Geowissenschaften
Refine
Year of publication
Document Type
- Article (593)
- Doctoral Thesis (139)
- Book (25)
- Contribution to a Periodical (21)
- Conference Proceeding (19)
- Working Paper (19)
- Part of Periodical (10)
- Diploma Thesis (8)
- diplomthesis (7)
- Preprint (6)
- Part of a Book (5)
- Report (5)
- Master's Thesis (4)
- Review (3)
- Bachelor Thesis (2)
- Habilitation (2)
- Other (2)
- Periodical (2)
Is part of the Bibliography
- no (872)
Keywords
- climate change (13)
- Climate change (5)
- Geochemistry (5)
- Klimaänderung (5)
- Atmospheric chemistry (4)
- Boden (4)
- Deutschland (4)
- Klima (4)
- Modellierung (4)
- Stratosphäre (4)
Institute
- Geowissenschaften (872)
- Senckenbergische Naturforschende Gesellschaft (59)
- Präsidium (49)
- Biodiversität und Klima Forschungszentrum (BiK-F) (45)
- Geographie (26)
- Biowissenschaften (15)
- Medizin (11)
- Physik (7)
- Institut für Ökologie, Evolution und Diversität (6)
- Biochemie und Chemie (5)
The growth of freshly formed aerosol particles can be the bottleneck in their survival to cloud condensation nuclei. It is therefore crucial to understand how particles grow in the atmosphere. Insufficient experimental data has impeded a profound understanding of nano-particle growth under atmospheric conditions. Here we study nano-particle growth in the CLOUD (Cosmics Leaving OUtdoors Droplets) chamber, starting from the formation of molecular clusters. We present measured growth rates at sub-3 nm sizes with different atmospherically relevant concentrations of sulphuric acid, water, ammonia and dimethylamine. We find that atmospheric ions and small acid-base clusters, which are not generally accounted for in the measurement of sulphuric acid vapour, can participate in the growth process, leading to enhanced growth rates. The availability of compounds capable of stabilizing sulphuric acid clusters governs the magnitude of these effects and thus the exact growth mechanism. We bring these observations into a coherent framework and discuss their significance in the atmosphere.
The main objective of this PhD work is to assess the impact of fine-scale air-sea interaction on the performance of a regional climate prediction model in marginal sea regions. Focus is on the North and Baltic Seas, the largest marginal sea area in the mid-latitudes. Motivation for this work is to better understand the interaction between the different components of the climate system, namely atmosphere, ocean and sea-ice. In addition to that, the sea regions of interest, the North and Baltic Seas, are orographically complex and cannot be resolved by a global ocean model. The ice coverage on the Baltic Sea is underestimated in the stand-alone atmospheric model COSMO-CLM due to the low water freezing temperature value assumed, which is not applicable for such brackish water body. To fulfil the thesis goal, a new regional coupled atmosphere-ocean-ice system was developed for these two seas, named COSMO-CLM/NEMO. The two-way coupling system involves active feedback from both component models: the limited-area climate model COSMO-CLM and the regional ocean model NEMO-NORDIC.
The coupled system COSMO-CLM/NEMO for the North and Baltic Seas was used to study the impact of sea surface temperature and sea ice on the atmosphere on diffrent topics. The long term impact of the North and Baltic Seas was studied through 15- year long simulations driven by European Center for Medium-Range Weather Forecasts (ECMWF) Interim reanalysis (ERA-Interim) data. Furthermore, to see whether the marginal sea modelling can advance the simulation of extreme climate events, the coupled model was used to reproduce six extreme snowband phenomena over the Baltic Sea in simulations driven by ERA-interim data. Last but not least, the role of the North and Baltic Sea model in improving long-term regional climate prediction was examined. Two sets of experiments with coupled and uncoupled models, each set has five independent decadal hindcasts forced by global climate model, were carried out.
All results were compared with observations and the stand-alone atmospheric model COSMO-CLM results. In all experiments, COSMO-CLM/NEMO showed good agreement with observations. Improvements compared with the uncoupled COSMO-CLM were also found. Coupling was found to affect the air temperature not only around the coupled sea region but also inland. The convective snowbands over the Baltic Sea were successfully reproduced by the coupled model. The high contrast of temperature in the air column, as well as considerably high amounts of surface heat fluxes exchanged between air and sea could not be simulated by COSMO-CLM without the help of reanalysis data. The coupled model also provided better forecasts in decadal scales compared with the uncoupled model and the global model. The added predictability came from the initialized regional seas and better simulated sea surface temperatures by the ocean model.
The impact of the North and Baltic Seas on the climate of the surrounding regions is in certain phases dominated by the North Atlantic Oscillation (NAO) activity. In this thesis, the relation between the NAO and the marginal sea influences was studied. It is confirmed by this study that, in strong phases, the NAO can overpower the impact of the local seas. During dominant phases of NAO, the European climate is mainly governed by large-scale circulation. On the other hand, the local seas play an important role in determining the European climate when NAO is in weak phases.
The added value of the coupled model raises promising perspectives for research in this field. It points to a potential benefit of using the coupled atmosphere-ocean-ice system for climate prediction in the region surrounding the North and Baltic Seas. Along with that, it is still a challenge to complete the model representation of the climate system by adding more climate components (such as a hydrological model). Further improvement of the coupled system can be achieved by coupling for a larger sea region, or by trying to reduce remaining low performance of the coupled model in some areas with a better configuration of the current system.
Here we present a comprehensive attempt to correlate aragonitic Na / Ca ratios from Lophelia pertusa, Madrepora oculata and a caryophylliid cold-water coral (CWC) species with different seawater parameters such as temperature, salinity and pH. Living CWC specimens were collected from 16 different locations and analyzed for their Na / Ca content using solution-based inductively coupled plasma-optical emission spectrometry (ICP-OES) measurements. The results reveal no apparent correlation with salinity (30.1–40.57 g/kg) but a significant inverse correlation with temperature (−0.31 mmol/mol/°C). Other marine aragonitic organisms such as Mytilus edulis (inner aragonitic shell portion) and Porites sp. exhibit similar results highlighting the consistency of the calculated CWC regressions. Corresponding Na / Mg ratios show a similar temperature sensitivity to Na / Ca ratios, but the combination of two ratios appear to reduce the impact of vital effects and domain-dependent geochemical variation. The high degree of scatter and elemental heterogeneities between the different skeletal features in both Na / Ca and Na / Mg however limit the use of these ratios as a proxy and/or make a high number of samples necessary. Additionally, we explore two models to explain the observed temperature sensitivity of Na / Ca ratios for an open and semi-enclosed calcifying space based on temperature sensitive Na and Ca pumping enzymes and transport proteins that change the composition of the calcifying fluid and consequently the skeletal Na / Ca ratio.
An accelerating Brewer-Dobson circulation (BDC) is a robust signal of climate change in model predictions but has been questioned by trace gas observations. We analyze stratospheric mean age of air and the full age spectrum as measures for the BDC and its trend. Age of air is calculated with the Chemical Lagrangian Model of the Stratosphere (CLaMS) driven by ERA-Interim, JRA-55 and MERRA-2 reanalysis data to assess the robustness of the representation of the BDC in current generation meteorological reanalyses. We find that climatological mean age significantly depends on the reanalysis, with JRA-55 showing the youngest and MERRA-2 the oldest mean age. Consideration of the age spectrum indicates that the older age for MERRA-2 is related to a stronger spectrum tail, likely related to weaker tropical upwelling and stronger recirculation. Seasonality of stratospheric transport is robustly represented in reanalyses, with similar mean age variations and age spectrum peaks. Long-term changes over 1989–2015 turn out to be similar for the reanalyses with mainly decreasing mean age accompanied by a shift of the age spectrum peak towards shorter transit times, resembling the forced response in climate model simulations to increasing greenhouse gas concentrations. For the shorter periods 1989–2001 and 2002–2015 age of air changes are less robust. Only ERA-Interim shows the hemispheric dipole pattern in age changes during 2002–2015 as viewed by recent satellite observations. Consequently, the representation of decadal variability of the BDC in current generation reanalyses appears less robust and a major uncertainty of modelling the BDC.
The Paleocene-Eocene Thermal Maximum (PETM) offers insight into massive short-term carbon cycle perturbations that caused significant warming during a high-pCO2 world, affecting both marine and terrestrial ecosystems. PETM records from the marine-terrestrial interface (e.g. estuarine swamps and mire deposits) are, therefore, of great interest as their present-day counterparts are highly vulnerable to future climate and sea level change. Here, we assess paleoenvironmental changes of mid-latitudinal Late Paleocene-Early Eocene peat mire records along the paleo-North Sea coast. We provide carbon isotope data of bulk organic matter (δ13CTOC), organic carbon content (%TOC), and palynological data from an extensive peat mire deposited at a mid-latitudinal (ca. 41 °N) coastal site (Schöningen, Germany). The δ13CTOC data show a carbon isotope excursion (CIE) of −1.7 ‰ coeval with a conspicuous Apectodinium acme, calling for the presence of the PETM in this coastal section. Due to the exceptionally large stratigraphic thickness of the PETM at Schöningen (10 m of section) we established a detailed palynological record that indicates only minor changes in paleovegetation leading to and during the PETM. Instead, paleovegetation changes mostly follow natural successions in response to changes along the marine-terrestrial interface. Compared to other available peat mire records (Cobham, UK; Vasterival, France) it appears that wetland deposits around the Paleogene North Sea have a typical CIE magnitude of ca. −1.3 ‰ in δ13CTOC. Moreover, the Schöningen record shares major characteristics with the Cobham Lignite, including evidence for increased fire activity prior to the PETM, minor PETM-related plant species changes, a reduced CIE in δ13CTOC, and drowning of the mire (marine ingressions) during much of the PETM. This suggests that paleoenvironmental conditions during the Late Paleocene-Early Eocene, including the PETM, consistently affected major segments of the paleo-North Sea coast.
In global hydrological models, groundwater storages and flows are generally simulated by linear reservoir models. Recently, the first global gradient-based groundwater models were developed in order to improve the representation of groundwater-surface water interactions, capillary rise, lateral flows and human water use impacts. However, the reliability of model outputs is limited by a lack of data as well as model assumptions required due to the necessarily coarse spatial resolution. The impact of data quality is presented by showing the sensitivity of a groundwater model to changes in the only available global hydraulic conductivity data-set. To better understand the sensitivity of model output to uncertain spatially distributed parameter inputs, we present the first application of a global sensitivity method for a global-scale groundwater model using nearly 2000 steady-state model runs of the global gradient-based groundwater model G3M. By applying the Morris method in a novel domain decomposition approach that identifies global hydrological response units, spatially distributed parameter sensitivities are determined for a computationally expensive model. Results indicate that globally simulated hydraulic heads are equally sensitive to hydraulic conductivity, groundwater recharge and surface water body elevation, though parameter sensitivities vary regionally. For large areas of the globe, rivers are simulated to be either losing or gaining, depending on the parameter combination, indicating a high uncertainty of simulating the direction of flow between the two compartments. Mountainous and dry regions show a high variance in simulated head due to numerical difficulties of the model, limiting the reliability of computed sensitivities in these regions. This instability is likely caused by the uncertainty in surface water body elevation. We conclude that maps of spatially distributed sensitivities can help to understand complex behaviour of models that incorporate data with varying spatial uncertainties. The findings support the selection of possible calibration parameters and help to anticipate challenges for a transient coupling of the model.
Global impact models represent process-level understanding of how natural and human systems may be affected by climate change. Their projections are used in integrated assessments of climate change. Here we test, for the first time, systematically across many important systems, how well such impact models capture the impacts of extreme climate conditions. Using the 2003 European heat wave and drought as a historical analogue for comparable events in the future, we find that a majority of models underestimate the extremeness of impacts in important sectors such as agriculture, terrestrial ecosystems, and heat-related human mortality, while impacts on water resources and hydropower are overestimated in some river basins; and the spread across models is often large. This has important implications for economic assessments of climate change impacts that rely on these models. It also means that societal risks from future extreme events may be greater than previously thought.
In late 2013, a whole air flask collection program started at the Taunus Observatory (TO) in central Germany. Being a rural site in close vicinity to the densely populated Rhein-Main area, Taunus Observatory allows to assess local and regional emissions. Owed to its altitude of 825 m, the site also regularly experiences background conditions, especially when air masses approach from north-westerly directions. With a large footprint area mainly covering central Europe north of the Alps, halocarbon measurements at the site have the potential to improve the data base for estimation of regional and total European halogenated greenhouse gas emissions. Flask samples are collected weekly for offline analysis using a GC-MS system employing a quadrupole as well as a time-of-flight mass spectrometer. As background reference, additional samples are collected approximately bi-weekly at the Mace Head Atmospheric Research Station (MHD) when air masses approach from the site’s clean air sector. Thus the TO time series can be linked to the in-situ AGAGE measurements and the NOAA flask sampling program at MHD. An iterative baseline identification procedure separates polluted samples from baseline data. While there is good agreement of baseline mixing ratios between TO and MHD, with a larger variability of mixing ratios at the continental site, measurements at TO are regularly influenced by elevated halocarbon mixing ratios. Here, first time series are presented for CFC-11, CFC-12, HCFC-22, HFC-134a, HFC-227ea, HFC-245fa, and dichloromethane. While atmospheric mixing ratios of the CFCs decrease, they increase for the HCFC and the HFCs. Small unexpected differences between CFC-11 and CFC-12 are found with regard to the occurrence of high mixing ratio events and seasonality, although production and use of both compounds are strictly regulated by the Montreal Protocol, and therefore a similar decrease of atmospheric mixing ratios should occur. Dichloromethane, a solvent about which recently concerns have risen regarding its growing influence on stratospheric ozone depletion, does not show a significant trend with regard to both, baseline mixing ratios and the occurrence of pollution events at Taunus Observatory for the time period covered, indicating stable emissions in the regions that influence the site. An analysis of HYSPLIT trajectories reveals differences in halocarbon mixing ranges depending on air mass origin.
In late 2013, a whole air flask collection programme was started at Taunus Observatory (TO) in central Germany. Being a rural site in close proximity to the Rhine–Main area, Taunus Observatory allows assessment of emissions from a densely populated region. Owing to its altitude of 825 m, the site also regularly experiences background conditions, especially when air masses approach from north-westerly directions. With a large footprint area mainly covering central Europe north of the Alps, halocarbon measurements at the site have the potential to improve the database for estimation of regional and total European halogenated greenhouse gas emissions. Flask samples are collected weekly for offline analysis using a GC/MS system simultaneously employing a quadrupole as well as a time-of-flight mass spectrometer. As background reference, additional samples are collected approximately once every 2 weeks at the Mace Head Atmospheric Research Station (MHD) when air masses approach from the site's clean air sector. Thus the time series at TO can be linked to the in situ AGAGE measurements and the NOAA flask sampling programme at MHD. An iterative baseline identification procedure separates polluted samples from baseline data. While there is good agreement of baseline mixing ratios between TO and MHD, with a larger variability of mixing ratios at the continental site, measurements at TO are regularly influenced by elevated halocarbon mixing ratios. Here, first time series are presented for CFC-11, CFC-12, HCFC-22, HFC-134a, HFC-227ea, HFC-245fa, and dichloromethane. While atmospheric mixing ratios of the chlorofluorocarbons (CFCs) decrease, they increase for the hydrochlorofluorocarbons (HCFCs) and the hydrofluorocarbons (HFCs). Small unexpected differences between CFC-11 and CFC-12 are found with regard to frequency and relative enhancement of high mixing ratio events and seasonality, although production and use of both compounds are strictly regulated by the Montreal Protocol, and therefore a similar decrease in atmospheric mixing ratios should occur. Dichloromethane, a solvent about which recently concerns have been raised regarding its growing influence on stratospheric ozone depletion, does not show a significant trend with regard to both baseline mixing ratios and the occurrence of pollution events at Taunus Observatory for the time period covered, indicating stable emissions in the regions that influence the site. An analysis of trajectories from the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model reveals differences in halocarbon mixing ranges depending on air mass origin.
A new method for size resolved chemical analysis of nucleation mode aerosol particles (size range from ~10 to ~30 nm) is presented. The Thermal Desorption Differential Mobility Analyzer (TD-DMA) uses an online, discontinuous principle. The particles are charged, a specific size is selected by differential mobility analysis and they are collected on a filament by electrostatic precipitation. Subsequently, the sampled mass is evaporated in a clean carrier gas and analyzed by a chemical ionization mass spectrometer. Gas phase measurements are performed with the same mass spectrometer during the sampling of particles. The characterization shows reproducible results, with a particle size resolution of 1.19 and the transmission efficiency for 15 nm particles being slightly above 50 %. The signal from the evaporation of a test substance can be detected starting from 0.01 ng and shows a linear response in the mass spectrometer. Instrument operation in the range of pg/m3 is demonstrated by an example measurement of 15 nm particles produced by nucleation from dimethylamine, sulfuric acid and water.
A new method for size-resolved chemical analysis of nucleation mode aerosol particles (size range from ∼10 to ∼30 nm) is presented. The Thermal Desorption Differential Mobility Analyzer (TD-DMA) uses an online, discontinuous principle. The particles are charged, a specific size is selected by differential mobility analysis and they are collected on a filament by electrostatic precipitation. Subsequently, the sampled mass is evaporated in a clean carrier gas and analyzed by a chemical ionization mass spectrometer. Gas-phase measurements are performed with the same mass spectrometer during the sampling of particles. The characterization shows reproducible results, with a particle size resolution of 1.19 and the transmission efficiency for 15 nm particles being slightly above 50 %. The signal from the evaporation of a test substance can be detected starting from 0.01 ng and shows a linear response in the mass spectrometer. Instrument operation in the range of pg m−3 is demonstrated by an example measurement of 15 nm particles produced by nucleation from dimethylamine, sulfuric acid and water.
Increasing atmospheric CO2 stimulates photosynthesis which can increase net primary production (NPP), but at longer timescales may not necessarily increase plant biomass. Here we analyse the four decade-long CO2-enrichment experiments in woody ecosystems that measured total NPP and biomass. CO2 enrichment increased biomass increment by 1.05 ± 0.26 kg C m−2 over a full decade, a 29.1 ± 11.7% stimulation of biomass gain in these early-secondary-succession temperate ecosystems. This response is predictable by combining the CO2 response of NPP (0.16 ± 0.03 kg C m−2 y−1) and the CO2-independent, linear slope between biomass increment and cumulative NPP (0.55 ± 0.17). An ensemble of terrestrial ecosystem models fail to predict both terms correctly. Allocation to wood was a driver of across-site, and across-model, response variability and together with CO2-independence of biomass retention highlights the value of understanding drivers of wood allocation under ambient conditions to correctly interpret and predict CO2 responses.
Diverse epidermal appendages including grouped filaments closely resembling primitive feathers in non-avian theropods, are associated with skeletal elements in the primitive ornithischian dinosaur Kulindadromeus zabaikalicus from the Kulinda locality in south-eastern Siberia. This discovery suggests that “feather-like” structures did not evolve exclusively in theropod dinosaurs, but were instead potentially widespread in the whole dinosaur clade. The dating of the Kulinda locality is therefore particularly important for reconstructing the evolution of “feather-like” structures in dinosaurs within a chronostratigraphic framework. Here we present the first dating of the Kulinda locality, combining U-Pb analyses (LA-ICP-MS) on detrital zircons and monazites from sedimentary rocks of volcaniclastic origin and palynological observations. Concordia ages constrain the maximum age of the volcaniclastic deposits at 172.8 ± 1.6 Ma, corresponding to the Aalenian (Middle Jurassic). The palynological assemblage includes taxa that are correlated to Bathonian palynozones from western Siberia, and therefore constrains the minimum age of the deposits. The new U-Pb ages, together with the palynological data, provide evidence of a Bathonian age—between 168.3 ± 1.3 Ma and 166.1 ± 1.2 Ma—for Kulindadromeus. This is older than the previous Late Jurassic to Early Cretaceous ages tentatively based on local stratigraphic correlations. A Bathonian age is highly consistent with the phylogenetic position of Kulindadromeus at the base of the neornithischian clade and suggests that cerapodan dinosaurs originated in Asia during the Middle Jurassic, from a common ancestor that closely looked like Kulindadromeus. Our results consequently show that Kulindadromeus is the oldest known dinosaur with “feather-like” structures discovered so far.
Formation of new aerosol particles from trace gases is a major source of cloud condensation nuclei (CCN) in the global atmosphere, with potentially large effects on cloud optical properties and Earth’s radiative balance. Controlled laboratory experiments have resolved, in detail, the different nucleation pathways likely responsible for atmospheric new particle formation, yet very little is known from field studies about the molecular steps and compounds involved in different regions of the atmosphere. The scarcity of primary particle sources makes secondary aerosol formation particularly important in the Antarctic atmosphere. Here, we report on the observation of ion-induced nucleation of sulfuric acid and ammonia—a process experimentally investigated by the CERN CLOUD experiment—as a major source of secondary aerosol particles over coastal Antarctica. We further show that measured high sulfuric acid concentrations, exceeding 107 molecules cm−3, are sufficient to explain the observed new particle growth rates. Our findings show that ion-induced nucleation is the dominant particle formation mechanism, implying that galactic cosmic radiation plays a key role in new particle formation in the pristine Antarctic atmosphere.
During the Late Cretaceous and early Cenozoic the Earth experienced prolonged climatic cooling most likely caused by decreasing volcanic activity and atmospheric CO2 levels. However, the causes and mechanisms of subsequent major global warming culminating in the late Paleocene to Eocene greenhouse climate remain enigmatic. We present deep and intermediate water Nd-isotope records from the North and South Atlantic to decipher the control of the opening Atlantic Ocean on ocean circulation and its linkages to the evolution of global climate. The marked convergence of Nd-isotope signatures 59 million years ago indicates a major intensification of deep-water exchange between the North and South Atlantic, which coincided with the turning point of deep-water temperatures towards early Paleogene warming. We propose that this intensification of Atlantic overturning circulation in concert with increased atmospheric CO2 from continental rifting marked a climatic tipping point contributing to a more efficient distribution of heat over the planet.
The multi-valence nature of vanadium means that its geochemical behaviour will be ƒO2-dependent, so that its concentration or V/Sc (or V/Ga), can serve as proxies for oxidation state in mantle peridotites. Compared to Fe3+/Fe2+-based equilibria, such trace elements may be less sensitive to metasomatic processes. To investigate these systematics, we have measured V, Sc, Ga and Fe3+ contents in clinopyroxene from well-characterised spinel peridotite xenoliths from the Massif Central, France. These samples were metasomatised by a variety of agents with different oxidation states.V contents can be modified by metasomatic interactions, and other geochemically similar elements including Sc and Ga can also be added, removed or remain constant. A link between V/Sc and Fe3+-Fe2+ equilibria is apparent. Partial removal of V is caused by different metasomatic agents; the common factor is that all agents were significantly more oxidised than the initial ambient mantle peridotite. This extraction can be understood by a decreasing partition coefficient for V for ΔlogƒO2 > ~FMQ-2. Considering that mineral/melt partitioning of V decreases similarly for all peridotite minerals, the bulk-rock V/Sc will also change during relatively oxidising metasomatic interactions and mirror the results obtained for clinopyroxene.
Nucleation and growth of aerosol particles from atmospheric vapors constitutes a major source of global cloud condensation nuclei (CCN). The fraction of newly formed particles that reaches CCN sizes is highly sensitive to particle growth rates, especially for particle sizes <10 nm, where coagulation losses to larger aerosol particles are greatest. Recent results show that some oxidation products from biogenic volatile organic compounds are major contributors to particle formation and initial growth. However, whether oxidized organics contribute to particle growth over the broad span of tropospheric temperatures remains an open question, and quantitative mass balance for organic growth has yet to be demonstrated at any temperature. Here, in experiments performed under atmospheric conditions in the Cosmics Leaving Outdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN), we show that rapid growth of organic particles occurs over the range from −25 ∘C to 25 ∘C. The lower extent of autoxidation at reduced temperatures is compensated by the decreased volatility of all oxidized molecules. This is confirmed by particle-phase composition measurements, showing enhanced uptake of relatively less oxygenated products at cold temperatures. We can reproduce the measured growth rates using an aerosol growth model based entirely on the experimentally measured gas-phase spectra of oxidized organic molecules obtained from two complementary mass spectrometers. We show that the growth rates are sensitive to particle curvature, explaining widespread atmospheric observations that particle growth rates increase in the single-digit-nanometer size range. Our results demonstrate that organic vapors can contribute to particle growth over a wide range of tropospheric temperatures from molecular cluster sizes onward.
Subduction zone magmas are more oxidised on eruption than those at mid-ocean ridges. This is attributed either to oxidising components, derived from subducted lithosphere (slab) and added to the mantle wedge, or to oxidation processes occurring during magma ascent via differentiation. Here we provide direct evidence for contributions of oxidising slab agents to melts trapped in the sub-arc mantle. Measurements of sulfur (S) valence state in sub-arc mantle peridotites identify sulfate, both as crystalline anhydrite (CaSO4) and dissolved SO42− in spinel-hosted glass (formerly melt) inclusions. Copper-rich sulfide precipitates in the inclusions and increased Fe3+/∑Fe in spinel record a S6+–Fe2+ redox coupling during melt percolation through the sub-arc mantle. Sulfate-rich glass inclusions exhibit high U/Th, Pb/Ce, Sr/Nd and δ34S (+ 7 to + 11‰), indicating the involvement of dehydration products of serpentinised slab rocks in their parental melt sources. These observations provide a link between liberated slab components and oxidised arc magmas.
Dating of extensive alluvial fan surfaces and fluvial features in the hyperarid core of the Atacama Desert, Chile, using cosmogenic nuclides provides unrivalled insights about the onset and variability of aridity. The predominantly hyperarid conditions help to preserve the traces of episodic climatic and/or slow tectonic change. Utilizing single clast exposure dating with cosmogenic 10Be and 21Ne, we determine the termination of episodes of enhanced fluvial erosion and deposition occurring at ~19, ~14, ~9.5 Ma; large scale fluvial modification of the landscape had ceased by ~2–3 Ma. The presence of clasts that record pre-Miocene exposure ages (~28 Ma and ~34 Ma) require stagnant landscape development during the Oligocene. Our data implies an early onset of (hyper-) aridity in the core region of the Atacama Desert, interrupted by wetter but probably still arid periods. The apparent conflict with interpretation that favour a later onset of (hyper-) aridity can be reconciled when the climatic gradients within the Atacama Desert are considered.
The mechanisms of transfer of crustal material from the subducting slab to the overlying mantle wedge are still debated. Mélange rocks, formed by mixing of sediments, oceanic crust, and ultramafics along the slab-mantle interface, are predicted to ascend as diapirs from the slab-top and transfer their compositional signatures to the source region of arc magmas. However, the compositions of melts that result from the interaction of mélanges with a peridotite wedge remain unknown. Here we present experimental evidence that melting of peridotite hybridized by mélanges produces melts that carry the major and trace element abundances observed in natural arc magmas. We propose that differences in nature and relative contributions of mélanges hybridizing the mantle produce a range of primary arc magmas, from tholeiitic to calc-alkaline. Thus, assimilation of mélanges into the wedge may play a key role in transferring subduction signatures from the slab to the source of arc magmas.
Kontinuierlich hohe Stickstofffrachten der Elbe und weiterer Nordseezuflüsse haben die Internationale Nordseeschutzkonferenz (INK) Ende der 80er Jahre dazu veranlasst, eine 50%ige Reduzierung der N-Einträge in die Nordsee innerhalb von 10 Jahren zu beschließen. Diese Reduzierung wurde in diesem Zeitraum nicht erreicht. Für Oberflächengewässer wurde im Jahr 2001 zur Umsetzung der EU-Wasserrahmenrichtlinie in Bundesdeutsches Recht von der Länderarbeitsgemeinschaft Wasser (LAWA) in Zusammenarbeit mit dem Umweltbundesamt (UBA 2001d) eine Güteklassifikation für Nährstoffe erstellt, die einen Wert von 3 mg/l N für Oberflächengewässer festgelegt. Am Beispiel der mittleren Mulde, die kontinuierlich hohe Stickstoffkonzentrationen von durchschnittlich 6 mg N /l aufweist, wird deutlich, dass eine Reduzierung der N-Einträge zur Erzielung der geforderten Gewässergüte unabdingbar ist. Sowohl für die Meere als auch für die Oberflächengewässer ist eine Halbierung der N-Einträge eine umweltpolitische Notwendigkeit. Im Rahmen des Projektes „Gebietswasserhaushalt und Stoffhaushalt in der Lößregion des Elbegebietes als Grundlage für die Durchsetzung einer nachhaltigen Landnutzung“ wurden deshalb die Wasser- und Stickstoffflüsse im Einzugsgebiet der mittleren Mulde (2700 km²) flächendifferenziert erfasst, um die N-Eintragpfade zu quantifizieren und Maßnahmen zur Minderung der N-Frachten abzuleiten. ...
The African continent is regularly portrayed as an indolent space with a well-known reputation as a chaotic continent. Viewed as lacking vision, means and capacities, Africa is perceived at best as a place that is marked by a permanent status quo, stagnation, or in worst case scenarios, as a declining continent. Various references to the continent are synonymous with famine, poverty, war, etc. Such portrayals are all the more intriguing given that the continent is known for its abundant natural resources, such as timber, oil, natural gas, minerals, etc., whose reserves are, moreover, not well known both by the African people and their leaders. As a result, there is still much progress to be made in tapping into the resources in order to improve the daily lives of African citizens.
In such a context dominated by infantile carelessness throughout the continent, the interventions of actors from outside the continent are the only hopes of bringing some vitality to this continent which is cloaked in "la grande nuit – the great darkness" (Mbembé 2013). Thus during the main sequences of recent history, representing different forms of Western penetration and activity on the African continent (slavery, imperialism, colonization), all the Western world’s contributions have obviously not sufficed to boost Africa and take it out of its never ending childhood. It has remained just as passive and apathetic today as it was yesterday.
The attraction of Asian actors to the continent is even more recent. And consistent with its abovementioned indolence, Africa is seen as an easy and defenceless prey for the Korean, Japanese, Indian, Malaysian, or Chinese conquerors. In the latter case, the insatiable appetite for natural resources whose reserves are being rapidly depleted is the cornerstone of their foreign aid policy. This led China to colonize the continent, showing a preference for Pariah Regimes which held no appeal for the West, by sending an army of workers to extract those resources (Lum et al. 2009), in defiance of all national and international regulations and based on completely opaque contracts.
Although the concept of African Agency was rapidly developed in several African countries, the aim of this study was more specific to Cameroon’s mining sector in which different entrepreneurs from abroad got involved over time. The thesis investigates whether indigenous citizens took part in any way in the development of mining projects in the country. Thus, the work assesses and analyses actions and reactions initiated and undertaken by local people in the context of China’s presence within Cameroon’s mining sector to promote and advance their interests over those of foreign investors. In addition, the author has no knowledge of any other study investigating African Agency in the mining sector as a whole in Cameroon.
In conducting this study, a multi-method research framework was developed including a series of methods used to collect data and analyse concepts of African Agency associated Political Ecology as they developed within Cameroon’s mining sector. Specifically, those methods comprised quantitative research when it came to collecting data using a positivist and empirical approach constructed by deducing evidence from statistical data collected by means of the 167 questionnaire surveys administered to local inhabitants and workers randomly selected on mining sites and in riparian communities. The questionnaires helped to capture Cameroonians' perceptions of the recent phenomenon of the gradual but significant influx of international actors and precisely Chinese players in the mining sector on the one hand, and on the other hand, observational data was collected across the GVC as developed in the Betare-Oya region. As a complement to the former technique, qualitative methods helped to study and deepen understanding of human behaviour and the social world in a holistic perspective through individual interviews, focus groups, and direct observations on the ground. In addition, the spatial analysis method based on the land use classification technique served to detect changes to land use/land cover that have been brought on by mechanised mining activities undertaken in this region. The sequencing of data collected and their processing from a ground theory perspective led to the formulation and specification of Cameroon’s Ecological Agency theory.
One of the earliest steps of this work consisted in a literature review and in placing the African Agency concept in a broader context. It then led to the state of the art, specifications about research content of the work and the main theories undergirding this thesis. Before examining developments that emerged during the last decade, a historical perspective was provided to the topic in order to show how African societies started mining operations and how they dealt with foreign partners interested in their mining resources. The aim was to show that while Western imperialism presented a challenge for the sector, it did not erase local participation, even despite the constraints associated with such involvement.
...
During the Holocene, North American ice sheet collapse and rapid sea-level rise reconnected the Black Sea with the global ocean. Rapid meltwater releases into the North Atlantic and associated climate change arguably slowed the pace of Neolithisation across southeastern Europe, originally hypothesized as a catastrophic flooding that fueled culturally-widespread deluge myths. However, we currently lack an independent record linking the timing of meltwater events, sea-level rise and environmental change with the timing of Neolithisation in southeastern Europe. Here, we present a sea surface salinity record from the Northern Aegean Sea indicative of two meltwater events at ~8.4 and ~7.6 kiloyears that can be directly linked to rapid declines in the establishment of Neolithic sites in southeast Europe. The meltwater events point to an increased outflow of low salinity water from the Black Sea driven by rapid sea level rise >1.4 m following freshwater outbursts from Lake Agassiz and the final decay of the Laurentide ice sheet. Our results shed new light on the link between catastrophic sea-level rise and the Neolithisation of southeastern Europe, and present a historical example of how coastal populations could have been impacted by future rapid sea-level rise.
A recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently, and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are re-analyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 nm and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range (up to ca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically-controlled) new particle formation for the conditions during the CLOUD7 experiment (278 K, 38% RH, sulfuric acid concentration between 1×106 and 3×107 cm-3 and dimethylamine mixing ratio of ~40 pptv). Finally, the simulation of atmospheric new particle formation reveals that even tiny mixing ratios of dimethylamine (0.1 pptv) yield NPF rates that could explain significant boundary layer particle formation. This highlights the need for improved speciation and quantification techniques for atmospheric gas-phase amine measurements.
A recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are reanalyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at a larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range of sizes (up to ca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement for the high base-to-acid ratios (∼ 100) relevant for this study. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically controlled) NPF for the conditions during the CLOUD7 experiment (278 K, 38 % relative humidity, sulfuric acid concentration between 1 × 106 and 3 × 107 cm−3, and dimethylamine mixing ratio of ∼ 40 pptv, i.e., 1 × 109 cm−3).
Chlorine and bromine atoms can lead to catalytic destruction of ozone in the stratosphere. Therefore the use and production of ozone depleting substances (ODS) containing chlorine and bromine is regulated by the Montreal Protocol to protect the ozone layer. Equivalent Effective Stratospheric Chlorine (EESC) has been adapted as an appropriate metric to describe the combined effects of chlorine and bromine released from halocarbons on stratospheric ozone. Here we revisit the concept of calculating EESC. We derive a new formulation of EESC based on an advanced concept of ODS propagation into the stratosphere and reactive halogen release. A new transit time distribution is introduced in which the age spectrum for an inert tracer is weighted with the release function for inorganic halogen from the source gases. This distribution is termed the “release time distribution”. The improved formulation shows that EESC levels in the year 1980 for the mid latitude lower stratosphere were significantly lower than previously calculated. 1980 marks the year commonly defined as the onset of anthropogenic ozone depletion in the stratosphere. Assuming that the EESC value must return to the same level in order for ozone to fully recover, we show that it will take more than 10 years longer than currently assumed in this region of the stratosphere. Based on the improved formulation, EESC level at mid-latitudes will reach this landmark only in 2060. We also present a range of sensitivity studies to investigate the effect of changes and uncertainties in the fractional release factors and in the assumptions on the shape of the release time distributions. We conclude that, under the assumptions that all other atmospheric parameters like stratospheric dynamics and chemistry are unchanged, the recovery of mid latitude stratospheric ozone would be expected to be delayed by about a 10 years, in a similar way as EESC.
Chlorine and bromine atoms lead to catalytic depletion of ozone in the stratosphere. Therefore the use and production of ozone-depleting substances (ODSs) containing chlorine and bromine is regulated by the Montreal Protocol to protect the ozone layer. Equivalent effective stratospheric chlorine (EESC) has been adopted as an appropriate metric to describe the combined effects of chlorine and bromine released from halocarbons on stratospheric ozone. Here we revisit the concept of calculating EESC. We derive a refined formulation of EESC based on an advanced concept of ODS propagation into the stratosphere and reactive halogen release. A new transit time distribution is introduced in which the age spectrum for an inert tracer is weighted with the release function for inorganic halogen from the source gases. This distribution is termed the release time distribution. We show that a much better agreement with inorganic halogen loading from the chemistry transport model TOMCAT is achieved compared with using the current formulation. The refined formulation shows EESC levels in the year 1980 for the mid-latitude lower stratosphere, which are significantly lower than previously calculated. The year 1980 is commonly used as a benchmark to which EESC must return in order to reach significant progress towards halogen and ozone recovery. Assuming that – under otherwise unchanged conditions – the EESC value must return to the same level in order for ozone to fully recover, we show that it will take more than 10 years longer than estimated in this region of the stratosphere with the current method for calculation of EESC. We also present a range of sensitivity studies to investigate the effect of changes and uncertainties in the fractional release factors and in the assumptions on the shape of the release time distributions. We further discuss the value of EESC as a proxy for future evolution of inorganic halogen loading under changing atmospheric dynamics using simulations from the EMAC model. We show that while the expected changes in stratospheric transport lead to significant differences between EESC and modelled inorganic halogen loading at constant mean age, EESC is a reasonable proxy for modelled inorganic halogen on a constant pressure level.
Convection-permitting models (CPMs) have proven their usefulness in representing precipitation on a sub-daily scale. However, investigations on sub-hourly scales are still lacking, even though these are the scales for which showers exhibit the most variability. A Lagrangian approach is implemented here to evaluate the representation of showers in a CPM, using the limited-area climate model COSMO-CLM. This approach consists of tracking 5‑min precipitation fields to retrieve different features of showers (e.g., temporal pattern, horizontal speed, lifetime). In total, 312 cases are simulated at a resolution of 0.01 ° over Central Germany, and among these cases, 78 are evaluated against a radar dataset. The model is able to represent most observed features for different types of convective cells. In addition, the CPM reproduced well the observed relationship between the precipitation characteristics and temperature indicating that the COSMO-CLM model is sophisticated enough to represent the climatological features of showers.
Chlorine monoxide (ClO) plays a key role in stratospheric ozone loss processes at midlatitudes. We present two balloon-borne in situ measurements of ClO conducted in northern hemisphere midlatitudes during the period of the maximum of total inorganic chlorine loading in the atmosphere. Both ClO measurements were conducted on board the TRIPLE balloon payload, launched in November 1996 in León, Spain, and in May 1999 in Aire sur l'Adour, France. For both flights a ClO daylight and night-time vertical profile was derived over an altitude range of approximately 15-35 km. ClO mixing ratios are compared to model simulations performed with the photochemical box model version of the Chemical Lagrangian Model of the Stratosphere (CLaMS). Simulations along 24-hour backward trajectories were performed to study the diurnal variation of ClO in the midlatitude lower stratosphere. Model simulations for the flight launched in Aire sur l'Adour 1999 show an excellent agreement with the ClO measurements. For the flight launched in León 1996, an overall good agreement is found, whereas the flight is characterized by a more complex dynamical situation due to a possible mixture of vortex and non-vortex air. We note that for both flights at solar zenith angles greater than 86°-87° simulated ClO mixing ratios are higher than observed ClO mixing ratios. However, the present findings indicate that no substantial uncertainties exist in midlatitude chlorine chemistry of the stratosphere.
Fractional release factors of long-lived halogenated organic compounds in the tropical stratosphere
(2009)
Fractional release factors (FRFs) of organic trace gases are time-independent quantities that influence the calculation of Global Warming Potentials and Ozone Depletion Potentials. We present the first set of vertically resolved FRFs for 15 long-lived halo carbons in the tropical stratosphere up to 34 km altitude. They were calculated from measurements on air samples collected on board balloons and a high altitude aircraft. We compare the derived dependencies of FRFs on the mean stratospheric transit times (the so-called mean ages of air) with similarly derived FRFs originating from measurements at higher latitudes and find significant differences. Moreover a comparison with averaged FRFs currently used by the World Meteorological Organisation revealed the latter to be imprecise measures due to their observed vertical and latitudinal variability. The presented data set could thus be used to improve future ozone level and climate projections.
The abiotic and biotic drivers of rapid diversification in Andean bellflowers (Campanulaceae)
(2016)
The tropical Andes of South America, the world's richest biodiversity hotspot, are home to many rapid radiations. While geological, climatic, and ecological processes collectively explain such radiations, their relative contributions are seldom examined within a single clade. We explore the contribution of these factors by applying a series of diversification models that incorporate mountain building, climate change, and trait evolution to the first dated phylogeny of Andean bellflowers (Campanulaceae: Lobelioideae). Our framework is novel for its direct incorporation of geological data on Andean uplift into a macroevolutionary model. We show that speciation and extinction are differentially influenced by abiotic factors: speciation rates rose concurrently with Andean elevation, while extinction rates decreased during global cooling. Pollination syndrome and fruit type, both biotic traits known to facilitate mutualisms, played an additional role in driving diversification. These abiotic and biotic factors resulted in one of the fastest radiations reported to date: the centropogonids, whose 550 species arose in the last 5 million yr. Our study represents a significant advance in our understanding of plant evolution in Andean cloud forests. It further highlights the power of combining phylogenetic and Earth science models to explore the interplay of geology, climate, and ecology in generating the world's biodiversity.
Brachiopod shells are the most widely used geological archive for the reconstruction of the temperature and the oxygen isotope composition of Phanerozoic seawater. However, it is not conclusive whether brachiopods precipitate their shells in thermodynamic equilibrium. In this study, we investigated the potential impact of kinetic controls on the isotope composition of modern brachiopods by measuring the oxygen and clumped isotope compositions of their shells. Our results show that clumped and oxygen isotope compositions depart from thermodynamic equilibrium due to growth rate-induced kinetic effects. These departures are in line with incomplete hydration and hydroxylation of dissolved CO2. These findings imply that the determination of taxon-specific growth rates alongside clumped and bulk oxygen isotope analyses is essential to ensure accurate estimates of past ocean temperatures and seawater oxygen isotope compositions from brachiopods.
A primordial state of matter consisting of free quarks and gluons that existed in the early universe a few microseconds after the Big Bang is also expected to form in high-energy heavy-ion collisions. Determining the equation of state (EoS) of such a primordial matter is the ultimate goal of high-energy heavy-ion experiments. Here we use supervised learning with a deep convolutional neural network to identify the EoS employed in the relativistic hydrodynamic simulations of heavy ion collisions. High-level correlations of particle spectra in transverse momentum and azimuthal angle learned by the network act as an effective EoS-meter in deciphering the nature of the phase transition in quantum chromodynamics. Such EoS-meter is model-independent and insensitive to other simulation inputs including the initial conditions for hydrodynamic simulations.
Despite mounting evidence of the anthropogenic influence on the Earth's climate, underlying mechanisms of climate change often remain elusive. The investigation of periods of rapid climate change from geological archives may provide crucial information about magnitude, duration, teleconnections of and regional responses to global and hemispheric scale climate perturbations. Thus, paleoclimate reconstructions may help in mitigating and adapting to the challenges of the coming decades. The '8.2 kyr B.P. climatic event' has previously been proposed as a possible analogue for the future climatic scenario of a reduced Atlantic Meridional Overturning Circulation (AMOC). The catastrophic drainage of the Laurentide meltwater lakes through the Hudson Bay and into the Labrador Sea, that occurred ca. 8.47 kyr B.P., caused the slowdown of the AMOC around 8.2 kyr B.P.. Subsequently, reduced heat transfer towards Europe triggered a substantial decline in (winter) temperature and pronounced changes in atmospheric circulation patterns in many regions of the northern hemisphere, especially the North Atlantic realm and Europe. Among the regions affected by the 8.2 kyr B.P. climatic event, the Eastern Mediterranean region is of particular interest for both past and future climate developments. Traditionally characterized as a region highly sensitive to variations in the climate systems of the high and low latitudes, abrupt climate changes have the potential to strongly alter atmospheric circulation patterns and thus precipitation distribution in the region that may have severe socioeconomical consequences. The analysis of stable hydrogen (δD) and oxygen isotopes (δ18O) in precipitation is an excellent tool to trace changes in atmospheric circulation. Here, we present a comparative study of δD and δ18O in precipitation from the Eastern Mediterranean region both in a present day scenario and during the 8.2 kyr B.P. climatic event. We analyze the influences of topography, air mass trajectory, climate and seasonality among others the stable isotopic compositions of meteoric waters from the Central Anatolian Plateau (CAP), Turkey, in order to create a first-order template which may serve as a reference against which paleoenvironmental proxy data may be more accurately interpreted and tested. Further, we employ a multiproxy approach on the early Holocene peat deposits of the classical site of Tenaghi Philippon (TP), NE Greece, to investigate paleoenvironmental responses to northern hemisphere cooling during the 8.2 kyr B.P. climatic event and aim to determine changes atmospheric circulation from δD of leaf wax n-alkanes (δDwax).
Based on δD and δ18O data from more than 480 surface water samples from the CAP, we characterize moisture sources affecting the net isotopic budget of precipitation, manifesting in a systematic north-south difference in near-sea level moisture compositions. Rainout, induced by the major orographic barriers of the plateau, the Pontic Mountains to the north and the Taurus Mountains to the south, strongly shape the modern patterns of δD and δ18O. Stable isotope data from the semi-arid plateau interior provide clear evidence for an evaporitic regime that drastically affects surface water compositions. Strong evaporative enrichment contrasts rainfall patterns along the plateau margins, in part obfuscating the effects of topography and air mass trajectory.
Consequently, in order to address possible influences of evaporation on δD and δ18O in paleoprecipitation from TP, we analyze n-alkane abundances and distributions along with stable carbon isotope compositions of total organic carbon (δ13CTOC) and palynological data to estimate surface moisture conditions during the early Holocene (ca. 8.7 - 7.5 kyr B.P.) and especially during the 8.2 kyr B.P. climatic event. A period of relatively dry surface conditions from ca. 8.7 to 8.2 kyr B.P., indicated by low values of the 'aquatic index' (Paq ) and by elevated Average Chain Length (ACL) values, in concert with elevated δ13CTOC values, precedes the 8.2 kyr B.P. climatic event. The event itself is characterized by slightly wetter, more humid conditions, as suggested by an increase in Paq values as well as reduced ACL and δ13CTOC values between ca. 8.2 and 7.9 kyr B.P.. In the upper section of the core, a distinct change in paleohydrology becomes. A steep increase in Paq and a decrease in ACL values as well as variations in δ13CTOC from 7.9 kyr B.P. onwards imply considerably elevated surface moisture levels, likely caused by the increased activity of the karstic system of the surrounding mountains. Collectively, the biomarker proxies presented here, reveal a concise picture of changing moisture conditions at TP that is consistent with palynological data and provide detailed paleoenvironmental information for the analysis of δDwax as a paleoprecipitation proxy. The long-term decline in δDwax values characterizes the lower section of the core until ca. 8.2 kyr B.P.. The 8.2 kyr B.P. climatic event itself is connected to two distinct positive hydrogen isotope excursions: a minor shift in δDwax around 8.2 kyr B.P. and a major shift in δDwax between ca. 8.1 and 8.0 kyr B.P.. The upper part of the section shows a progressive trend towards higher δDwax values. With no indication of increased evaporitic conditions at TP during the 8.2 kyr B.P. climatic event, as evident in biomarker proxies and pollen data, we link shifts in δDwax to changes in Mediterranean air mass trajectories supplying precipitation to northeastern Greece, with variations in the relative contributions of northerly derived, D-depleted moisture and southerly-derived, D-enriched moisture. Possible control mechanisms include changes in the influence of the Siberian High and differences in the influence of the African and Asian monsoon circulations on anticyclonic conditions in the Mediterranean region as well as regional inflow of moist air from the Aegean Sea.
The East African Rift System (EARS) was initiated in the Eocene epoch between 50 and 21 Ma probably due to the influence of mantle plumes that caused volcanism, flood basalts and rifting extensions in Ethiopa and the Afar region. As a result of magmatic intrusions and adiabatic decompression melting within the lithosphere caused by the impact of the Kenya plume, there was a southward propagation of the EARS of about 30 – 15 Ma from Ethiopia to Kenya, which coincide with the occurrence of volcanism. The EARS developed towards the south along the margins of the Tanzania Craton between 15 and 8 Ma. Previous findings of low-velocity anomalies within the upper mantle and the mantle transition zone indicate an upwelling of hot mantle material in the vicinity of the Afar region and the East African Rift. This study includes the analysis of P- and S-receiver functions in order to determine further impacts on the lithosphere from below. The aim was to determine the topographic undulations of further boundary layers and to identify their variability owing to the rifting processes and the formation of the EARS. The study area included the Tanzania Craton and the surrounding rift branches of the East African Rift System.
The region of the Rwenzori Mountains can be analysed in detail because of the large dataset of the RiftLink project. The use of the P-receiver function technique and the H-K stacking method enabled to determine different vP /vS ratios depending on the tectonic setting in the Rwenzori region: Rift shoulders (vP /vS =1.74), Albert Rift segment (vP /vS =1.80), Edward Rift segment (vP /vS =1.87) and Rwenzori Mountains (vP /vS =1.86). To determine the topography of the Moho, it is necessary to take into account the thickness of the sedimentary layer, the surface topography, the azimuthal variations in crustal thickness and the impact of local anomalies. After correcting these effects on the Moho depths, significant variations in Moho topography could be determined. The Moho depths range from 29 to 39 km beneath the rift shoulders of the Albertine Rift. Within the rift valley, the crustal thickness varies between 25 – 31 km in the Edward Rift segment and 22 – 30 km in the Albert Rift segment. An averaged crustal thickness of about 26 km within the rift valley indicates the lack of the crustal root beneath the Rwenzoris. Similar variations in crustal thickness were determined by using an automatic procedure for analysing S-receiver functions that was developed in this study.
The S-receiver functions are created by applying a rotation criterion in order to rotate the Z, N and E components into the L, Q and T components. It is necessary to perform trial rotations using different incident and azimuth angles to determine the correct rotation angles. The latter are identified by the use of the rotation criterion, including the amplitude ratio of the converted Moho signal to the direct S/SKS-wave signal. The L component is rotated correctly in the direction of the incident shear wave in the case of the maximum amplitude ratio. After analysing the frequency content of the receiver functions in order to sort out harmonic and long-periodic traces, the individual Moho signals are checked for consistency in order to remove atypic signals. To increase the signal-to-noise ratios on the traces, the S-receiver functions are stacked. For this purpose, the signals of the direct shear waves must originate from similar epicenters. On the basis of similar ray paths, the receiver functions show comparable waveforms and converted signals. To perform the stacking procedure, it is necessary to merge the datasets of the adjacent stations in order to obtain a sufficient number of receiver functions. This analysis is based on the assumption that the incident seismic waves arriving at the adjacent stations penetrate to some extent the same underground structures in the case of similar wave propagation paths. This approach accounts for the fact that the converted signals do not result exclusively from the piercing points at the boundary layers. Further signals originate from the conversions at the boundary layer within the Fresnel Zone. The piercing points are derived from the significant signals in the receiver functions. Depending on the order of arrival of the converted phases on the traces, the signals are attributed to the theoretical discontinuities DIS1, DIS2, DIS3 and DIS4. However, partly due to the low signal-to-noise ratios on the traces, it is difficult to identify the real conversions on the traces and to ensure that the converted signals are attributed to the correct boundary layers. For this reason, it is necessary to check the consistency of the conversion depths among each other. In the case of inconsistent conversion depths, the corresponding signals are either adjusted to another seismic boundary layer or removed from the dataset. To verify the functionality of the automatic procedure and to determine the resolvability with respect to two boundary layers, several models are tested including horizontal and dipping discontinuities. To resolve distinct discontinuities, their depths must differ by at least 60 km, otherwise, due to similar depth ranges of the different boundary layers, the converted signals cannot be separated from each other. As a consequence, the converted signals that originate from different discontinuities are attributed to a single one. Further tests including break-off edges of seismic discontinuities are performed to check the attributions of the converted signals to the discontinuities. Owing to the varying number of boundary layers, the converted signals cannot be attributed to the discontinuities according to the order of their arrivals on the traces. It is necessary to correct their attributions to the seismic discontinuities in order to resolve the boundary layers.
The crust-mantle boundary and further discontinuities within the lithospheric mantle are investigated by applying this automatic procedure. Depending on the tectonic setting, the conversion depths of the Moho range from about 30 – 45 km beneath the western rift shoulder to 20 – 35 km within the rift valley up to 30 – 40 km beneath the eastern rift shoulder. The long wavelengths of the shear waves hamper the correct identification of the converted phases in the S-receiver functions. With respect to the relative differences in conversion depth, the topographic undulations of the crust-mantle boundary are consistent with the Moho depths derived from P-receiver functions. In contrast to the Rwenzori region, it is difficult to resolve completely the trend of the Moho in the remaining area of the East African Rift due to the small dataset provided by IRIS. The results exibit an increase in crustal thickness to up to 45 km in the region of the Cenozoic volcanics such as Virunga, Kivu, Rungwe and Kenya. The greatest Moho depths of more than 50 km are located near Mount Kilimanjaro. In addition to the Moho, the analysis of the S-receiver functions revealed two further boundary layers at depths of 60 – 140 km and 110 – 260 km, which are associated with a mid-lithospheric discontinuity and the lithosphere-asthenosphere boundary, respectively. The shallowest conversion depths of the LAB are focussed to small-scale regions within the rift branches, namely the northern Albertine Rift, the Chyulu Hills and the Mozambique Belt, which are located around the Tanzania Craton. The larger thickness of the lithosphere beneath the cratonic terrain indicates that the Tanzania Craton is not significantly eroded. However, there are indications that the lithosphere beneath the craton and the rift branches is penetrated by ascending asthenospheric melts to depths of up to 140 and 60 km, respectively. The top of the ascending melts is associated with the occurrence of the mid-lithospheric discontinuity. The shallowest conversion depths of this boundary layer (60 – 90 km) are related to the rifted areas of the EARS and the Cenozoic volcanic provinces, which are located along the Albertine Rift, the Kenya Rift and the Rukwa-Malawi rift zones. The deepest conversion depths of up to 140 km are related to the Rwenzori Belt, the Ugandan Basement Complex and the interior of the Tanzania Craton.
Over the last several decades, spinel-structured minerals with the chemical formula AB2O4 (where A and B stand for divalent and trivalent cations, respectively) have attracted more and more attention, particularly with regards to their breakdown at high pressures and temperatures and the nature of the so-called "post-spinel" phases. Spinel-structured phases with different endmember compositions, like magnetite (Fe3O4), hercynite (FeAl2O4) or spinel (MgAl2O4), are known to breakdown differently at high pressure-temperature conditions (e.g., Akaogi et al. 1999; Schollenbruch et al. 2010; Woodland et al. 2012). Such phases are of particular interest when they incorporate ferric (Fe3+) and ferrous (Fe2+) cations as this makes their stability sensitive to redox conditions. Since magnetite and magnesioferrite (MgFe3+ 2O4) have been found as inclusions in diamond (e.g., Stachel et al. 1998; Harte et al. 1999; Wirth et al. 2014; Palot et al. 2016; Jacob et al. 2016), understanding their phase relations is important for setting constraints on the conditions of their formation.
This study aimed to experimentally investigate the phase relations of Fe-Mg spinel-structured phases at conditions of the deep upper mantle and transition zone. Exploring the stability of new post-spinel phases and their characterization were also major goals of this study. Approaching a pyrolitic mantle composition by adding amounts of SiO2 in the system allowed constraints on the relevance of Fe-Mg post-spinel phases coexisting with mantle silicates to be made. ...
Indian Ocean came into existence with the breakup of Gondwana in the Mesozoic era. The presence of complex aseismic ridges and plateaus in the Indian Ocean makes it the least-understood of all the oceans. Mascarene Plateau, apart from Central Indian Ridge (CIR) running north-south between 2◦N and 25◦S in the Indian Ocean, is one such complex feature in the Indian Ocean that consists of Seychelles microcontinent in the north and the volcanic islands of Mauritius, La Réunion and Rodrigues in the south.
Most of the previous seismological studies on the islands of Mauritius, Rodrigues and Seychelles are restricted as each of them has only one operational permanent station. In the current study, I present the results obtained from the investigations of the seismological data obtained from the deployment of temporary seismic network on Mauritius (November, 2012–August, 2014) and Seychelles (March, 2013–March, 2015) under Réunion Hotspot and Upper Mantle–Réunions Unterer Mantel (RHUM–RUM) project and later in Rodrigues (September, 2014–June, 2016) under a collaborative project between Goethe-Universität, Frankfurt, Germany and Mauritius Oceanography Institute (MOI), Mauritius. Additional data from the permanent stations were also used in this study. The investigations and results are presented under three themes, namely: (1) crustal structure beneath Mauritius, (2) upper mantle anisotropy below Mauritius, Rodrigues and Seychelles and (3) intraplate seismicity in the Rodrigues–CIR region.
Upper mantle anisotropy in south-west Indian Ocean region are very limited, especially from the islands of Mauritius and Rodrigues. With the new data from the seismic stations deployed in Mauritius and Seychelles, under RHUM–RUM, and permanent stations in Rodrigues, I constrain the upper mantle flow pattern beneath these islands. From the joint-splitting analysis, I obtain fast-polarisation direction (φ) dominant in N80◦E and delay time (δt) of ≈0.85 s for Mauritius and φ tending east–west in Rodrigues with δt of ≈1.1 s. Parabolic asthenospheric flow model explains the orientation of the fast-polarisation direction beneath Mauritius, whereas deep mantle circulation patterns best explain the horizontal alignment of the fast-polarisation direction in Rodrigues. From Seychelles data, the results show φ trending NE and δt ≈0.74 s, even for the island close to Amirante Ridge, suggesting an asthenospheric deformation induced by relative motion between the plate and the deep mantle flow.
It has recently been suggested that the volcanic island of Mauritius may be underlain by a remnant of continental origin termed “Mauritia.” To constrain the crustal thickness beneathMauritius, I analysed data from 11 land stations, 10 of which were deployed recently under the RHUM–RUM project. From the recordings, I obtained 382 P-receiver functions. On the obtained receiver functions, I applied the H–κ stacking technique and derived the crustal thickness of ≈10–15 km. I observe a considerable variation in the VP/VS ratio caused by a lack of clear multiples. Using forward modelling of receiver functions, I show that the lack of clear multiples can be explained by a transitional Moho, where the velocity increases gradually. The modelling further indicates that the thickness of this gradient zone is estimated to be ≈10 km. I argue that my findings suggest oceanic crust thickened by crustal underplating due to the mantle plume currently located beneath La Réunion.
Seismicity around Rodrigues Island is generally associated with events recorded by the global networks along the CIR. Using seismological array techniques on the data collected by the temporary deployment of seismic array on Rodrigues Island for a period of 22 months (September, 2014–June 2016), 62 new events were located, which were not reported by any global network. Determination of backazimuth and apparent velocity were performed by applying array methods in the time-domain instead of the more conventional frequency-domain analysis. Event distances were calculated using a 1-D velocity model and the measured travel-time differences between S- and P-wave arrivals. Local magnitudes of the events were obtained by removing the velocity response from the seismographs and then convolving with Wood–Anderson transfer function to obtain ground motion in nanometers. Most of the newly-detected events are located off the ridge axis and can be classified as intraplate events. Three different seismic clusters were observed around the island. Most of the events were localised in the north-east of Rodrigues at a distance of ≈138 km from the reference station. A distinguishable swarm of earthquakes was observed on the west of the spreading segment from March to April 2015. The local magnitudes (ML) of the events varied between 1.6 and 3.7.
Eisnukleierende Partikel (INP) sind ein wichtiger Bestandteil des atmosphärischen Aerosols. Trotz ihrer geringen Konzentrationen in der Atmosphäre haben sie Einfluss auf die Bildung von Eiskristallen und auf den Niederschlag. Durch Änderungen in Anzahlkonzentration oder anderer Eigenschaften der INP können sich Wolkenparameter wie Lebensdauer und Tröpfchendichte ändern, was weiter eine Ursache für Änderungen im globalen Strahlungshaushalt sein kann.
Der Anteil zum globalen Strahlungshaushalt durch „Wolken-Anpassungen aufgrund von Aerosolen“, stellt weiterhin die größte Unsicherheit des Strahlungsantriebes dar. Aus diesem Grund sind Messungen und Studien über atmosphärische Aerosole und INP notwendig. Im Rahmen dieser Arbeit wurde der Eiskeimzähler FINCH („fast ice nucleus chamber“) grundlegend überholt und für Messungen von INP optimiert. FINCH ist ein in-situ Eiskeimzähler der durch Mischung unterschiedlicher Luftströme eine Übersättigung der Probeluft mit Wasserdampf erzeugt, um auf diese Weise die zu untersuchenden Aerosolpartikel zu Eiskristallen wachsen zu lassen. Am Ende einer Wachstumskammer werden die Partikel durch eine Optik, dem FINCH-OPS, anhand von Streueigenschaften klassifiziert und ausgewertet. Um FINCH im erwarteten Umfang benutzen zu können, wurden am F-OPS der Laser und die zur Detektion des Streulichts benutzen Photomultiplier ersetzt. Weiter wurde die Software zur Detektion der Partikel neu entwickelt. Durch diese Änderungen ist es möglich Partikelanzahl, Partikelgröße sowie eine Information über die Form der Partikel abzuleiten. Über einen weiteren Photomultiplier im F-OPS ist es zudem möglich eine Information über Fluoreszenz des Partikels zu gewinnen, um so auf einen biologischen Ursprung des Partikels zu schließen. Vorangegangene Probleme durch elektromagnetische Einstrahlung und dadurch entstandene Inkonsistenzen während Messungen konnten im Rahmen dieser Arbeit identifiziert und ausgeschlossen werden. Ebenfalls konnten die zur Flusskühlung benutzen Wärmetaucher als Ursache für Verunreinigungen und Kontamination ausgemacht werden. Auch dieser, für Messungen ungeeignete Zustand, wurde im Rahmen dieser Arbeit behoben.
Ausführliche Charakterisierungsmessungen konnte die Funktionsfähigkeit des F-OPS, als einzelnes Messgerät ohne FINCH-Kammer, belegen. Durch Messungen mit einer steuerbaren Lichtquelle in der Optik konnte zudem die elektrische Verarbeitung sowie die Zählqualität der Optik verifiziert werden. Weiter kann durch diese Experimente gezeigt werden, dass mit dem F-OPS größenaufgelöst gemessen werden kann.
Auch in den ersten Streulichtexperimenten mit Testaerosol kann die Funktionsfähigkeit der Optik gezeigt werden. Für Partikelgröße von Dp > 400 nm wird eine Zähleffizienz von 25% eines TSI 3025 CPCs erreicht. Die über den F-OPS abgeleitete Partikelgröße kann durch Messungen mit monodispersen Aerosolpartikeln und einer parallelen Messung mit einem TSI 3330 OPS parametrisiert werden. Weiter kann die Fluoreszenz von ausgewählten Referenzstoffen gezeigt werden.
Im Betrieb von F-OPS hinter der FINCH-Kammer, also FINCH als Komplettsystem, wurden weitere Charakterisierungsmessungen durchgeführt. Es wurde festgestellt, dass die Anzahlkonzentration der Partikel nach Schließen eines Ventils exponentiell abfällt. Die Partikel folgen demnach nicht nur einem laminaren Fluss durch die Kammer. 50% der Partikel haben nach ca. 13 s die Kammer verlassen. Auch wurde ermittelt, dass ca. 40% der Partikel in der Kammer verloren gehen.
Erste Aktivierungsexperimente zeigen, dass Eispartikel in der Kammer auf eine Größe von Dp > 6 µm anwachsen. Durch Nullfiltermessungen in Aktivierungsphasen, sowie Ändern des zur Aktivierung notwendigen feuchten Flusses, wird zudem gezeigt, dass die Aktivierung der INP durch Mischung erfolgt und außerdem keine Fremdpartikel aktiviert werden. Die neue Steuerung der Kammer lässt es zu Temperaturen in etwa einer Stunde gezielt anzusteuern. Es wird gezeigt, dass Schwankungen in der Sättigung hauptsächlich durch Temperaturphänomene beeinflusst werden.
Abschließend wurden beispielhaft Laborexperimente mit Snomax© durchgeführt, welche sehr gut mit Werten aus der Literatur verglichen werden konnten. Auch eine erste Außenluftmessung am Jungfraujoch (Schweiz) wird in dieser Arbeit präsentiert. Die gemessenen INP-Konzentrationen im gezeigten Zeitraum liegen zwischen 1,4 ± 4,1 L-1 und 53 ± 30 L-1 und entsprechen somit wiederum bekannten Literaturwerten.
Size-resolved measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations and hygroscopicity were conducted at the remote Amazon Tall Tower Observatory (ATTO) in the central Amazon Basin over a full seasonal cycle (Mar 2014–Feb 2015). In a companion part 1 paper, we presented an in-depth CCN characterization based on annually as well as seasonally averaged time intervals and discuss different parametrization strategies to represent the Amazonian CCN cycling in modelling studies (M. Pöhlker et al., 2016b). The present part 2 study analyzes the aerosol and CCN variability in original time resolution and, thus, resolves aerosol advection and transformation for the following case studies, which represent the most characteristic states of the Amazonian atmosphere:
1. Near-pristine (NP) conditions, defined as the absence of detectable black carbon (< 0.01 µg m−3), showed their highest occurrence (up to 30 %) in the wet season (i.e., Mar–May). On average, the NP episodes are characterized by a bimodal aerosol size distribution (strong Aitken mode: DAit = 70 nm, NAit = ~ 200 cm−3 vs. weaker accumulation mode: Dacc = 170 nm, Nacc = ~ 60 cm−3), a mostly organic particle composition, and relatively low hygroscopicity levels (κAit = 0.12 vs. κacc = 0.18). The NP CCN efficiency spectrum shows that the CCN population is sensitive to changes in supersaturation (S) over a wide S range.
2. Long-range transport (LRT) conditions frequently mix Saharan dust, African combustion smoke, and sea spray aerosols into the Amazonian wet season atmosphere. The LRT episodes (i.e., Feb–Apr) are characterized by an accumulation mode dominated size distribution (DAit = 80 nm, NAit = 120 cm−3 vs. Dacc = 180 nm, Nacc = 300 cm−3), a clearly increased abundance of dust and salt compounds, and relatively high hygroscopicity levels (κAit = 0.18, κacc = 0.34). The LRT CCN efficiency spectrum shows that the CCN population is highly sensitive to changes in S in the low S regime.
3. Biomass burning (BB) conditions dominate the Amazonian dry season. A selected characteristic BB episode shows a very strong accumulation mode (DAit = 70 nm, NAit = ~ 140 cm−3 vs. Dacc = 170 nm, Nacc = ~ 3400 cm−3), particles with very high organic fractions (> 90 %), and correspondingly low hygroscopicity levels (κAit = 0.14, κacc = 0.17). The BB CCN efficiency spectrum shows that the CCN population is highly sensitive to changes in S in the low S regime.
4. Mixed pollution conditions show the superposition of African (i.e., volcanic) and Amazonian (i.e., biomass burning) aerosol emissions during the dry season. The African aerosols showed a broad monomodal distribution (D = 130 nm, N = ~ 1300 cm−3), with very high sulfate fractions (20 %), and correspondingly high hygroscopicity (κAit = 0.14, κacc = 0.22). This was superimposed by fresh smoke from nearby fires with one strong mode (D = 113 nm, Nacc = ~ 2800 cm−3), an organic-dominated aerosol, and sharply decreased hygroscopicity (κAit = 0.10, κacc = 0.20). These conditions underline the rapidly changing pollution regimes with clear impacts on the aerosol and CCN properties.
Overall, this study provides detailed insights into the CCN cycling in relation to aerosol-cloud interaction in the vulnerable and climate-relevant Amazon region. The detailed analysis of aerosol and CCN key properties and particularly the extracted CCN efficiency spectra with the associated fit parameters provide a basis for an in-depth analysis of aerosol-cloud interaction in the Amazon and beyond.
We developed a coupled regional climate system model based on the CCLM regional climate model. Within this model system, using OASIS3-MCT as a coupler, CCLM can be coupled to two land surface models (the Community Land Model (CLM) and VEG3D), the NEMO-MED12 regional ocean model for the Mediterranean Sea, two ocean models for the North and Baltic seas (NEMO-NORDIC and TRIMNP+CICE) and the MPI-ESM Earth system model.
We first present the different model components and the unified OASIS3-MCT interface which handles all couplings in a consistent way, minimising the model source code modifications and defining the physical and numerical aspects of the couplings. We also address specific coupling issues like the handling of different domains, multiple usage of the MCT library and exchange of 3-D fields.
We analyse and compare the computational performance of the different couplings based on real-case simulations over Europe. The usage of the LUCIA tool implemented in OASIS3-MCT enables the quantification of the contributions of the coupled components to the overall coupling cost. These individual contributions are (1) cost of the model(s) coupled, (2) direct cost of coupling including horizontal interpolation and communication between the components, (3) load imbalance, (4) cost of different usage of processors by CCLM in coupled and stand-alone mode and (5) residual cost including i.a. CCLM additional computations.
Finally a procedure for finding an optimum processor configuration for each of the couplings was developed considering the time to solution, computing cost and parallel efficiency of the simulation. The optimum configurations are presented for sequential, concurrent and mixed (sequential+concurrent) coupling layouts. The procedure applied can be regarded as independent of the specific coupling layout and coupling details.
We found that the direct cost of coupling, i.e. communications and horizontal interpolation, in OASIS3-MCT remains below 7 % of the CCLM stand-alone cost for all couplings investigated. This is in particular true for the exchange of 450 2-D fields between CCLM and MPI-ESM. We identified remaining limitations in the coupling strategies and discuss possible future improvements of the computational efficiency.
The formation of secondary particles in the atmosphere accounts for more than half of global cloud condensation nuclei. Experiments at the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber have underlined the importance of ions for new particle formation, but quantifying their effect in the atmosphere remains challenging. By using a novel instrument setup consisting of two nano-particle counters, one of them equipped with an ion filter, we were able to further investigate the ion-related mechanisms of new particle formation. In autumn 2015, we carried out experiments at CLOUD on four systems of different chemical compositions involving monoterpenes, sulfuric acid, nitrogen oxides, and ammonia. We measured the influence of ions on the nucleation rates under precisely controlled and atmospherically relevant conditions. Our results indicate that ions enhance the nucleation process when the charge is necessary to stabilize newly formed clusters, i.e. in conditions where neutral clusters are unstable. For charged clusters that were formed by ion-induced nucleation, we were able to measure, for the first time, their progressive neutralization due to recombination with oppositely charged ions. A large fraction of the clusters carried a charge at 1.2 nm diameter. However, depending on particle growth rates and ion concentrations, charged clusters were largely neutralized by ion–ion recombination before they grew to 2.2 nm. At this size, more than 90 % of particles were neutral. In other words, particles may originate from ion-induced nucleation, although they are neutral upon detection at diameters larger than 2.2 nm. Observations at Hyytiälä, Finland, showed lower ion concentrations and a lower contribution of ion-induced nucleation than measured at CLOUD under similar conditions. Although this can be partly explained by the observation that ion-induced fractions decrease towards lower ion concentrations, further investigations are needed to resolve the origin of the discrepancy.
The CLOUD (Cosmics Leaving OUtdoor Droplets) experiment at CERN is studying the nucleation and growth of aerosol particles under atmospheric conditions, and their activation into cloud droplets. A key feature of the CLOUD experiment is precise control of the experimental parameters. Temperature uniformity and stability in the chamber are important since many of the processes under study are sensitive to temperature and also to contaminants that can be released from the stainless steel walls by upward temperature fluctuations. The air enclosed within the 3 m CLOUD chamber is equipped with several arrays (strings) of high precision, fast-response thermometers to measure its temperature. Here we present a study of the air temperature uniformity inside the CLOUD chamber under various experimental conditions. Measurements were performed under calibration conditions and run conditions, which are distinguished by the flow rate of fresh air and trace gases entering the chamber: 20 l/min and up to 210 l/min, respectively. During steady-state calibration runs between −70 °C and +20 °C, the air temperature uniformity is better than +/−0.06 °C in the radial direction and +/−0.1 °C in the vertical direction. Larger non-uniformities are present during experimental runs, depending on the temperature control of the make-up air and trace gases (since some trace gases require elevated temperatures until injection into the chamber). The temperature stability is a few times 0.01 °C over periods of several hours during either calibration or steady-state run conditions. During rapid adiabatic expansions to activate cloud droplets and ice particles, the chamber walls are up to 10 °C warmer than the enclosed air. This results in larger non-uniformities while the air returns to its equilibrium temperature with time constant of about 200 s.
Evaluation of radiation components in a global freshwater model with station-based observations
(2016)
In many hydrological models, the amount of evapotranspired water is calculated using the potential evapotranspiration (PET) approach. The main driver of several PET approaches is net radiation, whose downward components are usually obtained from meteorological input data, whereas the upward components are calculated by the model itself. Thus, uncertainties can be large due to both the input data and model assumptions. In this study, we compare the radiation components of the WaterGAP Global Hydrology Model, driven by two meteorological input datasets and two radiation setups from ERA-Interim reanalysis. We assess the performance with respect to monthly observations provided by the Baseline Surface Radiation Network (BSRN) and the Global Energy Balance Archive (GEBA). The assessment is done for the global land area and specifically for energy/water limited regions. The results indicate that there is no optimal radiation input throughout the model variants, but standard meteorological input datasets perform better than those directly obtained by ERA-Interim reanalysis for the key variable net radiation. The low number of observations for some radiation components, as well as the scale mismatch between station observations and 0.5° × 0.5° grid cell size, limits the assessment.
The Earth's future depends on how we manage the manifold risks of climate change (CC). It is state-of-the-art to assume that risk reduction requires participatory management involving a broad range of stakeholders and scientists. However, there is still little knowledge about the optimal design of participatory climate change risk management processes (PRMPs), in particular with respect to considering the multitude of substantial uncertainties that are relevant for PRMPs. To support the many local to regional PRMPs that are necessary for a successful global-scale reduction of CC risks, we present a roadmap for designing such transdisciplinary knowledge integration processes. The roadmap suggests ways in which uncertainties can be comprehensively addressed within a PRMP. We discuss the concept of CC risks and their management and propose an uncertainty framework that distinguishes epistemic, ontological, and linguistic uncertainty as well as ambiguity. Uncertainties relevant for CC risk management are identified. Communicative and modeling methods that support social learning as well as the development of risk management strategies are proposed for each of six phases of a PRMP. Finally, we recommend how to evaluate PRMPs as such evaluations and their publication are paramount for achieving a reduction of CC risks.
The present PhD thesis comprises structural geology, petrographic and geochronological investiga-tions on crystalline rocks of the Uppermost Unit in the southern Aegean realm. Studies were carried out in three areas: (1) on the island of Anafi, (2) in the area west of Melambes in central Crete and (3) between the villages of Pefkos, Kalami and Sykologos in the municipality of Viannos in eastern Crete.
The Uppermost Unit forms together with the underlying, non-metamorphic Pindos Unit the upper nappe system of the Cretan nappe pile that, unlike the units of the lower nappe system, was not affected by Late Oligocene to Early Miocene subduction-related metamorphism. The upper nappe system must therefore have been at upper levels of the lithosphere in the Late Oligocene. This is of particular im-portance when reconstructing the tectonometamorphic evolution of the Uppermost Unit. The Upper-most Unit is very heterogeneous in composition and is subdivided into several subunits, which differ mainly in their lithological composition and the degree of metamorphic overprint. Usually, it is subdi-vided into several low-grade metamorphic subunits and one high-grade metamorphic subunit. Within the scope of this PhD thesis, three of these subunits were examined; (1) the anchimetamorphic Arvi Unit, (2) the newly described Greenschist Unit and (3) the Asterousia Crystalline Complex (ACC).
The analyses conducted during this PhD thesis include: (1) structural geology investigations in the field, (2) microstructural and petrographic analyses on thin sections, (3) radiometric dating of zircons using isotope dilution thermal ionisation mass spectrometry (ID-TIMS) and laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS), (4) electron microprobe (EMP) analysis, (5) quartz texture analysis using electron-backscattered diffraction (EBSD), (6) semiquantitative analysis of min-eral phases using X-ray powder diffraction (XRD), (7) analysis of the modal composition of intrusive rocks applying point counting on thin sections and (8) X-ray microtomography (micro-CT) on chias-tolite hornfels.
...
Binary nucleation of sulphuric acid-water particles is expected to be an important process in the free troposphere at low temperatures. SAWNUC (Sulphuric Acid Water Nucleation) is a model of binary nucleation that is based on laboratory measurements of the binding energies of sulphuric acid and water in charged and neutral clusters. Predictions of SAWNUC are compared for the first time comprehensively with experimental binary nucleation data from the CLOUD chamber at European Organization for Nuclear Research. The experimental measurements span a temperature range of 208–292 K, sulphuric acid concentrations from 1·106 to 1·109 cm−3, and distinguish between ion-induced and neutral nucleation. Good agreement, within a factor of 5, is found between the experimental and modeled formation rates for ion-induced nucleation at 278 K and below and for neutral nucleation at 208 and 223 K. Differences at warm temperatures are attributed to ammonia contamination which was indicated by the presence of ammonia-sulphuric acid clusters, detected by an Atmospheric Pressure Interface Time of Flight (APi-TOF) mass spectrometer. APi-TOF measurements of the sulphuric acid ion cluster distributions (math formula with i = 0, 1, ..., 10) show qualitative agreement with the SAWNUC ion cluster distributions. Remaining differences between the measured and modeled distributions are most likely due to fragmentation in the APi-TOF. The CLOUD results are in good agreement with previously measured cluster binding energies and show the SAWNUC model to be a good representation of ion-induced and neutral binary nucleation of sulphuric acid-water clusters in the middle and upper troposphere.
Chemical reduction-oxidation mechanisms within mantle rocks link to the terrestrial carbon cycle by influencing the depth at which magmas can form, their composition, and ultimately the chemistry of gases released into the atmosphere. The oxidation state of the uppermost mantle has been widely accepted to be unchanged over the past 3800 m.y., based on the abundance of redox-sensitive elements in greenstone belt–associated samples of different ages. However, the redox signal in those rocks may have been obscured by their complex origins and emplacement on continental margins. In contrast, the source and processes occurring during decompression melting at spreading ridges are relatively well constrained. We retrieve primary redox conditions from metamorphosed mid-oceanic ridge basalts (MORBs) and picrites of various ages (ca. 3000–550 Ma), using V/Sc as a broad redox proxy. Average V/Sc values for Proterozoic suites (7.0 ± 1.4, 2σ, n = 6) are similar to those of modern MORB (6.8 ± 1.6), whereas Archean suites have lower V/Sc (5.2 ± 0.4, n = 5). The lower Archean V/Sc is interpreted to reflect both deeper melt extraction from the uppermost mantle, which becomes more reduced with depth, and an intrinsically lower redox state. The pressure-corrected oxygen fugacity (expressed relative to the fayalite-magnetite-quartz buffer, ΔFMQ, at 1 GPa) of Archean sample suites (ΔFMQ –1.19 ± 0.33, 2σ) is significantly lower than that of post-Archean sample suites, including MORB (ΔFMQ –0.26 ± 0.44). Our results imply that the reducing Archean atmosphere was in equilibrium with Earth’s mantle, and further suggest that magmatic gases crossed the threshold that allowed a build-up in atmospheric O2 levels ca. 3000 Ma, accompanied by the first “whiffs” of oxygen in sediments of that age.
We have developed and characterized the novel PTR3, a proton transfer reaction-time-of-flight mass spectrometer (PTR-TOF) using a new gas inlet and an innovative reaction chamber design. The reaction chamber consists of a tripole operated with rf voltages generating an electric field only in the radial direction. An elevated electrical field is necessary to reduce clustering of primary hydronium (H3O+) and product ions with water molecules present in the sample gas. The axial movement of the ions is achieved by the sample gas flow only. Therefore, the new design allows a 30-fold longer reaction time and a 40-fold increase in pressure compared to standard PTR-TOF-MS. First calibration tests show sensitivities of up to 18000 counts per second/parts per billion and volume (cps/ppbv) at a mass resolution of >8000 m/Δm (fwhm). The new inlet using center-sampling through a critical orifice reduces wall losses of low volatility compounds. Therefore, the new PTR3 instrument is sensitive to VOC typically present in the ppbv range as well as to semivolatile organic compounds (SVOC) and even highly oxidized organic molecules (HOMs) present in the parts per quadrillion per volume (ppqv) range in the atmosphere.
The Global Irrigation Model (GIM) is used within the framework of the global hydrological model WaterGAP to calculate monthly irrigation crop water use. Results on a 0.5 degrees grid include, consumption (ICU) and, via division by irrigation efficiencies, water withdrawal (IWU). The model distinguishes up to two cropping periods of rice and non-rice crops, each grown for 150 days, using a grid of area equipped for irrigation (AEI). Historical development of AEI and fraction of area actually irrigated (AAI) was previously considered via scaling of cell-specific results with country-specific factors for each year. In this study, GIM was adapted to use the new Historical Irrigation Data set (HID) with cell-specific AEI for 14 time slices between 1900 and 2005. AEI grids were temporally interpolated, and using the optional grid of AAI/AEI, results for years 1901-2014 were generated (runs "HID-ACT"). Thus, new installation or abandonment of irrigation infrastructure in new grid cells can be represented in a spatially explicit manner. For evaluated years 1910, 1960, 1995, and 2005, ICU from HID-ACT was superior to country-specific scaled results (run "HID-ACTHIST") in representing historical development of the spatial pattern. Compared to US state-level reference data, spatial patterns were better, while country totals were not always better. For calculating the cropping periods, 30-years climate means are needed, the choice of which is relevant. Four chosen periods before 1981-2010 all resulted in considerable, pertaining changes of ICU spatial pattern, and various percent changes in country totals. This might be because of already present climate change.
This study examines the urban heat island (UHI) of Brussels, for both current (2000–2009) and projected future (2060–2069) climate conditions, by employing very high resolution (250 m) modelling experiments, using the urban boundary layer climate model UrbClim. Meteorological parameters that are related to the intensity of the UHI are identified and it is investigated how these parameters and the magnitude of the UHI evolve for two plausible trajectories for future climate conditions. UHI intensity is found to be strongly correlated to the inversion strength in the lowest 100 m of the atmosphere. The results for the future scenarios indicate that the magnitude of the UHI is expected to decrease slightly due to global warming. This can be attributed to the increased incoming longwave radiation, caused by higher air temperature and humidity values. The presence of the UHI also has a significant impact on the frequency of extreme temperature events in the city area, both in present and future climates, and exacerbates the impact of climate change on the urban population as the amount of heat wave days in the city increases twice as fast as in the rural surroundings.
Das Ziel dieser Arbeit ist die Untersuchung der stratosphärischen Meridionalzirkulation mit Hilfe von chemisch aktiven Spurengasen. Diese motiviert sich durch die Tatsache, dass der Klimawandel neben den viel erforschten Auswirkungen auf die Troposphäre, auch Reaktionen in der Stratosphäre zur Folge hat, welche bisher weit weniger tiefgehend untersucht wurden. Das macht die Stratosphäre zu einem aktuellen und frequentierten Forschungsgebiet der experimentellen und theoretischen Meteorologie. Neben vereinzelten hochaufgelösten in-situ Messungen und globalen Satellitendaten sind es hier vor allem globale numerische Klima-Chemiemodelle, die für Analysen genutzt werden. Für diese Arbeit wurden Daten des EMAC-Modells (engl.: ECHAM/MESSy Atmospheric Chemistry) ausgwertet, welche im Rahmen der ESCiMo (engl.: Earth System Chemistry integrated Modelling) Initiative vom MESSy-Konsortium (engl.: Modular Earth Submodel System) erstellt wurden. Die Zielsetzung dieser Arbeit war, ob sich etwaige Änderungen des stratosphärischen Transports anhand von modellierten, chemisch aktiven, idealisierten Spurengasen feststellen lassen. Idealisiert bedeutet hierbei, dass diese Gase ein konstantes Mischungsverhältnis am Erdboden aufweisen und den identischen chemischen Prozessen unterliegen wie die realistischen Tracer. Dies hat zur Folge, dass diese Spurengase somit nicht in das Strahlungsbudget des Modells rückkoppeln und ihre Verteilung nicht durch zeitliche troposphärische Trends beeinflusst wird. Zur Analyse des stratosphärischen Transports wurden die Differenzen der monatlich gemittelten Mischungsverhältnisse zweier Zeitpunkte der verschiedenen Substanzen im Vertikalprofil betrachtet und ausgewertet, wobei hier die photolytische Lebenszeit und die Zeitskala des Transports zu berücksichtigen war. Um die Saisonalität von Transport und Chemie zu berücksichtigen, wurden dazu die Monate März, Juni, September und Dezember analysiert.
Die Resultate zeigten, dass chemisch aktive Substanzen in der Tat geeignet sind Änderungen in der Dynamik festzustellen. So stellte sich heraus, dass mit einer allgemeinen Intensivierung der stratosphärischen Meridionalzirkulation im kommenden Jahrhundert gerechnet werden kann, wobei hiervon besonders die untere Stratosphäre betroffen ist. Eine Differenzierung welche Komponente der Zirkulation (Residualtransport oder bidirektionale quasi-horizontale Mischung) hierbei von übergeordneter Bedeutung ist, konnte nicht spezifiziert werden. Um abzuschätzen, ob sich die Änderung der Zirkulation durch Änderungen in den Mischungsverhältnissen von chemisch aktiven Substanzen mit Hilfe von direkten Messungen nachweisen lässt, wurde die atmosphärische Variabilität des Modells bestimmt und mit den Veränderungen dieser Mischungsverhältnisse verglichen. Es zeigte sich, dass diese modellierte atmosphärische Variabilität zum Teil deutlich größer war, als die Differenzen der Mischungsverhältnisse und so ohne eine Vielzahl von in-situ Messungen keine eindeutige Aussage zulassen. Um eine statistisch valide Aussage treffen zu können, müssen daher mehrere Messreihen innerhalb eines Monats durchgeführt werden. Zudem stellte sich heraus, dass der Monat Juni der bestmögliche Messzeitraum ist, da hier die natürliche Variabilität am geringsten ist. Zuletzt wurden die Spurengase mit vergleichsweise kleiner chemischer Lebenszeit auf normierten N2O-Isoplethen untersucht und die Verschiebung dieser Kurve zwischen den zwei Zeitpunkten analysiert. Die so gewonnenen Resultate ließen den Schluss zu, dass sich auf diese Weise die atmosphärische Variabilität reduzieren lässt und bei Nutzung mit experimentellen Daten eine zu den Tracer-Differenzen konsistente Aussage zulässt. So bestärkte diese Methode die These, dass sich der stratosphärische Transport innerhalb des 21. Jahrhunderts wahrscheinlich verstärken wird.
Evidence of widespread wildfires in a coal seam from the middle Permian of the North China Basin
(2017)
The North China Basin is the largest coal-bearing basin in China, and has an areal extent of 800,000 km2. We analyzed 138 coal samples and in situ pillar coal samples of the middle Permian from this basin by macropetrography, microscope, scanning electron microscope, gas chromatography, and gas chromatography–mass spectrometer in order to study wildfires. High contents of inertinite (charcoal) and natural coke particles observed in coal samples indicate that vegetation in precursor mires and peats of the middle Permian coal from north China was exposed to far-ranging wildfires. In addition, high-molecular-weight polycyclic aromatic hydrocarbons were detected in the coal samples. These aromatic compounds were formed under high temperatures and provide further evidence of wildfire. These wildfires would have discharged significant CO and CO2 gases into the atmosphere and affected the paleoclimate and paleoecosystem.
Coccolithophores are an abundant phytoplankton group that exhibit remarkable diversity in their biology, ecology and calcitic exoskeletons (coccospheres). Their extensive fossil record is a testament to their important biogeochemical role and is a valuable archive of biotic responses to environmental change stretching back over 200 million years. However, to realise the full potential of this archive for (palaeo-)biology and biogeochemistry requires an understanding of the physiological processes that underpin coccosphere architecture. Using culturing experiments on four modern coccolithophore species (Calcidiscus leptoporus, Calcidiscus quadriperforatus, Helicosphaera carteri and Coccolithus braarudii) from three long-lived families, we investigate how coccosphere architecture responds to shifts from exponential (rapid cell division) to stationary (slowed cell division) growth phases as cell physiology reacts to nutrient depletion. These experiments reveal statistical differences in coccosphere size and the number of coccoliths per cell between these two growth phases, specifically that cells in exponential-phase growth are typically smaller with fewer coccoliths, whereas cells experiencing growth-limiting nutrient depletion have larger coccosphere sizes and greater numbers of coccoliths per cell. Although the exact numbers are species-specific, these growth-phase shifts in coccosphere geometry demonstrate that the core physiological responses of cells to nutrient depletion result in increased coccosphere sizes and coccoliths per cell across four different coccolithophore families (Calcidiscaceae, Coccolithaceae, Isochrysidaceae and Helicosphaeraceae), a representative diversity of this phytoplankton group. Building on this, the direct comparison of coccosphere geometries in modern and fossil coccolithophores enables a proxy for growth phase to be developed that can be used to investigate growth responses to environmental change throughout their long evolutionary history. Our data also show that changes in growth rate and coccoliths per cell associated with growth-phase shifts can substantially alter cellular calcite production. Coccosphere geometry is therefore a valuable tool for accessing growth information in the fossil record, providing unprecedented insights into the response of species to environmental change and the potential biogeochemical consequences.
When assessing global water resources with hydrological models, it is essential to know the methodological uncertainties in the water resources estimates. The study presented here quantifies effects of the uncertainty in the spatial and temporal patterns of meteorological variables on water balance components at the global, continental and grid cell scale by forcing the global hydrological model WaterGAP 2.2 (ISI-MIP 2.1) with five state-of-the-art climate forcing input data-sets. While global precipitation over land during 1971–2000 varies between 103 500 and 111 000 km3 yr−1, global river discharge varies between 39 200 and 42 200 km3 yr−1. Temporal trends of global wa- ter balance components are strongly affected by the uncertainty in the climate forcing (except human water abstractions), and there is a need for temporal homogenization of climate forcings (in particular WFD/WFDEI). On about 10–20 % of the global land area, change of river discharge between two consecutive 30 year periods was driven more strongly by changes of human water use including dam construction than by changes in precipitation. This number increases towards the end of the 20th century due to intensified human water use and dam construction. The calibration approach of WaterGAP against observed long-term average river discharge reduces the impact of climate forcing uncertainty on estimated river discharge significantly. Different homgeneous climate forcings lead to a variation of Q of only 1.6 % for the 54 % of global land area that are constrained by discharge observations, while estimated renewable water resources in the remaining uncalibrated regions vary by 18.5 %. Uncertainties are especially high in Southeast Asia where Global Runoff Data Centre (GRDC) data availability is very sparse. By sharing already available discharge data, or installing new streamflow gauging stations in such regions, water balance uncertainties could be reduced which would lead to an improved assessment of the world’s water resources.
Ice nucleating particles over the Eastern Mediterranean measured by unmanned aircraft systems
(2016)
During an intensive field campaign on aerosol, clouds and ice nucleation in the Eastern Mediterranean in April 2016, we have measured the abundance of ice nucleating particles (INP) in the lower troposphere from unmanned aircraft systems (UAS). Aerosol samples were collected by miniaturized electrostatic precipitators onboard the UAS at altitudes up to 2.5 km. The number of INP in these samples, which are active in the deposition and condensation modes at temperatures from −20 to −30 ◦C, were analyzed immediately after collection on site using the ice nucleus counter FRIDGE. During the one month campaign we encountered a series of Saharan dust plumes that traveled at several kilometers altitude. Here we present INP data from 42 individual flights, together with aerosol number concentrations, observations of lidar backscattering, dust concentrations derived by the dust transport model DREAM (Dust Regional Atmospheric Model), and results from scanning electron microscopy. The effect of the dust plumes is reflected by the coincidence of INP with the particulate mass (PM), the lidar signal and with the predicted dust mass of the model. This suggests that mineral dust or a constituent related to dust was a major contributor to the ice nucleating properties of the aerosol. Peak concentrations of above 100 INP std.l -1 were measured at −30 ◦C. The INP concentration in elevated plumes was on average a factor of 10 higher than at ground level. Since desert dust is transported for long distances over wide areas of the globe predominantly at several km altitude we conclude that INP measurements at ground level may be of limited significance for the situation at the level of cloud formation.
Mean age of stratospheric air can be derived from observations of sufficiently long-lived trace gases with approximately linear trends in the troposphere. Mean age can serve as a tracer to investigate stratospheric transport and long-term changes in the strength of the overturning Brewer–Dobson circulation of the stratosphere. For this purpose, a low-cost method is required in order to allow for regular observations up to altitudes of about 30 km. Despite the desired low costs, high precision and accuracy are required in order to determine mean age. We present balloon-borne AirCore observations from two midlatitude sites: Timmins in Ontario/Canada and Lindenberg in Germany. During the Timmins campaign, five AirCores sampled air in parallel with a large stratospheric balloon and were analysed for CO2, CH4 and partly CO. We show that there is good agreement between the different AirCores (better than 0.1 %), especially when vertical gradients are small. The measurements from Lindenberg were performed using small low-cost balloons and yielded very comparable results. We have used the observations to extend our long-term data set of mean age observations at Northern Hemisphere midlatitudes. The time series now covers more than 40 years and shows a small, statistically non-significant positive trend of 0.15 ± 0.18 years decade−1. This trend is slightly smaller than the previous estimate of 0.24 ± 0.22 years decade−1 which was based on observations up to the year 2006. These observations are still in contrast to strong negative trends of mean age as derived from some model calculations.
AirCore-HR : a high-resolution column sampling to enhance the
vertical description of CH₄ and CO₂
(2017)
An original and innovative sampling system called AirCore was presented by NOAA in 2010 (Karion et al., 2010). It consists of a long ( > 100 m) and narrow (< 1 cm) stainless steel tube that can retain a profile of atmospheric air. The captured air sample has then to be analyzed with a gas analyzer for trace mole fraction. In this study, we introduce a new AirCore aiming to improve resolution along the vertical with the objectives to (i) better capture the vertical distribution of CO2 and CH4, (ii) provide a tool to compare AirCores and validate the estimated vertical resolution achieved by AirCores. This (high-resolution) AirCore-HR consists of a 300 m tube, combining 200 m of 0.125 in. (3.175 mm) tube and a 100 m of 0.25 in. (6.35 mm) tube. This new configuration allows us to achieve a vertical resolution of 300 m up to 15 km and better than 500 m up to 22 km (if analysis of the retained sample is performed within 3 h). The AirCore-HR was flown for the first time during the annual StratoScience campaign from CNES in August 2014 from Timmins (Ontario, Canada). High-resolution vertical profiles of CO2 and CH4 up to 25 km were successfully retrieved. These profiles revealed well-defined transport structures in the troposphere (also seen in CAMS-ECMWF high-resolution forecasts of CO2 and CH4 profiles) and captured the decrease of CO2 and CH4 in the stratosphere. The multi-instrument gondola also carried two other low-resolution AirCore-GUF that allowed us to perform direct comparisons and study the underlying processing method used to convert the sample of air to greenhouse gases vertical profiles. In particular, degrading the AirCore-HR derived profiles to the low resolution of AirCore-GUF yields an excellent match between both sets of CH4 profiles and shows a good consistency in terms of vertical structures. This fully validates the theoretical vertical resolution achievable by AirCores. Concerning CO2 although a good agreement is found in terms of vertical structure, the comparison between the various AirCores yields a large and variable bias (up to almost 3 ppm in some parts of the pro- files). The reasons of this bias, possibly related to the drying agent used to dry the air, are still being investigated. Finally, the uncertainties associated with the measurements are assessed, yielding an average uncertainty below 3 ppb for CH4 and 0.25 ppm for CO2 with the major source of uncertainty coming from the potential loss of air sample on the ground and the choice of the starting and ending point of the collected air sample inside the tube. In an ideal case where the sample would be fully retained, it would be possible to know precisely the pressure at which air was sampled last and thus to improve the overall uncertainty to about 0.1 ppm for CO2 and 2 ppb for CH4
Recent analysis of long-term balloon-borne measurements of Antarctic stratospheric condensation nuclei (CN) and temperature combined with global model calculations showed the wide extent of a mid stratospheric layer of new particles. Here the nucleation model SAWNUC is used to derive Antarctic stratospheric gaseous sulfuric acid profiles and to investigate the nucleation process of this CN layer. The sulfuric acid profiles were derived for an altitude range of 18-32 km between July and October by simulating air parcel trajectories that descend inside the polar vortex and calculating the sulfuric acid amount that reproduces the observations. The derived sulfuric acid concentrations (volume mixing ratios) are of the order of magnitude of 104 cm-3 (10-14) in July. In the following months the concentrations increase to about 107 cm-3 (10 exp -11) in October. They depend strongly on the temperature because a given temperature leaves only a small sulfuric acid range to reproduce the observed magnitude of CN. Ion-induced nucleation occurs. However, while it dominates nucleation at higher temperatures it has no significant influence on the nucleation rates at lower temperatures. Preexisting particles significantly reduce nucleation at sulfuric acid mixing ratios below 1 ppt. First estimates of sulfuric acid production rates range from 0.5 to about 500 molecules cm-3 s-1. A production mechanism for gaseous sulfuric acid during the Antarctic winter seems to be necessary to fully explain the observations. The derived sulfuric acid profiles compare well with midlatitude and Arctic sulfuric acid concentrations.
Nucleation modeling of the Antarctic stratospheric CN layer and derivation of sulfuric acid profiles
(2017)
Recent analysis of long-term balloon-borne measurements of Antarctic stratospheric condensation nuclei (CN) between July and October showed the formation of a volatile CN layer at 21–27 km altitude in a background of existing particles. We use the nucleation model SAWNUC to simulate these CN in subsiding air parcels and study their nucleation and coagulation characteristics. Our simulations confirm recent analysis that the development of the CN layer can be explained with neutral sulfuric acid–water nucleation and we show that outside the CN layer the measured CN concentrations are well reproduced just considering coagulation and the subsidence of the air parcels. While ion-induced nucleation is expected as the dominating formation process at higher temperatures, it does not play a significant role during the CN layer formation as the charged clusters recombine too fast. Further, we derive sulfuric acid concentrations for the CN layer formation. Our concentrations are about 1 order of magnitude higher than previously presented concentrations as our simulations consider that nucleated clusters have to grow to CN size and can coagulate with preexisting particles. Finally, we calculate threshold sulfuric acid profiles that show which concentration of sulfuric acid is necessary for nucleation and growth to observable size. These threshold profiles should represent upper limits of the actual sulfuric acid outside the CN layer. According to our profiles, sulfuric acid concentrations seem to be below midlatitude average during Antarctic winter but above midlatitude average for the CN layer formation.
Der "Regionalatlas Rhein-Main" wird zum 75-jährigen Jubiläum der "Rhein-Mainischen Forschung" veröffentlicht. Er verfolgt das Ziel,
- einne Überblick über die regionale Struktur des Rhein-Main-Gebietes zu verschaffen,
- Politik, Wirtschaft und Verwaltung Grundlagendaten in regionalisierter Form für ihre Entscheidungen an die Hand zu geben, und
- den im Rhein-Main-Gebiet lebenden Menschen die regionalen Strukturen ihres Lebensraumes näher zu bringen.
Im Rahmen einer Zusammenarbeit zwischen der Thüringer Landesanstalt für Umwelt und Geologie und der Goethe-Universität Frankfurt fand in Kooperation mit dem Deutschen Wetterdienst (DWD) eine umfassende Studie zum konvektiven Unwetterpotential über Thüringen statt. Unwetterereignisse, die durch konvektive Prozesse in der Atmosphäre verursacht werden, besitzen ein nicht unerhebliches Schadenspotential, obwohl sie oftmals eine räumlich eng begrenzte Ausdehnung aufweisen. Aufgrund ihrer Charakteristik ist sowohl die Vorhersage solcher Ereignisse, als auch eine vollständige, systematische Erfassung für eine detaillierte Auswertung längerer Zeitreihen noch immer eine Herausforderung. Zusätzliches Interesse besteht in der Abschätzung der durch den Klimawandel abhängigen Entwicklung des zukünftigen Gefährdungspotentials konvektiver Unwetter. Für eine gezielte Untersuchung des Themenkomplexes ist eine Vielzahl unterschiedlicher Daten und Methoden verwendet worden. Mit Hilfe von Fernerkundungsdatensätzen wird ein räumlich differenziertes Gefährdungspotential über Thüringen nachgewiesen. Bedingt durch das Relief ist das Auftreten von Konvektion am häufigsten und intensivsten über dem südlichen Thüringer Wald und dessen Ostrand zu beobachten, während Nordthüringen eine deutlich geringere Aktivität solcher Unwetterereignisse aufweist. Eine Abschätzung mittels globaler Klimamodelle und daraus abgeleiteten Wetterlagen zeigt unter Berücksichtigung des RCP8.5 Klimaszenarios für die nahe Zukunft (2016-2045) eine Zunahme des Gefährdungspotentials durch konvektive Unwetter. Aufgrund des Anstiegs feuchter Wetterlagen (49 % auf 82 %) erhöht sich die Zunahme der Gefährdung für den Zeitraum 2071-2100 noch deutlicher. Im Vergleich zu diesem statistischen Ansatz nimmt die projizierte Gefährdung durch extreme Ereignisse erheblich zu (Faktor 6), wenn die Ergebnisse expliziter Simulationen konvektiver Ereignisse mit einem regionalen Klimamodell (mit horizontaler Gitterdistanz von 1 km) und eine Zunahme der Tage mit konvektiven Extremereignissen berücksichtigt werden. Ein Anstieg der Gefährdung durch konvektive Unwetter in der Zukunft ist wahrscheinlich. Eine Quantifizierung bleibt jedoch unsicher.
Laut jüdischem Kalender entstand die Welt vor genau 5778 Jahren, nach der Bibel vor 6021 Jahren. Doch als Forscher begannen, auf und in der Erde selbst nach Spuren ihres Alters zu suchen, mussten sie die Zahl immer weiter nach oben korrigieren. Nach heutigen Datierungsmethoden ist unser Planet zwischen 4,5 und 4,6 Milliarden Jahre alt.
The Earth’s surface condition we find today is a result of long exposure to metabolism of life forms. Particularly, molecular oxygen in the atmosphere is a feature which developed over time. The first substantial and lasting rise of atmospheric oxygen level happened ≈ 2.5 Ga ago, but localities are reported where transiently elevated oxygen levels appeared before this time-point. To trace the timing and circumstances of the earliest availability of free oxygen in the atmosphere is important to understand the habitats of early microbial life forms on Earth.
This thesis focuses to obtain information of oxygen levels and the related atmospheric cycling of metals in sediments of the 3.5 to 3.2 Ga Barberton Greenstone Belt. First, as iron was a ubiquitous constituent of Archean seawater, I investigated its isotopic composition in minerals of chemical sediments. Hereby, I tried to resolve the changes within the water basin on small scale sedimentary sequence cycles. Second, I focused on the minor constituents of Archean seawater. The Re-Os geochronologic system and the abundance patterns of the platinum-group elements were chosen to integrate information of oxygen promoted weathering of a large source area. To integrate information of a large time interval, the isotopes of uranium were investigated over a large stratigraphic section.
The two key findings of this thesis are:
• Quantitative oxidation of ferrous iron in surface layers of Paleoarchean seawater occurred during the onset and termination of hydrothermal FeIIaq delivery into shallow waters.
• Paleoarchean sedimentary successions of the Barberton Greenstone Belt lack any evidence of transient basin-scale oxygenation.
The Manzimnyama Iron Formation (IF, Fig Tree Group, Barberton Greenstone Belt, South Africa) has been deciphered to exist of cyclic stacks of lithostratigraphic units with varying amounts of iron oxide and carbonate minerals. In-situ femtosecond-Laser-Ablation ICP-MS iron isotope measurements showed that the majority of siderite (γ56Fe ≈ −0.5 ‰) precipitated directly from seawater of γ56Fe ≈ 0 ‰. Ferric iron from the surface layers is preserved in ≤ 1μ m hematite and in magnetite that has been grown within the consolidated sediment. During FeIIaq events, fine-grained hematite (γ56Fe ≈ 2.2 ‰) and magnetite (γ56Fe 0.5 to 0.8 ‰) indicate oxygen levels in surface waters of lower than 0.0002 μM. Upon onset and termination of iron oxide abundance, magnetite with γ56Fe ≈ 0 ‰ indicates that low concentrations of FeIIaq in surface waters were oxidized quantitatively. These observations demonstrate the existence of iron oxidation in Paleoarchean surface waters independent of FeIIaq concentration. This is the first investigation of Paleoarchean IF showing that lithostratigraphic cyclicity can be traced in iron isotopic composition of oxide minerals.
ID-ICP-MS measurement of Re, Ir, Ru, Pt and Pd, trace element (SF-ICP-MS) and ID-MCICP- MS uranium isotope determination have been applied to carbonaceous shale of the Mapepe Fm. (Fig Tree Group) after inverse Aqua Regia leaching and bulk digestion. The sediments reveal a silicified fraction which exhibits a seawater REE signature and a mixture of detrital and meteoritic PGE. Neither enrichment of the redox-sensitive elements Re or Mo nor fractionated uranium isotopes have been found on a stratigraphic interval of several hundred meters. The non-silica fraction shows no depletion of Re which indicates that the detrital material had no contact to oxidizing fluids. ID-TIMS measurements of Re and Os after the CrO3-SO4 Carius Tube method of two sample intervals showed that the Re-Os isotopic systems of the non-silica fractions are identical to two komatiite occurrences. Weltevreden Fm. and Komati Fm. rocks were uplifted, eroded and transported to the deep part of the sedimentary basin without any change to the Re-Os system. Negative fractionated uranium isotopes (γ238U = −0.41 ± 0.01 ‰) associated with detrital Ba-Cr-U occurrences suggest the existence of distal redox-processes that involve uranium species. This study demonstrates that over the time of exposure and deposition of the Mapepe Fm. sedimentation, free oxygen was not available for weathering in the catchment area.
Ice nucleating particles over the eastern mediterranean measured by unmanned aircraft systems
(2017)
During an intensive field campaign on aerosol, clouds, and ice nucleation in the Eastern Mediterranean in April 2016, we measured the abundance of ice nucleating particles (INPs) in the lower troposphere from unmanned aircraft systems (UASs). Aerosol samples were collected by miniaturized electrostatic precipitators onboard the UASs at altitudes up to 2.5 km. The number of INPs in these samples, which are active in the deposition and condensation modes at temperatures from −20 to −30 °C, were analyzed immediately after collection on site using the ice nucleus counter FRIDGE (FRankfurt Ice nucleation Deposition freezinG Experiment). During the 1-month campaign, we encountered a series of Saharan dust plumes that traveled at several kilometers' altitude. Here we present INP data from 42 individual flights, together with aerosol number concentrations, observations of lidar backscattering, dust concentrations derived by the dust transport model DREAM (Dust Regional Atmospheric Model), and results from scanning electron microscopy. The effect of the dust plumes is reflected by the coincidence of INPs with the particulate matter (PM), the lidar signal, and the predicted dust mass of the model. This suggests that mineral dust or a constituent related to dust was a major contributor to the ice nucleating properties of the aerosol. Peak concentrations of above 100 INPs std L−1 were measured at −30 °C. The INP concentration in elevated plumes was on average a factor of 10 higher than at ground level. Since desert dust is transported for long distances over wide areas of the globe predominantly at several kilometers' altitude, we conclude that INP measurements at ground level may be of limited significance for the situation at the level of cloud formation.
Geoelektrische Methoden sind weit verbreitet und werden häufig zur Erkundung des oberflächennahen Untergrundes eingesetzt. Angewendet werden standardmäßig meist nur linienhafte Anordnungen der Sender- und Empfängerelektroden, die nur wenige Zehner Meter lang sind. Hierdurch haben diese Methoden nur geringe Eindringtiefen. Um größere Eindringtiefen und 3-dimensionale Informationen über den Untergrund zu erhalten, sind in der vorgestellten Studie die Empfänger- und Senderdipole in mehr oder weniger regelmäßigen Abständen über das Untersuchungsgebiet verteilt worden. Mit jeder Empfängerstation sind kontinuierlich die elektrischen Spannungen in bis zu drei Richtungen aufgezeichnet worden. Für die Einspeisungen wurde ein Rechtecksignal verwendet, das sich gut von den Störfrequenzen und den natürlichen Spannungen abhebt. Die Richtungen der Einspeisedipole sind entsprechend den örtlichen Gegebenheiten, jedoch möglichst parallel zu den Messrichtungen, gewählt worden. Zur Auswertung der erhobenen Messdaten wurde ein Programmpaket entwickelt, das eine weitestgehend automatisierte Auswertung der Daten erlaubt. Die Bestimmung der scheinbaren spezifischen Widerstände und ihrer Messfehler wurde an den fouriertransformierten Datenzeitreihen durchgeführt. Hierdurch konnten Störeinflüsse minimiert werden und es wurde möglich selbst stark verrauschte Datensätze auszuwerten. Um die erhobenen Daten interpretieren zu können sind die berechneten scheinbaren spezifischen Widerstände als Grundlage für Inversionen und Modellstudien verwendet worden. Die oben beschriebene Methode wurde im Rahmen der vorliegenden Arbeit in zwei unterschiedlichen Messgebieten angewandt.
Messgebiet im Hohen Vogelsberg
Im Juli 2007 wurde damit begonnen, die Forschungsbohrung Sichenhausen-Eschwald im Hohen Vogelsberg abzuteufen. Ziel war es, Informationen über den strukturellen Aufbau des größten geschlossenen Vulkankomplexes Mitteleuropas zu gewinnen. Die Gesteinsansprache der Tiefbohrung lieferte bereits relativ früh Hinweise darauf, dass ein großer magmatischer Körper aufgeschlossen wurde.Aufgrund der begrenzten räumlichen Aussagekraft der Bohrung und fehlender Geländebefunde war es nicht möglich, den Mechanismus der Platznahme und die Größe des Körpers näher zu beschreiben. Die Kampagne hatte das Ziel diese Lücke zu schließen und ein 3-dimensionales Modell des Untergrundes zu erstellen.In dem annähernd quadratischen Untersuchungsgebiet, das eine Fläche von ca. 25 $km²$ aufweist, wurden 20 Datenlogger zur Aufzeichnung der elektrischen Spannungen aufgebaut. Die Empfängerdipole waren zwischen 20 m und 30 m lang. Insgesamt wurden 36 Stromeinspeisungen mit Stromstärken zwischen 28 A und 40 A an 16 unterschiedlichen Positionen für jeweils 2 bis 3 verschiedene Dipolrichtungen vorgenommen. Die Einspeisedipole waren zwischen 100 m und 300 m lang. Insgesamt konnten 1.439 scheinbare spezifische Widerstände berechnet werden.Die Ergebnisse der Modellierungen und der Inversion der Daten zeigen, dass mit der Forschungsbohrung ein domartiger Körper angebohrt wurde. Anhand der Ergebnisse kann die räumliche Ausdehnung des Körpers eingegrenzt und ein vorher noch nicht kartierter Gang nachgewiesen werden.
Messgebiet im Bereich der Kinzigtalsperre
Das etwa Ost-West verlaufende Kinzigtal bildet die naturräumliche und geologische Grenze zwischen dem vulkanischen Vogelsberg im Norden und dem, in diesem Bereich aus Sedimentgesteinen aufgebauten, Spessart im Süden.Die zwischen Steinau a. d. Str. und Bad Soden-Salmünster befindliche Kinzigtalsperre dient dem Hochwasserschutz und der Regulierung des Pegels der Kinzig bei Dürreperioden. Der aufgestaute See ist relativ flach und weist im Normalstau maximale Tiefen von ca. 6~m auf. Der Stausee ist jedoch über weite Teile etwa 4~m tief. In dieser Kampagne betrug der Abstand zwischen den einzelnen Empfängerstationen etwa 100 m bis 300 m. Es wurde aufgrund der beengten Platzverhältnisse eine Dipollänge von ca. 48 m für die Einspeise- und die Empfängerdipole im Messgebiet gewählt. Insgesamt wurden 14 Empfängerstationen im Messgebiet aufgebaut, von denen sich Neun auf dem Seegrund befanden. Das Messraster orientierte sich am vermuteten Verlauf der Kinzigtalstörung. An 8 Positionen sind in 21 Richtungen elektrische Ströme mit Stärken zwischen 2,2 A und 40 A in den Untergrund eingespeist worden. Es konnten 536 scheinbare spezifische Widerstände berechnet werden. Ziel war es, den Verlauf der Störung näher zu bestimmen und die Tiefe der im Untergrund vorhandenen salinären Grundwässer zu bestimmen. Die Bestimmung des Verlaufs der Kinzigtalstörung sowie die Tiefenbestimmung der salinären Grundwässer war mit den erhobenen Daten jedoch nicht möglich.
Small-scale thermal upwellings under the northern East African Rift from S travel time tomography
(2016)
There is a long-standing debate over how many and what types of plumes underlie the East African Rift and whether they do or do not drive its extension and consequent magmatism and seismicity. Here we present a new tomographic study of relative teleseismic S and SKS residuals that expands the resolution from previous regional studies below the northern East African Rift to image structure from the surface to the base of the transition zone. The images reveal two low-velocity clusters, below Afar and west of the Main Ethiopian Rift, that extend throughout the upper mantle and comprise several smaller-scale (about 100 km diameter), low-velocity features. These structures support those of our recent P tomographic study below the region. The relative magnitude of S to P residuals is around 3.5, which is consistent with a predominantly thermal nature of the anomalies. The S and P velocity anomalies in the low-velocity clusters can be explained by similar excess temperatures in the range of 100–200°C, consistent with temperatures inferred from other seismic, geochemical, and petrological studies. Somewhat stronger VS anomalies below Afar than west of the Main Ethiopian Rift may include an expression of volatiles and/or melt in this region. These results, together with a comparison with previous larger-scale tomographic models, indicate that these structures are likely small-scale upwellings with mild excess temperatures, rising from a regional thermal boundary layer at the base of the upper mantle.
The Fire Modeling Intercomparison Project (FireMIP), phase 1: experimental and analytical protocols
(2016)
The important role of fire in regulating vegetation community composition and contributions to emissions of greenhouse gases and aerosols make it a critical component of dynamic global vegetation models and Earth system models. Over two decades of development, a wide variety of model structures and mechanisms have been designed and incorporated into global fire models, which have been linked to different vegetation models. However, there has not yet been a systematic examination of how these different strategies contribute to model performance. Here we describe the structure of the first phase of the Fire Model Intercomparison Project (FireMIP), which for the first time seeks to systematically compare a number of models. By combining a standardized set of input data and model experiments with a rigorous comparison of model outputs to each other and to observations, we will improve the understanding of what drives vegetation fire, how it can best be simulated, and what new or improved observational data could allow better constraints on model behavior. Here we introduce the fire models used in the first phase of FireMIP, the simulation protocols applied, and the benchmarking system used to evaluate the models. The works published in this journal are distributed under the Creative Commons Attribution 3.0 License. This license does not affect the Crown copy-right work, which is re-usable under the Open Government Licence (OGL). The Creative Commons Attribution 3.0 License and the OGL are interoperable and do not conflict with, reduce, or limit each other.
The important role of fire in regulating vegetation community composition and contributions to emissions of greenhouse gases and aerosols make it a critical component of dynamic global vegetation models and Earth system models. Over 2 decades of development, a wide variety of model structures and mechanisms have been designed and incorporated into global fire models, which have been linked to different vegetation models. However, there has not yet been a systematic examination of how these different strategies contribute to model performance. Here we describe the structure of the first phase of the Fire Model Intercomparison Project (FireMIP), which for the first time seeks to systematically compare a number of models. By combining a standardized set of input data and model experiments with a rigorous comparison of model outputs to each other and to observations, we will improve the understanding of what drives vegetation fire, how it can best be simulated, and what new or improved observational data could allow better constraints on model behavior. In this paper, we introduce the fire models used in the first phase of FireMIP, the simulation protocols applied, and the benchmarking system used to evaluate the models. We have also created supplementary tables that describe, in thorough mathematical detail, the structure of each model.
In this study, we aim to reconstruct a relevant and new database of monthly zonal mean distribution of carbon dioxide (CO2) at global scale extending from the upper-troposphere (UT) to stratosphere (S). This product can be used for model and satellite validation in the UT/S, as a prior for inversion modelling and mainly to analyse a plausible feature of the stratospherictropospheric exchange as well as the stratospheric circulation and its variability. To do so, we investigate the ability of a Lagrangian trajectory model guided by ERA-Interim reanalysis to construct the CO2 abundance in the UT/S. From 10 year backward trajectories and tropospheric observations of CO2, we reconstruct upper-tropospheric and stratospheric CO2 over the period 2000–2010. The inter-comparisons of the reconstructed CO2 with mid-latitude vertical profiles measured by balloon samples as well as quasi-horizontal air samples from ER-2 aircraft during SOLVE and CONTRAIL campaigns exhibit a remarkable agreement. That demonstrates the potential of Lagrangian model to reconstruct CO2 in the UT/S. The zonal mean distribution exhibits relatively large CO2 in the tropical stratosphere due to the seasonal variation of the tropical upwelling of Brewer-Dobson circulation. During winter and spring, the tropical pipe is relatively isolated but is less confined during summer and autumn so that high CO2 values are more readily transported out of the tropics to the mid- and high latitude stratosphere. The shape of the vertical profiles suggests that relatively high CO2 above 20 km altitude mainly enter the stratosphere through tropical upwelling. CO2 mixing ratio is relatively low in the polar and tropical regions above 25 km. On average the CO2 mixing ratio decreases with altitude by 6-8 ppmv from the UT to stratosphere (e.g. up to 35 km) and is nearly constant with altitude.
In this study, we construct a new monthly zonal mean carbon dioxide (CO2) distribution from the upper troposphere to the stratosphere over the 2000–2010 time period. This reconstructed CO2 product is based on a Lagrangian backward trajectory model driven by ERA-Interim reanalysis meteorology and tropospheric CO2 measurements. Comparisons of our CO2 product to extratropical in situ measurements from aircraft transects and balloon profiles show remarkably good agreement. The main features of the CO2 distribution include (1) relatively large mixing ratios in the tropical stratosphere; (2) seasonal variability in the extratropics, with relatively high mixing ratios in the summer and autumn hemisphere in the 15–20 km altitude layer; and (3) decreasing mixing ratios with increasing altitude from the upper troposphere to the middle stratosphere ( ∼ 35 km). These features are consistent with expected variability due to the transport of long-lived trace gases by the stratospheric Brewer–Dobson circulation. The method used here to construct this CO2 product is unique from other modelling efforts and should be useful for model and satellite validation in the upper troposphere and stratosphere as a prior for inversion modelling and to analyse features of stratosphere–troposphere exchange as well as the stratospheric circulation and its variability.
The fractional release factor (FRF) gives information on the amount of a halocarbon that is released at some point in the stratosphere from its source form to the inorganic form, which can harm the ozone layer through catalytic reactions. The quantity is of major importance because it directly affects the calculation of the Ozone Depletion Potential (ODP). To apply FRF in this context, steady-state values are needed, thus representing a molecular property for a given atmospheric situation. In particular, these values should be independent of the tropospheric trends of the respective halogenated trace gases.
We analyzed the temporal evolution of FRF from ECHAM/MESSy Atmospheric Chemistry (EMAC) model simulations for several halocarbons and nitrous oxide between 1965–2011 on different mean age levels and found that the current formulation of FRF yields highly time-dependent values. We show that this is caused by the way that the tropospheric trend is handled in the current calculation method of FRF.
Taking into account chemical loss in the calculation of stratospheric mixing ratios reduces the time-dependence in correlations of different tracers. Therefore we implemented a loss term in the formulation of FRF and applied the parameterization of a "mean arrival time" to our data set.
We find that the time-dependence in FRF can almost be compensated by applying a new trend correction in the calculation of FRF. We suggest that this new method should be used to calculate time-independent FRF, which can then be used e.g. for the calculation of ODP
The fractional release factor (FRF) gives information on the amount of a halocarbon that is released at some point into the stratosphere from its source form to the inorganic form, which can harm the ozone layer through catalytic reactions. The quantity is of major importance because it directly affects the calculation of the ozone depletion potential (ODP). In this context time-independent values are needed which, in particular, should be independent of the trends in the tropospheric mixing ratios (tropospheric trends) of the respective halogenated trace gases. For a given atmospheric situation, such FRF values would represent a molecular property.
We analysed the temporal evolution of FRF from ECHAM/MESSy Atmospheric Chemistry (EMAC) model simulations for several halocarbons and nitrous oxide between 1965 and 2011 on different mean age levels and found that the widely used formulation of FRF yields highly time-dependent values. We show that this is caused by the way that the tropospheric trend is handled in the widely used calculation method of FRF.
Taking into account chemical loss in the calculation of stratospheric mixing ratios reduces the time dependence in FRFs. Therefore we implemented a loss term in the formulation of the FRF and applied the parameterization of a mean arrival time to our data set.
We find that the time dependence in the FRF can almost be compensated for by applying a new trend correction in the calculation of the FRF. We suggest that this new method should be used to calculate time-independent FRFs, which can then be used e.g. for the calculation of ODP.
Medium range hydrological forecasts in mesoscale catchments are only possible with the use of hydrological models driven by meteorological forecasts, which in particular contribute quantitative precipitation forecasts (QPF). QPFs are accompanied by large uncertainties, especially for longer lead times, which are propagated within the hydrometeorological model system. To deal with this limitation of predictability, a probabilistic forecasting system is tested, which is based on a hydrological-meteorological ensemble prediction system. The meteorological component of the system is the operational limited-area ensemble prediction system COSMO-LEPS that downscales the global ECMWF ensemble to a horizontal resolution of 10 km, while the hydrological component is based on the semi-distributed hydrological model PREVAH with a spatial resolution of 500 m.
Earlier studies have mostly addressed the potential benefits of hydrometeorological ensemble systems in short case studies. Here we present an analysis of hydrological ensemble hindcasts for two years (2005 and 2006). It is shown that the ensemble covers the uncertainty during different weather situations with an appropriate spread-skill relationship. The ensemble also shows advantages over a corresponding deterministic forecast, even under consideration of an artificial spread.
Volatile organic compounds (VOCs) were analyzed in air and snow samples at the Jungfraujoch high alpine research station in Switzerland as part of CLACE 5 (CLoud and Aerosol Characterization Experiment) during February/March 2006. The fluxes of individual compounds in ambient air were calculated from gas phase concentrations and wind speed. The highest flux values were observed for the aromatic hydrocarbons benzene (14.3 µg m−2s−1), 1,3,5-trimethylbenzene (5.27 µg m−2s−1), toluene (4.40 µg m−2s−1), and the aliphatic hydrocarbons i-butane (7.87 µg m−2s−1), i-pentane (3.61 µg m−2s−1) and n-butane (3.23 µg m−2s−1). The fluxes were used to calculate the efficiency of removal of VOCs by snow, and the effect of temperature on removal efficiency. The removal efficiency was calculated at – 24◦C (−13.7◦C) and ranged from 37% (35%) for o-xylene to 93% (63%) for i-pentane. The distribution coefficients of VOCs between the air and snow phases were derived from published poly-parameter linear free energy relationship (pp-LFER) data, and compared with distribution coef- ficients obtained from the simultaneous measurements of VOC concentrations in air and snow at Jungfraujoch. The coefficients calculated from pp-LFER exceeded those values measured in the present study, which indicates more efficient snow scavenging of the VOCs investigated than suggested by theoretical predictions.
Quantification of spatially and temporally resolved water flows and water storage variations for all land areas of the globe is required to assess water resources, water scarcity and flood hazards, and to understand the Earth system. This quantification is done with the help of global hydrological models (GHMs). What are the challenges and prospects in the development and application of GHMs? Seven important challenges are presented. (1) Data scarcity makes quantification of human water use difficult even though significant progress has been achieved in the last decade. (2) Uncertainty of meteorological input data strongly affects model outputs. (3) The reaction of vegetation to changing climate and CO2 concentrations is uncertain and not taken into account in most GHMs that serve to estimate climate change impacts. (4) Reasons for discrepant responses of GHMs to changing climate have yet to be identified. (5) More accurate estimates of monthly time series of water availability and use are needed to provide good indicators of water scarcity. (6) Integration of gradient-based groundwater modelling into GHMs is necessary for a better simulation of groundwater–surface water interactions and capillary rise. (7) Detection and attribution of human interference with freshwater systems by using GHMs are constrained by data of insufficient quality but also GHM uncertainty itself. Regarding prospects for progress, we propose to decrease the uncertainty of GHM output by making better use of in situ and remotely sensed observations of output variables such as river discharge or total water storage variations by multi-criteria validation, calibration or data assimilation. Finally, we present an initiative that works towards the vision of hyperresolution global hydrological modelling where GHM outputs would be provided at a 1-km resolution with reasonable accuracy.
Samples of freshly fallen snow were collected at the high alpine research station Jungfraujoch (Switzerland) in February and March 2006 and 2007, during the Cloud and Aerosol Characterization Experiments (CLACE) 5 and 6. In this study a new technique has been developed and demonstrated for the measurement of organic acids in fresh snow. The melted snow samples were subjected to solid phase extraction and resulting solution analysed for organic acids by HPLC-MS-TOF using negative electrospray ionization. A series of linear dicarboxylic acids from C5 to C13 and phthalic acid, were identified and quantified. In several samples the biogenic acid pinonic acid was also observed. In fresh snow the median concentration of the most abundant acid, adipic acid, was 0.69 µg L−1 in 2006 and 0.70 µg L−1 in 2007. Glutaric acid was the second most abundant dicarboxylic acid found with median values of 0.46 µg L−1 in 2006 and 0.61 µg L−1 in 2007, while the aromatic acid phthalic acid showed a median concentration of 0.34 µg L−1 in 2006 and 0.45 µg L−1 in 2007. The concentrations in the samples from various snowfall events varied significantly, and were found to be dependent on the back trajectory of the air mass arriving at Jungfraujoch. Air masses of marine origin showed the lowest concentrations of acids whereas the highest concentrations were measured when the air mass was strongly influenced by boundary layer air.
This PhD thesis has been carried out within an interdisciplinary cooperational project between the Deutsches Bergbau-Museum Bochum and the Goethe-Universität Frankfurt, which is dedicated to ancient Pb-Ag mining and metal production in the hinterland of the municipium Ulpiana in central Kosovo. Geochemical analysis (OM, XRD, EMP, MC-ICP-MS) of ores, metallurgical (by-) products and metal artefacts allowed to reconstruct the local chaîne opératoire and to decipher significant chronological differences between presumably Roman/late antique and medieval/early modern metallurgical processing. Pb isotope provenance studies documented the relevance of local metal production within the Roman Empire and confirmed the actual existence of a Metalla Dardanica district, which until now solely has been suspected on basis of epigraphy.
The predominant abundance of the by-products matte (Cu, Pb, Fe and Zn sulphides) and speiss (ferrous speiss: Fe-As compounds; base metal speiss: ~(Cu,Ni,Fe,Ag )x(Sb,Sn,As )y ) at smelting sites with a preliminary Roman/late antique dating points to treatment of complex polymetallic ore. Pb isotope analysis demonstrated that the mining district of Shashkoc-Janjevo (partially) supplied six of the ten investigated metallurgical sites. In this mineralisation, parageneses with elevated Cu, As and Sb abundances comprise significant proportions of particularly tennantite-tetrahedrite minerals, chalcopyrite, arsenopyrite and were generated during the early and main stages of ore formation. Later precipitated ore in contrast is marked by a significantly less versatile mineralogy and consists almost exclusively of galena, sphalerite and pyrite/marcasite. Besides increased Cu, As and Sb contents, ore from the main formation stage also exhibits generally higher Ag abundances, which are mainly hosted by fahlore and locally abundant secondary Cu sulphides (chalcocite, digenite and covellite) and oxidised phases (e.g. malachite, azurite). The higher precious metal grades of this ore type, whose geochemical signature (i.e. higher proportions of Cu, As and Sb) is mirrored by the abundance of the metallurgical by-products matte and speiss (almost exclusively found at potentially Roman/late antique smelting sites; see above), presumably were a pivotal factor leading to its preferential exploitation in earlier times. Matte and base metal-rich speiss contain notable amounts of Ag, which are mainly present in Cu-(Fe) sulphides and particularly antimonides ((Cu,Ni)2Sb, Ag3Sb), respectively. While the speiss compounds due to their close association with Pb bullion presumably were cupelled automatically, the metallurgical treatment of matte could not have been proven unambiguously, but overall certainly is highly likely.
The beneficiated ore (i.e. crushed and sorted, potentially also treated by more lavish techniques such as grinding, sieving or wet-mechanical methods) possibly was partially roasted and subsequently together with fluxes and charcoal submitted to the furnaces. The working temperatures approximately ranged between 1100 and 1400 °C. Slags from all presumably Roman/late antique dated and few of their potentially medieval/early modern analogues were produced from smelting of (partially roasted) ore with charcoal and added siliceous material, thus resulting in fayalite-dominant phase assemblages or rarely observed glassy parageneses. Even though several subtypes of fayalite slags have been established on basis of the abundance of Fe-rich oxide phases (i.e. spinel ss and wüstite), late clinopyroxene and the general solidification sequence of the slags, the process conditions (i.e. temperature, fO2, added fluxing agents) must have been widely similar; chemical variations could be explained by varying degrees of interaction of the slag melt with charcoal ash and furnace material. The other investigated metallurgical remains indicate employment of a calcareous flux, which led to formation of Ca-rich olivine-, olivine+clinopyroxene-, clinopyroxene- or melilite-type slags. These types as well as glassy slags were generated at more oxidising conditions outside the fayalite stability field (FMQ buffer equilibrium, cf. Lindsley, 1976) than their olivine-dominant analogues. Conclusions on the furnace construction could be drawn on basis of the typology of the slags, which mostly were tapped into a basin located outside the furnace, but partially (at two presumably medieval/early modern sites) also accumulated in a reservoir within the smelter.
Lead artefacts excavated in Ulpiana could be isotopically related to ores from mineralisations in its vicinity and demonstrate that the resources were at least utilised for local metal production. However, also ship wreck cargo from Israel - including several lead ingots with the inscription 'MET DARD' (Raban, 1999) - and late antique lead-glazed pottery from Serbia and Romania (Walton & Tite, 2010) could be related to a possible Kosovarian/Serbian provenance of the raw material and thus indicate flourishing trade of metal from the Metalla Dardanica district within the Roman Empire.
References:
Lindsley, D. H. (1976). Experimental studies of oxide minerals. In D. Rumble, III (Hrsg.), Oxide minerals (61-88). Reviews in Mineralogy, Volume 3. Washington, DC: Mineralogical Society of America.
Raban, A. (1999). The lead ingots from the wreck site (area K8). Journal of Roman Archaeology, Supplementary Series, 35, 179-188.
Walton, M. S., & Tite, M. S. (2010). Production technology of Roman lead-glazed pottery and its continuance into late antiquity. Archaeometry, 52(5), 733-759.
Mean age of stratospheric air can be derived from observations of sufficiently long lived trace gases with approximately linear trends in the troposphere. Mean age can serve as a tracer to investigate stratospheric transport and long term changes in the strength of the overturning Brewer-Dobson circulation of the stratosphere. For this purpose, a low-cost method is required in order to allow for regular observations up to altitudes of about 30 km. Despite the desired low costs, high precision and accuracy are required in order to allow determination of mean age. We present balloon borne AirCore observations from two mid latitude sites: Timmins in Ontario/Canada and Lindenberg in Germany. During the Timmins campaign five AirCores sampled air in parallel from a large stratospheric balloon and were analysed for CO2, CH4 and partly CO. We show that there is good agreement between the different AirCores (better than 0.1 %) especially when vertical gradients are small. The measurements from Lindenberg were performed using small low-cost balloons and yielded very comparable results. We have used the observations to extend our long term data set of mean age observations at Northern Hemi-sphere mid latitudes. The time series now covers more than 40 years and shows a small, statis-tically not significant positive trend of 0.15 ± 0.18 years/decade. This trend is slightly smaller than the previous estimate of 0.24 ± 0.22 years/decade which was based on observations up to the year 2006. These observations are still in contrast to strong negative trends of mean age as derived from some model calculations.
Ziel der Arbeit war es, die Flugzeitmassenspektrometrie als neue Analysemethode für die instrumentelle Analytik halogenierter Spurengase in der Luft zu etablieren. Die grundle-gende Motivation dafür ist, dass anthropogene Emissionen vieler Vertreter dieser Sub-stanzklasse einen negativen Einfluss auf die Umwelt zeigen: in der Atmosphäre agieren die Substanzen bzw. ihre Abbauprodukte als Katalysatoren für den stratosphärischen Ozonab-bau und verstärken den Strahlungsantrieb der Erde durch Absorption elektromagnetischer Strahlung im sogenannten atmosphärischen Fenster. Um diese Effekte und deren Auswir-kung quantifizieren zu können, ist es notwendig, Konzentrationen und Trends der Substan-zen in der Atmosphäre zu überwachen. Nur so können Gegenmaßnahmen wie Produktions-reglementierungen geplant und bewertet werden. In Kombination mit inverser Modellie-rung können zudem Rückschlüsse über tatsächlich emittierten Mengen gezogen werden. Dies stellt den Anspruch an die Analytik, sehr geringe Mengen dieser Gase sehr präzise quantifizieren zu können, um auch schwache Trends zu erkennen. Zudem muss die Analy-semethode die Möglichkeit zu bieten, mit der wachsenden Anzahl bekannter und zu über-wachender Substanzen Schritt zu halten. Besonders für letzteren Aspekt bietet die Flug-zeitmassenspektrometrie einen entscheidenden Vorteil gegenüber der „konventionellen“ Methode, der Quadrupolmassenspektrometrie: sie zeichnet das gesamten Massenspektrum auf ohne dadurch an Empfindlichkeit einzubüßen. Um das atmosphärische Mischungsver-hältnis von Substanzen im Bereich von pmol mol−1 bis fmol mol−1 bestimmen zu können, muss das Quadrupolmassenspektrometer im Single Ion Monitoring Modus betrieben wer-den – so wird zwar eine hohe Sensitivität erreicht, es wird aber auch nur die Intensität eines bestimmten Masse zu Ladungsverhältnisses (kurz: Masse) zu einem Zeitpunkt aufgezeich-net. Ein Flugzeitmassenspektrometer hingegen extrahiert Ionen mit einer Frequenz im Ki-loherzbereich und zeichnet für jede Extraktion das vollständige Flugzeitspektrum und da-mit Massenspektrum auf.
Aufgabe dieser Arbeit war es, ein Flugzeitmassenspektrometer mit vorgeschalteter Pro-benanreicherungseinheit sowie Gaschromatograph zur Trennung des Subtanzgemisches vor der Detektion aufzubauen und Werkzeuge zur Datenauswertung zu entwickeln. Um einen zukünftigen Feldeinsatz vorzubereiten, sollte der Aufbau möglichst kompakt, mobil und vollständig automatisiert sein. Anschließend sollte Empfindlichkeit, Präzision und dynami-scher Messbereich geprüft, optimiert und die Anwendbarkeit zur Analyse halogenierter Spurengase gezeigt werden. Die Ergebnisse aus der in der vorliegenden Arbeit präsentier-ten Geräteentwicklung finden sich in drei Publikationen wieder, welche in thematischer Reihenfolge die Probenanreicherung (Obersteiner et al., 2016b), den Vergleich von Quadrupol- und Flugzeitmassenspektrometrie (Hoker et al., 2015) sowie Eigenschaften und Anwendung des neuen Aufbaus (Obersteiner et al., 2016a) behandeln. Mit den genannten Aufsätzen ist die Arbeitsgruppe Engel weltweit die erste, welche hochpräzise Analytik ha-logenierter Spurengase routinemäßig mittels Flugzeitmassenspektrometrie durchführt. Der nächste Schritt ist der Übergang von der Laboranwendung zur Feldmessung, z.B. in Form von bodenbasierter in situ Analyse troposphärischer Luftmassen am Taunus Observatorium auf dem Kleinen Feldberg. Da es bisher keine Messstation für die hier beschriebene analy-tische Fragestellung in Deutschland gibt, könnte eine deutliche Verbesserung der Überwa-chung halogenierter Treibhausgase und ozonzerstörender Substanzen in Europa erzielt wer-den. Weiterhin wäre eine Flugzeugapplikation in Zukunft denkbar, welche neben der durch das Flugzeitmassenspektrometer abgedeckten Substanzbandbreite auch von dessen hoher möglicher Spektrenrate profitieren könnte. In Kombination mit Hochgeschwindigkeitsgas-chromatographie könnte eine bisher unerreichte Zeitauflösung der Beprobung der Atmo-sphäre mittels Gaschromatographie-Massenspektrometrie erzielt werden.
Aerosolteilchen agieren als Kondensationskeime für Wolkentröpfchen (engl. Cloud Condensation Nuclei, CCN) oder Eiskristalle und sind deswegen für die Wolken- und Niederschlagsbildung entscheidend. Sowohl die Aerosolpartikel als auch die Wolken können Sonnenlicht effizient streuen, wodurch ein kühlender Effekt auf das Klima ausgeübt wird. Einige der Teilchen, wie z. B. aufgewirbelter Staub oder Seesalz, werden direkt in die Atmosphäre injiziert; der größte Anteil der Teilchen und etwa die Hälfte der CCN werden allerdings durch die Kondensation gasförmiger Substanzen gebildet. Dieser Prozess wird als Nukleation oder Partikelneubildung (engl. New Particle Formation, NPF) bezeichnet. Trotz intensiver Forschung ist die NPF noch nicht vollständig verstanden, was an der Komplexität der chemischen Abläufe in der Atmosphäre und an der Schwierigkeit liegt, die relevanten Substanzen bei extrem geringen Mischungsverhältnissen (etwa ein Molekül oder Cluster per 1012 bis 1015 Moleküle) zu identifizieren und zu quantifizieren. Neben der Frage nach den bei der Nukleation beteiligten Substanzen ist außerdem noch unklar, ob Ionen-induzierte Nukleation ein wichtiger Prozess für das Klima ist. Das CLOUD-Projekt (Cosmics Leaving OUtdoor Droplets) am CERN soll diesen Fragen nachgehen, indem dort die Partikelbildung in einem Kammer-Experiment unter extrem gut kontrollierten Bedingungen simuliert wird. Die chemischen Systeme, die in dieser Schrift diskutiert werden, umfassen das binäre (H2SO4-H2O), das ternäre Ammoniak (H2SO4-H2O-NH3) und das ternäre Dimethylamin (H2SO4-H2O-(CH3)2NH)-System.
Einige der wesentlichen Ergebnisse von Experimenten an der CLOUD-Kammer werden diskutiert. Diese zeigen, dass das binäre und das ternäre Ammoniak System die atmosphärische Nukleation bei niedrigen Temperaturen erklären können, wohingegen das ternäre Dimethylamin System prinzipiell in der Lage ist, die hohen bodennahen Nukleationsraten bei atmosphärisch relevanten Schwefelsäure-Konzentrationen zu beschreiben. Des Weiteren werden zwei für Nukleationsstudien wesentliche Messmethoden vorgestellt. Das Chemical Ionization Mass Spectrometer (CIMS) wird zur Messung von gasförmiger Schwefelsäure verwendet, da H2SO4 vermutlich die wichtigste Substanz bei der atmosphärischen Nukleation ist. Das Chemical Ionization-Atmospheric Pressure interface-Time Of Flight (CI-APi-TOF) Massenspektrometer misst Schwefelsäure und neutrale Cluster. Beide Geräte wurden für den Einsatz bei CLOUD optimiert und instrumentelle Entwicklungen wurden in Bezug auf die Ionenquelle vorgenommen, die eine Korona-Entladung verwendet. Außerdem wurden eine Kalibrationseinheit zur Bereitstellung definierter Schwefelsäure-Konzentrationen entwickelt und das CI-APi-TOF aufgebaut. In Bezug auf das ternäre Dimethylamin System werden Nukleationsraten und die ersten Messungen von gro en nukleierenden neutralen Clustern präsentiert. Monomer- und Dimer-Konzentrationen der Schwefelsäure, die mit dem CIMS bei tiefen Temperaturen gemessen wurden, dienten der Ableitung der thermodynamischen Eigenschaften bei der Dimer-Bildung im binären und ternären Ammoniak System. Um möglichst exakte Nukleationsraten zu bestimmen, wurde eine neue Methode entwickelt, die es erlaubt, den Effekt der Selbst-Koagulation bei der Nukleation miteinzubeziehen.
Die zusammengefassten Studien tragen signifikant zum Verständnis der Partikelneubildung bei.
Desert dust is one of the most abundant ice nucleating particle types in the atmosphere. Traditionally, clay minerals were assumed to determine the ice nucleation ability of desert dust and constituted the focus of ice nucleation studies over several decades. Recently some feldspar species were identified to be ice active at much higher temperatures than clay minerals, redirecting studies to investigate the contribution of feldspar to ice nucleation on desert dust. However, so far no study has shown the atmospheric relevance of this mineral phase.
For this study four dust samples were collected after airborne transport in the troposphere from the Sahara to different locations (Crete, the Peloponnese, Canary Islands, and the Sinai Peninsula). Additionally, 11 dust samples were collected from the surface from nine of the biggest deserts worldwide. The samples were used to study the ice nucleation behavior specific to different desert dusts. Furthermore, we investigated how representative surface-collected dust is for the atmosphere by comparing to the ice nucleation activity of the airborne samples. We used the IMCA-ZINC setup to form droplets on single aerosol particles which were subsequently exposed to temperatures between 233 and 250 K. Dust particles were collected in parallel on filters for offline cold-stage ice nucleation experiments at 253–263 K. To help the interpretation of the ice nucleation experiments the mineralogical composition of the dusts was investigated. We find that a higher ice nucleation activity in a given sample at 253 K can be attributed to the K-feldspar content present in this sample, whereas at temperatures between 238 and 245 K it is attributed to the sum of feldspar and quartz content present. A high clay content, in contrast, is associated with lower ice nucleation activity. This confirms the importance of feldspar above 250 K and the role of quartz and feldspars determining the ice nucleation activities at lower temperatures as found by earlier studies for monomineral dusts. The airborne samples show on average a lower ice nucleation activity than the surface-collected ones. Furthermore, we find that under certain conditions milling can lead to a decrease in the ice nucleation ability of polymineral samples due to the different hardness and cleavage of individual mineral phases causing an increase of minerals with low ice nucleation ability in the atmospherically relevant size fraction. Comparison of our data set to an existing desert dust parameterization confirms its applicability for climate models. Our results suggest that for an improved prediction of the ice nucleation ability of desert dust in the atmosphere, the modeling of emission and atmospheric transport of the feldspar and quartz mineral phases would be key, while other minerals are only of minor importance.
Desert dust is one of the most abundant ice nucleating particle types in the atmosphere. Tra ditionally, clay minerals were assumed to determine the ice nucleation ability of desert dust and constituted the focus of ice nucleation studies. Only recently some feldspar species were identified to be ice-active at much higher temperatures than clay minerals, redirecting studies to investigate the contribution of feldspar to ice nucleation on desert dust. However, so far no study has shown the atmospheric relevance of this mineral phase.
For this study four dust samples were collected after airborne transport in the troposphere from the Sahara to different locations (Crete, the Peloponnese, Canary Islands and the Sinai Peninsula). Additionally, eleven dust samples were collected from the surface from nine of the biggest deserts worldwide. The samples were used to study the ice nucleation behavior specific to different desert dusts. Furthermore we investigated how representative ice nucleation on surface-collected dust is for that in the atmosphere by comparing to the ice nucleation activity of the airborne samples. We used the IMCA-ZINC set-up to form droplets on single aerosol particles which were subsequently exposed to temperatures between 233 - 250 K. Dust particles were collected in parallel on filters for offline cold stage ice nucleation experiments at 253 - 263 K. To help the interpretation of the results from the ice nucleation experiments the mineralogical composition of the dusts was investigated.We found that a higher ice nucleation activity in a given sample can be attributed at 253 K to the K-feldspar content present in this sample whereas at temperatures between 238 - 245 K it is attributed to the sum of feldspar and quartz content present. A high clay content on the other hand is associated with a lower ice nucleation activity of a sample. This confirms the importance of feldspar at T > 250 K and the role of quartz and feldspars determining the ice nucleation activities at lower T as found by earlier studies for monomineral dust surrogates. Furthermore, we find that milling may lead to a decrease in the ice nucleation ability of polymineral samples due to a change in mineralogical composition in the atmospherically relevant size fraction arising from the different hardness and cleavage of individual mineral phases. Comparison of our comprehensive data set to an existing desert dust parameterization confirms its applicability for climate models. Our results suggest that for an improved prediction of the ice nucleation ability of desert dust in the atmosphere, the modelling of emission and atmospheric transport of the feldspar and quartz mineral phases would be key while other minerals are only of minor importance.
In situ single particle analysis of ice particle residuals (IPRs) and out-of-cloud aerosol particles was conducted by means of laser ablation mass spectrometry during the intensive INUIT-JFJ/CLACE campaign at the high alpine research station Jungfraujoch (3580 m a.s.l.) in January–February 2013. During the 4-week campaign more than 70 000 out-of-cloud aerosol particles and 595 IPRs were analyzed covering a particle size diameter range from 100 nm to 3 µm. The IPRs were sampled during 273 h while the station was covered by mixed-phase clouds at ambient temperatures between −27 and −6 °C. The identification of particle types is based on laboratory studies of different types of biological, mineral and anthropogenic aerosol particles. The outcome of these laboratory studies was characteristic marker peaks for each investigated particle type. These marker peaks were applied to the field data. In the sampled IPRs we identified a larger number fraction of primary aerosol particles, like soil dust (13 ± 5 %) and minerals (11 ± 5 %), in comparison to out-of-cloud aerosol particles (2.4 ± 0.4 and 0.4 ± 0.1 %, respectively). Additionally, anthropogenic aerosol particles, such as particles from industrial emissions and lead-containing particles, were found to be more abundant in the IPRs than in the out-of-cloud aerosol. In the out-of-cloud aerosol we identified a large fraction of aged particles (31 ± 5 %), including organic material and secondary inorganics, whereas this particle type was much less abundant (2.7 ± 1.3 %) in the IPRs. In a selected subset of the data where a direct comparison between out-of-cloud aerosol particles and IPRs in air masses with similar origin was possible, a pronounced enhancement of biological particles was found in the IPRs.
In-situ single particle analysis of ice particle residuals (IPR) and out-of-cloud aerosol particles was conducted by means of laser ablation mass spectrometry during the intensive INUIT-JFJ/CLACE campaign at the high alpine research station Jungfraujoch (3580 m a.s.l.) in January/February 2013. During the four week campaign more than 70000 out-of-cloud aerosol particles and 595 IPR were analyzed covering a particle size diameter range from 100 nm to 3 μm. The IPR were sampled during 273 hours while the station was covered by mixed-phase clouds at ambient temperatures between -27 °C and -6 °C. The identification of particle types is based on laboratory studies of different types of biological, mineral and anthropogenic aerosol particles. As outcome instrument specific marker peaks for the different investigated particle types were obtained and applied to the field data. The results show that the sampled IPR contain a larger relative amount of natural, primary aerosol, like soil dust (13 %) and minerals (11 %), in comparison to out-of-cloud aerosol particles (2 % and <1 %, respectively). Additionally, anthropogenic aerosol particles, like particles from industrial emissions and lead-containing particles, were found to be more abundant in the IPR than in the out-of-cloud aerosol. The out of-cloud aerosol contained a large fraction of aged particles (30 %, including organic material and secondary inorganics), whereas this particle type was much less abundant (3 %) in the IPR. In a selected subset of the data where a direct comparison between out-of-cloud aerosol particles and IPR in air masses with similar origin was possible, a pronounced enhancement of biological particles was found in the IPR.
Size-resolved long-term measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations and hygroscopicity were conducted at the remote Amazon Tall Tower Observatory (ATTO) in the central Amazon Basin over a 1-year period and full seasonal cycle (March 2014–February 2015). The measurements provide a climatology of CCN properties characteristic of a remote central Amazonian rain forest site.
The CCN measurements were continuously cycled through 10 levels of supersaturation (S = 0.11 to 1.10 %) and span the aerosol particle size range from 20 to 245 nm. The mean critical diameters of CCN activation range from 43 nm at S = 1.10 % to 172 nm at S = 0.11 %. The particle hygroscopicity exhibits a pronounced size dependence with lower values for the Aitken mode (κAit = 0.14 ± 0.03), higher values for the accumulation mode (κAcc = 0.22 ± 0.05), and an overall mean value of κmean = 0.17 ± 0.06, consistent with high fractions of organic aerosol.
The hygroscopicity parameter, κ, exhibits remarkably little temporal variability: no pronounced diurnal cycles, only weak seasonal trends, and few short-term variations during long-range transport events. In contrast, the CCN number concentrations exhibit a pronounced seasonal cycle, tracking the pollution-related seasonality in total aerosol concentration. We find that the variability in the CCN concentrations in the central Amazon is mostly driven by aerosol particle number concentration and size distribution, while variations in aerosol hygroscopicity and chemical composition matter only during a few episodes.
For modeling purposes, we compare different approaches of predicting CCN number concentration and present a novel parametrization, which allows accurate CCN predictions based on a small set of input data.
Size-resolved long-term measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations as well as hygroscopicity were conducted at the remote Amazon Tall Tower Observatory (ATTO) in the central Amazon Basin over a one-year period and full seasonal cycle (March 2014 - February 2015). The presented measurements provide a climatology of CCN properties for a characteristic central Amazonian rain forest site.
The CCN measurements were continuously cycled through 10 levels of supersaturation (S = 0.11 to 1.10 %) and span the aerosol particle size range from 20 to 245 nm. The observed mean critical diameters of CCN activation range from 43 nm at S = 1.10 % to 172 nm at S = 0.11 %. The particle hygroscopicity exhibits a pronounced size dependence with lower values for the Aitken mode (κAit = 0.14 ± 0.03), elevated values for the accumulation mode (κAcc = 0.22 ± 0.05), and an overall mean value of κmean = 0.17 ± 0.06, consistent with high fractions of organic aerosol.
The hygroscopicity parameter κ exhibits remarkably little temporal variability: no pronounced diurnal cycles, weak seasonal trends, and few short-term variations during long-range transport events. In contrast, the CCN number concentrations exhibit a pronounced seasonal cycle, tracking the pollution-related seasonality in total aerosol concentration. We find that the variability in the CCN concentrations in the central Amazon is mostly driven by aerosol particle number concentration and size distribution, while variations in aerosol hygroscopicity and chemical composition matter only during a few episodes.
For modelling purposes, we compare different approaches of predicting CCN number concentration and present a novel parameterization, which allows accurate CCN predictions based on a small set of input data.
The total stratospheric organic chlorine and bromine burden was derived from balloon-borne measurements in the tropics (Teresina, Brazil, 5°04´ S, 42°52´ W) in 2005. Whole air samples were collected cryogenically at altitudes between 15 and 34 km. For the first time, we report measurements of a set of 28 chlorinated and brominated substances in the tropical upper troposphere and stratosphere including ten substances with an atmospheric lifetime of less than half a year. The substances were quantified using pre-concentration techniques followed by Gas Chromatography with Mass Spectrometric detection. In the tropical tropopause layer at altitudes between 15 and 17 km we found 1.1–1.4% of the chlorine and 6–8% of the bromine to be present in the form of very short-lived organic compounds. By combining the data with tropospheric reference data and age of air observations the abundances of inorganic chlorine and bromine (Cly and Bry) were derived. At an altitude of 34 km we calculated 3062 ppt of Cly and 17.5 ppt of Bry from the decomposition of both long- and short-lived organic source gases. Furthermore we present indications for the presence of additional organic brominated substances in the tropical upper troposphere and stratosphere.
Climate change and its impacts already pose considerable challenges for societies that will further increase with global warming (IPCC, 2014a, b). Uncertainties of the climatic response to greenhouse gas emissions include the potential passing of large-scale tipping points (e.g. Lenton et al., 2008; Levermann et al., 2012; Schellnhuber, 2010) and changes in extreme meteorological events (Field et al., 2012) with complex impacts on societies (Hallegatte et al., 2013). Thus climate change mitigation is considered a necessary societal response for avoiding uncontrollable impacts (Conference of the Parties, 2010). On the other hand, large-scale climate change mitigation itself implies fundamental changes in, for example, the global energy system. The associated challenges come on top of others that derive from equally important ethical imperatives like the fulfilment of increasing food demand that may draw on the same resources. For example, ensuring food security for a growing population may require an expansion of cropland, thereby reducing natural carbon sinks or the area available for bio-energy production. So far, available studies addressing this problem have relied on individual impact models, ignoring uncertainty in crop model and biome model projections. Here, we propose a probabilistic decision framework that allows for an evaluation of agricultural management and mitigation options in a multi-impact-model setting. Based on simulations generated within the Inter-Sectoral Impact Model Intercomparison Project (ISI-MIP), we outline how cross-sectorally consistent multi-model impact simulations could be used to generate the information required for robust decision making.
Using an illustrative future land use pattern, we discuss the trade-off between potential gains in crop production and associated losses in natural carbon sinks in the new multiple crop- and biome-model setting. In addition, crop and water model simulations are combined to explore irrigation increases as one possible measure of agricultural intensification that could limit the expansion of cropland required in response to climate change and growing food demand. This example shows that current impact model uncertainties pose an important challenge to long-term mitigation planning and must not be ignored in long-term strategic decision making.
In order to achieve climate change mitigation, long-term decisions are required that must be reconciled with other societal goals that draw on the same resources. For example, ensuring food security for a growing population may require an expansion of crop land, thereby reducing natural carbon sinks or the area available for bio-energy production. Here, we show that current impact-model uncertainties pose an important challenge to long-term mitigation planning and propose a new risk-assessment and decision framework that accounts for competing interests.
Based on cross-sectorally consistent simulations generated within the Inter-Sectoral Impact Model Intercomparison Project (ISI-MIP) we discuss potential gains and limitations of additional irrigation and trade-offs of the expansion of agricultural land as two possible response measures to climate change and growing food demand. We describe an illustrative example in which the combination of both measures may close the supply demand gap while leading to a loss of approximately half of all natural carbon sinks.
We highlight current limitations of available simulations and additional steps required for a comprehensive risk assessment.
Comparing projections of future changes in runoff from hydrological and biome models in ISI-MIP
(2013)
Future changes in runoff can have important implications for water resources and flooding. In this study, runoff projections from ISI-MIP (Inter-sectoral Impact Model Intercomparison Project) simulations forced with HadGEM2-ES bias-corrected climate data under the Representative Concentration Pathway 8.5 have been analysed for differences between impact models. Projections of change from a baseline period (1981–2010) to the future (2070–2099) from 12 impacts models which contributed to the hydrological and biomes sectors of ISI-MIP were studied. The biome models differed from the hydrological models by the inclusion of CO2 impacts and most also included a dynamic vegetation distribution. The biome and hydrological models agreed on the sign of runoff change for most regions of the world. However, in West Africa, the hydrological models projected drying, and the biome models a moistening. The biome models tended to produce larger increases and smaller decreases in regionally averaged runoff than the hydrological models, although there is large inter-model spread. The timing of runoff change was similar, but there were differences in magnitude, particularly at peak runoff. The impact of vegetation distribution change was much smaller than the projected change over time, while elevated CO2 had an effect as large as the magnitude of change over time projected by some models in some regions. The effect of CO2 on runoff was not consistent across the models, with two models showing increases and two decreases. There was also more spread in projections from the runs with elevated CO2 than with constant CO2. The biome models which gave increased runoff from elevated CO2 were also those which differed most from the hydrological models. Spatially, regions with most difference between model types tended to be projected to have most effect from elevated CO2, and seasonal differences were also similar, so elevated CO2 can partly explain the differences between hydrological and biome model runoff change projections. Therefore, this shows that a range of impact models should be considered to give the full range of uncertainty in impacts studies.
Profiles of CFC-11 (CCl3F) and CFC-12 (CCl2F2) of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) aboard the European satellite Envisat have been retrieved from versions MIPAS/4.61 to MIPAS/4.62 and MIPAS/5.02 to MIPAS/5.06 level-1b data using the scientific level-2 processor run by Karlsruhe Institute of Technology (KIT), Institute of Meteorology and Climate Research (IMK) and Consejo Superior de Investigaciones Científicas (CSIC), Instituto de Astrofísica de Andalucía (IAA). These profiles have been compared to measurements taken by the balloon-borne cryosampler, Mark IV (MkIV) and MIPAS-Balloon (MIPAS-B), the airborne MIPAS-STRatospheric aircraft (MIPAS-STR), the satellite-borne Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) and the High Resolution Dynamic Limb Sounder (HIRDLS), as well as the ground-based Halocarbon and other Atmospheric Trace Species (HATS) network for the reduced spectral resolution period (RR: January 2005–April 2012) of MIPAS. ACE-FTS, MkIV and HATS also provide measurements during the high spectral resolution period (full resolution, FR: July 2002–March 2004) and were used to validate MIPAS CFC-11 and CFC-12 products during that time, as well as profiles from the Improved Limb Atmospheric Spectrometer, ILAS-II. In general, we find that MIPAS shows slightly higher values for CFC-11 at the lower end of the profiles (below ∼ 15 km) and in a comparison of HATS ground-based data and MIPAS measurements at 3 km below the tropopause. Differences range from approximately 10 to 50 pptv ( ∼ 5–20 %) during the RR period. In general, differences are slightly smaller for the FR period. An indication of a slight high bias at the lower end of the profile exists for CFC-12 as well, but this bias is far less pronounced than for CFC-11 and is not as obvious in the relative differences between MIPAS and any of the comparison instruments. Differences at the lower end of the profile (below ∼ 15 km) and in the comparison of HATS and MIPAS measurements taken at 3 km below the tropopause mainly stay within 10–50 pptv (corresponding to ∼ 2–10 % for CFC-12) for the RR and the FR period. Between ∼ 15 and 30 km, most comparisons agree within 10–20 pptv (10–20 %), apart from ILAS-II, which shows large differences above ∼ 17 km. Overall, relative differences are usually smaller for CFC-12 than for CFC-11. For both species – CFC-11 and CFC-12 – we find that differences at the lower end of the profile tend to be larger at higher latitudes than in tropical and subtropical regions. In addition, MIPAS profiles have a maximum in their mixing ratio around the tropopause, which is most obvious in tropical mean profiles. Comparisons of the standard deviation in a quiescent atmosphere (polar summer) show that only the CFC-12 FR error budget can fully explain the observed variability, while for the other products (CFC-11 FR and RR and CFC-12 RR) only two-thirds to three-quarters can be explained. Investigations regarding the temporal stability show very small negative drifts in MIPAS CFC-11 measurements. These instrument drifts vary between ∼ 1 and 3 % decade−1. For CFC-12, the drifts are also negative and close to zero up to ∼ 30 km. Above that altitude, larger drifts of up to ∼ 50 % decade−1 appear which are negative up to ∼ 35 km and positive, but of a similar magnitude, above.
The organic rich Livello Bonarelli formed as a result of oxygen deficiency and carbonate dissolution in the oceans during the Cenomanian/Turonian (C/T) transition. During this Ocean Anoxic Event 2 (OAE2), a combination of factors caused increased productivity, incomplete decomposition of organic matter and widespread deposition of black shales. Although these sediments are extensively studied, the exact extent, cause, timing and duration of oceanic anoxia are debated (Sinton and Duncan, 1997; Mitchell et al., 2008). Contrasting causal mechanisms have been suggested, including stratification of the water column (Lanci et al., 2010) versus intensification of the hydrological cycle driving a dynamic ocean circulation (Trabucho-Alexandre et al., 2010). Studies on trace-elemental and (radiogenic) isotope compositions of Cenomanian marine successions have suggested a volcanic origin of OAE2, by delivering nutrients to the semi-enclosed proto-North Atlantic (Zheng et al., 2013, and references therein; Du Vivier et al., 2014). Deciphering the importance of volcanic and oceanographic processes requires tight constraints on their relative timing. Regularly occurring black cherts and shales below the Livello Bonarelli demonstrate that oceanic conditions in the Umbria-Marche Basin were punctuated by episodes of regional anoxia from the mid-Cenomanian onwards. Their hierarchical stacking pattern suggests an orbital control on the deposition of organic rich horizons (Mitchell et al., 2008; Lanci et al., 2010). Stable carbon isotope data reveal that long-term 15 variations in eccentricity paced the carbon cycle (Sprovieri et al., 2013) and sea level changes (Voigt et al., 2006) of the Late Cretaceous. Here we investigate the role of orbital forcing on climate and the carbon cycle, and, specifically, on organic-rich sedimentation prior, during, and after OAE2.
We also explore the potential for establishing an anchored astrochronology for the C/T interval in Europe. Recent improvements in the astronomical solution (La2011; Laskar et al., 2011b) and in the intercalibration of radiometric and astronomical dating techniques (Kuiper et al., 2008; Renne et al., 2013) allow the extension of the astronomical time scale into the Cretaceous. The C/T boundary in the Western Interior (USA) has been dated at 93.90 ± 0.15 Ma by intercalibration of radio-isotopic and astrochronologic time scales (Meyers et al., 2012b). Also, reinterpretation of proxy records spanning the C/T interval seems to resolve discrepancies in reported durations of the OAE2 (Sageman et al., 2006; Meyers et al., 2012a). The well-documented Italian rhythmic successions, reference sections for climatic processes in the Tethyan realm, need to be tied in with the absolute time scale. Biostratigraphic correlation to radioisotopically-dated ash beds in the Western Interior is complicated by the provinciality of faunas and floras. However, δ13C stratigraphy provides a reliable correlation tool (Gale et al., 2005) and we present a new 40Ar/39Ar age for the Thatcher bentonite from the Western Interior occurring within the mid-Cenomanian δ13C event (MCE). This study integrates the well-developed cyclostratigraphy from the Umbria-Marche Basin with radioisotopic ages from the Western Interior and derives a numerical timescale for this critical interval in Earth’s history.
The oceans at the time of the Cenomanian–Turonian transition were abruptly perturbed by a period of bottom-water anoxia. This led to the brief but widespread deposition of black organic-rich shales, such as the Livello Bonarelli in the Umbria–Marche Basin (Italy). Despite intensive studies, the origin and exact timing of this event are still debated. In this study, we assess leading hypotheses about the inception of oceanic anoxia in the Late Cretaceous greenhouse world by providing a 6 Myr long astronomically tuned timescale across the Cenomanian–Turonian boundary. We procure insights into the relationship between orbital forcing and the Late Cretaceous carbon cycle by deciphering the imprint of astronomical cycles on lithologic, physical properties, and stable isotope records, obtained from the Bottaccione, Contessa and Furlo sections in the Umbria–Marche Basin. The deposition of black shales and cherts, as well as the onset of oceanic anoxia, is related to maxima in the 405 kyr cycle of eccentricity-modulated precession. Correlation to radioisotopic ages from the Western Interior (USA) provides unprecedented age control for the studied Italian successions. The most likely tuned age for the base of the Livello Bonarelli is 94.17 ± 0.15 Ma (tuning 1); however, a 405 kyr older age cannot be excluded (tuning 2) due to uncertainties in stratigraphic correlation, radioisotopic dating, and orbital configuration. Our cyclostratigraphic framework suggests that the exact timing of major carbon cycle perturbations during the Cretaceous may be linked to increased variability in seasonality (i.e. a 405 kyr eccentricity maximum) after the prolonged avoidance of seasonal extremes (i.e. a 2.4 Myr eccentricity minimum). Volcanism is probably the ultimate driver of oceanic anoxia, but orbital periodicities determine the exact timing of carbon cycle perturbations in the Late Cretaceous. This unites two leading hypotheses about the inception of oceanic anoxia in the Late Cretaceous greenhouse world.
The LPJ-GUESS dynamic vegetation model uniquely combines an individual- and patch-based representation of vegetation dynamics with ecosystem biogeochemical cycling from regional to global scales. We present an updated version that includes plant and soil N dynamics, analysing the implications of accounting for C-N interactions on predictions and performance of the model. Stand structural dynamics and allometric scaling of tree growth suggested by global databases of forest stand structure and development were well-reproduced by the model in comparison to an earlier multi-model study. Accounting for N cycle dynamics improved the goodness-of-fit for broadleaved forests. N limitation associated with low N mineralisation rates reduces productivity of cold-climate and dry-climate ecosystems relative to mesic temperate and tropical ecosystems. In a model experiment emulating free-air CO2 enrichment (FACE) treatment for forests globally, N-limitation associated with low N mineralisation rates of colder soils reduces CO2-enhancement of NPP for boreal forests, while some temperate and tropical forests exhibit increased NPP enhancement. Under a business-as-usual future climate and emissions scenario, ecosystem C storage globally was projected to increase by c. 10 %; additional N requirements to match this increasing ecosystem C were within the high N supply limit estimated on stoichiometric grounds in an earlier study. Our results highlight the importance of accounting for C-N interactions not only in studies of global terrestrial C cycling, but to understand underlying mechanisms on local scales and in different regional contexts.
The LPJ-GUESS dynamic vegetation model uniquely combines an individual- and patch-based representation of vegetation dynamics with ecosystem biogeochemical cycling from regional to global scales. We present an updated version that includes plant and soil N dynamics, analysing the implications of accounting for C–N interactions on predictions and performance of the model. Stand structural dynamics and allometric scaling of tree growth suggested by global databases of forest stand structure and development were well reproduced by the model in comparison to an earlier multi-model study. Accounting for N cycle dynamics improved the goodness of fit for broadleaved forests. N limitation associated with low N-mineralisation rates reduces productivity of cold-climate and dry-climate ecosystems relative to mesic temperate and tropical ecosystems. In a model experiment emulating free-air CO2 enrichment (FACE) treatment for forests globally, N limitation associated with low N-mineralisation rates of colder soils reduces CO2 enhancement of net primary production (NPP) for boreal forests, while some temperate and tropical forests exhibit increased NPP enhancement. Under a business-as-usual future climate and emissions scenario, ecosystem C storage globally was projected to increase by ca. 10%; additional N requirements to match this increasing ecosystem C were within the high N supply limit estimated on stoichiometric grounds in an earlier study. Our results highlight the importance of accounting for C–N interactions in studies of global terrestrial N cycling, and as a basis for understanding mechanisms on local scales and in different regional contexts.