1950er Jahren? Brücken zu methodologisch benachbarten Theorien und Philosophen werden ebenso geschlagen (z. B. Heidegger, Dürckheim, Müller-Freienfels) wie zu anderen thematisch relevanten Arbeiten von Bollnow.
Reconstructing Oligocene-Miocene paleoelevation contributes to our understanding of the evolutionary history of the European Alps and sheds light on geodynamic and Earth’s surface processes involved in the development of Alpine topography. Despite being one of the most intensively explored mountain ranges worldwide, constraints on the elevation history of the European Alps, however, remain scarce. Here we present stable and clumped isotope geochemistry 15 measurements to provide a new paleoelevation estimate for the mid-Miocene (~14.5 Ma) European Central Alps. We apply stable isotope δ-δ paleoaltimetry on near sea level pedogenic carbonate oxygen isotope (δ18O) records from the Northern Alpine Foreland Basin (Swiss Molasse Basin) and high-Alpine phyllosilicate hydrogen isotope (δD) records from the Simplon Fault Zone (Swiss Alps). We further explore Miocene paleoclimate and paleoenvironmental conditions in the Swiss Molasse Basin through carbonate stable (δ18O, δ13C) and clumped (Δ47) isotope data from three foreland basin sections in different 20 alluvial megafan settings (proximal, mid-fan, and distal). Combined pedogenic carbonate δ18O values and Δ47 temperatures (30 ± 5°C) yield a near sea level precipitation δ18Ow value of -5.8 ± 0.2‰ and in conjunction with the high-Alpine phyllosilicate δD record suggest that the region surrounding the SFZ attained surface elevations of >4000 m no later than the mid-Miocene. Our near sea level δ18Ow estimate is supported by paleoclimate (iGCM Echam5-wiso) modeled δ18O values, which vary between -4.2 and -7.6‰ for the Northern Alpine Foreland Basin.
Stratospheric inorganic chlorine (Cly) is predominantly released from long-lived chlorinated source gases and, to a small extent, very short-lived chlorinated substances. Cly includes the reservoir species (HCl and ClONO2) and active chlorine species (i.e., ClOx). The active chlorine species drive catalytic cycles that deplete ozone in the polar winter stratosphere. This work presents calculations of inorganic chlorine (Cly) derived from chlorinated source gas measurements on board the High Altitude and Long Range Research Aircraft (HALO) during the Southern Hemisphere Transport, Dynamic and Chemistry (SouthTRAC) campaign in austral late winter and early spring 2019. Results are compared to Cly in the Northern Hemisphere derived from measurements of the POLSTRACC-GW-LCYCLE-SALSA (PGS) campaign in the Arctic winter of 2015/2016. A scaled correlation was used for PGS data, since not all source gases were measured. Using the SouthTRAC data, Cly from a scaled correlation was compared to directly determined Cly and agreed well. An air mass classification based on in situ N2O measurements allocates the measurements to the vortex, the vortex boundary region, and midlatitudes. Although the Antarctic vortex was weakened in 2019 compared to previous years, Cly reached 1687±19 ppt at 385 K; therefore, up to around 50 % of total chlorine was found in inorganic form inside the Antarctic vortex, whereas only 15 % of total chlorine was found in inorganic form in the southern midlatitudes. In contrast, only 40 % of total chlorine was found in inorganic form in the Arctic vortex during PGS, and roughly 20 % was found in inorganic form in the northern midlatitudes. Differences inside the two vortices reach as much as 540 ppt, with more Cly in the Antarctic vortex in 2019 than in the Arctic vortex in 2016 (at comparable distance to the local tropopause). To our knowledge, this is the first comparison of inorganic chlorine within the Antarctic and Arctic polar vortices. Based on the results of these two campaigns, the differences in Cly inside the two vortices are substantial and larger than the inter-annual variations previously reported for the Antarctic.
Biogenic organic precursors play an important role in atmospheric new particle formation (NPF). One of the major precursor species is α-pinene, which upon oxidation can form a suite of products covering a wide range of volatilities. Highly oxygenated organic molecules (HOMs) comprise a fraction of the oxidation products formed. While it is known that HOMs contribute to secondary organic aerosol (SOA) formation, including NPF, they have not been well studied in newly formed particles due to their very low mass concentrations. Here we present gas- and particle-phase chemical composition data from experimental studies of α-pinene oxidation, including in the presence of isoprene, at temperatures (−50 and −30 ∘C) and relative humidities (20 % and 60 %) relevant in the upper free troposphere. The measurements took place at the CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber. The particle chemical composition was analyzed by a thermal desorption differential mobility analyzer (TD-DMA) coupled to a nitrate chemical ionization–atmospheric pressure interface–time-of-flight (CI-APi-TOF) mass spectrometer. CI-APi-TOF was used for particle- and gas-phase measurements, applying the same ionization and detection scheme. Our measurements revealed the presence of C8−10 monomers and C18−20 dimers as the major compounds in the particles (diameter up to ∼ 100 nm). Particularly, for the system with isoprene added, C5 (C5H10O5−7) and C15 compounds (C15H24O5−10) were detected. This observation is consistent with the previously observed formation of such compounds in the gas phase. However, although the C5 and C15 compounds do not easily nucleate, our measurements indicate that they can still contribute to the particle growth at free tropospheric conditions. For the experiments reported here, most likely isoprene oxidation products enhance the growth of particles larger than 15 nm. Additionally, we report on the nucleation rates measured at 1.7 nm (J1.7 nm) and compared with previous studies, we found lower J1.7 nm values, very likely due to the higher α-pinene and ozone mixing ratios used in the present study.
Reconstructing Oligocene–Miocene paleoelevation contributes to our understanding of the evolutionary history of the European Alps and sheds light on geodynamic and Earth surface processes involved in the development of Alpine topography. Despite being one of the most intensively explored mountain ranges worldwide, constraints on the elevation history of the European Alps remain scarce. Here we present stable and clumped isotope measurements to provide a new paleoelevation estimate for the mid-Miocene (∼14.5 Ma) European Central Alps. We apply stable isotope δ–δ paleoaltimetry to near-sea-level pedogenic carbonate oxygen isotope (δ18O) records from the Northern Alpine Foreland Basin (Swiss Molasse Basin) and high-Alpine phyllosilicate hydrogen isotope (δD) records from the Simplon Fault Zone (Swiss Alps). We further explore Miocene paleoclimate and paleoenvironmental conditions in the Swiss Molasse Basin through carbonate stable (δ18O, δ13C) and clumped (Δ47) isotope data from three foreland basin sections in different alluvial megafan settings (proximal, mid-fan, and distal). Combined pedogenic carbonate δ18O values and Δ47 temperatures (30±5 ∘C) yield a near-sea-level precipitation δ18Ow value of ‰ and, in conjunction with the high-Alpine phyllosilicate δD value of ‰, suggest that the region surrounding the Simplon Fault Zone attained surface elevations of >4000 m no later than the mid-Miocene. Our near-sea-level δ18Ow estimate is supported by paleoclimate (iGCM ECHAM5-wiso) modeled δ18O values, which vary between −4.2 ‰ and −7.6 ‰ for the Northern Alpine Foreland Basin.
Stratospheric inorganic chlorine (Cly) is predominantly released from long-lived chlorinated source gases and, to a small extent, very short-lived chlorinated substances. Cly includes the reservoir species (HCl and ClONO2) and active chlorine species (i.e., ClOx). The active chlorine species drive catalytic cycles that deplete ozone in the polar winter stratosphere. This work presents calculations of inorganic chlorine (Cly) derived from chlorinated source gas measurements on board the High Altitude and Long Range Research Aircraft (HALO) during the Southern Hemisphere Transport, Dynamic and Chemistry (SouthTRAC) campaign in austral late winter and early spring 2019. Results are compared to Cly in the Northern Hemisphere derived from measurements of the POLSTRACC-GW-LCYCLE-SALSA (PGS) campaign in the Arctic winter of 2015/2016. A scaled correlation was used for PGS data, since not all source gases were measured. Using the SouthTRAC data, Cly from a scaled correlation was compared to directly determined Cly and agreed well. An air mass classification based on in situ N2O measurements allocates the measurements to the vortex, the vortex boundary region, and midlatitudes. Although the Antarctic vortex was weakened in 2019 compared to previous years, Cly reached 1687±19 ppt at 385 K; therefore, up to around 50 % of total chlorine was found in inorganic form inside the Antarctic vortex, whereas only 15 % of total chlorine was found in inorganic form in the southern midlatitudes. In contrast, only 40 % of total chlorine was found in inorganic form in the Arctic vortex during PGS, and roughly 20 % was found in inorganic form in the northern midlatitudes. Differences inside the two vortices reach as much as 540 ppt, with more Cly in the Antarctic vortex in 2019 than in the Arctic vortex in 2016 (at comparable distance to the local tropopause). To our knowledge, this is the first comparison of inorganic chlorine within the Antarctic and Arctic polar vortices. Based on the results of these two campaigns, the differences in Cly inside the two vortices are substantial and larger than the inter-annual variations previously reported for the Antarctic.
Biogenic organic precursors play an important role in atmospheric new particle formation (NPF). One of the major precursor species is α-pinene, which upon oxidation can form a suite of products covering a wide range of volatilities. Highly oxygenated organic molecules (HOMs) comprise a fraction of the oxidation products formed. While it is known that HOMs contribute to secondary organic aerosol (SOA) formation, including NPF, they have not been well studied in newly formed particles due to their very low mass concentrations. Here we present gas- and particle-phase chemical composition data from experimental studies of α-pinene oxidation, including in the presence of isoprene, at temperatures (−50 and −30 ∘C) and relative humidities (20 % and 60 %) relevant in the upper free troposphere. The measurements took place at the CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber. The particle chemical composition was analyzed by a thermal desorption differential mobility analyzer (TD-DMA) coupled to a nitrate chemical ionization–atmospheric pressure interface–time-of-flight (CI-APi-TOF) mass spectrometer. CI-APi-TOF was used for particle- and gas-phase measurements, applying the same ionization and detection scheme. Our measurements revealed the presence of C8−10 monomers and C18−20 dimers as the major compounds in the particles (diameter up to ∼ 100 nm). Particularly, for the system with isoprene added, C5 (C5H10O5−7) and C15 compounds (C15H24O5−10) were detected. This observation is consistent with the previously observed formation of such compounds in the gas phase. However, although the C5 and C15 compounds do not easily nucleate, our measurements indicate that they can still contribute to the particle growth at free tropospheric conditions. For the experiments reported here, most likely isoprene oxidation products enhance the growth of particles larger than 15 nm. Additionally, we report on the nucleation rates measured at 1.7 nm (J1.7 nm) and compared with previous studies, we found lower J1.7 nm values, very likely due to the higher α-pinene and ozone mixing ratios used in the present study.
Vor dem Hintergrund der zunehmenden Veränderung des städtischen Lebensumfeldes durch Gentrifizierung, investorenfreundliche Stadtpolitik, Privatisierung öffentlicher Räume, Einsparung öffentlicher Investitionen und den Abbau demokratischer Beteiligungsinstrumente haben wir uns gefragt: Wie könnte eine solidarische Stadt der Zukunft aussehen? Welche Gegenentwürfe zu aktuell herrschenden Paradigmen in der Stadtentwicklung zeigen uns Wege aus der Alternativlosigkeit hin zu einer solidarischen Praxis auf Quartiersebene? Im Rahmen einer angewandten kritischen Geografie möchten wir zeigen, dass es eine Vielzahl an Projekten und Initiativen gibt, die die Kreativlosigkeit, zu der uns der Neoliberalismus erzogen hat, durchbrechen und an konkreten Ideen und deren praktischer Umsetzung arbeiten. Als theoretische Annäherung dafür setzen wir uns mit Utopien und deren Potenzialen für eine politische Praxis auseinander. Da wir selbst im Kontext stadtpolitischer Gruppen engagiert sind, nutzen wir die aktivistische Stadtforschung als methodischen Rahmen unserer Forschung. Daraus entstanden ist ein Faltblatt, der „Kompass für ein solidarisches Quartier“, welcher als aktivistisches Werkzeug und Ideengeber für die konkrete Umsetzung transformativer Stadtpolitik dienen soll.
Lightning climate change projections show large uncertainties caused by limited empirical knowledge and strong assumptions inherent to coarse-grid climate modeling. This study addresses the latter issue by implementing and applying the lightning potential index parameterization (LPI) into a fine-grid convection-permitting regional climate model (CPM). This setup takes advantage of the explicit representation of deep convection in CPMs and allows for process-oriented LPI inputs such as vertical velocity within convective cells and coexistence of microphysical hydrometeor types, which are known to contribute to charge separation mechanisms. The LPI output is compared to output from a simpler flash rate parameterization, namely the CAPE × PREC parameterization, applied in a non-CPM on a coarser grid. The LPI’s implementation into the regional climate model COSMO-CLM successfully reproduces the observed lightning climatology, including its latitudinal gradient, its daily and hourly probability distributions, and its diurnal and annual cycles. Besides, the simulated temperature dependence of lightning reflects the observed dependency. The LPI outperforms the CAPE × PREC parameterization in all applied diagnostics. Based on this satisfactory evaluation, we used the LPI to a climate change projection under the RCP8.5 scenario. For the domain under investigation centered over Germany, the LPI projects a decrease of 4.8% in flash rate by the end of the century, in opposition to a projected increase of 17.4% as projected using the CAPE × PREC parameterization. The future decrease of LPI occurs mostly during the summer afternoons and is related to (i) a change in convection occurrence and (ii) changes in the microphysical mixing. The two parameterizations differ because of different convection occurrences in the CPM and non-CPM and because of changes in the microphysical mixing, which is only represented in the LPI lightning parameterization.
Global analysis of halogenated trace gases in the UTLS: from long-lived to short-lived substances
(2023)
In this dissertation, the distribution of chlorinated and brominated substances in the upper troposphere and lower stratosphere is investigated. These substances contribute significantly to the catalytic decomposition of ozone and are involved in the recurrent formation of the polar ozone hole in the Antarctic winter and spring. The Montreal Protocol, a multilateral environmental treaty to protect the ozone layer, has successfully reduced emissions of long-lived chlorine- and bromine-containing substances. Short-lived chlorinated and brominated substances, some of which are natural and anthropogenic in origin, are not regulated by the Montreal Protocol and it can be assumed that their relative contribution to the stratospheric halogen budget will increase, while the contribution of long-lived compounds will steadily decrease. The distribution of long- and short-lived halogenated substances are part of current research. For the upper troposphere and lower stratosphere, the very short-lived substances are particularly important. The lower stratosphere needs special investigation in this respect, since its composition is influenced by different transport processes. The influences on ozone trends in the lower stratosphere are subject to great uncertainties. Especially in the Southern Hemisphere, the number of observations is very limited.
In this work, the GhOST (Gas chromatograph for Observational Studies using Tracers) instrument was used during the SouthTRAC measurement campaign on the German HALO (High Altitude and LOng range) research aircraft, providing observations of halogenated hydrocarbons in Antarctic late winter to early spring 2019, a generally poorly sampled region. The polar vortex was, compared to previous years, significantly weaker and shifted towards the eastern South Pacific and South America. From the airborne measurements of chlorinated source gases, inorganic chlorine (the sum of active chlorine and reservoir gases; Cly) could be inferred with the result that Cly within the vortex increased up to 1687 ± 19 ppt at 385 K potential temperature, accounting for about 50 % of the total chlorine within the vortex and only 15 % of the total chlorine in the southern mid-latitudes. A comparison with the Northern Hemisphere could be made using the PGS measurement campaign in the Arctic winter 2015/2016. Under comparable conditions (season and distance from the tropopause), only 40 % of the total chlorine was in the inorganic form within the Arctic polar vortex and about 20 % was found in the mid-latitudes of the Northern Hemisphere. In addition, about 540 ppt more Cly was present in the Antarctic vortex than in the Arctic vortex, exceeding the annual variations previously reported for Antarctica.
The mean age of air plays an essential role in the derivation of Cly via the organic source gases, as was done in this work. A new method for determining the mean age of air from observational data has been introduced that accounts for extra-tropical input to the stratosphere in addition to tropical input. This new method was compared with the previously used method, which considered only the tropical input. The new method shows more realistic values especially near the tropopause. On average, the air of the lower stratosphere in the Northern Hemisphere was older than in the Southern Hemisphere by about 0.5 ± 0.3 years. About 65 K above the tropopause, the pattern changed with older air in the mid-latitudes of the Northern Hemisphere, but older air in high latitudes of the Southern Hemisphere, which implies differences in the strength and isolation of the respective polar vortex as well as the wave forcing in the shallow branch of the Brewer-Dobson circulation of the respective hemisphere. This is in good agreement with the distribution of Cly. The difference in the lower stratosphere was not clearly evident with the old method and it can be assumed that investigations of the differences in Cly of Northern and Southern Hemisphere will benefit from the new method.
Finally, the global and seasonal distribution of the two most important representatives of the short-lived brominated substances, CH2Br2 and CHBr3, was investigated. For this purpose, two additional HALO measurement campaigns have been used, the 2012 TACTS measurement campaign and the 2017 WISE measurement campaign, as well as the HIAPER Pole-to-Pole Observations (HIPPO) and Atmospheric Tomography (ATom) measurement campaigns. Observations of CH2Br2 show a pronounced seasonality in the free and upper troposphere of both hemispheres with slightly larger values in the Northern Hemisphere. CHBr3, on the other hand, shows a generally higher variability and lower seasonality with larger mixing ratios at mid and high latitudes in the northern hemispheric winter and autumn. A comparison of the lower stratosphere is limited to autumn and spring of both hemispheres due to the limited data basis of the observations. The distributions in each spring are similar (less than 0.1 ppt differences for e.g., CH2Br2). In hemispheric autumn, larger differences are evident with substantially smaller mixing ratios in the southern hemispheric lower stratosphere. This suggests that the transport processes of the two hemispheres may be different and implies that the input of tropospheric air (flushing) to the Northern Hemisphere lowest stratosphere is more efficient than in the Southern Hemisphere. Vertical profiles of CH2Br2 and CHBr3 in the mid-latitudes of both hemispheres and resulting vertical gradients support this conjecture. However, the Southern Hemisphere data set is insufficient to quantify this difference and further measurements are needed.
First-principles modeling techniques offer the ability to simulate a wide range of systems under different physical conditions, such as temperature, pressure, and composition, without relying on empirical knowledge. Density functional theory (DFT), a quantum mechanical method, has become an exceptionally successful framework for materials science modeling. Employing DFT makes it possible to gain valuable insights into the fundamental state of a system, enabling the reliable determination of equilibrium crystal structures. Over time, DFT has become an essential tool that can be incorporated into various schemes for predicting the properties of a material related to its structure, insulating/metallic behavior, magnetism, and optics. DFT is regularly applied in numerous fields, spanning from fundamental subjects in condensed matter physics to the study of large-scale phenomena in geosciences. In the latter, the effectiveness of DFT stems from its ability to simulate the properties found on the Earth, other planets, and meteorites, which may pose challenges for their direct study or laboratory investigation.
In this thesis, a comprehensive examination of a family of monosulfides and a perovskite heterostructure was conducted. These materials are relevant for their potential applications in technology, energy harvesting, and in the case of monosulfides, their speculated abundance on the planet Mercury.
Firstly, a DFT approach was used to analyze two non-magnetic monosulfides, CaS and MgS. We determined their structural properties and then focused on the modeling of their reflectivity in the infrared region. The calculation of the reflectivity considered both harmonic and anharmonic contributions. In the harmonic limit, the non-analytic correction was employed to accurately determine the LO/TO splitting, which is necessary to delimit the retstrahlend band, that is, the maximum of the reflectivity. The anharmonic effects given by up to three-phonon and isotopic scatterings, which were included using perturbation theory, primarily smeared the reflectivity spectra edges in the high-wave region.
Secondly, four polymorphs of MnS were studied using a combination of first-principles methods to simulate their antiferromagnetic (AFM) and paramagnetic (PM) states. The integration of DFT+$U$ with special quasirandom structures (SQS) supercells, and occupation matrix control techniques was crucial for achieving convergence, structural optimization accuracy, and obtaining finite energy band gaps and local magnetic moments in the PM phases. The addition of the Hubbard $U$ correction was necessary to treat the highly-correlated Mn $d$-electrons. The success of our approach was clear based on our electronic structure predictions for the PM rock-salt B1-MnS polymorph. Experimentally this phase has been observed to be an insulator, but multiple \emph{ab initio} works resulted previously in metallic behavior. Our computations, on the other hand, predicted insulating and magnetic properties that compare well with available measurements. Additionally, the pressure-field stability of the four MnS polymorphs was studied. In the case of the PM phases, B1-MnS was identified to be the most stable up to about 21 GPa, then transforming into the B31-MnS polymorph. This finding was in close agreement with high-pressure experiments reporting a similar phase transformation. The optical properties of B1-, B4-, and B31-MnS were also simulated. The SQS technique was used to obtain soft-mode-free phonon band structures within the harmonic approximation. Then, the anharmonic effects were included, and the reflectivity was calculated for B1-MnS and B4-MnS. In both cases, a good agreement for the LO/TO splitting was achieved in comparison to experimental results.
Lastly, the oxygen-deficient heterostructure of LaAlO$_{3-\delta}$ /SrTiO$_{3-\delta}$ was investigated also employing DFT+$U$, with a particular emphasis on the potential impact of vacancy clustering at the interface. Six distinct configurations of pairs of vacancies were studied and their energies were compared to find the most stable one. The orbital reconstruction of Ti orbitals was also examined based on their location with respect to the vacancies and the local magnetic moments were calculated. The final results showed that linearly arranged vacancies located opposite to Ti ions give the most energetically stable configuration.
Auf Basis ethnographischer Feldforschung untersucht der Beitrag den Zusammenhang zwischen prekären Wohnverhältnissen und der Entstehung politischer Kollektivität unter Mieter*innen. Theoretisch-konzeptionell knüpft er dabei an Debatten der kritischen Stadtforschung zu Verdrängungsprozessen, Forschungsarbeiten zu Prekarisierung sowie poststrukturalistisch inspirierte Perspektiven der sozialen Bewegungsforschung an. Empirisch ist der Blick gerichtet auf die Lebensrealitäten von Bewohner*innen einer Frankfurter Vonovia-Wohnsiedlung. Gefragt wird danach, wie Mieter*innen ihre Wohnsituation in Anbetracht drohender Mieterhöhungen infolge von Modernisierungsarbeiten wahrnehmen, welche Bedeutung sie der Wohnungsfrage zuschreiben und welche sozialräumlichen Bedingungen, Handlungspraktiken und diskursiven Deutungsmuster die Entwicklung einer kollektiven politischen Handlungsfähigkeit erschweren.
Due to massive energetic investments in woody support structures, trees are subject to unique physiological, mechanical, and ecological pressures not experienced by herbaceous plants. Despite a wealth of studies exploring trait relationships across the entire plant kingdom, the dominant traits underpinning these unique aspects of tree form and function remain unclear. Here, by considering 18 functional traits, encompassing leaf, seed, bark, wood, crown, and root characteristics, we quantify the multidimensional relationships in tree trait expression. We find that nearly half of trait variation is captured by two axes: one reflecting leaf economics, the other reflecting tree size and competition for light. Yet these orthogonal axes reveal strong environmental convergence, exhibiting correlated responses to temperature, moisture, and elevation. By subsequently exploring multidimensional trait relationships, we show that the full dimensionality of trait space is captured by eight distinct clusters, each reflecting a unique aspect of tree form and function. Collectively, this work identifies a core set of traits needed to quantify global patterns in functional biodiversity, and it contributes to our fundamental understanding of the functioning of forests worldwide.
The Izu–Bonin–Mariana volcanic arc is situated at a convergent plate margin where subduction initiation triggered the formation of MORB-like forearc basalts as a result of decompression melting and near-trench spreading. International Ocean Discovery Program (IODP) Expedition 352 recovered samples within the forearc basalt stratigraphy that contained unusual macroscopic globular textures hosted in andesitic glass (Unit 6, Hole 1440B). It is unclear how these andesites, which are unique in a stratigraphic sequence dominated by forearc basalts, and the globular textures therein may have formed. Here, we present detailed textural evidence, major and trace element analysis, as well as B and Sr isotope compositions, to investigate the genesis of these globular andesites. Samples consist of K2O-rich basaltic globules set in a glassy groundmass of andesitic composition. Between these two textural domains a likely hydrated interface of devitrified glass occurs, which, based on textural evidence, seems to be genetically linked to the formation of the globules. The andesitic groundmass is Cl rich (ca. 3000 µg/g ), whereas globules and the interface are Cl poor (ca. 300 µg/g ). Concentrations of fluid-mobile trace elements also appear to be fractionated in that globules and show enrichments in B, K, Rb, Cs, and Tl, but not in Ba and W relative to the andesitic groundmass, whereas the interface shows depletions in the latter, but is enriched in the former. Interestingly, globules and andesitic groundmass have identical Sr isotopic composition within analytical uncertainty ( 87Sr∕86Sr of 0.70580 ± 10 ), indicating that they likely formed from the same source. However, globules show high δ11 B (ca. + 7 ‰ ), whereas their host andesites are isotopically lighter (ca. – 1 ‰ ), potentially indicating that whatever process led to their formation either introduced heavier B isotopes to the globules, or induced stable isotope fractionation of B between globules and their groundmass. Based on the bulk of the textural information and geochemical data obtained from these samples, we conclude that these andesites likely formed as a result of the assimilation of shallowly altered oceanic crust (AOC) during forearc basaltic magmatism. Assimilation likely introduced radiogenic Sr, as well as heavier B isotopes to comparatively unradiogenic and low δ11B forearc basalt parental magmas (average 87Sr∕86Sr of 0.703284). Moreover, the globular textures are consistent with their formation being the result of fluid-melt immiscibility that was potentially induced by the rapid release of water from assimilated AOC whose escape likely formed the interface. If the globular textures present in these samples are indeed the result of fluid-melt immiscibility, then this process led to significant trace element and stable isotope fractionation. The textures and chemical compositions of the globules highlight the need for future experimental studies aimed at investigating the exsolution process with respect to potential trace element and isotopic fractionation in arc magmas that have perhaps not been previously considered.
Observed weather and projected climate change suggest an increase in the transmission of vector-borne diseases (VBDs) in the Hindu Kush Himalayan (HKH) region. In this study, we systematically explore the literature for empiric associations between the climate variables and specific VBDs and their vectors in the HKH region. We conducted a systematic synthesis of the published literature on climate variables, VBDs and vectors in the HKH region until the 8th of December 2020. The majority of studies show significant positive associations of VBDs with climatic factors, such as temperature, precipitation, relative humidity, etc. This systematic review allowed us to identify the most significant variables to be considered for evidence-based trend estimates of the effects of climate change on VBDs and their vectors in the HKH region. This evidence-based trend was set into the context of climate change as well as the observed expansion of VBDs and disease vectors in the HKH region. The geographic range of VBDs expanded into previously considered non-endemic areas of highlands (mountains) in the HKH region. Based on scarce, but clear evidence of a positive relationship of most climate variables and VBDs and the observed climatic changes, we strongly recommend an expansion of vector control and surveillance programmes in areas of the HKH region that were previously considered to be non-endemic.
In this dissertation, different aspects of turbulent transport and thermally driven flows over complex terrain are investigated. Two publications concentrate on the vertical heat and moisture exchange in the convective boundary layer over mountainous terrain. To study this, Large-Eddy Simulation (LES) is used. Both turbulent and advective transport mechanisms are evaluated over the simple orography of a quasi-two-dimensional, periodic valley with prescribed surface fluxes. Here, terrain elevation varies along only one of the horizontal coordinate axes. Even a relatively shallow orography, possibly unresolved in existing numerical weather prediction models, modifies the domain-averaged moisture and temperature profiles. For the analysis, the flow is decomposed into a local turbulent part, a local mean circulation, and a large-scale part. An analysis of the turbulent kinetic energy and turbulent heat and moisture flux budgets shows that the thermal circulation significantly contributes to the vertical transport. It is found that thermal upslope winds are important for the moisture transport from the valley to the mountain tops. In total, moisture export out of the valley is mostly accomplished by the mean circulation. On the temperature distribution, which is horizontally relatively homogeneous, the thermal circulation has a weaker impact. If an upper-level wind is present, it interacts with the thermal circulation. This weakens the vertical transport of moisture and thus reduces its export out of the valley. The heat transport is less affected by the upper-level wind because of its weaker dependence on the thermal circulation. These findings were corroborated in a more realistic experiment simulating the full diurnal cycle using radiation forcing and an interactive land surface model.
Based on these results, coherent turbulent structures in the convective boundary layer over non-flat terrain are studied in further detail. A conditional sampling method based on the concentration of a decaying passive tracer is implemented in order to identify the boundary-layer plumes objectively. Conditional sampling allows to quantify the contribution of plume structures to the vertical transport of heat and moisture. In case of the idealized valley, vertical transport by coherent structures is the dominant contribution to the turbulent components of both heat and moisture flux. It is comparable in magnitude to the advective transport by the mean slope-wind circulation, although it is more important for heat than for moisture transport. A set of less idealized simulations considers the flow over three-dimensional terrain. In this case, conditional sampling is carried out by using a simple domain-decomposition approach. We demonstrate that thermal updrafts are generally more frequent on hill tops than over the surroundings, but they are less persistent on the windward sides when large-scale winds are present in the free atmosphere.
The tools for flow decomposition and budget analysis are also applied in another idealized case with a quasi-two-dimensional valley featuring the stable boundary layer. Here, the formation of a low stratus cloud is investigated. The main driver for the cloud formation is radiative cooling due to outgoing longwave radiation. Despite a purely horizontal flow, the advection terms in the prognostic equations for heat and moisture produce vertical mixing across the upper cloud edge leading to a loss of cloud water content. However, this behavior is not due to any kind of thermally-driven circulation. Instead, this spurious mixing is caused by the diffusive error of the advection scheme in regions where the sloping surfaces of the terrain-following vertical coordinate intersect the cloud top. It is shown that the intensity of the (spurious) numerical diffusion strongly depends on the horizontal resolution, the order of advection, and the choice of the scalar advection scheme. A LES with 4 m horizontal resolution serves as a reference. For horizontal resolutions of a few hundred meters, carried out with a model setup as it is used in Numerical Weather Prediction, a strong reduction of the simulated liquid-water path is observed. In order to keep the (spurious) numerical diffusion at coarser resolutions small, at least a fifth-order advection scheme should be used. In the present case, a WENO scalar advection scheme turns out to increase the numerical diffusion along a sharp cloud edge compared to an upwind scheme. Furthermore, the choice of the vertical coordinate has a strong impact on the simulated liquid-water path over orography. With a modified definition of the terrain-following sigma coordinate, it is possible to produce cloud water where the classical sigma coordinate does not allow any cloud formation.
An update of the two-energy turbulence scheme is presented, the 2TE + APDF scheme. The original version of the two-energy scheme is able to successfully model shallow convection without the need of an additional parameterization for non-local fluxes. However, the performance of the two-energy scheme is worse in stratocumulus cases, where it tends to overestimate the erosion of the stable layers. We have identified the causes: the non-local stability parameter does not consider local stratification, the scheme lacks an internal parameter that could distinguish between a shallow convection regime and a stratocumulus regime, and it uses an inflexible turbulence length scale formulation. To alleviate this problem, we propose several modifications: an update of the stability parameter, a modified computation of the turbulence length scale, and the introduction of the entropy potential temperature to distinguish between a shallow convection and a stratocumulus regime. In addition, the two-energy scheme is coupled to a simplified assumed probability density function method in order to achieve a more universal representation of the cloudy regimes. The updated turbulence scheme is evaluated for several idealized cases and one selected real case in the ICOsahedral Nonhydrostatic (ICON) modeling framework. The results show that the updated scheme corrects the overmixing problem in the stratocumulus cases. The performance of the updated scheme is comparable to the operational setup, and can be thus used instead of the operational turbulence and shallow convection scheme in ICON. Additionally, the updated scheme improves the coupling with dynamics, which is beneficial for the modeling of coherent flow structures in the atmospheric boundary layer.
The accessories perovskite, pyrochlore, zirconolite, calzirtite and melanite from carbonatites and carbonate-rich foidites from the Kaiserstuhl are variously suited for the in situ determination of their U–Pb ages and Sr, Nd- and Hf-isotope ratios by LA-ICP-MS. The 143Nd/144Nd ratios may be determined precisely in all five phases, the 176Hf/177Hf ratios only in calzirtite and the 87Sr/86Sr ratios in perovskites and pyrochlores. The carbonatites and carbonate-rich foidites belong to one of the three magmatic groups that Schleicher et al. (1990) distinguished in the Kaiserstuhl on the basis of their Sr, Nd and Pb isotope ratios. Tephrites, phonolites and essexites (nepheline monzogabbros) form the second and limburgites (nepheline basanites) and olivine nephelinites the third. Our 87Sr/86Sr isotope data from the accessories overlap with the carbonatite and olivine nephelinite fields defined by Schleicher et al. (1990) but exhibit a much narrower range. These and the εNd and εHf values plot along the mantle array in the field of oceanic island basalts relatively close to mid-ocean ridge basalts. Previously reported K–Ar, Ar–Ar and fission track ages for the Kaiserstuhl lie between 16.2 and 17.8 Ma. They stem entirely from the geologically older tephrites, phonolites and essexites. No ages existed so far for the geologically younger carbonatites and carbonate-rich foidites except for one apatite fission track age (15.8 Ma). We obtained precise U–Pb ages for zirconolites and calzirtites of 15.66, respectively 15.5 Ma (± 0.1 2σ) and for pyrochlores of 15.35 ± 0.24 Ma. Only the perovskites from the Badberg soevite yielded a U–P concordia age of 14.56 ± 0.86 Ma while the perovskites from bergalites (haüyne melilitites) only gave 206Pb/238U and 208Pb/232Th ages of 15.26 ± 0.21, respectively, 15.28 ± 0.48 Ma. The main Kaiserstuhl rock types were emplaced over a time span of 1.6 Ma almost 1 million years before the carbonatites and carbonate-rich foidites. These were emplaced within only 0.32 Ma.
Living on the edge: environmental variability of a shallow late Holocene cold-water coral mound
(2022)
Similar to their tropical counterparts, cold-water corals (CWCs) are able to build large three-dimensional reef structures. These unique ecosystems are at risk due to ongoing climate change. In particular, ocean warming, ocean acidification and changes in the hydrological cycle may jeopardize the existence of CWCs. In order to predict how CWCs and their reefs or mounds will develop in the near future one important strategy is to study past fossil CWC mounds and especially shallow CWC ecosystems as they experience a greater environmental variability compared to other deep-water CWC ecosystems. We present results from a CWC mound off southern Norway. A sediment core drilled from this relatively shallow (~ 100 m) CWC mound exposes in full detail hydrographical changes during the late Holocene, which were crucial for mound build-up. We applied computed tomography, 230Th/U dating, and foraminiferal geochemical proxy reconstructions of bottom-water-temperature (Mg/Ca-based BWT), δ18O for seawater density, and the combination of both to infer salinity changes. Our results demonstrate that the CWC mound formed in the late Holocene between 4 kiloannum (ka) and 1.5 ka with an average aggradation rate of 104 cm/kiloyears (kyr), which is significantly lower than other Holocene Norwegian mounds. The reconstructed BWTMg/Ca and seawater density exhibit large variations throughout the entire period of mound formation, but are strikingly similar to modern in situ observations in the nearby Tisler Reef. We argue that BWT does not exert a primary control on CWC mound formation. Instead, strong salinity and seawater density variation throughout the entire mound sequence appears to be controlled by the interplay between the Atlantic Water (AW) inflow and the overlying, outflowing Baltic-Sea water. CWC growth and mound formation in the NE Skagerrak was supported by strong current flow, oxygen replenishment, the presence of a strong boundary layer and larval dispersal through the AW, but possibly inhibited by the influence of fresh Baltic Water during the late Holocene. Our study therefore highlights that modern shallow Norwegian CWC reefs may be particularly endangered due to changes in water-column stratification associated with increasing net precipitation caused by climate change.
We performed an experiment under long-term microgravity conditions aboard the International Space Station (ISS) to obtain information on the energetics and experimental constraints required for the formation of chondrules in the solar nebula by ’nebular lightning’. As a simplified model system, we exposed porous forsterite (Mg2 SiO4) dust particles to high-energetic arc discharges. The characterization of the samples after their return by synchrotron microtomography and scanning electron microscopy revealed that aggregates had formed, consisting of several fused Mg2SiO4 particles. The partial melting and fusing of Mg2SiO4 dust particles under microgravity conditions leads to a strong reduction of their porosity. The experimental outcomes vary strongly in their appearance from small spherical melt-droplets (∅≈90 µm) to bigger and irregularly shaped aggregates (∅≈350 µm). Our results provided new constraints with respect to energetic aspects of chondrule formation and a roadmap for future and more complex experiments on Earth and in microgravity conditions.
Several past summer floods in Central Europe were associated with so-called Vb‑cyclones propagating from the Mediterranean Sea north-eastward to Central Europe. This study illustrates the usefulness of the parametric transfer entropy measure TE‑linear in investigating heavy Vb‑cyclone precipitation events in the Odra catchment (Poland). With the application of the TE‑linear approach, we confirm the impact of the Mediterranean Sea on precipitation intensification. Moreover, we also detect significant information exchange to Vb‑cyclone precipitation from evaporation over the European continent along the typical Vb‑cyclone pathway. Thus, the Mediterranean Sea could enhance the Vb‑cyclone precipitation by pre-moistening continental moisture source regions that contribute to precipitation downstream in the investigated catchments. Overall, the transfer entropy approach with the measure TE‑linear proved to be computationally effective and complementary to traditional methods such as Lagrangian and Eulerian diagnostics.
The infrastructure for parking and parked cars themselves (e.g., parked cars blocking bike lanes and sidewalks or the visibility range) can lead to conflicts for pedestrians and cyclists. The perception of conflicts could discourage walking and cycling in neighborhoods and undermine municipalities’ efforts to provide more sustainable urban mobility. The aim of this study was therefore to analyze the effect of on-street car parking in urban neighborhoods on perceived parking and traffic-related conflicts. In addition, it examines in what way the intention to reduce one’s car use influences the perception of the conflicts (Stage Model of Self-Regulated Behavior Change (SSBC)). A household survey was conducted in the inner-city neighborhood of Frankfurt-Bornheim, Germany (N=1027). The residents most often observed the conflicts in which parked cars impeded walking and cycling as well as situations in which pedestrians felt threatened by cyclists biking on the sidewalk. Results from multiple linear regression models revealed that the influencing factors for the perception of conflicts were the use of different means of transportation and the intention to change one’s behavior (SSBC model) to reduce car use rather than car ownership. In addition, a resident’s age and household structure seemed to affect awareness of conflicts in which pedestrians and cyclists were involved. The results suggest a group-serving bias, meaning that the residents mostly observed those conflicts that they did not cause. A separate infrastructure for pedestrians and cyclists could help prevent most of the conflicts described in this study.
Climatic and biogeographical drivers of functional diversity in the flora of the Canary Islands
(2022)
Aim: Functional traits can help us to elucidate biogeographical and ecological processes driving assemblage structure. We analysed the functional diversity of plant species of different evolutionary origins across an island archipelago, along environmental gradients and across geological age, to assess functional aspects of island biogeographical theory.
Location: Canary Islands, Spain.
Major taxa studied: Spermatophytes.
Time period: Present day.
Methods: We collected data for four traits (plant height, leaf length, flower length and fruit length) associated with resource acquisition, competitive ability, reproduction and dispersal ability of 893 endemic, non-endemic native and alien plant species (c. 43% of the Canary Island flora) from the literature. Linking these traits to species occurrences and composition across a 500 m × 500 m grid, we calculated functional diversity for endemic, non-endemic native and alien assemblages using multidimensional functional hypervolumes and related the resulting patterns to climatic (humidity) and island biogeographical (geographical isolation, topographic complexity and geological age) gradients.
Results: Trait space of endemic and non-endemic native species overlapped considerably, and alien species added novel trait combinations, expanding the overall functional space of the Canary Islands. We found that functional diversity of endemic plant assemblages was highest in geographically isolated and humid grid cells. Functional diversity of non-endemic native assemblages was highest in less isolated and humid grid cells. In contrast, functional diversity of alien assemblages was highest in arid ecosystems. Topographic complexity and geological age had only a subordinate effect on functional diversity across floristic groups.
Main conclusions: We found that endemic and non-endemic native island species possess similar traits, whereas alien species tend to expand functional space in ecosystems where they have been introduced. The spatial distribution of the functional diversity of floristic groups is very distinct across environmental gradients, indicating that species assemblages of different evolutionary origins thrive functionally in dissimilar habitats.
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.
Titanite is a potentially powerful U–Pb petrochronometer that may record metamorphism, metasomatism, and deformation. Titanite may also incorporate significant inherited Pb, which may lead to inaccurate and geologically ambiguous U–Pb dates if a proper correction is not or cannot be applied. Here, we present laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS)-derived titanite U–Pb dates and trace element concentrations for two banded calcsilicate gneisses from south-central Maine, USA (SSP18-1A and SSP18-1B). Single spot common Pb-corrected dates range from 400 to 280 Ma with ±12–20 Ma propagated 2SE. Titanite grains in sample SSP18-1B exhibit regular core-to-rim variations in texture, composition, and date. We identify four titanite populations: (1) 397 ± 5 Ma (95% CL) low Y + HREE cores and mottled grains, (2) 370 ± 7 Ma high Y + REE mantles and cores, (3) 342 ± 6 Ma cores with high Y + REE and no Eu anomaly, and (4) 295 ± 6 Ma LREE-depleted rims. We interpret the increase in titanite Y + HREE between ca. 397 and ca. 370 Ma to constrain the timing of diopside fracturing and recrystallization and amphibole breakdown. Apparent Zr-in-titanite temperatures (803 ± 36°C at 0.5 ± 0.2 GPa) and increased XDi suggest a thermal maximum at ca. 370 Ma. Population 3 domains dated to ca. 342 Ma exhibit no Eu anomaly and are observed only in compositional bands dominated by diopside (>80 vol%), suggesting limited equilibrium between titanite and plagioclase. Finally, low LREE and high U/Th in Population 4 titanite dates the formation of hydrous phases, such as allanite, during high XH2O fluid infiltration at ca. 295 Ma. In contrast to the well-defined date–composition–texture relationships observed for titanite from SSP18-1B, titanite grains from sample SSP18-1A exhibit complex zoning patterns and little correlation between texture, composition, and date. We hypothesize that the incorporation of variable amounts of radiogenic Pb from dissolved titanite into recrystallized domains resulted in mixed dates spanning 380–330 Ma. Although titanite may reliably record multiple phases of metamorphism, these data highlight the importance of considering U–Pb data along with chemical and textural data to screen for inherited radiogenic Pb.
Reliable identification of chondrules, calcium-aluminum-rich inclusions (CAIs), carbonate grains, and Ca-phosphate grains at depth within untouched, unprepared chondritic samples by a nondestructive analytical method, such as synchrotron X-ray fluorescence (SXRF) computed tomography (CT), is an essential first step before intrusive analytical and sample preparation methods are performed. The detection of a local Ca-enrichment could indicate the presence of such a component, all of which contain Ca as major element and/or Ca-bearing minerals, allowing it to be precisely located at depth within a sample. However, the depth limitation from which Ca-K fluorescence can travel through a chondrite sample (e.g., ∼115 µm through material of 1.5 g cm−3) to XRF detectors leaves many Ca-bearing components undetected at deeper depths. In comparison, Sr-K lines travel much greater distances (∼1700 µm) through the same sample density and are, thus, detected from much greater depths. Here, we demonstrate a clear, positive, and preferential correlation between Ca and Sr and conclude that Sr-detection can be used as proxy for the presence of Ca (and, thus, Ca-bearing components) throughout mm-sized samples of carbonaceous chondritic material. This has valuable implications, especially for sample return missions from carbonaceous C-type asteroids, such as Ryugu or Bennu. Reliable localization, identification, and targeted analysis by SXRF of Ca-bearing chondrules, CAIs, and carbonates at depth within untouched, unprepared samples in the initial stages of a multianalysis investigation insures the valuable information they hold of pre- and post-accretion processes in the early solar system is neither corrupted nor destroyed in subsequent processing and analyses.
Questions: Both species turnover and intraspecific trait variation can affect plant assemblage dynamics along environmental gradients. Here, we asked how community assemblage patterns in relation to species turnover and intraspecific variation differ between endemic and non-endemic species. We hypothesized that endemic species show lower intraspecific variation than non-endemic species because they tend to have high rates of in situ speciation, whereas non-endemic species are expected to have a larger gene pool and higher phenotypic plasticity.
Location: La Palma, Canary Islands.
Methods: We established 44 sampling sites along a directional gradient of precipitation, heat load, soil nitrogen, phosphorus and pH. Along this gradient, we estimated species abundances and measured three traits (plant height, leaf area and leaf thickness) on perennial endemic and non-endemic plant species. In total, we recorded traits for 1,223 plant individuals of 43 species. Subsequently, we calculated community-weighted mean traits to measure the relative contribution of species turnover, intraspecific variation and their covariation along the analysed gradient.
Results: The contribution of intraspecific variation to total variation was similar in endemic and non-endemic assemblages. For plant height, intraspecific variation explained roughly as much variation as species turnover. For leaf area and leaf thickness, intraspecific variation explained almost no variation. Species turnover effects mainly drove trait responses along the environmental gradient, but intraspecific variation was important for responses in leaf area to precipitation.
Conclusions: Despite their distinct evolutionary history, endemic and non-endemic plant assemblages show similar patterns in species turnover and intraspecific variation. Our results indicate that species turnover is the main component of trait variation in the underlying study system. However, intraspecific variation can increase individual species’ fitness in response to precipitation. Overall, our study challenges the theory that intraspecific trait variation is more important for the establishment of non-endemic species compared with endemic species.
Positive plant–plant interactions are thought to drive vegetation patterns in harsh environments, such as semi-arid areas. According to the stress-gradient hypothesis (SGH), the role of positive interactions between species (facilitation) is expected to increase with harshness, predicting associated variation in species composition along environmental gradients. However, the relation between stress and facilitation along environmental gradients is debated. Furthermore, differentiating facilitative interactions from other underlying mechanisms, such as microtopographic heterogeneity, is not trivial. We analysed the spatial co-occurrence relationships of vascular plant species that form patchy vegetation in arid lapilli fields (tephra) from recent volcanic eruptions on La Palma, Canary Islands. Assuming a harshness gradient negatively correlated with elevation because the lower elevations are more arid and water availability is considered the most limiting resource, and that an outcome of facilitation is plants co-occurring in the same patch, from the SGH we expected a greater degree of co-occurrence at lower elevation. We tested this at both the species and the individual plant level. We analysed the species composition of 1277 shrubby vegetation patches at 64 different sampling points, ranging from the coast to around 700 m a.s.l. Patch morphology and microtopographic heterogeneity variables were also measured, to account for their potential effects on the species composition of patches. We used generalized linear models and generalized mixed-effects models to analyse species richness, number of individuals in patches and percentage of patches with positive co-occurrences, and a pairwise co-occurrence analysis combined with a graphical network analysis to reveal positive links between 13 of the species. We found that the percentage of patches with positive co-occurrences increased at higher elevations, in contrast to the predictions of the SGH, but in accordance with a refined stress-gradient hypothesis for arid sites, in which characteristics of the interacting species are incorporated.
This thesis presents the experimental and numerical analysis of seismic waves that are produced by wind farms. With the aim to develop renewable energies rapidly, the number of wind turbines has been increased in recent years. Ground motions induced by their operation can be observed by seismometers several kilometers away. Hence, the seismic noise level can be significantly increased at the seismic station. Therefore, this study combines long-term experiments and numerical simulations to improve the understanding of the seismic wavefields emitted by complete wind farms and to advance the prediction of signal amplitudes.
Firstly, wind-turbine induced signals that are measured at a small wind farm close to Würzburg (Germany) are correlated with the operational data of the turbines. The frequency-dependent decay of signal amplitudes with distance from the wind farm is modeled using an analytical method including the complex effects of interferences of the wavefields produced by the multiple wind turbines. Specific interference patterns significantly affect the wave propagation and therefore the signal amplitude in the far field of a wind farm. Since measurements inside the wind turbines show that the assumption of in-phase vibrating wind turbines is inappropriate, an approach to calculate representative seismic radiation patterns from multiple wind turbines, which allows the prediction of amplitudes in the far field of a complete wind farm, is proposed.
In a second study, signals with a frequency of 1.15 Hz, produced by the Weilrod wind farm (north of Frankfurt, Germany) are observed at the seismological observatory TNS (Taunus), which is located at a distance of 11 km from the wind farm. The propagation of the wavefield emitted by the wind farm is numerically modeled in 3D, using the spectral element method. It is shown that topographic effects can cause local signal amplitude reductions, but also signal amplification along the travel path of the seismic wave. The comparison of simulations with and without topography reveals that the reduction and amplification are spatially linked to the shape of the topography, which could be an explanation for the relatively high signal amplitude observed at TNS.
Finally, the reduction of the impact of wind turbines on seismic measurements using borehole installations is studied using 2D numerical models. Possible effects of the seismic velocity, attenuation, and layering of the subsurface are demonstrated. Results show that a borehole can be very effective in reducing the observed high-frequency signals emitted by wind turbines. However, a borehole might not be beneficial if signals with frequencies of about 1 Hz (or lower) are of interest, due significant wavelength-dependent effects. The estimations of depth-dependent amplitudes with a layered subsurface are validated with existing data from wind-turbine-induced signals measured at the top and bottom of two boreholes.
The experimental analysis of measurements conducted at wind farms and the advances of modeling such signals improve the understanding of the propagation of wind-farm induced seismic wave fields. Furthermore, the methods developed in this work have a high potential of universal application to the prediction of signal amplitudes at seismometers close to wind farms with arbitrary layout and geographic location.
This thesis is focusing on the impact of Paratethys and Mediterranean water bodies over the Eurasian climate and the interplay between climate, tectonics and biosphere during the late Miocene. This target was the interval between 12.7 and 7.65 Ma for Paratethys, following the Eastern Paratethys restriction and isolation, and 7.2−6.5 Ma (the early Messinian) in Mediterranean, zooming on the effects of gateway restrictions over the eastern Mediterranean and the new born Aegean domain. In both cases restriction is overlapping with large scale climatic changes and tectonic reconfiguration, leading a sort of symbiotic relationship.
Paratethys was a giant epicontinental sea that covered a large part of Eurasia since Paleogene. Due to the Eurasia-Afro-Arabia collision and formation of the Alpine-Himalayan belt (Rögl, 1999; Popov et al., 2006), the Paratethys was divided during the late Miocene in smaller basins that in time were isolated of each other. The protracted isolation and intense continentalisation of paratethyan realm led to changes in humidity distribution, basin connectivity, sediment sources and salinity. These changes had in turn major consequences over water circulation, water availability, vegetation cover and biota. These changes are more intense after 11.6 Ma, when the Eastern Paratethys lost any sustained marine connection, evolving into an enclosed system with endemic fauna (Harzhauser and Piller, 2007).
Mediterranean Sea is a Mezozoic oceanic relic squeezed between Africa, Europe, Anatolia and Arabia, as Africa continued to subduct beneath the European plate. As opposed to Paratethys, it maintained the open connection with the ocean until Messinian, when the two Atlantic gateways (Betic and Rifian corridors) closed for a short time, isolating the basin. The cut off resulted in a dramatic drop down and onset of evaporitic precipitation in marginal basins, the event receiving the name of Messinian Salinity Crisis (5.97−5.55). The restriction affected all marine ecosystems, due to changes in salinity and stratification of water column.
The main objectives of this thesis were:
(1) build valid paleo-temperatures records for both basins based on biomarkers;
(2) reconstruct the hydrology for the late Miocene time interval;
(3) identify vegetation composition and changes;
(4) identify paleo-fires in the late Miocene sediment records;
(5) identify the biotic response to the overall climate and tectonic changes.
All the above objectives were attained with results published in specific journals (Chapters 5−7).
Based on Panagia section (Taman Peninsula, Russia) the longest Paratethys temperature record was completed (~5 Myr), covering the interval between 12.7 and 7.65 Ma. A comprehensive SST and MAT records was obtained, as well as soil pH and carbon (δ13C) and hydrogen (δ2H) stable isotopic compositions on n-alkanes and alkenones. The main findings are concentrated around three prolonged periods with severe droughts affecting the late Miocene circum-Paratethys region peaking at 9.65, 9.4 and 7.9 Ma, associated with a transition towards open land vegetation, intensification of fire activity and enhanced evaporation and aridity.
The time intervals with dryer conditions recorded in Panagia coincide with periods of mammal turnover and dispersal in Eurasia indicating that major environmental changes occurred in the circum-Paratethys region and Paratethys fragmentation had a great impact on the terrestrial ecosystems, when periods of prolonged droughts generated biotic crises and animal displacements across the Eurasian continent. The δ13CC29n-alkane values and charcoal morphologies from Panagia indicate an increased contribution of C4 plants adapted to drier conditions at 9.66 Ma. Similarly high δ13CC29n-alkane values continue until 9.4 Ma, when in Western Europe increased seasonality accelerated the demise of the evergreen subtropical woodlands and expansion of grasslands from Anatolia and Middle East to Europe.
As a result of basin fragmentation and climatic stress, the Eastern Paratethys sub-basins progressively lost their marine properties and turned into brackish-fresh water bodies fed primarily by riverine input. The shallower areas became in time emerged, obstructing connections and isolating the biota, inducing rapid adjusting or extinctions. Thus, the Paratethys harbored a highly endemic fauna (Rögl, 1999), such as dwarf whales, dolphins, seals (among mammals), as well as fish and other taxa (mollusks, ostracods, diatoms, foraminifera, algae, etc.).
Collectively the data structured and analyzed in chapter five support a model in which the Eastern Paratethys evolved as a largely (en)closed system, registering paleoenvironmental signals that are governed by interbasinal connectivity (or lack of it) and regional climate changes in the basin catchment. Acting as an important source of humidity for Western and Central Asia, the size and areal extent of the Paratethys water body is likely to have had a major impact on hydroclimate patterns in the Eurasian interior, with the cumulative fluctuations in both hydrology and surface temperature enhancing the aridity and seasonality, with different partition of moisture over the year. Our combined data suggests a decoupling of Paratethys from the global system as isolation advanced, dominated by regional tectonics and ultimately the Paratethys volume and areal extent reduction.
Ob Klimawandel oder Luftverschmutzung: Die chemischen und physikalischen Prozesse in der Atmosphäre haben wichtige Auswirkungen auf die menschliche Gesundheit und Ökosysteme. Dabei ist die Atmosphäre mehr als ein Gemisch aus Stickstoff, Sauerstoff, Wasserdampf, Helium und Kohlenstoffdioxid. Es gibt zahlreiche Spurengase, deren Gesamtanteil am Volumen weniger als 1 % ausmacht. In dieser Arbeit werden Stickstoffoxide, Schwefeldioxid, Kohlenstoffmonoxid und Schwefelsäure näher betrachtet, die im Rahmen der flugzeugbasierten Messkampagne Chemistry of the Atmosphere: field experiment in Europe (CAFE-EU)/BLUESKY gemessen wurden.
Die Stickstoffoxide NO und NO2, als NOx zusammengefasst, besitzen hauptsächlich anthropogene Quellen, allen voran fossile Verbrennung und industrielle Prozesse. Zwischen NO und NO2 besteht ein photochemisches Gleichgewicht, sodass in der Atmosphäre vor allem NO2 in relevanten Konzentrationen vorkommt; dies wirkt aufgrund der Bildung von Salpetersäure, HNO3, in wässriger Lösung beim Einatmen ätzend und ist entsprechend gesundheitsschädlich. Troposphärisches Ozon, O3, wesentlicher Bestandteil von Sommersmog, wird hauptsächlich durch die Reaktion von NO mit Peroxiden (HO2 und RO2) gebildet. In der Stratosphäre entstehen NOx hauptsächlich durch die Photodissoziation von Lachgas, N2O, das aufgrund seiner langen Lebenszeit von der Tropo- in die Stratosphäre transportiert werden kann und dort die wichtigste Stickstoffquelle darstellt. In der Stratosphäre tragen NOx zum katalytischen Abbaumechanismus des Ozons bei (Bliefert, 2002; Seinfeld and Pandis, 2016).
Schwefeldioxid, SO2, ist ein toxisches Gas, dessen atmosphärische Quellen hauptsächlich anthropogen sind, nämlich fossile Verbrennung und industrielle Prozesse; Senken sind trockene und feuchte Deposition, wobei letztere zu saurem Regen führen kann. Seit den 1980ern sinken die globalen SO2-Emissionen. SO2 kann in der Atmosphäre zu Sulfat und Schwefelsäure oxidiert werden, was Hauptbestandteil des Wintersmogs ist. Der wichtigste Mechanismus ist die Oxidation mit dem Hydroxylradikal, OH˙, unter Beteiligung von Wasserdampf. In der Stratosphäre ist Carbonylsulfid, OCS, die wichtigste Schwefelquelle, da es analog zum N2O dank seiner langen Lebenszeit von der Tropo- in die Stratosphäre transportiert werden kann (Bliefert, 2002; Seinfeld und Pandis, 2016). Typische Konzentrationen von Schwefelsäure sind 105 cm–3 nachts und 107 cm–3 tagsüber in der Troposphäre sowie 105 cm–3 tagsüber in der Stratosphäre (Clarke et al., 1999; Weber et al., 1999; Fiedler et al., 2005; Arnold, 2008; Kürten et al., 2016; Berresheim et al., 2000).
Kohlenstoffmonoxid, CO, ist ein toxisches Gas, das zu gleichen Teilen durch direkte Emissionen (v.a. Biomasseverbrennung und fossile Verbrennung) und In-situ-Oxidation (v.a. von Methan, Isopren und industriellen Kohlenwasserstoffen) in die Atmosphäre gelangt. Die Hauptsenke ist die Reaktion mit OH˙ in der Troposphäre. Seit 2000 sinkt die globale CO-Konzentration (Bliefert, 2002).
Doch neben Gasen sind auch Aerosolpartikel fester Bestandteil des Gemisches Luft, welche luftgetragene feste oder flüssige Teilchen sind. Primäre Aerosolpartikel werden direkt als solche in die Atmosphäre emittiert, während sekundäre Aerosolpartikel in der Atmosphäre gebildet werden, indem gasförmige Vorläufersubstanzen mit geringer Flüchtigkeit auf primären Partikeln kondensieren oder durch Zusammenclustern und Anwachsen komplett neue Partikel bilden. Aerosolpartikel ermöglichen als Wolkenkondensationskeime erst die Bildung von Wolken und wirken somit – neben ihrem direkten reflektierenden Effekt – durch Änderung der Wolkenbedeckung und -eigenschaften insgesamt kühlend aufs Klima und beeinflussen die lokalen und globalen Wasserkreisläufe. Doch sie haben auch negative Auswirkungen auf die menschliche Gesundheit und sind für eine Verkürzung der durchschnittlichen Lebensdauer in Regionen mit hohen Feinstaubbelastungen verantwortlich (Seinfeld und Pandis, 2016; Bellouin et al., 2020; World Health Organization, 2016).
Neben den bisher betrachteten neutralen, also ungeladenen Gasen und Partikeln sind Ionen in der Gasphase sowie geladene Partikel ebenfalls Bestandteil der Atmosphäre. Sie spielen bei vielen atmosphärischen Prozessen eine wichtige Rolle, wie etwa bei Gewittern, Radiowellenübertragung und ionen-induzierter Nukleation von Aerosolpartikeln. Die Hauptquellen für Ionisation in der Tropo- und Stratosphäre ist die galaktische kosmische Strahlung, die entgegen ihrem Namen hauptsächlich aus Protonen und α-Partikeln (primäre Partikel genannt) besteht und in der Erdatmosphäre durch Kollision mit Luftmolekülen Teilchenschauer von sekundären Partikeln (u.a. Myonen, Pionen und Neutrinos) hervorruft. Die primären und sekundären Partikel können die Luftmoleküle ionisieren unter Entstehung von N+, N2+, O+, O2+ und Elektronen. Sauerstoff reagiert rasch mit letzteren zu O– und O2–. Diese Kationen und Anionen reagieren weiter, bis Ionenclustern der Summenformeln (HNO3)n(H2O)mNO3– und H+(H2O)n(B)m gebildet werden, wobei B Basen wie Methanol, Aceton, Ammoniak oder Pyridin sind. Weitere Ionisationsquellen sind der Zerfall des Radioisotops 222Rn in Bodennähe und ionisierende Solarstrahlung oberhalb der Stratosphäre. Atmosphärische Ionen haben zwei wichtige Senken: die Wiedervereinigung, auch Rekombination genannt, bei der sich ein Kation und ein Anion gegenseitig neutralisieren sowie das Anhaften an Aerosolpartikeln. Letztere Senke ist vor allem in der Troposphäre aufgrund der relativ hohen Konzentration an Aerosolpartikeln relevant (Arnold, 2008; Viggiano und Arnold, 1995; Bazilevskaya et al., 2008; Hirsikko et al., 2011).
Melting inside earth is a common phenomenon and can be observed in many different regions where melt travels through the mantle and crust to eventually reach the surface where it crystallizes to build large volcanic provinces, whole stratigraphic layers of flood basalts, or even the oceanic crust. Often, melt reaching the surface is a good source of information. It can be used to achieve a better understanding about processes taking place in deeper regions inside the mantle and it is therefore essential to fundamentally understand melting and melt percolation processes. In order to achieve a deeper understanding, the aim of this thesis is to investigate processes that are connected to melting by using numerical models.
The physical model used is a so called two-phase flow model which describes the ability of melt to percolate through a viscously deforming, partially molten matrix. A famous feature of two-phase flow are solitary porosity waves, which are waves of locally higher porosity ascending through a partially molten background, keeping its shape constant, driven by decompaction and compaction of the solid matrix in front and behind the wave.
The viscosity law for shear- and volume viscosity was strongly simplified in most previous studies that modeled solitary waves. Often the porosity dependency is underestimated or its influence on the volume viscosity is even neglected, leading to too high viscosities. In this work more realistic laws are used that strongly decrease for small melt fractions. Those laws are incorporated into a 2D Finite Difference mantle convection code with two-phase flow to study the ascent of solitary porosity waves.
The model results show that an initial Gaussian-shaped wave rapidly evolves into a solitary wave with a certain amplitude, traveling upwards with constant velocity. Even though strongly weaker viscosities are used, the effect on dispersion curves and wave shape are only minor as long as the background porosity is rather small. The results are still in agreement to semi-analytical solutions which neglect shear stresses in the melt segregation equation. Higher background porosities and wave amplitudes lead to significant decrease in phase velocity and wave width, as the viscosity is strongly effected. However, the models show that solitary waves are still a possible mechanism for more realistic matrix viscosities.
While the ascending of porosity waves are mostly described by the movement of fluid melt, partially molten regions inside Earth trigger upwelling of both, solid and fluid phases, which can be called diapirism. While diapirs can have a wide variety of wavelengths, porosity waves are restricted to a few times the compaction length. The size of a melt perturbation in terms of compaction length therefore describes whether material is transported by diapirism or porosity waves. In this thesis we study the transition from diapiric rise to solitary porosity waves by systematically changing the size of a porosity perturbation from 1.8 to 120 times the compaction length. In case of a perturbation of the size of a few times the compaction length a single porosity wave will emerge, either with a positive or negative vertical matrix flux and if melt is not allowed to move relative to the matrix a diapir will emerge. In between these physical end members a regime can be observed where the partially molten perturbation will split up into numerous solitary waves, whose phase velocity is low compared to the Stokes velocity and the swarm of solitary waves will ascend jointly as a diapir, slowly elongating due to a higher amplitude main solitary wave.
Solitary waves will always emerge from a melt perturbation as long as two-phase flow is enabled, but the time for a solitary wave to emerge increases non-linearly with the perturbation radius in terms of compaction length. In nature, in many cases this time might be too long for solitary waves to emerge.
Another important feature when it comes to two-phase flow is the transport of trace elements in melt. Incompatible elements prefer to go into the melt, which eventually enriches the area where it crystallizes again. In order to model this redistribution, the code FDCON was extended to allow for fully consistent transport of elements in melt, including melting, freezing and re-equilibration with time. A 2D model, a simple representation of a volcanic back arc, is set up to investigate the behavior of trace elements. The influence of retention number and re-equilibration time is examined. Lava-lamp like convection can be observed in the lower part of the model, producing melt, that eventually leads to enrichment in trace elements in the upper high-viscous layer. The total enrichment in this layer approaches an asymptotic value and a 0D model is introduced to recreate this behavior.
Cratonic eclogite is the product of oceanic crust subduction into the subcontinental lithospheric mantle, and it also is a fertile diamond source rock. In contrast to matrix minerals in magma-borne xenoliths, inclusions in diamond are shielded from external fluids, retaining more pristine information on the state of the eclogite source at the time of encapsulation. Vanadium is a multi-valent element and a widely used elemental redox proxy. Here, we show that that xenolithic garnet has lower average V abundances than garnet inclusions. This partly reflects crystal-chemical controls, whereby higher average temperatures recorded by inclusions, accompanied by enhanced Na2O and TiO2 partitioning into garnet, facilitate V incorporation at the expense of clinopyroxene. Unexpectedly, although diamond formation is strongly linked to metasomatism and xenoliths remained open systems, V concentrations are similar for bulk eclogites reconstructed from inclusions and from xenoliths. This suggests an oxygen-conserving mechanism for eclogitic diamond formation, and implies that eclogite is an efficient system to buffer fO2 over aeons of lithospheric mantle modification by subduction-derived and other fluids.
Global water models (GWMs) simulate the terrestrial water cycle, on the global scale, and are used to assess the impacts of climate change on freshwater systems. GWMs are developed within different modeling frameworks and consider different underlying hydrological processes, leading to varied model structures. Furthermore, the equations used to describe various processes take different forms and are generally accessible only from within the individual model codes. These factors have hindered a holistic and detailed understanding of how different models operate, yet such an understanding is crucial for explaining the results of model evaluation studies, understanding inter-model differences in their simulations, and identifying areas for future model development. This study provides a comprehensive overview of how state-of-the-art GWMs are designed. We analyze water storage compartments, water flows, and human water use sectors included in 16 GWMs that provide simulations for the Inter-Sectoral Impact Model Intercomparison Project phase 2b (ISIMIP2b). We develop a standard writing style for the model equations to further enhance model improvement, intercomparison, and communication. In this study, WaterGAP2 used the highest number of water storage compartments, 11, and CWatM used 10 compartments. Seven models used six compartments, while three models (JULES-W1, Mac-PDM.20, and VIC) used the lowest number, three compartments. WaterGAP2 simulates five human water use sectors, while four models (CLM4.5, CLM5.0, LPJmL, and MPIHM) simulate only water used by humans for the irrigation sector. We conclude that even though hydrologic processes are often based on similar equations, in the end, these equations have been adjusted or have used different values for specific parameters or specific variables. Our results highlight that the predictive uncertainty of GWMs can be reduced through improvements of the existing hydrologic processes, implementation of new processes in the models, and high-quality input data.
This paper investigates the global stratospheric Brewer–Dobson circulation (BDC) in the ERA5 meteorological reanalysis from the European Centre for Medium-Range Weather Forecasts (ECMWF). The analysis is based on simulations of stratospheric mean age of air, including the full age spectrum, with the Lagrangian transport model CLaMS (Chemical Lagrangian Model of the Stratosphere), driven by reanalysis winds and total diabatic heating rates. ERA5-based results are compared to results based on the preceding ERA-Interim reanalysis. Our results show a significantly slower BDC for ERA5 than for ERA-Interim, manifesting in weaker diabatic heating rates and higher age of air. In the tropical lower stratosphere, heating rates are 30 %–40 % weaker in ERA5, likely correcting a bias in ERA-Interim. At 20 km and in the Northern Hemisphere (NH) stratosphere, ERA5 age values are around the upper margin of the uncertainty range from historical tracer observations, indicating a somewhat slow–biased BDC. The age trend in ERA5 over the 1989–2018 period is negative throughout the stratosphere, as climate models predict in response to global warming. However, the age decrease is not linear but steplike, potentially caused by multi-annual variability or changes in the observations included in the assimilation. During the 2002–2012 period, the ERA5 age shows a similar hemispheric dipole trend pattern as ERA-Interim, with age increasing in the NH and decreasing in the Southern Hemisphere (SH). Shifts in the age spectrum peak and residual circulation transit times indicate that reanalysis differences in age are likely caused by differences in the residual circulation. In particular, the shallow BDC branch accelerates in both reanalyses, whereas the deep branch accelerates in ERA5 and decelerates in ERA-Interim.