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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.
Ice nucleating particle concentrations of the past: insights from a
600 year old Greenland ice core
(2020)
Ice nucleating particles (INPs) affect the microphysics in cloud and precipitation processes. Hence, they modulate the radiative properties of clouds. However, atmospheric INP concentrations of the past are basically unknown. Here, we present INP measurements from an ice core in Greenland, which dates back to the year 1370. In total 135 samples were analyzed with the FRIDGE droplet freezing assay in the temperature range from −14 ◦C to −35 ◦C. The sampling frequency was set to 1 in 10 years from 1370 to 1960. From 1960 to 1990 the frequency was increased to 1 sample per year. Additionally, a number of special events were probed, including volcanic episodes. The typical time coverage of a sample was on the order of a few months. Historical atmospheric INP concentrations were estimated with a conversion factor, which depends on the snow accumulation rate of the ice core, particle dry deposition velocity and the wet scavenging ratio. Typical atmospheric INP concentrations were on the order of 0.1 L -1 at −25 ◦C. The INP variability was found to be about 1 – 2 orders of magnitude. Yet, the short-term variability from samples over a seasonal cycle was considerably lower. INP concentrations were significantly correlated to chemical tracers derived from continuous flow analysis (CFA) and ion chromatography (IC) over a broad range of nucleation temperatures. The highest correlation coefficients were found for the particle concentration (dp > 1.2 µm). The correlation is higher for the seasonal samples, where INP concentrations follow a clear annual pattern, highlighting the importance of the annual dust input in Greenland from East Asian deserts during spring. Scanning electron microscopy (SEM) of single particles retrieved from selected samples found particles of soil origin to be the dominant fraction, verifying the significance of mineral dust particles as INPs. Overall, the concentrations compare reasonably well to present day INP concentrations, albeit they are on the lower side. However, we found that the INP concentration at medium supercooled temperatures differed before and after 1960. Average INP concentrations at −23 ◦C, −24 ◦C, −25 ◦C, −26 ◦C and −28 ◦C were significantly higher (and more variable) in the modern day period, which could indicate a potential anthropogenic impact or some post-coring contamination of the topmost, very porous firn.
Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments
(2015)
Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e. particles that have grown to diameters of 10 and 15nm following nucleation, and measure their water uptake. Water uptake constrains their chemical composition. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90% relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) experiments performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation. The hygroscopicity parameter Κ decreased with increasing particle size indicating decreasing acidity of particles. No clear effect of the sulfuric acid monomer concentrations on the hygroscopicities of 10nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15nm particles sharply decreased with decreasing sulfuric acid monomer concentrations. In 20 particular, when the concentrations of sulfuric acid was 5.1 x 106 molecules cm exp -3 in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured Κ of 15nm particles was 0.3 ± 0.01 close to the value reported for dimethylamine sulfate (DMAS) (Κ DMAS ~ 0.28). Furthermore, the difference in Κ between sulfuric acid and sulfuric acid-dimethylamine experiments increased with increasing particle size. The Κ values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from α-pinene ozonolysis play a significant role in particle growth already at 10nm sizes.
Hygroscopicity of nanoparticles produced from homogeneous
nucleation in the CLOUD experiments
(2016)
Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15 nm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90 % relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid–dimethylamine, and sulfuric acid–organics derived from α-pinene oxidation. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles. No clear effect of the sulfuric acid concentration on the hygroscopicity of 10 nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15 nm particles sharply decreased with decreasing sulfuric acid concentrations. In particular, when the concentration of sulfuric acid was 5.1 × 106 molecules cm−3 in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured κ of 15 nm particles was 0.31 ± 0.01: close to the value reported for dimethylaminium sulfate (DMAS) (κDMAS ∼ 0.28). Furthermore, the difference in κ between sulfuric acid and sulfuric acid–imethylamine experiments increased with increasing particle size. The κ values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from α-pinene ozonolysis play a significant role in particle growth even at 10 nm sizes.
Convection-permitting climate model are promising tools for improved representation of extremes, but the number of regions for which these models have been evaluated are still rather limited to make robust conclusions. In addition, an integrated interpretation of near-surface characteristics (typically temperature and precipitation) together with cloud properties is limited. The objective of this paper is to comprehensively evaluate the performance of a ‘state-of-the-art’ regional convection-permitting climate model for a mid-latitude coastal region with little orographic forcing. For this purpose, an 11-year integration with the COSMO-CLM model at Convection-Permitting Scale (CPS) using a grid spacing of 2.8 km was compared with in-situ and satellite-based observations of precipitation, temperature, cloud properties and radiation (both at the surface and the top of the atmosphere). CPS clearly improves the representation of precipitation, in especially the diurnal cycle, intensity and spatial distribution of hourly precipitation. Improvements in the representation of temperature are less obvious. In fact the CPS integration overestimates both low and high temperature extremes. The underlying cause for the overestimation of high temperature extremes was attributed to deficiencies in the cloud properties: The modelled cloud fraction is only 46 % whereas a cloud fraction of 65 % was observed. Surprisingly, the effect of this deficiency was less pronounced at the radiation balance at the top of the atmosphere due to a compensating error, in particular an overestimation of the reflectivity of clouds when they are present. Overall, a better representation of convective precipitation and a very good representation of the daily cycle in different cloud types were demonstrated. However, to overcome remaining deficiencies, additional efforts are necessary to improve cloud characteristics in CPS. This will be a challenging task due to compensating deficiencies that currently exist in ‘state-of-the-art’ models, yielding a good representation of average climate conditions. In the light of using the CPS models to study climate change it is necessary that these deficiencies are addressed in future research.
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.
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.
A satellite-based climate record of monthly mean surface solar irradiance (SIS) is investigated with regard to possible inhomogeneities in time. The data record is provided by the European Organisation for the Exploitation of Meteorological Satellites (EUMETSAT) Satellite Application Facility on Climate Monitoring (CM SAF) for the period of 1983 to 2005, covering a disk area between ±70° in latitude and longitude. The Standard Normal Homogeneity Test (SNHT) and two other homogeneity tests are applied with and without the use of reference SIS data (from the Baseline Surface Radiation Network (BSRN) and from the ECMWF (European Centre for Medium-Range Weather Forecasts) ERA -Interim reanalysis. The focus is on the detection of break-like inhomogeneities, which may occur due to satellite or SIS retrieval algorithm changes. In comparison with the few suitable BSRN SIS observation series with limited extension in time (no data before 1992), the CM SAF SIS time series do not show significant inhomogeneities, even though slight discrepancies in the surface measurements appear. The investigation of the full CM SAF SIS domain reveal inhomogeneities related to most of the documented satellite and retrieval changes, but only for relatively small domain fractions (especially in mountainous desert-like areas in Africa). In these regions the retrieval algorithm is not capable of adjusting for the changes of the satellite instruments. For other areas, e.g., Europe, no such breaks in the time series are found. We conclude that the CM SAF SIS data record has to be further assessed and regionally homogenized before climate trend investigations can be conducted.
Barriereinseln und Außensände, geformt durch eine Kombination aus Wind, Wellen, Strömung und Küstenlängstransport gelten als morphologisch hoch aktive Küstenbereiche und variieren häufig in Ursprung, Genese und Entwicklung. Sie besitzen durch ihre dissipative Wirkungsweise eine bedeutende Schutzfunktion für rückwärtige Inseln, Halligen und Festlandbereiche und bilden vor der Küste Nordfrieslands die westliche Außengrenze des Wattenmeeres.
Ziel der nachfolgenden Studie ist es, anhand hochauflösender Georadarmessungen und sedimentologischer Daten aus Bohrungen die Landschaftsgeschichte an der Westküste Amrums sowie die Entstehung und interne sedimentäre Architektur des der Insel westlich angelagerten Kniepsandes zu untersuchen und die Prozesse, die zur Genese geführt haben, durch Datierungen zeitlich einzuordnen. Auf Grundlage der gewonnenen Daten wurden zwei stratigraphische Modelle entwickelt, welche die geologisch-geomorphologischen Prozesse und Sedimentationsbedingungen im Westküstenvorfeld erklären.
Ein Modell zeigt die Landschaftsentwicklung an der Westküste Amrums und beschreibt die Sedimentationsbedingungen, die im Vorfeld der Westküste herrschten, bevor der Kniepsand an die Insel heranwanderte. Auf der Landoberfläche des ertrinkenden saaleeiszeitlichen Geestkerns wurden zu Beginn der Flandrischen Transgression feinkörnige Sedimente eines Mischund Schlickwatts abgelagert. Es ist davon auszugehen, dass der damals noch weit vor der Küste Amrums liegende Kniepsand eine Barriere bildete und so an der heute hochenergetischen Westküste für strömungsberuhigte Sedimentationsbedingungen sorgte. Durch Erosion am Geestkern bildeten sich in unterschiedlichen Höhenpositionen fossile Kliffs, die dem damaligen Meeresspiegelstand entsprechen.
Ein weiteres Modell beschreibt den Andockmechanismus des Kniepsandes an die Insel Amrum. Durch die Anlagerung des ehemaligen Außensandes und den damit einhergehenden Sedimentinput wurden die Bedingungen für eine großflächige Dünenbildung geschaffen.
Accretion rates of Holocene tropical coral reefs in three areas in the Atlantic, Pacific and Indian Oceans have been quantified in 79 dated core sections in 34 reef cores from Belize, the Maldives and French Polynesia. Holocene vertical reef accretion rate averages 5.05 m/kyr and has decreased during the past 10 kyr. Accretion rates in branched and massive coral facies are statistically similar. Reef accretion rate is positively correlated with the rate of sea‐level rise, that is the degree of creation of accommodation space, and with climate as expressed in a Holocene sea surface temperature anomaly. Accommodation space is also created by subsidence, but at a rate one to two orders of magnitude lower than that created by glacio‐eustasy (0.04 to 0.16 m/kyr). Lagoonal background sedimentation in adjacent reef lagoons averages 0.89 m/kyr as measured in 72 dated core sections in 28 cores. Lagoonal carbonate sedimentation on top of underlying mangrove peat usually starts after a considerable hiatus of ca 3 kyr on average. The lagoonal background sedimentation rate increased during the Holocene, probably due to deepening. The differences between vertical reef accretion and lagoonal background sedimentation rates are a major factor in the production of the widely known saucer shapes typical of tropical reefs and carbonate platforms, that is the creation of unfilled accommodation space. Reef core recovery, used as a proxy for reef consolidation, and core depth exhibit a statistically negative correlation based on data from 326 core barrels. Recovery and marine cement abundance (average volume 8.6%) also decrease from windward to leeward core positions. These observations are presumably a result of both a decrease in the rate of sea‐level rise that is the increase in time available for submarine cementation during the Holocene and the amount of flushing of reef interstices by marine waters.
This study describes the Holocene sedimentary lagoonal deposition history, including event sedimentation and benthic foraminiferal analyzes, from about 10 kyrs BP until today. This is the first study describing the sedimentation of a Maldivian atoll lagoon in such detail. Thirty-nine sediment cores have been recovered from the deep Rasdhoo Atoll lagoon of the Maldives (4°N/73°W). Seventeen sediment cores were opened, described, and 296 sediment samples have been collected and analyzed. Different methods have been used to evaluate the coarse- and fine-grained carbonate components and a total of fifty-eight samples have been dated radiometrically by Beta Analytic Inc., Miami, Florida. In general, the Rasdhoo Atoll lagoon sediments can be divided into (1) a Late Pleistocene soil, (2) an early Holocene peat layer composed of mangrove deposits which mark the beginning inundation of the atoll lagoon by the rising Holocene sea-level at 10,320 ± 100 yrs BP, and (3) carbonate sediments starting to fill up the lagoon 7850 ± 140 yrs BP until today. The transition from peat to carbonate is characterized by a considerable hiatus. Six different carbonate sediment facies are classified by statistical analyses, listed in decreasing abundance:
(1) mollusk-coral-algal floatstone to rudstone (30%)
(2) mollusk-coral-red algae rudstone (23%)
(3) mollusk-coral-algal wackestone to floatstone (23%)
(4) mollusk-coral wackestone (13%)
(5) mollusk-coral mudstone to wackestone (9%)
(6) mollusk mudstone (2%)
Based on grain-sizes in combination with coral identification, the facies represent both lagoonal background sedimentation (mostly fine-grained sediments (matrix >50%)) and event sedimentation (coarse-grained sediment layers composing reefal components).
Six coarser grained layers in muddy background sediments of the Rasdhoo Atoll lagoon were interpreted as Holocene tsunami events, based on the increase of allochthonous skeletal material with shallow-water reef affinity such as fragments of shallow-water coral species, coralline red algae, and reef-dwelling foraminifera in these layers, as well as AMS dating:
• Event 1: 420 - 890 yrs BP (655 yrs BP)
• Event 2: 890 - 1560 yrs BP (1225 yrs BP)
• Event 3: 2040 - 2340 yrs BP (2190 yrs BP)
• Event 4: 2420 - 3380 yrs BP (2900 yrs BP)
• Event 5: 3890 - 4330 yrs BP (4110 yrs BP)
• Event 6: 5480 - 5760 yrs BP (5620 yrs BP)
Five of the six layers may be correlated to previously published tsunami events at adjacent coastal research sites. The mid-late Holocene atoll lagoon archive is incomplete though based on the assumption that major earthquakes at the Indonesian subduction zone generated more than six major tsunamis during the past 6.5 kyrs.
According to Gischler (2006), the sediments of the Rasdhoo Atoll lagoon can be divided into two areas: (1) a central to marginal deep lagoon with a lateral west-to-east gradient of sediment facies distribution, visible in sections <4 kyrs BP with sedimentary facies of mudstone to wackestone in the western part (e.g., cores 16, 18, and 34) and coarse-grained coral and algal-rich sediments in the eastern part of the lagoon (e.g., cores 30 and 31). (2) A northern enclosed and shallow area between the sand apron and the sand spit accumulating “sandy” sediments of wackestone facies (cores 2, 19, 25, and 26).
Comparing the sediment accumulation data of the lagoon with two reconstructed local sea-level curves, three different sequence-stratigraphical systems tracts are visible: (1) a lowstand systems tract (LST) >10 kyrs BP. Pleistocene brownish soil superposing subaerially exposed Pleistocene reef limestone. (2) A transgressive systems tract (TST) 10-6.5 kyrs BP. A peat layer marks the beginning of the inundation, and the carbonate sedimentation starts with very low sedimentation rates of 0.02 m/kyr. (3) A highstand systems tract (HST) 6.5-0 kyrs BP, further divided into three stages (6.5-3, 3-1, 1-0 kyrs BP). The sea-level rise slowed down, sedimentation rates are increasing continuously up to a maximum of 1.4 m/kyr, the sand spit developed some 4 kyrs BP, the lagoonal circulation got restricted, and the lateral west-to-east gradient of grain-size accumulation started. From 1-0 kyrs BP the sedimentation rates slowed down to modern mean sedimentation rates of 0.6 m/kyr.
Two cores, one core from the center of the lagoon (core 16) and one core from the northern margin of the lagoon (core 19), have been analyzed on diversity and assemblages of benthic foraminifera in high-resolution. The transitions of Ammonia spp. to a more even and diverse fauna marks a significant environmental change at 7.0 kyrs BP in core 16 (onset of a stable environment in the deep lagoon after the sea-level rise slowed down at HST stage 1) and at 4.0 kyrs BP in core 19. A continuing environmental change after 1.4 kyrs BP in core 16 caused the fauna to become more even, a recovery of diversity and a permanent decline of foraminiferal accumulation rate. The changes in the faunas at 4.0 kyrs BP and at 1.4 kyrs BP could be explained with the sand spit formation in the northwestern and western lagoon. The sand spit has apparently acted as an obstacle in lagoonal circulation and might have caused unstable environmental conditions due to a more rapid circulation at the shallow marine site of core 19 and a slowdown of bottom water circulation in the main lagoon (core 16) leading to higher residence times and to lower oxygen and higher nutrient concentrations.
In Belize, which is well known for the Belize Barrier Reef and its offshore atolls, coastal lagoons are frequent morphological features along the coast. They represent transitional environments between siliciclastic and carbonate settings. In order to shed light into the Holocene evolution of coastal lagoon environments, five localities along the central coast of Belize were selected as coring sites. These include four coastal lagoons and one marsh area, namely Mantatee Lagoon, Mullins River Beach, Colson Point Lagoon, Commerce Bight Lagoon and Sapodilla Lagoon. A total of 26 sediment cores with core lengths ranging from 109 cm to 500 cm, were drilled using a Lanesky-vibracorer. Overall, 73 m of Holocene sediments and Pleistocene soil were recovered. Together with 58 radiocarbon dates the sediments reveal details on the sediment architecture and depositional features of the localities.
Marine inundation of the mainland and coastal lagoon formation started around 6 kyrs cal BP.
As a response to sea-level rise during the Holocene transgression, facies retrograded towards the coast, as seen in marginal marine overlying brackish mollusk faunas. Evidence for late Holocene progradation of facies due to sea-level stagnation is largely lacking. The occurrence of landward thinning sand beds, hiatuses and marine fauna in lagoonal successions are indications of event (overwash) sedimentation. Sediments recovered are largely of Holocene age (<7980 cal BP), overlying Pleistocene sections. Analyses of sediment composition and texture, radiocarbon dating and mollusk shell identification were used to describe and correlate sedimentary facies.
XRD analyses have identified quartz as the dominant mineral, with the Maya Mountains as main source of coastal lagoon sediments. The most common sedimentary facies include peat and peaty sediment, mud, sand, and poorly sorted sediments. Pleistocene soil forms the basement of Holocene sediments. Holocene mud represents lagoon background permanent sedimentation.
Peats and peat-rich sequences were deposited in mangrove swamp environments, whereas sandy facies mainly occur in the shoreface, beach, barriers, bars, barrier spits and overwash deposits. Facies successions could be identified for each locality, but it has proven difficult to correlate the stratigraphic sequences, especially among localities. These differences among the five locations studied suggest that apart from regional influence such as sea-level rise, local environmental factors such as small-scale variation in geomorphology and resulting facies heterogeneity, connectivity of the lagoon with the sea, antecedent topography and river discharge, were responsible for coastal sedimentation and lagoon development in the Holocene of Belize.
Faunal composition and distribution patterns of mollusk assemblages from 20 shell concentrations in cores collected in coastal lagoons, a mangrove-fringed tidal inlet and the marginal marine area (shallow subtidal) show considerable variation due to environmental heterogeneity and the interplay of several environmental factors in the course of the mid-late Holocene (ca. 6000 cal BP to modern). The investigated fauna ≥2 mm comprises 2246 bivalve, gastropod and 11 scaphopod specimens. Fifty-three mollusk species, belonging to 42 families, were identified. The bivalve Anomalocardia cuneimeris and cerithid gastropods are the dominant species and account for 78% of the total fauna. Diversity indices are low in concentrations from lagoons and relatively high in the marginal marine and tidal inlet areas.
Based on cluster analysis and nonmetric multidimensional scaling (NMDS), seven lagoonal assemblages and three marginal marine/tidal inlet assemblages were defined. A separation between lagoonal and marginal marine/tidal inlet assemblages seen in ordination indicates a lagoon-onshore gradient. The statistical separation among lagoonal assemblages demonstrates environmental changes during the Holocene evolution of the coastal lagoons, which is probably related to the formation of barriers and spits. The controlling factors of species distribution patterns are difficult to figure out, probably due to the heterogeneity of the barrier-lagoon systems and the interaction of paleoecological and paleoenvironmental factors. In addition to the taxonomic analysis, a taphonomic analysis of 1827 valves of A. cuneimeris from coastal lagoons was carried out. There is no relationship between depth and age of shells and their taphonomic condition. Size-frequency distributions and right-left valve ratios of A. cuneimeris suggest that valves were not transported over long distances but were deposited parautochthonously in their original habitat. Shells from tidal inlet and marginal marine environments were also predominantly deposited in their original habitats.
Since the Belize coast was repeatedly affected by hurricanes and the paleohurricane record for this region is poor, the sediment cores have been examined in order to identify storm deposits.
The paleohurricane record presented in this study spans the past 8000 years and exhibits three periods with increased evidences of hurricane strikes occurring at 6000-4900 cal yr BP, 4200-3600 cal yr BP and 2200-1500 cal yr BP. Two earlier events around 7100 and 7900 cal yr BP and more recent events around 180 cal yr BP and during modern times have been detected. Sand layers, redeposited corals and lagoon shell concentrations have been used as proxies for storm deposition. Additionally, hiatuses and reversed ages may indicate storm influence. While sand layers and corals represent overwash deposits, the lagoon shell concentrations, which mainly comprise the bivalve Anomalocardia cuneimeris and cerithid gastropods, have been deposited due to changes in lagoon salinity during and after storm landfalls. Comparison with other studies reveals similarities with one record from Belize, but hardly any matches with other published records. The potential for paleotempestology reconstructions of the barrier-lagoon complexes along the central Belize coast differs depending on geomorphology, and deposition of washovers in the lagoon basins is limited, probably due to the interplay of biological, geological and geomorphological processes.
Measurements of OH, the sum of peroxy radicals (ROx), non-methane hydrocarbons (NMHCs) and various other trace gases were made at the Meteorological Observatory Hohenpeissenberg in June 2000. The data from an intensive measurement period characterised by high solar insolation (18-21 June) are analysed. The maximum midday OH concentration ranged between 4.5 x 106 molecules cm-3 and 7.4 x 106 molecules cm-3. The maximum total ROx mixing ratio increased from about 55 pptv on 18 June to nearly 70 pptv on 20 and 21 June. A total of 64 NMHCs, including isoprene and monoterpenes, were measured every 1 to 6 hours. The oxidation rate of the NMHCs by OH was calculated and reached a total of over 14 x 106 molecules cm-3 s-1 on two days. A simple photostationary state balance model was used to simulate the ambient OH and ROx concentrations with the measured data as input. The model was able to reproduce the main features of the diurnal profiles of both OH and ROx. The model results proved to be most sensitive to assumptions about the mixing ratio of formaldehyde (HCHO), which was included as a proxy for carbonyl compounds, and about the partitioning between HO2 and RO2. The measured OH concentration and ROx mixing ratios were reproduced well by assuming the presence of 3 ppbv HCHO and a ratio HO2/RO2 between 1:1 and 1:2. The most important source of OH, and conversely the greatest sink for ROx, was the recycling of HO2 radicals to OH. This reaction was responsible for the recycling of more than 45 x 106 molecules cm-3 s-1 on two days. The most important sink for OH, and the largest source of ROx, was the oxidation of NMHCs, in particular, of isoprene and the monoterpenes.
Measurements of OH, total peroxy radicals, non-methane hydrocarbons (NMHCs) and various other trace gases were made at the Meteorological Observatory Hohenpeissenberg in June 2000. The data from an intensive measurement period characterised by high solar insolation (18-21 June) are analysed. The maximum midday OH concentration ranged between 4.5x106 molecules cm-3 and 7.4x106 molecules cm-3. The maximum total ROx (ROx =OH+RO+HO2+RO2) mixing ratio increased from about 55 pptv on 18 June to nearly 70 pptv on 20 and 21 June. A total of 64 NMHCs, including isoprene and monoterpenes, were measured every 1 to 6 hours. The oxidation rate of the NMHCs by OH was calculated and reached a total of over 14x106 molecules cm-3 s-1 on two days. A simple photostationary state balance model was used to simulate the ambient OH and peroxy radical concentrations with the measured data as input. This approach was able to reproduce the main features of the diurnal profiles of both OH and peroxy radicals. The balance equations were used to test the effect of the assumptions made in this model. The results proved to be most sensitive to assumptions about the impact of unmeasured volatile organic compounds (VOC), e.g. formaldehyde (HCHO), and about the partitioning between HO2 and RO2. The measured OH concentration and peroxy radical mixing ratios were reproduced well by assuming the presence of 3 ppbv HCHO as a proxy for oxygenated hydrocarbons, and a HO2/ RO2 ratio between 1:1 and 1:2. The most important source of OH, and conversely the greatest sink for peroxy radicals, was the recycling of HO2 radicals to OH. This reaction was responsible for the recycling of more than 45x106 molecules cm-3 s-1 on two days. The most important sink for OH, and the largest source of peroxy radicals, was the oxidation of NMHCs, in particular, of isoprene and the monoterpenes.
Ca-Silikate als natürliche Einschlüsse in Diamanten sind so extrem selten und bislang wenig untersucht, daß der Weg, sie synthetisch herzustellen, um entsprechende Analysen durchführen zu können, gerechtfertigt wird. Um die Veränderungen über einen großen Druckbereich bis zu Bedingungen, die dem Unteren Erdmantel entsprechen, durchführen zu können, wurde ein neues Hochdrucklabor mit einer Multi-Anvil-Presse aufgebaut. In dieses Labor sind viele Erfahrungen aus eigenen Experimenten und aus anderen Arbeitsgruppen eingeflossen, sodaß eine leistungsfähige Hochdruckanlage zur Verfügung steht. Kernstück dieses Hochdrucksystems ist der innere Hochdruckaufbau, wobei nicht ein bereits etablierter Hochdruckaufbau kopiert, sondern - durch das Integrieren der Vorzüge von unterschiedlichen Systemen - ein eigenständiger Hochdruckaufbau entwickelt wurde. Das System ist für weitere Ausbaumöglichkeiten vorbereitet, sodaß z. B. großvolumige Kapseln zusammen mit den Ceramcast-Oktaedern bis 80 kbar eingesetzt werden können, bzw. der maximale Druckbereich mit einem 10/4 mm Aufbau bis über 200 kbar ausgeweitet werden kann. Die Untersuchung der Reaktionskinetik an den Ca-Silikatphasen stellt eine besondere Herausforderung dar. Aus vorangegangenen Experimenten und Untersuchungen ist die "nicht Quenchbarkeit" von Ca-Perovskit und die Amorphisierung von Ca-Walstromit bekannt, sodaß sich die Untersuchungen mittels der herkömmlichen Hochdruckmethoden für diese Fragestellung als nachteilig erweisen. Dank der Zusammenarbeit mit dem "Material Science Laboratory" am Synchrotron in Daresbury bot sich die Möglichkeit, in situ Hochdruckexperimente an den Ca-Silikatphasen durchzuführen. Es stand nur eine begrenzte Entwicklungszeit zur Verfügung, um die neuartige "fine-to-fine" Geometrie zu entwickeln und zu erproben. Mit diesem Hochdruckaufbau ist es gelungen, in situ Hochdruckexperimente bei bis zu 150 kbar und 1400°C durchzuführen und dabei Ca-Perovskit zu kristallisieren. Mit den kleineren 10mm MgO-Oktaedern und 5 bzw. 4 mm Truncation an den Wolframcarbid-Würfeln sind sogar bei gleicher Geometrie noch höhere Drücke realisierbar. Die Beobachtungen an den durchgeführten Experimente ermöglicht eine Aussage zur Reaktionskinetik der Phasenumwandlung bei Ca-Silikaten. Die Disproportionsreaktion von Ca-Perovskit zu den zwei Phasen Larnit und Si-Titanit läuft sehr rasch ab, wo hingegen die Rekombinationsreaktion dieser beiden Phasen zu Ca-Walstromit kinetisch gehemmt und innerhalb von Stunden keine Umwandlung beobachtet werden konnte. Darüber hinaus bestätigen die eigenen Experimente ein Einsetzen der Amorphisierung von Ca-Perovskit bei Drücken unterhalb von 10 kbar. Eine Amorphisierung von Ca-Walstromit wurde auch nach vollständiger Druckentlastung nicht beobachtet. Werden die Beobachtungen der kinetischen Experimente der Phasenumwandlung an Ca-Silikaten auf die natürlichen Bedingungen bei der Diamantentstehung und deren Aufstiegspfad übertragen, spricht dies für ein Modell des raschen Aufstiegs aus dem Unteren Mantel bzw. der Übergangszone und einem Steckenbleiben im Oberen Mantel bei moderaten Drücken. Der Weg an die Erdoberfläche findet dann zu einem späteren Zeitpunkt ebenfalls mit schnellen Aufstiegsgeschwindigkeiten statt. Die Ergebnisse der Löslichkeits-Hochdruckexperimente von Kalium und Phosphor bestätigen die Beobachtungen, die an den natürlichen Ca-Silikateinschlüssen gemacht wurden. In dem Zweiphasenfeld, in dem Larnit zusammen mit Si-Titanit koexsistiert, hebt sich vor allem die sehr hohe Löslichkeit von Kalium und Phosphor hervor. Zwar wurde bereits in den natürlichen Einschlüssen ein auffallend hoher Gehalt dieser Elemente beobacht, die Experimente zur maximalen Löslichkeit zeigen jedoch, daß sich weitaus höhere Gehalte im Larnit lösen können. Für diese Phase trifft die gekoppelte Substitution von Kalium und Phosphor gegen Calcium und Silicium im Verhältnis 1 : 1 zu. Interessant ist zudem die offenbare Druckhabhängigkeit der Löslichkeit in Larnit. Für eine geobarometrische Anwendung dieses Druckeffekts ist das Stabilitätsfeld mit nur 20 kbar relativ schmal, so daß der Druckgradient gering ist. Die Titanit-Struktur erweist sich im Gegensatz dazu als nicht kompatibel für diese Elemente. In Si-Titanit werden nur extrem geringe Gehalte an Kalium und Phosphor eingebaut. In den natürlichen Einschlüssen wurden gleichermaßen geringe Gehalte nachgewiesen. Damit kann vom Erreichen der maximalen Löslichkeit in den natürlichen Proben ausgegangen werden. Als potentieller Träger von Kalium und Phosphor in der Übergangszone ist die Phase Larnit. Sie kann sehr hohe Gehalte dieser Elemente aufnehmen, mit steigendem Druck nimmt die Löslichkeit jedoch ab. Direkte Messungen der Löslichkeit an Ca-Perovskit liegen bislang nicht vor. Die Experimente an der unteren Stabilitätsgrenze zeigen sehr geringe Gehalte an Kalium und Phosphor. Eine Substitution in dieser sehr dichten Struktur findet nicht statt. Die geringe Löslichkeit in Ca-Perovskit entspricht nicht dem erwarteten Ergebnis. Diese Phase galt bislang als möglicher Träger von Kalium und Phosphor im Unteren Mantel. Wenn davon ausgegangen wird, daß Einschlüsse, in denen Larnit und Si-Titanit nachgewiesen werden, möglicherweise ehemals Ca-Perovskit gewesen sind und damit eine Herkunft aus dem Unteren Mantel haben, so sprechen die hohen Gehalte an Kalium und Phosphor in Larnit gegen diese Annahme. Ein Einschluß, der als Ca-Perovskit im Unteren Mantel kristallisiert ist, kann nicht die großen Mengen an Kalium und Phosphor einbauen, wie sie dann im Larnit als direkte Umwandlungsphase nachgewiesen werden. Möglicherweise sind Einschlüsse, die hohe Gehalte an Kalium und Phosphor zeigen, in dem Zweiphasenstabilitätsfeld Larnit/Si-Titanit kristallisiert, und ein Hinweis darauf, daß sie kein Disproportionsprodukt aus vormaligem Ca-Perovskit sind. Bislang ungeklärt bleibt die Frage, ob mit höherem Druck die Löslichkeit von Kalium und Phosphor in Ca-Perovskit zunimmt. Wenn eine Druckabhängigkeit der Löslichkeit vorliegt, würde dies dafür sprechen, daß die Diamanten mit Ca-Perovskit-Einschlüssen aus dem Unteren Mantel stammen und nicht aus der Übergangszone. Die Annahme der Herkunft dieser speziellen Diamantparagenese aus dem Unteren Mantel wird auch durch das Auftreten von Ferro-Periklas und Stichovit zusammen mit Ca-Perovskit im gleichen Diamantkristall bekräftigt. Zukünftige Experimente bei höheren Drücken könnten die Frage klären, ob bei einer Druckerhöhung eine Zunahme der Löslichkeit in Ca-Perovskit beobachtet wird. Eine beachtliche Zunahme der Löslichkeit mit dem Druck würde das Modell der Herkunft der Ca-Silikateinschlüsse aus dem Unteren Mantel stützen. Die Löslichkeit von Kalium und Phosphor in Ca-Walstromit zeigt sowohl in den natürlichen Einschlüssen als auch in den Experimenten mittlere Gehalte dieser Elemente an. Abweichend von den Beobachtungen in den Einschlüssen ist jedoch der erhöhte Kaliumgehalt, der nicht den erwarteten stöchiometrischen Austausch von 1 : 1 wiedergibt. Untersuchungen an natürlichen Ca-Walstromit als Einschlüsse in Diamanten werden zukünftig von besonderem Interesse sein, da diese Einschlüsse entsprechend häufiger auftreten und als Probenmaterial vorliegen. Weitere Experimente im Ca-Walstromit-Stabilitätsfeld mit unterschiedlichen Gehalten an Spurenelementen und entsprechenden Strukturuntersuchungen können die Frage der Stabilität bzw. der Amorphisierung klären. Ein unmittelbares Amorphisieren von Ca-Walstromit nach der Druckentlastung wird nicht beobachtet und auch die energiereiche Strahlung der Mikrosonde bzw. des Synchrotrons hat keine Amorphisierung zur Folge. Beim Bestrahlen mit der sehr energiereichen Strahlung bei den TEM-Untersuchungen zeigt sich jedoch, daß Ca-Walstromit nicht sehr stabil ist und innerhalb weniger Minuten amorphisiert. Die TEM-Untersuchungen weisen auf mögliche Polymorphe von Ca-Walstromit hin. Wenn sich unterschiedliche Polymorphe nachweisen lassen, ist von abweichenden Löslichkeiten und unter Umständen anderen Einbaumechanismen in den Phasen auszugehen.
Die Seismizität des nördlichen Oberrheingrabens (ORG) ist aufgrund seines Potentials für die geothermische Nutzung und der damit möglicherweise verbundenen seismischen Risiken von allgemeinem Interesse. Detaillierte Kenntnisse der natürlichen Seismizität erlauben Rückschlüsse auf aktive Störungszonen und Spannungsverhältnisse im Untergrund. Sie liefert außerdem wichtige Hintergrundinformationen für die Abschätzung einer möglichen induzierten Seismizität. Untersuchungen zur Charakterisierung der natürlichen Seismizität, des Spannungsfeldes und der seismischen Gefährdung des nördlichen ORG sind Hauptbestandteil dieser Arbeit, die innerhalb des BMU/BMWi-Projektes SiMoN (Seismisches Monitoring im Zusammenhang mit der geothermischen Nutzung des Nördlichen Oberrheingrabens) entstanden ist. Aufzeichnungen eines Netzwerkes aus 13 seismischen Stationen dienen als Datengrundlage zur Charakterisierung der Seismizität innerhalb eines etwa 50 x 60 km2 großen Areals im dichtbesiedelten Rhein-Main Gebiet. Untersuchungen der Rauschbedingungen zur Bewertung der Eignung der Stationsorte für das Aufzeichnen der natürlichen Seismizität lieferten bei den Stationen auf felsigem Untergrund sehr gute spektrale Eigenschaften, während alle Stationen im Sediment des ORG deutlich höhere Rauschanteile aufzeigten. Anhand systematischer Messungen in flachen Bohrlöchern konnten laterale und vertikale Variationen des seismischen Rauschens beschrieben werden und dadurch eine Verbesserung der Detektionsschwelle beobachtet werden.
Es werden die Ergebnisse des seismischen Monitorings für den Zeitraum November 2010 bis Dezember 2014 dargestellt. Die Detektionsschwelle für das Netzwerk liegt bei einer Lokalmagnitude von etwa 0,5, die Vollständigkeitsmagnitude beträgt Mc = 1,2. Seit Beginn der Datenaufzeichnung konnten 243 Erdbeben im unmittelbaren Bereich des Stations-netzwerkes mit Magnituden im Bereich zwischen ML = -0,5 und ML = 4,2 lokalisiert werden. Die Epizentren liegen hauptsächlich entlang der östlichen Grabenschulter und im Graben; entlang der westlichen Grabenschulter ist die seismische Aktivität deutlich geringer. Eine weitere aktive Region konnte entlang der südlichen Ausläufer des Taunus im Nordwesten des Untersuchungsgebietes identifiziert werden. Die Seismizität erstreckt sich bis in eine Tiefe von 24 km mit einem Maximum der hypozentralen Tiefenverteilung im Bereich von 12-18 km. Im Graben ist die Seismizität dabei auf die tiefere Kruste im Bereich von 9-24 km beschränkt. Das Fehlen von seismischer Aktivität in der oberen Kruste bis ca. 9 km Tiefe im Graben könnte auf eine aseismische Deformation in diesem Tiefenbereich hindeuten. Seit Mai 2014 konnte südöstlich von Darmstadt bei der Ortschaft Ober-Ramstadt zum ersten Mal seit fast 150 Jahren eine Schwarmbebenaktivität im Bereich des nördlichen ORG registriert werden. Die Hypozentren sind in zwei Cluster unterteilt, die räumlich voneinander getrennt sind und unterschiedliche Aktivitätsraten aufweisen. Die Herdtiefen liegen im Bereich von 1-8 km.
Zusätzlich zu den Daten des SiMoN Netzwerkes wurden Aufzeichnungen der regionalen Erdbebendienste in Herdflächenanalysen für insgesamt 58 Erdbeben einbezogen. Die Herdflächenlösungen weisen überwiegend Blattverschiebungen (Strike-slip-Mechanismen) auf. Auf- und Abschiebungen spielen nur eine untergeordnete Rolle. Die berechneten Herdmechanismen bestätigen, dass sich das Spannungsfeld des nördlichen ORG transtensional verhält, im Vergleich zu früheren Studien konnte jedoch eine deutlich ausgeprägte Blattverschiebungskomponente identifiziert werden. Zur Bestimmung der Hauptspannungsachsen wurde eine Inversion der Herdflächenlösungen durchgeführt und die Richtung der maximalen horizontalen Spannung, welche hauptsächlich in N135°E orientiert ist, bestimmt.
Aufbauend auf den neu gewonnen Erkenntnissen zur natürlichen Seismizität und zum Spannungsfeld des nördlichen ORG wurde eine probabilistische seismische Gefährdungsanalyse durchgeführt. Um Unsicherheiten in den seismischen Quellregion-modellen zu berücksichtigen, wurden sechs unterschiedliche Modelle entwickelt. Für jede Quellregion wurden spezifische Parameter bestimmt. Ihre Unsicherheiten werden in einem logischen Baum behandelt. Auf der Grundlage eines neu zusammengestellten Momentmagnituden-basierten Erdbebenkatalogs wurden die Magnitudenhäufigkeits-parameter bestimmt. Unter Berücksichtigung des tektonischen Regimes in jeder Quelle wurden unterschiedliche Dämpfungsrelationen der Bodenbeschleunigung verwendet. Zur Quantifizierung der maximal zu erwartenden Magnitude in jeder Quelle wurden Wahrscheinlichkeitsdichtefunktionen berechnet. Die Resultate der Gefährdungsanalyse werden in Form von Karten der Spektralbodenbeschleunigungen und Spitzenboden-beschleunigungen für Wiederkehrperioden von 475 und 2475 Jahren und Antwortbeschleunigungsspektren dargestellt. Im Vergleich zu früheren Studien konnte eine erhöhte seismische Gefährdung für den nördlichen ORG festgestellt werden.
Climate change research is increasingly focusing on the dynamics among species, ecosystems and climates. Better data about the historical behaviours of these dynamics are urgently needed. Such data are already available from ecology, archaeology, palaeontology and geology, but their integration into climate change research is hampered by differences in their temporal and geographical scales. One productive way to unite data across scales is the study of functional morphological traits, which can form a common denominator for studying interactions between species and climate across taxa, across ecosystems, across space and through time—an approach we call ‘ecometrics’. The sampling methods that have become established in palaeontology to standardize over different scales can be synthesized with tools from community ecology and climate change biology to improve our understanding of the dynamics among species, ecosystems, climates and earth systems over time. Developing these approaches into an integrative climate change biology will help enrich our understanding of the changes our modern world is undergoing.
During SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) we performed measurements of a wide range of trace gases with different lifetimes and sink/source characteristics in the northern hemispheric upper troposphere (UT) and lowermost stratosphere (LMS). A large number of in-situ instruments were deployed on board a Learjet 35A, flying at altitudes up to 13.7 km, at times reaching to nearly 380 K potential temperature. Eight measurement campaigns (consisting of a total of 36 flights), distributed over all seasons and typically covering latitudes between 35° N and 75° N in the European longitude sector (10° W–20° E), were performed. Here we present an overview of the project, describing the instrumentation, the encountered meteorological situations during the campaigns and the data set available from SPURT. Measurements were obtained for N2O, CH4, CO, CO2, CFC12, H2, SF6, NO, NOy, O3 and H2O. We illustrate the strength of this new data set by showing mean distributions of the mixing ratios of selected trace gases, using a potential temperature – equivalent latitude coordinate system. The observations reveal that the LMS is most stratospheric in character during spring, with the highest mixing ratios of O3 and NOy and the lowest mixing ratios of N2O and SF6. The lowest mixing ratios of NOy and O3 are observed during autumn, together with the highest mixing ratios of N2O and SF6 indicating a strong tropospheric influence. For H2O, however, the maximum concentrations in the LMS are found during summer, suggesting unique (temperature- and convection-controlled) conditions for this molecule during transport across the tropopause. The SPURT data set is presently the most accurate and complete data set for many trace species in the LMS, and its main value is the simultaneous measurement of a suite of trace gases having different lifetimes and physical-chemical histories. It is thus very well suited for studies of atmospheric transport, for model validation, and for investigations of seasonal changes in the UT/LMS, as demonstrated in accompanying and elsewhere published studies.
During SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) we performed measurements of a wide range of trace gases with different lifetimes and sink/source characteristics in the northern hemispheric upper troposphere (UT) and lowermost stratosphere (LMS). A large number of in-situ instruments were deployed on board a Learjet 35A, flying at altitudes up to 13.7 km, at times reaching to nearly 380 K potential temperature. Eight measurement campaigns (consisting of a total of 36 flights), distributed over all seasons and typically covering latitudes between 35° N and 75° N in the European longitude sector (10° W–20° E), were performed. Here we present an overview of the project, describing the instrumentation, the encountered meteorological situations during the campaigns and the data set available from SPURT. Measurements were obtained for N2O, CH4, CO, CO2, CFC12, H2, SF6, NO, NOy, O3 and H2O. We illustrate the strength of this new data set by showing mean distributions of the mixing ratios of selected trace gases, using a potential temperature – equivalent latitude coordinate system. The observations reveal that the LMS is most stratospheric in character during spring, with the highest mixing ratios of O3 and NOy and the lowest mixing ratios of N2O and SF6. The lowest mixing ratios of NOy and O3 are observed during autumn, together with the highest mixing ratios of N2O and SF6 indicating a strong tropospheric influence. For H2O, however, the maximum concentrations in the LMS are found during summer, suggesting unique (temperature- and convection-controlled) conditions for this molecule during transport across the tropopause. The SPURT data set is presently the most accurate and complete data set for many trace species in the LMS, and its main value is the simultaneous measurement of a suite of trace gases having different lifetimes and physical-chemical histories. It is thus very well suited for studies of atmospheric transport, for model validation, and for investigations of seasonal changes in the UT/LMS, as demonstrated in accompanying and elsewhere published studies.
High-pressure/high-temperature synthesis of the new boron-rich terbium hydroxyborate Tb3B12O19(OH)7
(2023)
Monoclinic Tb3B12O19(OH)7 was obtained by multianvil high-pressure/high-temperature syntheses at 6 GPa and 650 °C. The crystal structure was investigated by single-crystal X-ray diffraction methods and space group C2 (no. 5) with the unit cell parameters a = 24.2299(5) Å, b = 4.4667(1) Å, c = 7.0964(2) Å, β = 94.58(1)°, and two formula units per cell were revealed. Powder X-ray diffraction, infrared spectroscopy and the investigation of its second harmonic generation properties support the proposed structural model.
Herein, the high-pressure/high-temperature synthesis (11 GPa, 650 °C) of Tb3B10O17(OH)5 in a modified Walker-type multianvil device is presented. The structure of this rare-earth borate was determined by single-crystal X-ray diffraction methods and was found to crystallize orthorhombically in the space group Pmn21 (no. 31) with the unit cell parameters a = 16.2527(4), b = 4.4373(1), and c = 8.8174(2) Å. The new compound was further characterized using infrared spectroscopy, energy-dispersive X-ray spectroscopy, second harmonic generation (SHG) measurements, and temperature-dependent X-ray powder diffraction. Tb3B10O17(OH)5 decomposes to β-Tb(BO2)3 at temperatures higher than 460 °C. With increasing temperatures, the formation of μ-TbBO3 was observed, which transforms to π-TbBO3 upon cooling.
The current study tested the assumption that floristic and functional diversity patterns are negatively related to soil nitrogen content. We analyzed 20 plots with soil N-contents ranging from 0.63% to 1.06% in a deciduous forest near Munich (Germany). To describe species adaptation strategies to different nitrogen availabilities, we used a plant functional type (PFT) approach. Each identified PFT represents one realized adaptation strategy to the current environment. These were correlated, next to plant species richness and evenness, to soil nitrogen contents. We found that N-efficient species were typical for low soil nitrogen contents, while N-requiring species occur at high N-contents. In contrast to our initial hypotheses, floristic and functional diversity measures (number of PFTs) were positively related to nitrogen content in the soil. Every functional group has its own adaptation to the prevailing environmental conditions; in consequence, these functional groups can co-exist but do not out-compete one another. The increased number of functional groups at high N-contents leads to increased species richness. Hence, for explaining diversity patterns we need to consider species groups representing different adaptations to the current environmental conditions. Such co-existing ecological strategies may even overcome the importance of competition in their effect on biodiversity.
High field strength element systematics and Lu-Hf & Sm-Nd garnet geochronology of orogenic eclogites
(2008)
Concerning the Bulk Silicate Earth (BSE), the depleted mantle and the continental crust are thought to balance the budget of refractory and lithophile elements, resulting in complementary trace element patterns. However, the two high field strength elements (HFSE) Niob and Tantal appear to contradict this mass balance. All reservoirs of the silicate Earth exhibit subchondritic Nb/Ta ratios, possibly as a result of Nb depletion. The two HFSE Zr and Hf on the other hand seem not to be fractionated between the silicate reservoirs. They show more or less chondritic Zr/Hf ratios. In this study a series of orogenic eclogites from different localities was analyzed to determine their HFSE concentrations and to contribute to the question if eclogites could form a hidden reservoir to account for the mass imbalance of the BSE. The results show that the orogenic eclogites have subchondritic Nb/Ta ratios and near chondritic Zr/Hf ratios. The investigated eclogites show no fractionation of Nb/Ta ratios and no enrichment of Nb compared to e.g. MOR-basalts, the likely precursor of these rocks. With an average Nb/Ta ratio of 14.9 these eclogites could not balance the differences between BSE and chondrite. Additionally, with an average Nb/Ta ≈ MORB they also cannot balance the small differences in the Nb/Ta of the crust and the mantle. LA-ICPMS analyses of rutiles in these eclogites reveal a zonation of Nb/Ta ratios in this mineral, with rutile cores having higher Nb/Ta than rutile rims. As a consequence, Laser Ablation data of rutiles have to be evaluated carefully and cannot necessarily reflect a bulk rock Nb and Ta composition, although over 90% of these elements reside in rutile.
Understanding how temperature affects cod (Gadus morhua) ecology is important for forecasting how populations will develop as climate changes in future. The effects of spawning-season temperature and habitat size on cod recruitment dynamics have been investigated across the North Atlantic. Ricker and Beverton and Holt stock–recruitment (SR) models were extended by applying hierarchical methods, mixed-effects models, and Bayesian inference to incorporate the influence of these ecosystem factors on model parameters representing cod maximum reproductive rate and carrying capacity. We identified the pattern of temperature effects on cod productivity at the species level and estimated SR model parameters with increased precision. Temperature impacts vary geographically, being positive in areas where temperatures are <5°C, and negative for higher temperatures. Using the relationship derived, it is possible to predict expected changes in population-specific reproductive rates and carrying capacities resulting from temperature increases. Further, carrying capacity covaries with available habitat size, explaining at least half its variability across stocks. These patterns improve our understanding of environmental impacts on key population parameters, which is required for an ecosystem approach to cod management, particularly under ocean-warming scenarios. Key words: carrying capacity , cod , hierarchical models , North Atlantic , temperature , uncertainty
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.
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.
There are strong indications that particles containing secondary organic aerosol (SOA) exhibit amorphous solid or semi-solid phase states in the atmosphere. This may facilitate deposition ice nucleation and thus influence cirrus cloud properties. However, experimental ice nucleation studies of biogenic SOA are scarce. Here, we investigated the ice nucleation ability of viscous SOA particles.
The SOA particles were produced from the ozone initiated oxidation of α-pinene in an aerosol chamber at temperatures in the range from −38 to −10 ◦C at 5–15 % relative humidity with respect to water to ensure their formation in a highly viscous phase state, i.e. semi-solid or glassy. The ice nucleation ability of SOA particles with different sizes was investigated with a new continuous flow diffusion chamber. For the first time, we observed heterogeneous ice nucleation of viscous α-pinene SOA in the deposition mode for ice saturation ratios between 1.3 and 1.4 significantly below the homogeneous freezing limit. The maximum frozen fractions found at temperatures between −36.5 and −38.3 °C ranged from 6 to 20 % and did not depend on the particle surface area. Global modelling of monoterpene SOA particles suggests that viscous biogenic SOA particles are indeed present in regions where cirrus cloud formation takes place. Hence, they could make up an important contribution to the global ice nuclei (IN) budget.
There are strong indications that particles containing secondary organic aerosol (SOA) exhibit amorphous solid or semi-solid phase states in the atmosphere. This may facilitate heterogeneous ice nucleation and thus influence cloud properties. However, experimental ice nucleation studies of biogenic SOA are scarce. Here, we investigated the ice nucleation ability of viscous SOA particles.
The SOA particles were produced from the ozone initiated oxidation of α-pinene in an aerosol chamber at temperatures in the range from −38 to −10 °C at 5–15 % relative humidity with respect to water to ensure their formation in a highly viscous phase state, i.e. semi-solid or glassy. The ice nucleation ability of SOA particles with different sizes was investigated with a new continuous flow diffusion chamber. For the first time, we observed heterogeneous ice nucleation of viscous α-pinene SOA for ice saturation ratios between 1.3 and 1.4 significantly below the homogeneous freezing limit. The maximum frozen fractions found at temperatures between −39.0 and −37.2 °C ranged from 6 to 20 % and did not depend on the particle surface area. Global modelling of monoterpene SOA particles suggests that viscous biogenic SOA particles are indeed present in regions where cirrus cloud formation takes place. Hence, they could make up an important contribution to the global ice nucleating particle budget.
We report measurements of the deuterium content of molecular hydrogen (H2) obtained from a suite of air samples that were collected during a stratospheric balloon flight between 12 and 33 km at 40º N in October 2002. Strong deuterium enrichments of up to 400 permil versus Vienna Standard Mean Ocean Water (VSMOW) are observed, while the H2 mixing ratio remains virtually constant. Thus, as hydrogen is processed through the H2 reservoir in the stratosphere, deuterium is accumulated in H2 . Using box model calculations we investigated the effects of H2 sources and sinks on the stratospheric enrichments. Results show that considerable isotope enrichments in the production of H2 from CH4 must take place, i.e., deuterium is transferred preferentially to H2 during the CH4 oxidation sequence. This supports recent conclusions from tropospheric H2 isotope measurements which show that H2 produced photochemically from CH4 and non-methane hydrocarbons must be enriched in deuterium to balance the tropospheric hydrogen isotope budget. In the absence of further data on isotope fractionations in the individual reaction steps of the CH4 oxidation sequence, this effect cannot be investigated further at present. Our measurements imply that molecular hydrogen has to be taken into account when the hydrogen isotope budget in the stratosphere is investigated.
We present a new experimental dataset on the impact of the heavy halogens chlorine, bromine and iodine on the Raman water bands concerning pressure and their concentration at room temperature. These experiments were conducted at ambient temperature, with variations in halogen concentration and pressure ranging from 0 to 1.4 GPa.
The strength of the Raman water band shift change increases with the ionic size from chlorine, over bromine, to iodine. Our experiments further demonstrate that increased pressure diminishes the impact of the halogen shift change to a varying extent for each of the three halogens. This finding can have significant implications for the salinity calculation of fluid inclusions in minerals such as quartz or olivine. Particularly in the low salinity range, the concentration can be markedly underestimated if the pressure effect is neglected. For experiments in diamond anvil cells involving halogens dissolved in water, the change in Raman water band shifts can serve either as a new tool to monitor pressure, or to monitor the salinity.
The 99th Annual Meeting of the Geologische Vereinigung (GV) and International Conference on Earth Control on Planetary Life and Environment, held in October 2009 at the Geosciences Centre of the Georg-August-Universität Göttingen, brings together researchers from all fields of Earth Sciences and beyond to shape an attractive interdisciplinary program on the geological history of Planet Earth and its control over and interaction with biological evolution, development of habitats, environmental and climate change as well as history and culture of Homo sapiens. This volume contains the abstracts of invited keynote lectures as well as all oral and poster presentations.
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.
Chloritoid and kyanite coexist in metapelites from the high-pressure/low-temperature Massa Unit in the Alpi Apuane metamorphic complex (Northern Apennines, Italy). The composition of chloritoid is extremely variable throughout the Massa Unit. Fe-chloritoid occurs in association with hematite-free, graphite-bearing schists, whereas strongly zoned Fe-Mg chloritoid is found with hematite and kyanite. We investigated the effect of different bulk Fe2O3 contents in controlling chloritoid composition through phase equilibria modelling of four selected samples, representative of the different chloritoid-bearing parageneses found in the Massa Unit. The ferric iron content, measured through wet chemical titration, ranges from 0 (graphite-chloritoid schist) to 73% of the total iron (hematite-chloritoid schist). We show that Mg-rich chloritoid compositions and stability of kyanite at greenschist to blueschist facies conditions can be reproduced in the MnO–Na2O–K2O–FeO–MgO–Al2O3–SiO2–H2O–TiO2–O (MnNKFMASHTO) chemical system only considering the presence of significant amounts of ferric iron as part of the bulk composition. The stabilization of kyanite at lower grade is directly linked to the presence of Fe2O3, which renders the reactive bulk rock composition effectively enriched in Al2O3 with respect to Fe and Mg. We also document that high Fe2O3 contents exacerbate the effect of chloritoid fractionation, producing strongly zoned Fe-Mg-chloritoid grains. Finally, the P–T modelling of the Massa Units performed in this study allows, for the first time, the recognition of a two-stage evolution at peak conditions, with an earlier pressure peak (1.2–1.3 GPa at 350–400°C), and a later thermal peak (0.7–1.1 GPa at 440–480°C), compatible with subduction, underthrusting and exhumation of the Adria continental margin during growth of the Northern Apennine orogenic wedge.
An evaluation scheme is presented in this paper which can be used to assess groundwater vulnerability according to the requirements of the European Water Framework Directive (WFD). The evaluation scheme results in a groundwater vulnerability map identifying areas of high, medium and low vulnerability, as necessary for the measurement planning of the WFD. The evaluation scheme is based on the definition of the vulnerability of the Intergovernmental Panel on Climate Change (IPCC). It considers exposure, sensitivity and the adaptive capacity of the region. The adaptive capacity is evaluated in an actors' platform, which was constituted for the region in the PartizipA ("Participative modelling, Actor and Ecosystem Analysis in Regions with Intensive Agriculture") project. As a result of the vulnerability assessment, 21% of the catchment area was classified as being highly vulnerable, whereas 73% has medium vulnerability and 6% has low vulnerability. Thus, a groundwater vulnerability assessment approach is presented, which can be used in practice on a catchment scale for the WFD measurement planning.
Irrigation is the most important water use sector accounting for about 70% of the global freshwater withdrawals and 90% of consumptive water uses. While the extent of irrigation and related water uses are reported in statistical databases or estimated by model simulations, information on the source of irrigation water is scarce and very scattered. Here we present a new global inventory on the extent of areas irrigated with groundwater, surface water or non-conventional sources, and we determine the related consumptive water uses. The inventory provides data for 15 038 national and sub-national administrative units. Irrigated area was provided by census-based statistics from international and national organizations. A global model was then applied to simulate consumptive water uses for irrigation by water source. Globally, area equipped for irrigation is currently about 301 million ha of which 38% are equipped for irrigation with groundwater. Total consumptive groundwater use for irrigation is estimated as 545 km3 yr−1, or 43% of the total consumptive irrigation water use of 1 277 km3 yr−1. The countries with the largest extent of areas equipped for irrigation with groundwater, in absolute terms, are India (39 million ha), China (19 million ha) and the United States of America (17 million ha). Groundwater use in irrigation is increasing both in absolute terms and in percentage of total irrigation, leading in places to concentrations of users exploiting groundwater storage at rates above groundwater recharge. Despite the uncertainties associated with statistical data available to track patterns and growth of groundwater use for irrigation, the inventory presented here is a major step towards a more informed assessment of agricultural water use and its consequences for the global water cycle.
Irrigation is the most important water use sector accounting for about 70% of the global freshwater withdrawals and 90% of consumptive water uses. While the extent of irrigation and related water uses are reported in statistical databases or estimated by model simulations, information on the source of irrigation water is scarce and very scattered. Here we present a new global inventory on the extent of areas irrigated with groundwater, surface water or non-conventional sources, and we determine the related consumptive water uses. The inventory provides data for 15 038 national and sub-national administrative units. Irrigated area was provided by census-based statistics from international and national organizations. A global model was then applied to simulate consumptive water uses for irrigation by water source. Globally, area equipped for irrigation is currently about 301 million ha of which 38% are equipped for irrigation with groundwater. Total consumptive groundwater use for irrigation is estimated as 545 km3 yr−1, or 43% of the total consumptive irrigation water use of 1277 km3 yr−1. The countries with the largest extent of areas equipped for irrigation with groundwater, in absolute terms, are India (39 million ha), China (19 million ha) and the USA (17 million ha). Groundwater use in irrigation is increasing both in absolute terms and in percentage of total irrigation, leading in places to concentrations of users exploiting groundwater storage at rates above groundwater recharge. Despite the uncertainties associated with statistical data available to track patterns and growth of groundwater use for irrigation, the inventory presented here is a major step towards a more informed assessment of agricultural water use and its consequences for the global water cycle.
Gridded maps of meteorological variables are needed for the evaluation of weather and climate models and for climate change monitoring. In order to produce them, values at locations where no observing stations are available need to be estimated from point-wise observations. For the interpolation of meteorological observations deterministic and stochastic methods are often combined. Deterministic methods can account for ancillary information such as elevation, continentality or satellite observations. Stochastic methods such as kriging reproduce observed values at the station locations and also account for spatial variability. In the first two studies of this thesis, a flexible interpolation method for the gridding of locally observed daily extreme temperatures is developed that also provides an optimal estimate of the interpolation ncertainty. In the third study, an observational dataset is created using this interpolation method and then applied to evaluate a climate simulation for Africa.
In the first study, the Regression-Kriging-Kriging (RKK) method is tested for the interpolation of daily minimum and maximum temperatures (Tmin and Tmax) in different regions in Europe. RKK accounts for elevation, continentality index and zonal mean temperature and is applicable in regions of differing station density and climate. The accuracy of RKK is compared to Inverse Distance Weighting, a common deterministic interpolation method, and to Ordinary Kriging, a common stochastic interpolation method. The first step in RKK is to use regression kriging, in which multiple linear regression accounts for topographical effects on the temperature field and kriging minimizes the regression error, to interpolate climatological means. In the second step daily deviations from the monthly climatology are interpolated using simple kriging. Owing to the large climatological differences across the investigation area the interpolation is performed in homogeneous subregions defined according to the Köppen-Geiger climate classification. Cross validation demonstrates the superiority of RKK over the simpler algorithms in terms of accuracy and preservation of spatial variability. The interpolation performance however strongly varies across Europe, being considerably higher over Central Europe (highest station density) than over Greenland (few stations along the coast line). This illustrates the strong impact of the station density on the accuracy of the interpolation result. Satellites provide comprehensive observations of climate variables such as land surface temperature (LST) and cloud cover (CC). However, LST is associated with high uncertainty (standard error ~ 1-2°C), preventing its direct application in meteorology and climatology. The second study investigates the usefulness of LST and CC as predictors for the gridding of daily Tmin and Tmax. The RKK algorithm is compared with similar interpolation methods that apply LST and CC in addition to the predictors used with the RKK algorithm. The investigation is conducted in two regions, Central Europe and the Iberian Peninsula, which differ strongly in average cloud cover (Central Europe is approximately 30% cloud free and the Iberian Peninsula approximately 60 % cloud free). RKKLST (in which monthly mean LST is used as an additional predictor) yields for Central Europe no clear improvement over RKK, yet it reduces the interpolation error over the Iberian Peninsula. This finding can be explained by the higher percentage of cloud free pixels over that region in summer which enables a more robust determination of monthly mean LST. Adding a regression step for daily anomalies (using the predictor CC) yields the RKRK method and improves the preservation of spatial variability over the Iberian Peninsula. Moreover, a successive reduction of the station number (from 140 to 10 stations) reveals an increasing superiority of RKKLST and RKRK over RKK in both regions.
The application of a gridded observational dataset for climate monitoring or climate model validation requires knowledge of the uncertainties associated with the dataset. The estimation of the interpolation uncertainty, here the inter quartile range is the used uncertainty measure, is therefore an important issue within the frame of this thesis. By means of cross validation it is shown that the largest uncertainties occur in regions of low station density (e.g. Greenland), in mountainous regions and along coastlines (in these regions model evaluation results should be interpreted carefully). The magnitude of the interpolation error mainly depends on the station density, while the complexity of terrain has substantially less influence. On average over all regions and investigation days the target precision of the uncertainty estimate is reached. However, on local scales and for single days it can be clearly over- or underestimated. The application of satellite-derived predictors (LST and CC) yields no noteworthy improvement of the uncertainty estimate.
In the last study two regional climate simulations for Africa using the ERA-Interim driven COSMO-CLM (CCLM) model at two different horizontal resolutions (0.22° and 0.44°) are validated. It is assessed whether observed patterns and statistical properties of daily Tmin and Tmax are correctly represented in the model. The ERA-Interim reanalysis and a specially created observational dataset are used as reference. The observational dataset is generated by applying the RKRK algorithm (developed within the second study). The investigations show an occasionally large bias in Tmin and Tmax. The hemispheric summers are generally too warm and the temporal variability in temperature is too high, particularly over extra tropical Africa. The diurnal temperature range is overestimated by about 2°C in the northern subtropics but underestimated by about 2°C over large parts of the African tropics. CCLM reproduces the observed frequency distribution of daily Tmin and Tmax in all African climate regions, and the extreme values in the lower percentiles (5, 10, 20%) for Tmin are well simulated. The higher percentiles (80, 90, 95%) for Tmax are however overestimated by 2-5°C. For both Tmin and Tmax the 0.22° simulation is on average 0.5°C warmer than the 0.44° simulation. Additionally, the higher percentiles are about 1°C warmer for both Tmin and Tmax in the higher resolution run, while the lower percentiles in both runs match very well. Although the temperature pattern is represented in more detail along the coastlines and in topographically complex regions, the higher resolution simulation yields no qualitative improvement.
To summarize, the choice of the appropriate algorithm mainly depends on the interpolation conditions. In cases where the station density is high across the target region and the predictor space is adequately covered by observing stations, the computationally less demanding RK algorithm should be preferred. In regions where the station density is low the more robust RKRK algorithm should be the first choice. Due to the strong physical relation of both CC and LST to Tmin and Tmax the missing information is at least partially compensated for. The estimation of the interpolation uncertainty could be improved by applying a normal score transformation to the data prior to a kriging step. This is because the kriging assumption that the increments of the variable of interest are second order stationary can be approximately met by a normal score transformation.
This work analyses several granitic bodies of the Variscan Orogen of Central and Western Europe in order to improve our knowledge about different aspects of their evolution, regarding their ascent and emplacement mechanisms, as well as their deformation history. In the Iberian Massif two granitoid bodies, namely the La Bazana pluton and the Nisa-Alburquerque batholith, were studied in order to decipher their ascent and emplacement history. The La Bazana pluton is a small, sub-circular body in map view that intruded into rocks of the Ossa-Morena Zone in the core of a late upright antiform. Its three-dimensional drop-pipe shape, its internal dome foliation pattern and the structure of the host rock suggest that the magma ascended and emplaced diapirically. The Nisa-Alburquerque batholith is a large body that intruded into rocks of the Central Iberian Zone, the Central Unit, and the Ossa-Morena Zone. Its cartographic shape is elongate and parallel to the NW—SE to WNW—ESE Variscan structures. In the light of the available structural data and the gravimetric models, the intrusion is viewed as a continuous lateral magma flow from the eastern root guided towards the west through the southern limb of a kilometre-scale antiform. As mass-transfer mechanisms, a combination of rigid translation of the country rocks, stoping, and possibly ballooning is proposed. In the Bohemian Massif several small granitoid bodies showing a strong solid-state deformation were studied in order to integrate their tectonometamorphic history in the geotectonic framework of the south-western Bohemian Massif, focusing principally on the deformation phase referred to as D3. Four ductile deformation phases are proposed for the study area. D1 produced high-temperature fabrics under upper amphibolite to granulite facies conditions. Its kinematics is unknown. D2 occurred under amphibolite to upper greenschist facies conditions under N—S to NNW—SSE compression. It is responsible for a subvertical NW—SE striking foliation in migmatites developed under dextral simple shear and for the deformation at the Bayerischer Pfahl shear-zone system at its earlier stages. Many granitoid dykes and stocks were found to be affected by sinistral shear along subvertical planes trending ENE to ESE. Since this deformation, which is called D3 in the present work, is not compatible with a N—S to NNW—SSE compression, it is proposed that these sinistral shear zones in granites do not belong to the Bayerischer Pfahl shear-zone system and constitute themselves a separated one, which is called “D3 shear-zone system”. D3 took place under upper greenschist to lower amphibolite facies conditions (~480-550°C). Both the intrusion and the deformation of the granites affected by D3 occurred at deep to intermediate levels of the crust, whereas the deformation took place under NE—SW compression. Datings on two of the deformed granites yielded 324.4 ± 0.8 Ma and 315.0 ± 1.0 Ma: Thus, the age of D3 is most probably ~315 Ma. The intrusion of most of the sheared granitoids was pre-kinematic with respect to D3. After D3 the N—S to NNW—SSE compression which governed D2 was restored, giving way to the next deformation phase D4, which was linked to further deformation at and next to the principal shears of the Bayerischer Pfahl shear-zone system under greenschist facies conditions. The causes for the change of the stress field leading to a NE—SW compression during D3 might be related to (1) global changes in the dynamics of the tectonic plates in late Variscan times, (2) orogenic collapse leading to the sinking of the Teplá-Barrandian and lateral extrusion of the surrounding Moldanubian rocks, (3) distortion of the regional stress field by local intrusion of large stocks, such as the Saldenburg granite of the Fürstenstein Massif, or (4) distortion of the regional stress field due to the existence of ephemeral releasing bends in the Bayerischer Pfahl shear zone during its early evolution.
Invasive plant species are increasingly altering species composition and the functioning of ecosystems from a local to a global scale. The grass species Pennisetum setaceum has recently raised concerns as an invader on different archipelagos worldwide. Among these affected archipelagos are the Canary Islands, which are a hotspot of endemism. Consequently, conservation managers and stakeholders are interested in the potential spreading of this species in the archipelago. We identify the current extent of the suitable habitat for P. setaceum on the island of La Palma to assess how it affects island ecosystems, protected areas (PAs), and endemic plant species richness. We recorded in situ occurrences of P. setaceum from 2010 to 2018 and compiled additional ones from databases at a 500 m × 500 m resolution. To assess the current suitable habitat and possible distribution patterns of P. setaceum on the island, we built an ensemble model. We projected habitat suitability for island ecosystems and PAs and identified risks for total as well as endemic plant species richness. The suitable habitat for P. setaceum is calculated to cover 34.7% of the surface of La Palma. In open ecosystems at low to mid elevations, where native ecosystems are already under pressure by land use and human activities, the spread of the invader will likely lead to additional threats to endemic plant species. Forest ecosystems (e.g., broadleaved evergreen and coniferous forests) are not likely to be affected by the spread of P. setaceum because of its heliophilous nature. Our projection of suitable habitat of P. setaceum within ecosystems and PAs on La Palma supports conservationists and policymakers in prioritizing management and control measures and acts as an example for the potential threat of this graminoid invader on other islands.
Die Zunahme der Konzentration von CO2 und anderen "Treibhausgasen" in der Atmosphäre ist unzweifelhaft, und ebenso unzweifelhaft reagiert das Klima darauf. Christian-Dietrich Schönwiese, Professor für Meteorologische Umweltforschung und Klimatologie an der Universität Frankfurt am Main, sieht dringenden politischen Handlungsbedarf und plädiert gleichzeitig dafür, die Debatte rund um den Klimaschutz zu versachlichen.
Long-term average groundwater recharge, which is equivalent to renewable groundwater resources, is the major limiting factor for the sustainable use of groundwater. Compared to surface water resources, groundwater resources are more protected from pollution, and their use is less restricted by seasonal and inter-annual flow variations. To support water management in a globalized world, it is necessary to estimate groundwater recharge at the global scale. Here, we present a best estimate of global-scale long-term average diffuse groundwater recharge (i.e. renewable groundwater resources) that has been calculated by the most recent version of the WaterGAP Global Hydrology Model WGHM (spatial resolution of 0.5° by 0.5°, daily time steps). The estimate was obtained using two state-of-the-art global data sets of gridded observed precipitation that we corrected for measurement errors, which also allowed to quantify the uncertainty due to these equally uncertain data sets. The standard WGHM groundwater recharge algorithm was modified for semi-arid and arid regions, based on independent estimates of diffuse groundwater recharge, which lead to an unbiased estimation of groundwater recharge in these regions. WGHM was tuned against observed long-term average river discharge at 1235 gauging stations by adjusting, individually for each basin, the partitioning of precipitation into evapotranspiration and total runoff. We estimate that global groundwater recharge was 12 666 km3/yr for the climate normal 1961–1990, i.e. 32% of total renewable water resources. In semi-arid and arid regions, mountainous regions, permafrost regions and in the Asian Monsoon region, groundwater recharge accounts for a lower fraction of total runoff, which makes these regions particularly vulnerable to seasonal and inter-annual precipitation variability and water pollution. Average per-capita renewable groundwater resources of countries vary between 8 m3/(capita yr) for Egypt to more than 1 million m3/(capita yr) for the Falkland Islands, the global average in the year 2000 being 2091 m3/(capita yr). Regarding the uncertainty of estimated groundwater resources due to the two precipitation data sets, deviation from the mean is 1.1% for the global value, and less than 1% for 50 out of the 165 countries considered, between 1 and 5% for 62, between 5 and 20% for 43 and between 20 and 80% for 10 countries. Deviations at the grid scale can be much larger, ranging between 0 and 186 mm/yr.
Long-term average groundwater recharge, which is equivalent to renewable groundwater resources, is the major limiting factor for the sustainable use of groundwater. Compared to surface water resources, groundwater resources are more protected from pollution, and their use is less restricted by seasonal and inter-annual flow variations. To support water management in a globalized world, it is necessary to estimate groundwater recharge at the global scale. Here, we present a best estimate of global-scale long-term average diffuse groundwater recharge (i.e. renewable groundwater resources) that has been calculated by the most recent version of the WaterGAP Global Hydrology Model WGHM (spatial resolution of 0.5° by 0.5°, daily time steps). The estimate was obtained using two state-of-the art global data sets of gridded observed precipitation that we corrected for measurement errors, which also allowed to quantify the uncertainty due to these equally uncertain data sets. The standard WGHM groundwater recharge algorithm was modified for semi-arid and arid regions, based on 15 independent estimates of diffuse groundwater recharge, which lead to an unbiased estimation of groundwater recharge in these regions. WGHM was tuned against observed long-term average river discharge at 1235 gauging stations by adjusting, individually for each basin, the partitioning of precipitation into evapotranspiration and total runoff. We estimate that global groundwater recharge was 12 666 km3/yr for the climate nor20 mal 1961–1990, i.e. 32% of total renewable water resources. In semi-arid and arid regions, mountainous regions, permafrost regions and in the Asian Monsoon region, groundwater recharge accounts for a lower fraction of total runoff, which makes these regions particularly vulnerable to seasonal and inter-annual precipitation variability and water pollution. Average per-capita renewable groundwater resources of countries vary 25 between 8m3/(capita yr) for Egypt to more than 1 million m3/(capita yr) for the Falkland Islands, the global average in the year 2000 being 2091m3/(capita yr). Regarding the uncertainty of estimated groundwater resources due to the two precipitation data sets, deviation from the mean is less than 1% for 50 out of the 165 countries considered, between 1 and 5% for 62, between 5 and 20% for 43 and between 20 and 80% for 10 countries. Deviations at the grid scale can be much larger, ranging between 0 and 186 mm/yr.
Within the framework of the Transboundary Waters Assessment Programme (TWAP), initiated by the Global Environment Facility (GEF), we contributed to a comprehensive baseline assessment of transboundary aquifers (TBAs) by quantifying different groundwater indicators using the global water resources and water use model WaterGAP 2.2. All indicators were computed under current (2010) and projected conditions in 2030 and 2050 for 91 selected TBAs larger than 20,000 km2 and for each nation’s share of the TBAs (TBA-CU: country unit). TBA outlines were provided by the International Groundwater Resources Assessment Centre (IGRAC). The set of indicators comprises groundwater recharge, groundwater depletion, per-capita groundwater recharge, dependency on groundwater, population density, and groundwater development stress (groundwater withdrawals to groundwater recharge). Only the latter four indicators were projected to 2030 and 2050. Current-state indicators were quantified using the Watch Forcing Data climate dataset, while projections were based on five climate scenarios that were computed by five global climate models for the high-emissions scenario RCP 8.5. Water use projections were based on the Shared Socio-economic Pathway SSP2 developed within ISI-MIP. Furthermore, two scenarios of future irrigated areas were explored. For individual water use sectors, the fraction of groundwater abstraction was assumed to remain at the current level.
According to our assessment, aquifers with the highest current groundwater depletion rates worldwide are not transboundary. Exceptions are the Neogene Aquifer System (Syria) with 53 mm/yr between 2000 and 2009 and the Indus River Plain aquifer (India) with 28 mm/yr. For current conditions, we identified 20 out of 258 TBA-CUs suffering from medium to very high groundwater development stress, which are located in the Middle East and North Africa region, in South Asia, China, and the USA. Considering projections, ensemble means of per-cent changes or percent point changes to current conditions were determined. Per-capita groundwater recharge is projected to decrease in 80-90% of all TBA-CUs until 2030/2050. Due to the strongly varying projections of the global climate models, we applied a worst-case scenario approach to define future hotspots of groundwater development stress, taking into account the strongest computed increase until either 2030 or 2050 among all scenarios and individual GCMs. Based on this approach, the number of TBA-CUs under at least medium groundwater development stress increases from 20 to 58, comprising all hotspots under current conditions. New hotspots are projected to develop mainly in Sub-Saharan Africa, China, and Mexico.
Floodplains play an important role in the terrestrial water cycle and are very important for biodiversity. Therefore, an improved representation of the dynamics of floodplain water flows and storage in global hydrological and land surface models is required. To support model validation, we combined monthly time series of satellite-derived inundation areas (Papa et al., 2010) with data on irrigated rice areas (Portmann et al., 2010). In this way, we obtained global-scale time series of naturally inundated areas (NIA), with monthly values of inundation extent during 1993–2004 and a spatial resolution of 0.5°. For most grid cells (0.5°×0.5°), the mean annual maximum of NIA agrees well with the static open water extent of the Global Lakes and Wetlands database (GLWD) (Lehner and Döll, 2004), but in 16% of the cells NIA is larger than GLWD. In some regions, like Northwestern Europe, NIA clearly overestimates inundated areas, probably because of confounding very wet soils with inundated areas. In other areas, such as South Asia, it is likely that NIA can help to enhance GLWD. NIA data will be very useful for developing and validating a floodplain modeling algorithm for the global hydrological model WGHM. For example, we found that monthly NIAs correlate with observed river discharges.
Global-scale information on natural river flows and anthropogenic river flow alterations is required to identify areas where aqueous ecosystems are expected to be strongly degraded. Such information can support the identification of environmental flow guidelines and a sustainable water management that balances the water demands of humans and ecosystems. This study presents the first global assessment of the anthropogenic alteration of river flow regimes, in particular of flow variability, by water withdrawals and dams/reservoirs. Six ecologically relevant flow indicators were quantified using an improved version of the global water model WaterGAP. WaterGAP simulated, with a spatial resolution of 0.5 degree, river discharge as affected by human water withdrawals and dams around the year 2000, as well as naturalized discharge without this type of human interference. Compared to naturalized conditions, long-term average global discharge into oceans and internal sinks has decreased by 2.7% due to water withdrawals, and by 0.8% due to dams. Mainly due to irrigation, long-term average river discharge and statistical low flow Q90 (monthly river discharge that is exceeded in 9 out of 10 months) have decreased by more than 10% on one sixth and one quarter of the global land area (excluding Antarctica and Greenland), respectively. Q90 has increased significantly on only 5% of the land area, downstream of reservoirs. Due to both water withdrawals and reservoirs, seasonal flow amplitude has decreased significantly on one sixth of the land area, while interannual variability has increased on one quarter of the land area mainly due to irrigation. It has decreased on only 8% of the land area, in areas downstream of reservoirs where consumptive water use is low. The impact of reservoirs is likely underestimated by our study as small reservoirs are not taken into account. Areas most affected by anthropogenic river flow alterations are the Western and Central USA, Mexico, the western coast of South America, the Mediterranean rim, Southern Africa, the semi-arid and arid countries of the Near East and Western Asia, Pakistan and India, Northern China and the Australian Murray-Darling Basin, as well as some Arctic rivers. Due to a large number of uncertainties related e.g. to the estimation of water use and reservoir operation rules, the analysis is expected to provide only first estimates of river flow alterations that should be refined in the future.
Global-scale information on natural river flows and anthropogenic river flow alterations is required to identify areas where aqueous ecosystems are expected to be strongly degraded. Such information can support the identification of environmental flow guidelines and a sustainable water management that balances the water demands of humans and ecosystems. This study presents the first global assessment of the anthropogenic alteration of river flow regimes by water withdrawals and dams, focusing in particular on the change of flow variability. Six ecologically relevant flow indicators were quantified using an improved version of the global water model WaterGAP. WaterGAP simulated, with a spatial resolution of 0.5 degree, river discharge as affected by human water withdrawals and dams, as well as naturalized discharge without this type of human interference. Mainly due to irrigation, long-term average river discharge and statistical low flow Q90 (monthly river discharge that is exceeded in 9 out of 10 months) have decreased by more than 10% on one sixth and one quarter of the global land area (excluding Antarctica and Greenland), respectively. Q90 has increased significantly on only 5% of the land area, downstream of reservoirs. Due to both water withdrawals and dams, seasonal flow amplitude has decreased significantly on one sixth of the land area, while interannual variability has increased on one quarter of the land area mainly due to irrigation. It has decreased on only 8% of the land area, in areas with little consumptive water use that are downstream of dams. Areas most affected by anthropogenic river flow alterations are the western and central USA, Mexico, the western coast of South America, the Mediterranean rim, Southern Africa, the semi-arid and arid countries of the Near East and Western Asia, Pakistan and India, Northern China and the Australian Murray-Darling Basin, as well as some Arctic rivers. Due to a large number of uncertainties related e.g. to the estimation of water use and reservoir operation rules, the analysis is expected to provide only first estimates of river flow alterations that should be refined in the future.
This study presents a global scale analysis of cropping intensity, crop duration and fallow land extent computed by using the global dataset on monthly irrigated and rainfed crop areas MIRCA2000. MIRCA2000 was mainly derived from census data and crop calendars from literature. Global cropland extent was 16 million km2 around the year 2000 of which 4.4 million km2 (28%) was fallow, resulting in an average cropping intensity of 0.82 for total cropland extent and of 1.13 when excluding fallow land. The lowest cropping intensities related to total cropland extent were found for Southern Africa (0.45), Central America (0.49) and Middle Africa (0.54), while highest cropping intensities were computed for Eastern Asia (1.04) and Southern Asia (1.0). In remote or arid regions where shifting cultivation is practiced, fallow periods last 3–10 years or even longer. In contrast, crops are harvested two or more times per year in highly populated, often irrigated tropical or subtropical lowlands where multi-cropping systems are common. This indicates that intensification of agricultural land use is a strategy that may be able to significantly improve global food security. There exist large uncertainties regarding extent of cropland, harvested crop area and therefore cropping intensity at larger scales. Satellite imagery and remote sensing techniques provide opportunities for decreasing these uncertainties and to improve the MIRCA2000 inventory.
Global modelling of continental water storage changes : sensitivity to different climate data sets
(2007)
Since 2002, the GRACE satellite mission provides estimates of the Earth's dynamic gravity field with unprecedented accuracy. Differences between monthly gravity fields contain a clear hydrological signal due to continental water storage changes. In order to evaluate GRACE results, the state-of-the-art WaterGAP Global Hydrological Model (WGHM) is applied to calculate terrestrial water storage changes on a global scale. WGHM is driven by different climate data sets to analyse especially the influence of different precipitation data on calculated water storage. The data sets used are the CRU TS 2.1 climate data set, the GPCC Full Data Product for precipitation and data from the ECMWF integrated forecast system. A simple approach for precipitation correction is introduced. WGHM results are then compared with GRACE data. The use of different precipitation data sets leads to considerable differences in computed water storage change for a large number of river basins. Comparing model results with GRACE observations shows a good spatial correlation and also a good agreement in phase. However, seasonal variations of water storage as derived from GRACE tend to be significantly larger than those computed by WGHM, regardless of which climate data set is used.
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.
We report on HCFC-22 data acquired by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) in the reduced spectral resolution nominal observation mode. The data cover the period from January 2005 to April 2012 and the altitude range from the upper troposphere (above cloud top altitude) to about 50 km. The profile retrieval was performed by constrained nonlinear least squares fitting of modelled spectra to the measured limb spectral radiances. The spectral ν4-band at 816.5 ± 13 cm−1 was used for the retrieval. A Tikhonov-type smoothing constraint was applied to stabilise the retrieval. In the lower stratosphere, we find a global volume mixing ratio of HCFC-22 of about 185 pptv in January 2005. The rate of linear growth in the lower latitudes lower stratosphere was about 6 to 7 pptv year−1 in the period 2005–2012. The profiles obtained were compared with ACE-FTS satellite data v3.5, as well as with MkIV balloon profiles and cryosampler balloon measurements. Between 13 and 22 km, average agreement within −3 to +5 pptv (MIPAS – ACE) with ACE-FTS v3.5 profiles is demonstrated. Agreement with MkIV solar occultation balloon-borne measurements is within 10–20 pptv below 30 km and worse above, while in situ cryosampler balloon measurements are systematically lower over their full altitude range by 15–50 pptv below 24 km and less than 10 pptv above 28 km. MIPAS HCFC-22 time series below 10 km altitude are shown to agree mostly well to corresponding time series of near-surface abundances from the NOAA/ESRL and AGAGE networks, although a more pronounced seasonal cycle is obvious in the satellite data. This is attributed to tropopause altitude fluctuations and subsidence of polar winter stratospheric air into the troposphere. A parametric model consisting of constant, linear, quasi-biennial oscillation (QBO) and several sine and cosine terms with different periods has been fitted to the temporal variation of stratospheric HCFC-22 for all 10°-latitude/1-to-2-km-altitude bins. The relative linear variation was always positive, with relative increases of 40–70 % decade−1 in the tropics and global lower stratosphere, and up to 120 % decade−1 in the upper stratosphere of the northern polar region and the southern extratropical hemisphere. Asian HCFC-22 emissions have become the major source of global upper tropospheric HCFC-22. In the upper troposphere, monsoon air, rich in HCFC-22, is instantaneously mixed into the tropics. In the middle stratosphere, between 20 and 30 km, the observed trend is inconsistent with the trend at the surface (corrected for the age of stratospheric air), hinting at circulation changes. There exists a stronger positive trend in HCFC-22 in the Southern Hemisphere and a more muted positive trend in the Northern Hemisphere, implying a potential change in the stratospheric circulation over the observation period.
We report on HCFC-22 data acquired by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) in reduced spectral resolution nominal mode in the period from January 2005 to April 2012 from version 5.02 level-1b spectral data and covering an altitude range from the upper troposphere (above cloud top altitude) to about 50 km. The profile retrieval was performed by constrained nonlinear least squares fitting of measured limb spectral radiances to modelled spectra. The spectral v4-band at 816.5 ± 13 cm-1 was used for the retrieval. A Tikhonov-type smoothing constraint was applied to stabilise the retrieval. In the lower stratosphere, we find a global volume mixing ratio of HCFC-22 of about 185 pptv in January 2005. The linear growth rate in the lower latitudes lower stratosphere was about 6 to 7 pptv yr-1 in the period 2005–2012. The obtained profiles were compared with ACE-FTS satellite data v3.5, as well as with MkIV balloon profiles and in situ cryosampler balloon measurements. Between 13 and 22 km, average agreement within -3 to +5 pptv (MIPAS–ACE) with ACE-FTS v3.5 pro files is demonstrated. Agreement with MkIV solar occultation balloon-borne measurements is within 10–20 pptv below 30 km and worse above, while in situ cryosampler balloon measurements are systematically lower over their full altitude range by 15– 50 pptv below 24 km and less than 10 pptv above 28 km. Obtained MIPAS HCFC-22 time series below 10 km altitude are shown to agree mostly well to corresponding time series of near-surface abundances from NOAA/ESRL and AGAGE networks, although a more pronounced seasonal cycle is obvious in the satellite data, probably due to tropopause altitude fluctuations and subsidence of polar winter stratospheric air into the troposphere. A parametric model consisting of constant, linear, quasi-biennial oscillation (QBO) and several sine and cosine terms with different periods has been fitted to the temporal variation of stratospheric HCFC-22 for all 10° latitude/1 to 2 km altitude bins. The relative linear variation was always positive, with relative increases of 40–70%decade-1 in the tropics and global lower stratosphere, and up to 120%decade-1 in the upper stratosphere of the northern polar region and the southern extratropical hemisphere. In the middle stratosphere between 20 and 30 km, the observed trend is not consistent with the age of stratospheric air-corrected trend at ground, but stronger positive at the Southern Hemisphere and less strong increasing in the Northern Hemisphere, hinting towards changes in the stratospheric circulation over the observation period.
In this study, we use simulations from seven global vegetation models to provide the first multi‐model estimate of fire impacts on global tree cover and the carbon cycle under current climate and anthropogenic land use conditions, averaged for the years 2001–2012. Fire globally reduces the tree covered area and vegetation carbon storage by 10%. Regionally, the effects are much stronger, up to 20% for certain latitudinal bands, and 17% in savanna regions. Global fire effects on total carbon storage and carbon turnover times are lower with the effect on gross primary productivity (GPP) close to 0. We find the strongest impacts of fire in savanna regions. Climatic conditions in regions with the highest burned area differ from regions with highest absolute fire impact, which are characterized by higher precipitation. Our estimates of fire‐induced vegetation change are lower than previous studies. We attribute these differences to different definitions of vegetation change and effects of anthropogenic land use, which were not considered in previous studies and decreases the impact of fire on tree cover. Accounting for fires significantly improves the spatial patterns of simulated tree cover, which demonstrates the need to represent fire in dynamic vegetation models. Based upon comparisons between models and observations, process understanding and representation in models, we assess a higher confidence in the fire impact on tree cover and vegetation carbon compared to GPP, total carbon storage and turnover times. We have higher confidence in the spatial patterns compared to the global totals of the simulated fire impact. As we used an ensemble of state‐of‐the‐art fire models, including effects of land use and the ensemble median or mean compares better to observational datasets than any individual model, we consider the here presented results to be the current best estimate of global fire effects on ecosystems.
Global distributions of profiles of sulphur hexafluoride (SF6) have been retrieved from limb emission spectra recorded by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat covering the period September 2002 to March 2004. Individual SF6 profiles have a precision of 0.5 pptv below 25 km altitude and a vertical resolution of 4–6 km up to 35 km altitude. These data have been validated versus in situ observations obtained during balloon flights of a cryogenic whole-air sampler. For the tropical troposphere a trend of 0.230±0.008 pptv/yr has been derived from the MIPAS data, which is in excellent agreement with the trend from ground-based flask and in situ measurements from the National Oceanic and Atmospheric Administration Earth System Research Laboratory, Global Monitoring Division. For the data set currently available, based on at least three days of data per month, monthly 5° latitude mean values have a 1 o standard error of 1%. From the global SF6 distributions, global daily and monthly distributions of the apparent mean age of air are inferred by application of the tropical tropospheric trend derived from MIPAS data. The inferred mean ages are provided for the full globe up to 90° N/S, and have a 1 o standard error of 0.25 yr. They range between 0 (near the tropical tropopause) and 7 years (except for situations of mesospheric intrusions) and agree well with earlier observations. The seasonal variation of the mean age of stratospheric air indicates episodes of severe intrusion of mesospheric air during each Northern and Southern polar winter observed, long-lasting remnants of old, subsided polar winter air over the spring and summer poles, and a rather short period of mixing with midlatitude air and/or upward transport during fall in October/November (NH) and April/May (SH), respectively, with small latitudinal gradients, immediately before the new polar vortex starts to form. The mean age distributions further confirm that SF6 is destroyed in the mesosphere to a considerable degree. Model calculations with the Karlsruhe simulation model of the middle atmosphere (KASIMA) chemical transport model agree well with observed global distributions of the mean age only if the SF6 sink reactions in the mesosphere are included in the model.
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.
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.
A data set of monthly growing areas of 26 irrigated crops (MGAG-I) and related crop calendars (CC-I) was compiled for 402 spatial entities. The selection of the crops consisted of all major food crops including regionally important ones (wheat, rice, maize, barley, rye, millet, sorghum, soybeans, sunflower, potatoes, cassava, sugar cane, sugar beets, oil palm, rapeseed/canola, groundnuts/peanuts, pulses, citrus, date palm, grapes/vine, cocoa, coffee), major water-consuming crops (cotton), and unspecified other crops (other perennial crops, other annual crops, managed grassland). The data set refers to the time period 1998-2002 and has a spatial resolution of 5 arc minutes by 5 arc minutes which is 8 km by 8 km at the equator. This is the first time that a data set of cell-specific irrigated growing areas of irrigated crops with this spatial resolution was created. The data set is consistent to the irrigated area and water use statistics of the AQUASTAT programme of the Food and Agriculture Organization of the United Nations (FAO) (http://www.fao.org/ag/agl/aglw/aquastat/main/index.stm) and the Global Map of Irrigation Areas (GMIA) (http://www.fao.org/ag/agl/aglw/aquastat/irrigationmap/index.stm). At the cell-level it was tried to maximise consistency to the cropland extent and cropland harvested area from the Department of Geography and Earth System Science Program of the McGill University at Montreal, Quebec, Canada and the Center for Sustainability and the Global Environment (SAGE) of the University of Wisconsin at Madison, USA (http://www.geog.mcgill.ca/~nramankutty/ Datasets/Datasets.html and http://geomatics.geog.mcgill.ca/~navin/pub/Data/175crops2000/). The consistency between the grid product and the input data was quantified. MGAG-I and CC-I are fully consistent to each other on entity level. For input data other than CC-I, the consistency of MGAG-I on cell level was calculated. The consistency of MGAG-I with respect to the area equipped for irrigation (AEI) of GMIA and to the cropland extent of SAGE was characterised by the sum of the cell-specific maximum difference between the MGAG-I monthly total irrigated area and the reference area when the latter was exceeded in the grid cell. The consistency of the harvested area contained in MGAG-I with respect to SAGE harvested area was characterised by the crop-specific sum of the cell-specific difference between MGAG-I harvested area and the SAGE harvested area when the latter was exceeded in the grid cell. In all three cases, the sums are the excess areas that should not have been distributed under the assumption that the input data were correct. Globally, this cell-level excess of MGAG-I as compared to AEI is 331,304 ha or only about 0.12 % of the global AEI of 278.9 Mha found in the original grid. The respective cell-level excess of MGAG-I as compared to the SAGE cropland extent is 32.2 Mha, corresponding to about 2.2 % of the total cropland area. The respective cell-level excess of MGAG-I as compared to the SAGE harvested area is 27 % of the irrigated harvested area, or 11.5 % of the AEI. In a further step that will be published later also rainfed areas were compiled in order to form the Global data set of monthly irrigated and rainfed crop areas around the year 2000 (MIRCA2000). The data set can be used for global and continental-scale studies on food security and water use. In the future, it will be improved, e.g. with a better spatial resolution of crop calendars and an improved crop distribution algorithm. The MIRCA2000 data set, its full documentation together with future updates will be freely available through the following long-term internet site: http://www.geo.uni-frankfurt.de/ipg/ag/dl/forschung/MIRCA/index.html. The research presented here was funded by the German Research Foundation (Deutsche Forschungsgemeinschaft, DFG) within the framework of the research project entitled "Consistent assessment of global green, blue and virtual water fluxes in the context of food production: regional stresses and worldwide teleconnections". The authors thank Navin Ramankutty and Chad Monfreda for making available the current SAGE datasets on cropland extent (Ramankutty et al., 2008) and harvested area (Monfreda et al., 2008) prior to their publication.
Geoprax : Newsletter
(1999)
The endemic argan tree (Argania spinosa) populations in South Morocco are highly degraded due to their use as a biomass resource in dry years and illegal firewood extraction. The intensification and expansion of agricultural land lead to a retreat of the wooded area, while the remaining argan open woodlands are often overgrazed. Thus, canopy-covered areas decrease while areas without vegetation cover between the argan trees increase. In total, 36 rainfall simulation experiments as well as 60 infiltration measurements were conducted to investigate the potential difference between tree-covered areas and bare intertree areas. In addition, 60 soil samples were taken under the trees and in the intertree areas parallel to the contour lines. Significant differences using a t-test were found between tree and intertree areas for the studied parameters Ksat, Kh, pH, electric conductivity, percolation stability, total C-content, total N-content, K-content, Na-content, and Mg-content. Surface runoff and soil losses were not as conclusive but showed similar trends. The results showed that argan trees influence the soil underneath significantly, while the soil in intertree areas is less protected and more degraded. It is therefore reasonable to assume further degradation of the soil when intertree areas extend further due to lack of rejuvenation of argan trees.
This paper provides new geochemical data focusing on valuable elements in the coal, parting, and floor samples in the No. 5 coal seam of the Taiyuan Formation from the Wujiawan mine, Datong coalfield, northern China. The minerals mainly consist of kaolinite, calcite, and pyrite, as well as trace amounts of quartz and illite. The No. 5 coal is enriched in Li, Ga, high field strength elements (HFSEs), and rare earth elements and yttrium (REY) when compared with world hard coals. Of particular interest is the high average concentration of Li (67.66 μg/g), which is around seven times higher than the value for world hard coals. Lithium, Ga, and HFSEs have strong inorganic affinities, whereas REY have organic affinities. The main carrier of Li, Ga, and HFSEs is aluminosilicate minerals, while REY appear to occur with organophosphorus. These HFSEs are enriched, both in the parting and in the adjacent coal samples. This suggests that these elements are likely to leach out during the diagenetic process. The distribution patterns of REY, along with the ratio of Al2O3/TiO2 and the figure of Zr/TiO2 vs. Nb/Y are suggestive of their derivation from felsic parent material. In the northern and eastern part of the Datong coalfield, there are several regions where the Li content is higher than the mineable grade, in particular in the northern Datong coalfield where there is a mine with an Li content of 294.6 μg/g. This is significantly higher than the mineable grade. Therefore, there is a potential for financially viable recovery of Li in these coals of the Datong coalfield.
Trace elemental concentrations of bivalve shells content a wealthy of environmental and climatic information of the past, and therefore the studies of trace elemental distributions in bivalve shells gained increasing interest lately. However, after more than half century of research, most of the trace elemental variations are still not well understood and trace elemental proxies are far from being routinely applicable. This dissertation focuses on a better understanding of the trace elemental chemistry of Arctica islandica shells from Iceland, and paving the way for the application of the trace elemental proxies to reconstruct the environmental and climatic changes. Traits of trace elemental concentrations on A. islandica shells were explored and evaluated. Then based the geochemical traits of the shells, four non-environmental/climatic controlling is indentified. (1) Trace elemental concentrations of bivalve shells are effected by early diagenesis by the leach or exchange of elemental ions, especially in shell tip part, even with the protection of periostrucum; (2) The analytical methods also affect the results of trace elemental concentrations, especially for the element, such as Mg, which is highly enriched in organic matrices; (3) Shell organic matrices are found play a dominating role on the concentration of trace elements on A. islandica shells. Most trace elements only occurred in insoluble organic matrices (IOM), although others are only found in the carbonate fraction. IOM of A. islandica shells is significantly enriched in Mg, while Li and Na are more deplete in IOM, but enriched in shell carbonate. Ba is more or less even contented in IOM and shell carbonate. The concentrations of certain elements vary between primary layer and secondary layer; (4) The vital /physiological controlling on trace elemental distributions of bivalve shells is also confirmed. Six elemental (B, Na, Mg, Mn, Sr, and Ba) concentrations show significant correlation (exponential functions) with ontogenetic age and shell grow rates (logarithmic equations). It is worthy to remark that B, Mg, Sr and Ba concentrations are negatively correlated with shell growth rate, positive with ontogenetic age, while the concentrations of Na and Mn show the opposite trends. At last, all the controlling described above can be taken into account and corrected to extract the environmental and climatic signal by a kind of standardization. The derived six exponential functions of the high correlations between six trace elemental concentrations and ontogenetic year are applied to make the standardization of these element-Ca ratios. The gotten standardized indices are compared with the variations of environmental and climatic parameters in this region, and many correlations are found. Standardized indices of Sr/Ca ratios are strongly related to the sun spot number, autumn NAO, autumn Europe surface air temperature (SAT) and Arctic sea surface temperature anomaly (TA), and those of Mg/Ca ratios are strongly associated with Arctic TA, Europe SAT and Solar variation (irradiance). The variations of autumn Europe SAT demonstrated more similarity with standardized indices of B/Ca than other parameters. Except for the SAT index of Arctic, the standardized indices of Na/Ca showed no distinct relation to temperature. European precipitation and the Arctic sea level pressure index compared well the Na/Ca ratios of the shells, and so did the autumn NAO. Standardized indices of Mn/Ca were correlated with the number of hurricanes in the North Atlantic, Northern Europe SAT and sun spot number.
In subduction zones, sediments and hydrothermally altered oceanic crust, which together form part of the subducting slab, contribute to the chemical composition of lavas erupted at the surface to form volcanic arcs. Transport of this material from the slab to the overlying mantle wedge is thought to involve discreet melts and fluids that are released from various portions of the slab. We use a meta-analysis of geochemical data from eight globally representative arcs to show that melts and fluids from individual slab components cannot be responsible for the formation of arc lavas. Instead, the data are compatible with models that first invoke physical mixing of slab components and the mantle wedge, widely referred to as high-pressure mélange, before arc magmas are generated.
Driven by globalization, urbanization and climate change, the distribution range of invasive vector species has expanded to previously colder ecoregions. To reduce health-threatening impacts on humans, insect vectors are extensively studied. Population genomics can reveal the genomic basis of adaptation and help to identify emerging trends of vector expansion. By applying whole genome analyses and genotype-environment associations to populations of the main dengue vector Aedes aegypti, sampled along an altitudinal gradient in Nepal (200–1300 m), we identify putatively adaptive traits and describe the species' genomic footprint of climate adaptation to colder ecoregions. We found two differentiated clusters with significantly different allele frequencies in genes associated to climate adaptation between the highland population (1300 m) and all other lowland populations (≤800 m). We revealed nonsynonymous mutations in 13 of the candidate genes associated to either altitude, precipitation or cold tolerance and identified an isolation-by-environment differentiation pattern. Other than the expected gradual differentiation along the altitudinal gradient, our results reveal a distinct genomic differentiation of the highland population. Local high-altitude adaptation could be one explanation of the population's phenotypic cold tolerance. Carrying alleles relevant for survival under colder climate increases the likelihood of this highland population to a worldwide expansion into other colder ecoregions.
Background: Driven by globalization, urbanization and climate change, the distribution range of invasive vector species has expanded to previously colder ecoregions. To reduce health-threatening impacts on humans, insect vectors are extensively studied. Population genomics can reveal the genomic basis of adaptation and help to identify emerging trends of vector expansion.
Results: By applying whole genome analyses and genotype-environment associations to populations of the main dengue vector Ae. aegypti, sampled along an altitudinal temperature gradient in Nepal (200- 1300m), we identify adaptive traits and describe the species’ genomic footprint of climate adaptation to colder ecoregions. We found two clusters of differentiation with significantly different allele frequencies in genes associated to climate adaptation between the highland population (1300m) and all other lowland populations (≤ 800 m). We revealed non-synonymous mutations in 13 of the candidate genes associated to either altitude, precipitation or cold tolerance and identified an isolation-by-environment differentiation pattern.
Conclusion: Other than the expected gradual differentiation along the altitudinal gradient, our results reveal a distinct genomic differentiation of the highland population. This finding either indicates a differential invasion history to Nepal or local high-altitude adaptation explaining the population’s phenotypic cold tolerance. In any case, this highland population can be assumed to carry pre-adapted alleles relevant for the species’ invasion into colder ecoregions worldwide that way expanding their climate niche.
Global warming, changes in the hydrological cycle and enhanced marine primary productivity all have been invoked as having contributed to the occurrence of widespread ocean anoxia during the Cenomanian–Turonian oceanic anoxic event (OAE2; ~94 Ma), but disentangling these factors on a regional scale has remained problematic. In an attempt to separate these forcing factors, we generated palynological and organic geochemical records using a core spanning the OAE2 from Wunstorf, Lower Saxony Basin (LSB; northern Germany), which exhibits cyclic black shale–marl alternations related to the orbital precession cycle.
Despite the widely varying depositional conditions complicating the interpretation of the obtained records, TEX86H indicates that sea-surface temperature (SST) evolution in the LSB during OAE2 resembles that of previously studied sites throughout the proto-North Atlantic. Cooling during the so-called Plenus Cold Event interrupted black shale deposition during the early stages of OAE2. However, TEX86 does not vary significantly across black shale–marl alternations, suggesting that temperature variations did not force the formation of the cyclic black shale horizons. Relative (i.e., with respect to marine palynomorphs) and absolute abundances of pollen and spores are elevated during phases of black shale deposition, indicative of enhanced precipitation and run-off. High abundances of cysts from inferred heterotrophic and euryhaline dinoflagellates supports high run-off, which likely introduced additional nutrients to the epicontinental shelf resulting in elevated marine primary productivity.
We conclude that orbitally forced enhanced precipitation and run-off, in tandem with elevated marine primary productivity, were critical in cyclic black shale formation on the northern European epicontinental shelf and potentially for other OAE2 sections in the proto-Atlantic and Western Interior Seaway at similar latitudes as well.
Global warming, changes in the hydrological cycle and enhanced marine primary productivity all have been invoked to have contributed to the occurrence of widespread ocean anoxia during the Cenomanian-Turonian Oceanic Anoxic Event (OAE2; ~ 94 Ma), but disentangling these factors on a regional scale has remained problematic. We generated palynological and organic geochemical records that allow the separation of these forcing factors in a core spanning the OAE2 from Wunstorf, Lower Saxony Basin (LSB; North Gemany), which exhibits cyclic black shale–marl alternations related to the orbital precession cycle.
Despite the widely varying depositional conditions complicating the interpretation of the obtained records, TEX86H indicates that sea-surface temperature (SST) evolution in the LSB during OAE2 resembles that of previously studied sites throughout the proto-North Atlantic. Cooling during the so-called Plenus Cold Event interrupted black shale deposition during the early stages of OAE2. However, TEX86 does not vary significantly across marl–black shale alternations, suggesting that temperature variations did not force the formation of the cyclic black shale horizons. Relative (i.e., with respect to marine palynomorphs) and absolute abundances of pollen and spores are elevated during phases of black shale deposition, indicative of enhanced precipitation and run-off. High abundances of cysts from inferred heterotrophic and euryhaline dinoflagellates supports high run-off, which likely introduced additional nutrients to the epicontinental shelf resulting in elevated marine primary productivity.
We conclude that orbitally-forced enhanced precipitation and run-off, in tandem with elevated marine primary productivity, were critical in cyclic black shale formation on the northwest European epicontinental shelf and potentially for other OAE2 sections in the proto-Atlantic and Western Interior Seaway at similar latitudes as well.
Fractional release factors of long-lived halogenated organic compounds in the tropical stratosphere
(2010)
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 halocarbons 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 limitations of these measures due to their observed vertical and latitudinal variability. The presented data set could be used to improve future ozone level and climate projections.
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.
Fossil records of early solar irradiation and cosmolocation of the CAI factory: a reappraisal
(2021)
Calcium-aluminum–rich inclusions (CAIs) in meteorites carry crucial information about the environmental conditions of the nascent Solar System prior to planet formation. Based on models of 50V–10Be co-production by in-situ irradiation, CAIs are considered to have formed within ~0.1 AU from the proto-Sun. Here, we present vanadium (V) and strontium (Sr) isotopic co-variations in fine- and coarse-grained CAIs and demonstrate that kinetic isotope effects during partial condensation and evaporation best explain V isotope anomalies previously attributed to solar particle irradiation. We also report initial excesses of 10Be and argue that CV CAIs possess essentially a homogeneous level of 10Be, inherited during their formation. Based on numerical modeling of 50V–10Be co-production by irradiation, we show that CAI formation during protoplanetary disk build-up likely occurred at greater heliocentric distances than previously considered, up to planet-forming regions (~1AU), where solar particle fluxes were sufficiently low to avoid substantial in-situ irradiation of CAIs.
To reconstruct ocean circulation changes during specific periods of Earth history, benthic and planktic foraminifera were used as proxies in the different parts of this thesis. Both studied time periods, the Late Cretaceous and the early Pleistocene, are characterized by long-term climate cooling and major changes in ocean circulation. The first part of this thesis concentrated in the Late Cretaceous. During the Late Cretaceous long-term cooling phase, benthic foraminiferal δ18O values show a positive shift lasting about 1.5 Myr (71.5–70 Ma). This shift can be observed on a global scale and has become known as the Campanian-Maastrichtian Boundary Event (CMBE). It is proposed that this δ18O excursion is influenced either by changing intermediate- to deep-water circulation or by temporal build-up of Antarctic ice sheets. Benthic foraminiferal assemblage counts from a southern high-latitudinal site near Antarctica (ODP Site 690) are analyzed to test if the influence of the CMBE on the benthic species composition. One of the two discussed hypotheses for the causation of the δ18O transition is a change in intermediate- to deep-water circulation from low-latitude to high-latitude water masses. This change would result in cooler temperatures, higher oxygen concentration, and possibly lower organic-matter flux at the seafloor, causing a major benthic foraminiferal assemblage change. Another possible explanation of the δ18O transition of the CMBE is significant ice formation on Antarctica. However no major benthic foraminiferal assemblage change would be expected in this case. The benthic foraminiferal assemblage of Site 690 shows a separation of the studied succession into two parts with significantly different species composition. The older part (73.0–70.5 Ma) is dominated by species, which are typical for lower bottom water oxygen concentration and more common in low-latitude assemblages. Species dominating the younger part (70.0–68.0 Ma) are indicators for well-oxygenated bottom waters and more common in high-latitude assemblages. This change in the benthic foraminiferal assemblages is interpreted to represent a shift of low-latitude toward high-latitude dominated intermediateto deep-water sources. A change in oceanic circulation was therefore at least a major component of the CMBE. The Pacific Ocean contributed significantly to the climatic development during the Late Cretaceous cooling period. The contribution of ocean circulation changes in the Pacific Ocean to the Late Cretaceous climatic development in general and the CMBE and Mid-Maastrichtian Event (MME) in particular, however, is poorly understood. Previously measured high resolution planktic and benthic stable isotope data and a neodymium (Nd) isotope record from the Pacific ODP Site 1210 (Shatsky Rise, tropical Pacific Ocean) for the Campanian to Maastrichtian (69.5 to 72.5 Ma) are used to reconstruct changes in surface- and bottom water temperatures as well as changes in the source region of deep- to intermediate waters [see Appendix 4; Jung et al. 2013]. The results of the benthic foraminiferal δ18O and Nd isotope records in combination with Nd isotope records from other studies indicate changes in the intensity of intermediate- to deep ocean circulation in the tropical Pacific across the Campanian-Maastrichtian interval [see Appendix 4; Jung et al. 2013]. During the early Maastrichtian (72.5 to 69.5 Ma), a three-million-year-long period of cooler conditions and a simultaneous change towards less radiogenic Nd isotope signatures is interpreted to represent a period of increased admixture and northward flow of deep waters from the Southern Ocean (Southern Component Water, SCW). This change was probably caused by an intensified formation of deep waters in the Southern Ocean. This was reduced again during the MME (69.5 to 68.5 Ma). This early Maastrichtian cold interval is similar to the CMBEδ13C fall and succeeding δ13C rise towards the MME and is therefore also interpreted to represent tectonically forced, long-term changes in the global carbon cycle and thus a tectonic forcing of the early Maastrichtian climate cooling. Overall, the Campanian-Maastrichtian Nd and stable isotope records of Shatsky Rise indicate changes in ocean circulation that are paralleled by global warming and cooling periods. The fluctuating strength of SCW contribution in the tropical Pacific points towards an increased respectively weakened ocean circulation, which is probably related to the strength of deep-water formation in the Southern Ocean [see Appendix 4; Jung et al. 2013]. For this study, the analysis of benthic foraminiferal assemblages of Site 1210 is carried out for the same time interval (69.5 to 72.5 Ma) as Nd and stable isotopes to evaluate the influence of intermediate- to deep ocean circulation changes on the benthic foraminiferal community. The possible reaction of benthic foraminiferal assemblages is compared to the results of stable isotope and neodymium isotopes. The observed changes in species abundances only partly reflect the circulation changes reconstructed with Nd and stable oxygen istopes. For example, Stensioina spp., Aragonia spp. and Lenticulina spp., cold-water preferring species, start to be increasingly abundant at the beginning of enhanced influence of SCW. However, their abundance pattern does not follow the varying strength of the cold SCW influence at Shatsky Rise. Other species prefer lesser oxygen concentrations and warmer bottom water, e.g. Paralabamina spp. and Globorotalites spp. Paralabamina spp. has its highest relativ abundance at the beginning of the studied succession, where the influence of SCW is small. However, this taxa occurs throughout the record, even though the influence of SCW increases. Globorotalites spp. is even most abundance after the CMBE, where bottom waters are till cold and influenced by SCW. This leads to the conclusion that the varying strength of SCW in the tropical Pacific at Shatsky Rise through the studied interval is not facilitating a significant faunal turnover as has been observed at the South Atlantic Site 690 (Chapter 3). These results of the benthic foraminiferal assemblage analysis suggest a rather minor influence of the SCW on the major environmental factors that are generally influencing benthic foraminiferal communities (e.g., oxygen concentration, organic matter flux to the sea floor, bottom-water temperature). The second major part of this thesis focused on the late Pliocene-earliest Pleistocene. The late Pliocene is characterized by a long-term global cooling trend resulting in a major increase of Arctic ice sheets from around 3 Ma onwards, culminating in the Plio-Pleistocene intensification of the Northern Hemisphere glaciation. At around 2.7 Ma, large amplitude glacial-interglacial excursions (~1‰ δ18O in benthic foraminiferal calcite) in benthic oxygen isotopes can be observed. Marine isotope stage (MIS) 100 at around 2.55 Ma is the first glacial, when widespread ice rafted debris has been found in sediments in the North Atlantic Ocean. To gain a deeper understanding of the climatic evolution of the latest Pliocene-early Pleistocene, it is necessary to improve the reconstructions of North Atlantic paleohydrography, as the North Atlantic provides a key region for global climate. The consequences of the intensification of Northern Hemisphere on the early Pleistocene North Atlantic thermocline stratification and intermediate waters are still poorly understood. However, surface hydrography, the history of the thermocline and development of North Atlantic intermediate waters are well-studied for the Last Glacial Maximum (LGM). These well-known mechanisms responsible for the LGM in comparison with the present-day interglacial North Atlantic are used as an analogue for te early Pleistocene glacialinterglacials cycles. In this study, suborbitally resolved stable oxygen and carbon isotope and Mg/Ca records are measured from a deep-dwelling planktic foraminifera (Globorotaliacrassaformis) from Integrated Ocean Drilling Program Site U1313 (North Atlantic, 41°N) covering marine oxygen isotope stages MIS 103 to 95 (early Pleistocene, 2.6 to 2.4 Ma). The results are interpreted to represent a change in intermediate-water masses on glacialinterglacial timescales. During glacials geochemical records in G. crassaformis (~500–1000 m) bear the imprint of Glacial North Atlantic Intermediate Water (GNAIW), while during interglacials this species reflects the signature of the influence of Mediterranean Outflow Water (MOW) in combination with the subtropical gyre. The comparison of this data with the published records from G. ruber from the same samples facilitates the reconstruction of glacial-interglacial stratification changes of the upper water column at Site U1313. The results show that larger gradients of temperature, salinity and δ13C prevailed during glacials, suggesting a stronger stratification of the upper water column. This can be seen to indicate glacial-interglacial changes in ntermediate water masses in the North Atlantic similar to those reconstructed for the latest Pleistocene. As an additional proxy, the clumped isotope paleothermometer is applied for the Late Cretaceous study as well as for the early Pleistocene. This proxy is commonly assumed to be independent of other factors than temperature. Clumped isotopes are measured for the Late Cretaceous Site 690 on the planktic foraminiferal species Archaeoglobigerina australis and compared to already existing stable oxygen isotopes of this species. This is assumed to enable the reconstruction of paleotemperature independent of ice volume and therefore contribute to the long-lasting discussion whether there was a temporal ice build-up on Antarctic during the Campanian-Maastrichtian cooling period. For the early Pleistocene, the planktic foraminiferal species G. crassaformis is used from Site U1313 from MIS 99 (interglacial) and MIS 98 (glacial). This provides the opportunity to separate ice volume, salinity and temperature effects on the measured δ18O record of G. crassaformis. The results of the clumped isotope measurements reveal comparatively large standard errors. For the Late Cretaceous the standard error of the clumped isotope measurements proved too large to allow any conclusions on the temperature component on the δ18O record of A. australis. For the early Pleistocene, the temperature difference is also too small to be reconstructed with the standard error of the clumped isotope measurements in this study. Measuring many replicates of one sample would minimize the standard error considerably. However, the amount necessary to measure replicates cannot be gained for either time period, as almost all foraminifera were picked from the respective samples. It is concluded that the respective questions may be solved with a different method of clumped isotope analysis requiring less sample material. This method is, for example, available at the ETH Zurich.
One possible approach to study systematically the influence of the deformation regime on the geometry of geological structures like folds and boudins is analogue modelling. For a complete understanding of the resulting structures, consideration of the third dimension is required. This PhD study deals with scaled analogue modelling under constriction and plane-strain conditions to improve our knowledge of folding and boudinage of lower crustal rocks in space and time. Plasticine is an appropriate analogue material for rocks in the lower crust. Therefore, this material was used for the experiments. The macroscopic behaviour of most types of plasticine is quite similar to rocks undergoing strain-rate softening and strain hardening regardless of the different microscopic aspects of deformation. Therefore, if one is aware that the stress exponent and viscosity increase with increasing strain, the original plasticine types used with stress exponents ranging from 5.8 to 8.0 are adequate for modelling geologic structures. The same holds for plasticine/oil mixtures. Thus, plasticine and plasticine/oil mixtures can be used to model the viscous flow of different rock types in the lower crust. If climb-accommodated dislocation creep and associated steady-state flow is assumed for the natural rocks, the plasticine/oil mixtures should be used, which flow under steady-state conditions. Three different experimental studies of plane-strain coaxial deformation of stiff layers, with viscosity η2 and stress exponent n2, embedded in a weak matrix, with viscosity η1 and stress exponent n1, have been carried out. The undeformed samples (matrix plus layer) were cubes with an edge length of 12 cm. All experimental runs have been carried out at T = 25 ± 1°C and varying strain rates ė, ranging from 7.9 x 10 high -6 s high -1 to 1.7 x 10 high -2 s high -1, until a finite longitudinal strain of 30% – 40% was achieved. The first experimental study improved the understanding about the evolution of folds and boudins when the layer is oriented perpendicular to the Y-axis of the finite strain ellipsoid. The rock analogues used were Beck’s green plasticine (matrix) and Beck’s black plasticine (competent layer), both of which are strain-rate softening modelling materials with stress exponent n = ca. 8. The effective viscosity η of the matrix plasticine was changed by adding different amounts of oil to the original plasticine. At a strain rate ė of 10 high -3 s high -1 and a finite strain e of 10%, the effective viscosity of the matrix ranges from 1.2 x 10 high 6 to 7.2 x 10 high 6 Pa s. The effective viscosity of the competent layer has been determined as 4.2 x 10 high 7 Pa s. If the viscosity ratio is large (> ca. 20) and the initial thickness of the competent layer is small, both folds and boudins develop simultaneously. Although the growth rate of the folds seems to be higher than the growth rate of the boudins, the wavelength of both structures is approximately the same as is suggested by analytical solutions. A further unexpected, but characteristic, aspect of the deformed competent layer is a significant increase in thickness, which can be used to distinguish plane-strain folds and boudins from constrictional folds and boudins. In the second experimental study, the impact of varying strain rates on growing folds and boudins under plane strain have been investigated. The strain rates used range from 7.9 x 10 high -6 s high -1 to 1.7 x 10 high -2 s high -1. The stiff layer and matrix consist of non-linear viscous Kolb grey and Beck’s green plasticine, respectively, both of which are strain-rate softening modelling materials with power law exponents (n) and apparent viscosities (η) ranging from 6.5 to 7.9 and 8.5 x 10 high 6 to 7.2 x 10 high 6 Pa s, respectively. The effective viscosity (η) of the matrix plasticine was partly modified by adding oil to the original plasticine. At the strain rates used in the experiments the viscosity ratio between layer and matrix ranges between 3 and 10. Different runs have been carried out where the layer was oriented perpendicular to the principal strain axes (X>Y>Z). The results suggest a considerable influence of the strain rate on the geometry of the deformed stiff layer including its thickness. This holds for every type of layer orientation (S ┴ X, S ┴ Y, S ┴ Z). If the stiff layer is oriented perpendicular to the short axis Z of the finite strain ellipsoid, the number of the resulting boudins and the thickness of the stiff layer increase, whereas the length of boudins decreases with increasing strain rate. If the stiff layer is oriented perpendicular to the long axis, X, of the finite strain ellipsoid, enlargement of the strain rate results in increasing wavelength of folds, whereas the number of folds and the degree of thickening of the stiff layer decreased. If the stiff layer is oriented perpendicular to the intermediate Y-axis of the finite strain ellipsoid enlargement of the strain rate results in a decreasing number of boudins and folds associated with increasing wavelengths of both structures. The wavelength of folds is approximately half of the boudins wavelength. This is true for the case where folds and boudins develop simultaneously (S ┴ Y) and for cases where both structures develop independently (folds at S ┴ X and boudins at S ┴ Z). In the third experimental study, scaled analogue experiments have been carried out to demonstrate the growth of plane-strain folds and boudins through space and time. Previous 3D-studies are based only on finite deformation structures. Their results can therefore not be used to prove if both structures grew simultaneously or in sequence. Plane strain acted on a single stiff layer that was embedded in a weak matrix, with the layer oriented perpendicular to the intermediate Y-axis of the finite strain ellipsoid. Two different experimental runs have been carried out using computer tomography (CT) to analyse the results. The first run was carried out without interruption. During the second run, the deformation was stopped in each case at longitudinal strain increments of 10%. Every experiment was carried out at a temperature T of 25°C and a strain rate, ė, of ca. 4 x 10 high -3 s high -1 until a finite longitudinal strain of 40% was achieved with a viscosity contrast m of 18.6 between the non-linear viscous layer (Kolb brown plasticine) and the matrix (Beck’s green plasticine with 150 ml oil kg high -1). The apparent viscosity, η, and the stress exponent, n, for the layer at a strain rate ė = ca. 10 high -3 s high -1 and a finite strain e = 10% are 2.23 x 10 high 7 Pa s and n = 5.8 and for the matrix 1.2 x 10 high 6 Pa s and 10.5. These new data that result from incremental analogue modelling corroborate previous suggestions that folds and boudins are coeval structures in cases of plane-strain coaxial deformation with the stiff layer oriented perpendicular to the intermediate Y-axis of the finite strain ellipsoid. They will be of interest for all workers who are dealing with plane-strain boudins and folds, where the fold axes are parallel to the major axis (X) of the finite strain ellipsoid. As has been demonstrated by the first experimental study, coeval folding and boudinage under plane strain, with S ┴ Y, are associated with a significant increase in the thickness of the competent layer. The latter phenomenon does not occur in other cases of simultaneous folding and boudinage, such as bulk pure constriction. To study the impact of layer thickness on the geometry of folds and boudins under pure constriction, we carried out additional experiments using different types of plasticine for a stiff layer and a weaker matrix to model folding and boudinaging under pure constriction, with the initially planar layer oriented parallel to the Xaxis of the finite strain ellipsoid. The stiff layer and matrix consist of non-linear viscous Kolb brown and Beck’s green plasticine, respectively, both of which are strain-rate softening modelling materials. Six runs have been carried out using thicknesses of the stiff layer of 1, 2, 4, 6, 8 and 10 ± 0.2 mm. All experimental runs were carried out at a temperature T of 30 ± 2°C and a strain rate, ė, of ca. 1.1 x 10 high -4 s high -1 until a finite longitudinal strain of 40% was achieved with a viscosity contrast m of 3.1 between the stiff layer (Kolb brown plasticine) and the matrix (Beck’s green plasticine). The apparent viscosity, η, and the stress exponent, n, for the layer at a strain rate ė = ca. 10 high -3 s high -1 and a finite strain e = 10% are 2.23 x 10 high 7 Pa s and n = 5.8 and for the matrix 7.2 x 10 high 6 Pa s and 7.9. Our results suggest a considerable influence of the initial thickness of the stiff layer on the geometry of the deformed stiff layer. There is no evidence for folding in XY=XZ-sections if the initial thickness of the competent layer is larger than ca. 8 mm. If the initial thickness of the competent layer is set at ca. 10 ± 0.2 mm, both folds and boudins develop simultaneously. However, the growth rate of the boudins seems to be higher than the growth rate of the folds. A further expected, but characteristic, aspect of the deformed competent layer is no change in thickness of the competent layer, which can be used to distinguish plane-strain folds and boudins from constrictional folds and boudins. The model results are important for the analysis and interpretation of deformation structures in rheologically stratified rocks undergoing dislocation creep under bulk constriction. Tectonic settings where constrictional folds and boudins may develop simultaneously are stems of salt diapirs, subduction zones or thermal plumes. To make (paleo) viscosimetric statements possible, the rheological data of the different plasticine types were related to the geometrical data. When comparing the normalized dominant wavelength Wd obtained from the deformed layer of the models with the theoretical dominant wavelength (Ld) calculated using the Smith equation (1977, 1979), the latter probably also holds when folding and boudinage develop simultaneously (S ┴ Y) and when boudins develop independently (S ┴ Z), but can obviously not be applied at very low viscosity ratios as is indicated by the low-strain-rate experiments.
Metasomatic reaction zones between mafic and ultramafic rocks exhumed from subduction zones provide a window into mass-transfer processes at high pressure. However, accurate interpretation of the rock record requires distinguishing high-pressure metasomatic processes from inherited oceanic signatures prior to subduction. We integrated constraints from bulk-rock geochemical compositions and petrophysical properties, mineral chemistry, and thermodynamic modeling to understand the formation of reaction zones between juxtaposed metagabbro and serpentinite as exemplified by the Voltri Massif (Ligurian Alps, Italy). Distinct zones of variably metasomatized metagabbro are dominated by chlorite, amphibole, clinopyroxene, epidote, rutile, ilmenite, and titanite between serpentinite and eclogitic metagabbro. Whereas the precursor serpentinite and oxide gabbro formed and were likely already in contact in an oceanic setting, the reaction zones formed by diffusional Mg-metasomatism between the two rocks from prograde to peak, to retrograde conditions in a subduction zone. Metasomatism of mafic rocks by Mg-rich fluids that previously equilibrated with serpentinite could be widespread along the subduction interface, within the subducted slab, and the mantle wedge. Furthermore, the models predict that talc formation by Si-metasomatism of serpentinite in subduction zones is limited by pressure-dependent increase in the silica activity buffered by the serpentine-talc equilibrium. Elevated activities of aqueous Ca and Al species would also favor the formation of chlorite and garnet. Accordingly, unusual conditions or processes would be required to stabilize abundant talc at high P-T conditions. Alternatively, a different set of mineral assemblages, such as serpentine- or chlorite-rich rocks, may be controlling the coupling-decoupling transition of the plate interface.
Active chlorine species play a dominant role in the catalytic destruction of stratospheric ozone in the polar vortices during the late winter and early spring seasons. Recently, the correct understanding of the ClO dimer cycle was challenged by the release of new laboratory absorption cross sections (Pope et al., 2007) yielding significant model underestimates of observed ClO and ozone loss (von Hobe et al., 2007). Under this aspect, Arctic stratospheric limb emission measurements carried out by the balloon version of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) from Kiruna (Sweden) on 11 January 2001 and 20/21 March 2003 have been reanalyzed with regard to the chlorine reservoir species ClONO2 and the active species, ClO and ClOOCl (Cl2O2). New laboratory measurements of IR absorption cross sections of ClOOCl for various temperatures and pressures allowed for the first time the retrieval of ClOOCl mixing ratios from remote sensing measurements. High values of active chlorine (ClOx) of roughly 2.3 ppbv at 20 km were observed by MIPAS-B in the cold mid-winter Arctic vortex on 11 January 2001. While nighttime ClOOCl shows enhanced values of nearly 1.1 ppbv at 20 km, ClONO2 mixing ratios are less than 0.1 ppbv at this altitude. In contrast, high ClONO2 mixing ratios of nearly 2.4 ppbv at 20 km have been observed in the late winter Arctic vortex on 20 March 2003. No significant ClOx amounts are detectable on this date since most of the active chlorine has already recovered to its main reservoir species ClONO2. The observed values of ClOx and ClONO2 are in line with the established chlorine chemistry. The thermal equilibrium constants between the dimer formation and its dissociation, as derived from the balloon measurements, are on the lower side of reported data and in good agreement with values recommended by von Hobe et al. (2007). Calculations with the ECHAM/MESSy Atmospheric Chemistry model (EMAC) using established kinetics show similar chlorine activation and deactivation, compared to the measurements in January 2001 and March 2003, respectively.
Active chlorine species play a dominant role in the catalytic destruction of stratospheric ozone in the polar vortices during the late winter and early spring seasons. Recently, the correct understanding of the ClO dimer cycle was challenged by the release of new laboratory absorption cross sections (Pope et al., 2007) yielding significant model underestimates of observed ClO and ozone loss (von Hobe et al., 2007). Under this aspect, nocturnal Arctic stratospheric limb emission measurements carried out by the balloon version of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) from Kiruna (Sweden) on 11 January 2001 and 20/21 March 2003 have been reanalyzed with regard to the chlorine reservoir species ClONO2 and the active species, ClO and ClOOCl (Cl2O2). New laboratory measurements of IR absorption cross sections of ClOOCl for various temperatures and pressures allowed for the first time the retrieval of ClOOCl mixing ratios from remote sensing measurements. High values of active chlorine (ClOx) of roughly 2.3 ppbv at 20 km were observed by MIPAS-B in the cold mid-winter Arctic vortex on 11 January 2001. While nighttime ClOOCl shows enhanced values of nearly 1.1 ppbv at 20 km, ClONO2 mixing ratios are less than 0.1 ppbv at this altitude. In contrast, high ClONO2 mixing ratios of nearly 2.4 ppbv at 20 km have been observed in the late winter Arctic vortex on 20 March 2003. No significant ClOx amounts are detectable on this date since most of the active chlorine has already recovered to its main reservoir species ClONO2. The observed values of ClOx and ClONO2 are in line with the established polar chlorine chemistry. The thermal equilibrium constants between the dimer formation and its dissociation, as derived from the balloon measurements, are on the lower side of reported data and in good agreement with values recommended by von Hobe et al. (2007). Calculations with the ECHAM/MESSy Atmospheric Chemistry model (EMAC) using established kinetics show similar chlorine activation and deactivation, compared to the measurements in January 2001 and March 2003, respectively.
We report the first atmospheric observations of the Chlorofluorocarbons (CFCs) trifluorochloroethene, 3-chloropentafluoropropene and 4,4-dichlorohexafluoro-1-butene by means of Gas Chromatography with Electron Capture and Mass Spectrometric detection (GC-ECD-MS) in air samples taken at the Taunus Observatory operated by the University of Frankfurt (Main) and the Jungfraujoch High Altitude Research Station in Switzerland. These substances belong to a class of CFCs containing a double bond and are suspected to originate from the production and thermal degradation of widely used fluoropolymers like polychlorotrifluoroethene (PCTFE). Their atmospheric lifetimes are expected to be rather short. A quantitative calibration could only be derived for trifluorochloroethene but not for the other species by now. Thus, we use a relative sensitivity method to get a first indication of the observed atmospheric abundances. Identification was possible because of an air plume containing high concentrations of these substances. We suggest that the abundances found on this occasion originated from a local source. However, we have also observed the novel CFCs in air masses representative of background conditions, though with much lower concentrations. These species and some of their degradation products are toxic and could also be relevant for stratospheric and tropospheric ozone depletion.
Die konventionelle Extremwertstatistik die sich an der Über- bzw. Unterschreitungshäufigkeit bestimmter Schwellenwerte orientiert, beinhaltet den Nachteil, daß Änderungen der Parameter der Häufigkeitsverteilung die Extremwertwahrscheinlichkeit beeinflussen. So kann allein das Vorhandensein eines Trends für derartige Veränderungen verantwortlich sein. Die hier gewählte Methodik vermeidet diesen Nachteil, indem sie eine Zerlegung der betrachteten Zeitreihen in einen strukturierten und einen unstrukturierten Anteil durchführt. Dabei setzt sich der strukturierte Anteil aus einer Trend-, Saison- und glatten Komponente zusammen. Aus der Summe dieser in der Zeitreihe signifikant enthaltenen Komponenten läßt sich die Eintrittswahrscheinlichkeit von Extremwerten ableiten. Ähnliches gilt für den unstrukturierten Anteil insbesondere für die Varianz des Residuums. Das Residuum kann aber auch Werte enthalten, die nicht zu ihrer ansonsten angepaßten Häufigkeitsverteilung passen. Solche Werte werden als Extremereignisse bezeichnet und sind von den Extremwerten zu unterschieden. In der vorliegenden Arbeit werden nun, getrennt voneinander, durch Änderungen in den Parametern der Häufigkeitsverteilung hervorgerufene Variationen der Extremwertwahrscheinlichkeit als auch parameterunabhängige Extremereignisse der bodennahen Lufttemperatur betrachtet. Als Datenbasis dienten 41, wahrscheinlich homogene, europäische Stationszeitreihen von Monatsmitteltemperaturen, die den Zeitraum von 1871 bis 1990 abdecken. In den untersuchten Temperaturzeitreihen wurde an 37 von 41 Stationen ein positiver Trend detektiert, woraus ein Anstieg der Extremwertwahrscheinlichkeit mit der Zeit resultiert. Die glatten, niederfrequenten Schwingungen wirken sich in den meisten Fällen um 1890 und 1975 negativ und um 1871, 1940 und 1990 positiv auf die Extremwertwahrscheinlich keit aus. Desweiteren treten Änderungen in der Saisonfigur bezüglich der Amplitude und der Phasenlage auf. Detektierte Zunahmen in der Amplitude des Jahresgangs führen zu einer positiven Änderung der Extremwertwahrscheinlichkeit. Signifikante Änderungen in der Phasenlage der Saisonfigur erzeugen in den Anomaliezeitreihen einen saisonal unterschiedlichen Trend, dessen Amplitude, in den betrachteten Fällen, in der Größenordnung der Trendkomponente liegt. Saisonal unterschiedliche Trends beeinflussen saisonal unterschiedlich die Wahrscheinlichkeit für das Eintreten von Extremwerten. Die Residuen von fünf Temperaturzeitreihen weisen signifikante Varianzinstationaritäten auf, wobei in nur einem Fall die Varianz mit der Zeit zunimmt und somit einen Anstieg der Extremwertwahrscheinlichkeit erzeugt. Extremereignisse treten vorwiegend in Form besonders kalter Winter auf und können wahrscheinlich als Realisation eines Poisson-Prozesses interpretiert werden. Sie erscheinen zufällig über den Beobachtungszeitraum verteilt mit einer mittleren Wiederkehrzeit von mehr als 10 Jahren.
Highlights
• We present the first results of a deep learning model based on a convolutional neural network for earthquake magnitude estimation, using HR-GNSS displacement time series.
• The influence of different dataset configurations, such as station numbers, epicentral distances, signal duration, and earthquake size, were analyzed to figure out how the model can be adapted to various scenarios.
• The model was tested using real data from different regions and magnitudes, resulting in the best cases with 0.09 ≤ RMS ≤ 0.33.
Abstract
High-rate Global Navigation Satellite System (HR-GNSS) data can be highly useful for earthquake analysis as it provides continuous high-frequency measurements of ground motion. This data can be used to analyze diverse parameters related to the seismic source and to assess the potential of an earthquake to prompt strong motions at certain distances and even generate tsunamis. In this work, we present the first results of a deep learning model based on a convolutional neural network for earthquake magnitude estimation, using HR-GNSS displacement time series. The influence of different dataset configurations, such as station numbers, epicentral distances, signal duration, and earthquake size, were analyzed to figure out how the model can be adapted to various scenarios. We explored the potential of the model for global application and compared its performance using both synthetic and real data from different seismogenic regions. The performance of our model at this stage was satisfactory in estimating earthquake magnitude from synthetic data with 0.07 ≤ RMS ≤ 0.11. Comparable results were observed in tests using synthetic data from a different region than the training data, with RMS ≤ 0.15. Furthermore, the model was tested using real data from different regions and magnitudes, resulting in the best cases with 0.09 ≤ RMS ≤ 0.33, provided that the data from a particular group of stations had similar epicentral distance constraints to those used during the model training. The robustness of the DL model can be improved to work independently from the window size of the time series and the number of stations, enabling faster estimation by the model using only near-field data. Overall, this study provides insights for the development of future DL approaches for earthquake magnitude estimation with HR-GNSS data, emphasizing the importance of proper handling and careful data selection for further model improvements.
We use observations of total particle number concentration at 36 worldwide sites and a global aerosol model to quantify the primary and secondary sources of particle number. We show that emissions of primary particles can reasonably reproduce the spatial pattern of observed condensation nuclei (CN) (R2=0.51) but fail to explain the observed seasonal cycle at many sites (R2=0.1). The modeled CN concentration in the free troposphere is biased low (normalised mean bias, NMB=−88%) unless a secondary source of particles is included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%). Simulated CN concentrations in the continental boundary layer (BL) are also biased low (NMB=−74%) unless the number emission of anthropogenic primary particles is increased or an empirical BL particle formation mechanism based on sulfuric acid is used. We find that the seasonal CN cycle observed at continental BL sites is better simulated by including a BL particle formation mechanism (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). Using sensitivity tests we derive optimum rate coefficients for this nucleation mechanism, which agree with values derived from detailed case studies at individual sites.
We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300–2000 cm -3 in the marine boundary layer and free troposphere (FT) and 1000–10 000 cm -3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2–10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=& -88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB= -25%). Simulated CN concentrations in the continental BL were also biased low (NMB= -74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation-type nucleation parameterizations gave similar agreement with observed monthly mean CN concentrations.
Bayesian Networks are computer-based environmental models that are frequently used to support decision-making under uncertainty. Under data scarce conditions, Bayesian Networks can be developed, parameterized, and run based on expert knowledge only. However, the efficiency of expert-based Bayesian Network modeling is limited by the difficulty in deriving model inputs in the time available during expert workshops. This thesis therefore aimed at developing a simple and robust method for deriving conditional probability tables from expert estimates in a time-efficient way. The design and application of this new elicitation and conversion method is demonstrated using a case study in Xinjiang, Northwest China. The key characteristics of this method are its time-efficiency and the approach to use different conversion tables based on varying levels of confidence. Although the method has its limitations, e.g. it can only be applied for variables with one conditioning variable; it provides the opportunity to support the parameterization of Bayesian Networks which would otherwise remain half-finished due to time constraints. In addition, a case study in the Murray-Darling Basin, Australia, is used to compare Bayesian Network types and software to improve the presentation clarity of large Bayesian Networks. Both case studies aimed at gaining insights on how to improve the applicability of Bayesian Networks to support environmental management.
Als Voraussetzung für die experimentellen Arbeiten wurde am Mineralogischen Institut in Frankfurt eine Hochdruckpresse mit einer Multi-Anvil-Apparatur vom Walker-Typ aufgebaut und kalibriert. Diese Arbeiten nahmen einen beträchtlichen Teil der Promotionszeit ein. In einer Reihe von Hochdruck-Experimenten wurde dann die maximale Löslichkeit von Aluminium und den Seltenerd-Elementen Lanthan, Gadolinium und Lutetium in den Phasen des CaSiO3-Systems im Druckbereich zwischen 2.0 und 13.0 GPa untersucht. Unsere Experimente ergaben eine Zunahme der maximalen Löslichkeit mit steigendem Druck, von Wollastonit über Ca-Walstromit, Larnit + Si-Titanit bis Ca-Perowskit. Ca-Perowskit zeigt extrem hohe SEE-Konzentrationen mit einem Maximum bei den mittleren SEE. In den anderen Phasen nimmt die Löslichkeit mit zunehmender Kompatibilität der SEE zu. Innerhalb der Stabilitätsfelder zeigte sich keine signifikante Druck- oder Temperatur-Abhängigkeit der maximalen Löslichkeit. Anhand der Mikrosonden-Analysen konnte gezeigt werden, dass der Einbau von Al und SEE in Ca-Walstromit nicht über eine gekoppelte Substitution erfolgt, sondern wahrscheinlich über eine Defektstruktur. Dies deckt sich mit unseren TEM-Untersuchungen an diesen synthetischen Produkten, die eine hohe Dichte an planaren Baufehlern mit leicht erhöhten SEE-Konzentrationen ergaben. In allen Ca-Silikat-Phasen lag die maximale Löslichkeit der Seltenen Erden höher als die Konzentration in natürlichen Proben. Damit steht fest, dass die in Einschlüssen gemessenen SEE-Gehalte „primär“ sind und sich nicht durch etwaige Entmischungen im Zuge einer Anpassung der Kristallstruktur an die veränderten P,T-Bedingungen verändert haben. Entmischungen in Form einer SEE-reichen Phase würden eine an LSEE extrem angereicherte Quelle voraussetzen. Ein Vergleich unserer Subsolidus-Experimente mit CaSiO3-Einschlüssen in Diamanten aus Guinea zeigt, dass einige mit bis zu 0.13 Gew.% Al2O3 an Aluminium gesättigt sind. Diese Tatsache ist besonders interessant bei der Interpretation Alhaltiger Einschlussphasen. Neben absoluten Spurenelement-Konzentrationen sind Verteilungskoeffizienten äußerst wertvolle Hilfsmittel bei der Bewertung natürlicher Proben. Die in der Literatur bestehenden Datensätze wurden mit unseren Kristall/Schmelz-Verteilungskoeffizienten bzw. Verteilungskoeffizienten zwischen Ca-Silikatphasen erweitert. Verteilungskoeffizienten der Seltenerd-Elemente zwischen Ca-Walstromit und Karbonat sind um eine Größenordnung höher als Ca-Walstromit/Schmelz-Verteilungskoeffizienten und zeigen eine größere Steigung zwischen den MSEE und den SSEE (Lu/Gd). Die Seltenen Erden verhalten sich sowohl in Larnit als auch in Si-Titanit inkompatibel, wobei DX/L La für Larnit etwa 0.1 und für CaSi2O5 etwa 0.002 ist, d.h. auch, dass die LSEE im Vergleich zu Si-Titanit bevorzugt in Larnit eingebaut werden. Al verhält sich in Si-Titanit Zusammenfassung 147 kompatibel (DX/LAl=4) und in Larnit leicht inkompatibel. Diese Ergebnisse decken sich mit Analysen an natürlichen Proben. Die SEE-Verteilungskoeffizienten zwischen Ca-Perowskit und Schmelze liegen mit Ausnahme von La über eins und zeigen in Übereinstimmung mit Literaturdaten ein Maximum bei Gd. Für Granat konnte gezeigt werden, dass der Einbau der SEE und Si in MgO-haltigen Kristallen in Abhängigkeit von Druck und Startzusammensetzung über eine Ca SEE2 Mg2 Si3O12- Komponente bzw. über eine Ca3 MgSi Si3O12-Komponente mit 6-fach koordiniertem Silizium erfolgt. In zahlreichen Experimenten kristallisierte eine neue Ca-SEE-Silikat-Phase mit Feldspat-Stöchiometrie. Dabei handelt es sich offenbar um ein Mischkristallsystem mit einem Endglied, in das vorwiegend die leichten SEE eingebaut werden und in einem zweiten mit vorwiegend schweren SEE. Ab einem Druck von etwa 10.0 GPa trennt ein Solvus die beiden Endglieder voneinander. In der Literatur ist bisher nur ein CaLa2Si2O8-Endglied beschrieben worden. In einigen Experimenten mit P und Li wurde zusätzlich untersucht, ob diese Elemente zur Rekonstruktion der Bildungsbedingungen von Diamanten verwendet werden können. Dabei zeigte sich, dass die max. Löslichkeit von Li in CaSiO3 näher an den natürlichen Probenzusammensetzungen liegt und damit möglicherweise Potential für die Rekonstruktion von Bildungsbedingungen hat. In einem weiteren Teil dieser Arbeit wurde die Kinetik retrograder Reaktionen im CaSiO3-System untersucht. Die für die In-Situ-Experimente mit Synchrotron-Strahlung notwendigen Versuchsaufbauten wurden von uns entwickelt und die entsprechenden Entwicklungsschritte und technischen Probleme ausführlich beschrieben. Anhand von Entlastungsexperimenten wurden die Disproportionierung von Ca-Perowskit zu Larnit + Si-Titanit und die Rekombination zu Ca-Walstromit bei unterschiedlichen Temperaturen und unter dem Einfluss von Wasser untersucht. Aufgrund der wenigen verwertbaren Daten, die uns vorliegen, konnten zwar keine Aktivierungsenergien berechnet werden, es sind aber aufgrund unser Beobachtungen folgende Feststellungen zu treffen: Die Reaktion von Ca-Perowskit zu Larnit + Si-Titanit erfolgt bei gleicher Temperatur offenbar um Größenordnungen schneller als die sich bei niedrigen Drucken anschließende Rekombination zu Ca-Walstromit. Dies deckt sich mit Beobachtungen an natürlichen Proben, bei denen Larnit und Si-Titanit teilweise unvollständig zu Ca-Walstromit reagierten. Dadurch erscheint es eher unwahrscheinlich, dass amorphes CaSiO3 in Diamanten ein direktes Umwandlungsprodukt von Ca-Perowskit ist. Aber auch für die in der Literatur beschriebene Amorphisierung von Ca-Walstromit-Einschlüssen (Stachel 2000) noch innerhalb des umgebenden Diamanten ließ sich durch unsere In-Situ-Entlastungsexperimente nicht stützen. Eine Amorphisierung von Ca-Walstromit beobachteten wir nur bei einer Untersuchung am TEM, wo die Phase sehr instabil war und selbst in einem Kryohalter rasch unter dem Einfluss der Elektronenstrahls amorphisierte. Die Beugungs-Spektren, die nach einer Druckentlastung im Ca-Walstromit-Stabilitätsfeld aufgenommen wurden, unterschieden sich trotz der CaSiO3-Chemie der neu gebildeten Phase deutlich von unseren Ca-Walstromit-Referenz-Spektren, so dass die Umwandlung möglicherweise über eine metastabile Zwischenstufe erfolgt. Vor dem Hintergrund von unterschiedlichen, in der Literatur beschriebenen Strukturtypen von Ca-Walstromit wäre eine systematische Untersuchung der Struktur innerhalb des gesamten Stabilitätsfeldes wichtig.
During the measurement campaign FROST 2 (FReezing Of duST 2), the Leipzig Aerosol Cloud Interaction Simulator (LACIS) was used to investigate the influence of various surface modifications on the ice nucleating ability of Arizona Test Dust (ATD) particles in the immersion freezing mode. The dust particles were exposed to sulfuric acid vapor, to water vapor with and without the addition of ammonia gas, and heat using a thermodenuder operating at 250 °C. Size selected, quasi monodisperse particles with a mobility diameter of 300 nm were fed into LACIS and droplets grew on these particles such that each droplet contained a single particle. Temperature dependent frozen fractions of these droplets were determined in a temperature range between −40 °C ≤T≤−28 °C. The pure ATD particles nucleated ice over a broad temperature range with their freezing behavior being separated into two freezing branches characterized through different slopes in the frozen fraction vs. temperature curves. Coating the ATD particles with sulfuric acid resulted in the particles' IN potential significantly decreasing in the first freezing branch (T>−35 °C) and a slight increase in the second branch (T≤−35 °C). The addition of water vapor after the sulfuric acid coating caused the disappearance of the first freezing branch and a strong reduction of the IN ability in the second freezing branch. The presence of ammonia gas during water vapor exposure had a negligible effect on the particles' IN ability compared to the effect of water vapor. Heating in the thermodenuder led to a decreased IN ability of the sulfuric acid coated particles for both branches but the additional heat did not or only slightly change the IN ability of the pure ATD and the water vapor exposed sulfuric acid coated particles. In other words, the combination of both sulfuric acid and water vapor being present is a main cause for the ice active surface features of the ATD particles being destroyed. A possible explanation could be the chemical transformation of ice active metal silicates to metal sulfates. The strongly enhanced reaction between sulfuric acid and dust in the presence of water vapor and the resulting significant reductions in IN potential are of importance for atmospheric ice cloud formation. Our findings suggest that the IN concentration can decrease by up to one order of magnitude for the conditions investigated.
During the measurement campaign FROST 2 (FReezing Of duST 2), the Leipzig Aerosol Cloud Interaction Simulator (LACIS) was used to investigate the influences of various surface modifications on the immersion freezing behavior of Arizona Test Dust (ATD) particles. The dust particles were exposed to sulfuric acid vapor, to water vapor with and without the addition of ammonia gas, and heat using a thermodenuder operating at 250 °C. Size selected, quasi monodisperse particles with a mobility diameter of 300 nm were fed into LACIS and droplets grew on these particles such that each droplet contained a single particle. Temperature dependent frozen fractions of these droplets were determined in a temperature range between −40 °C ≤ T ≤ −28 °C. The pure ATD particles nucleated ice over a~broad temperature range with their freezing behavior being separated into two freezing branches characterized through different slopes in the frozen fraction vs. temperature curves. Coating the ATD particles with sulfuric acid resulted in the particles' IN potential significantly decreasing in the first freezing branch (T > −35 °C) and a slight increase in the second branch (T≤ −35 °C). The addition of water vapor after the sulfuric acid coating caused the disappearance of the first freezing branch and a strong reduction of the IN ability in the second freezing branch. The presence of ammonia gas during water vapor exposure had a negligible effect on the particles' IN ability compared to the effect of water vapor. Heating in the thermodenuder led to a decreased IN ability of the sulfuric acid coated particles for both branches but the additional heat did not or only slightly change the IN ability of the pure ATD and the water vapor exposed sulfuric acid coated particles. In other words, the combination of both sulfuric acid and water vapor being present is a main cause for the ice active surface features of the ATD particles being destroyed. A possible explanation could be the chemical transformation of ice active metal silicates to metal sulfates. From an atmospheric point of view, and here specifically the influences of atmospheric aging on the IN ability of dust particles, the strongly enhanced reaction between sulfuric acid and dust in the presence of water vapor, and the resulting significant reductions in IN potential, are certainly very interesting.
his study aims at a detailed characterization of an ultra-fine aerosol particle counting system for operation on board the Russian high altitude research aircraft M-55 "Geophysica" (maximum ceiling of 21 km). The COndensation PArticle counting Systems (COPAS) consists of an aerosol inlet and two dual-channel continuous flow Condensation Particle Counters (CPCs).
The aerosol inlet, adapted for COPAS measurements on board the M-55 "Geophysica", is described concerning aspiration, transmission, and transport losses. The counting efficiencies of the CPCs using the chlorofluorocarbon FC-43 as the working fluid are studied experimentally at two pressure conditions, 300 hPa and 70 hPa. Three COPAS channels are operated with different temperature differences between the saturator and the condenser block yielding smallest detectable particle sizes (dp50 – as 50% detection "cut off" diameters) of 6 nm, 11 nm, and 15 nm, respectively, at ambient pressure of 70 hPa. The fourth COPAS channel is operated with an aerosol heating line (250°C) for a determination of the non-volatile number of particles. The heating line is experimentally proven to volatilize pure H2SO4-H2O particles for a particle diameter (dp) range of 11 nm<dp<200 nm.
Additionally this study includes investigation to exclude auto-nucleation of the working fluid inside the CPCs. An instrumental inter-comparison (cross-correlation) has been performed for several measurement flights and mission flights in the Arctic and the Tropics are discussed. Finally, COPAS measurements are used for an aircraft plume crossing analysis.
A characterization of the ultra-fine aerosol particle counter COPAS (COndensation PArticle counting System) for operation on board the Russian high altitude research aircraft M-55 Geophysika is presented. The COPAS instrument consists of an aerosol inlet and two dual-channel continuous flow Condensation Particle Counters (CPCs) operated with the chlorofluorocarbon FC-43. It operates at pressures between 400 and 50 hPa for aerosol detection in the particle diameter (dp) range from 6 nm up to 1 micro m. The aerosol inlet, designed for the M-55, is characterized with respect to aspiration, transmission, and transport losses. The experimental characterization of counting efficiencies of three CPCs yields dp50 (50% detection particle diameter) of 6 nm, 11 nm, and 15 nm at temperature differences (DeltaT) between saturator and condenser of 17°C, 30°C, and 33°C, respectively. Non-volatile particles are quantified with a fourth CPC, with dp50=11 nm. It includes an aerosol heating line (250°C) to evaporate H2SO4-H2O particles of 11 nm<dp<200 nm at pressures between 70 and 300 hPa. An instrumental in-flight inter-comparison of the different COPAS CPCs yields correlation coefficients of 0.996 and 0.985. The particle emission index for the M-55 in the range of 1.4–8.4×10 16 kg -1 fuel burned has been estimated based on measurements of the Geophysika's own exhaust.
The exchange of heat, momentum, and mass in the atmosphere over mountainous terrain is controlled by synoptic-scale dynamics, thermally driven mesoscale circulations, and turbulence. This article reviews the key challenges relevant to the understanding of exchange processes in the mountain boundary layer and outlines possible research priorities for the future. The review describes the limitations of the experimental study of turbulent exchange over complex terrain, the impact of slope and valley breezes on the structure of the convective boundary layer, and the role of intermittent mixing and wave–turbulence interaction in the stable boundary layer. The interplay between exchange processes at different spatial scales is discussed in depth, emphasizing the role of elevated and ground-based stable layers in controlling multi-scale interactions in the atmosphere over and near mountains. Implications of the current understanding of exchange processes over mountains towards the improvement of numerical weather prediction and climate models are discussed, considering in particular the representation of surface boundary conditions, the parameterization of sub-grid-scale exchange, and the development of stochastic perturbation schemes.
Parabens and sorbic acid are commonly used as food preservatives due to their antimicrobial effect. However, their use in foods for infants and young children is not permitted in the European Union. Previous studies found these compounds in some gel-filled baby teethers, whereby parabens, which are well-known as endocrine disruptors, were identified in the polymer-based chewing surface consisting of ethylene-vinyl acetate (EVA). To assess the exposure of infants and young children to these products, the application of parabens in teethers should be thoroughly investigated. Therefore, the present study aimed to apply a representative migration test procedure combined with an accurate analytical method to examine gel-filled baby teethers without elaborate sample preparation, high costs, and long processing times. Accordingly, solid-phase extraction (SPE), in combination with a stable isotope dilution assay (SIDA) and subsequent gas chromatography–mass spectrometry (GC–MS) for analysis of methyl-, ethyl-, and n-propylparaben (MeP, EtP, and n-PrP), was found to be well-suited, with recoveries ranging from 93 to 99%. The study compared the release of these parabens from intact teether surfaces into water and saliva simulant under real-life conditions, with total amounts of detected parabens found to be in the range of 101–162 µg 100 mL−1 and 57–148 µg 100 mL−1, respectively. Furthermore, as a worst-case scenario, the release into water was examined using a long-term migration study.
Sulphuric acid, ammonia, amines, and oxidised organics play a crucial role in nanoparticle formation in the atmosphere. In this study, we investigate the composition of nucleated nanoparticles formed from these compounds in the CLOUD (Cosmics Leaving Outdoor Droplets) chamber experiments at CERN (Centre européen pour la recherche nucléaire). The investigation was carried out via analysis of the particle hygroscopicity, ethanol affinity, oxidation state, and ion composition. Hygroscopicity was studied by a hygroscopic tandem differential mobility analyser and a cloud condensation nuclei counter, ethanol affinity by an organic differential mobility analyser and particle oxidation level by a high-resolution time-of-flight aerosol mass spectrometer. The ion composition was studied by an atmospheric pressure interface time-of-flight mass spectrometer. The volume fraction of the organics in the particles during their growth from sizes of a few nanometers to tens of nanometers was derived from measured hygroscopicity assuming the Zdanovskii–Stokes–Robinson relationship, and compared to values gained from the spectrometers. The ZSR-relationship was also applied to obtain the measured ethanol affinities during the particle growth, which were used to derive the volume fractions of sulphuric acid and the other inorganics (e.g. ammonium salts). In the presence of sulphuric acid and ammonia, particles with a mobility diameter of 150 nm were chemically neutralised to ammonium sulphate. In the presence of oxidation products of pinanediol, the organic volume fraction of freshly nucleated particles increased from 0.4 to ~0.9, with an increase in diameter from 2 to 63 nm. Conversely, the sulphuric acid volume fraction decreased from 0.6 to 0.1 when the particle diameter increased from 2 to 50 nm. The results provide information on the composition of nucleated aerosol particles during their growth in the presence of various combinations of sulphuric acid, ammonia, dimethylamine and organic oxidation products.
Sulphuric acid, ammonia, amines, and oxidised organics play a crucial role in nanoparticle formation in the atmosphere. In this study, we investigate the composition of nucleated nanoparticles formed from these compounds in the CLOUD chamber experiments at CERN. The investigation is carried out via analysis of the particle hygroscopicity, ethanol affinity, oxidation state, and ion composition. Hygroscopicity was studied by a hygroscopic tandem differential mobility analyser and a cloud condensation nuclei counter, ethanol affinity by an organic differential mobility analyser and particle oxidation level by a high-resolution time-of-flight aerosol mass spectrometer. The ion composition was studied by an atmospheric pressure interface time-of-flight mass spectrometer. The volume fraction of the organics in the particles during their growth from sizes of a few nanometers to tens of nanometers was derived from measured hygroscopicity assuming the Zdanovski-Stokes-Robinson relationship, and compared to values gained from the spectrometers. The ZSR-relationship was also applied to obtain the measured ethanol affinities during the particle growth, which were used to derive the volume fractions of sulphuric acid and the other inorganics (e.g. ammonium salts). In the presence of sulphuric acid and ammonia, particles with a mobility diameter of 150 nm were chemically neutralised to ammonium sulphate. In the presence of oxidation products of pinanediol, the organic volume fraction of freshly nucleated particles increased from 0.4 to ∼0.9, with an increase in diameter from 2 to 63 nm. Conversely, the sulphuric acid volume fraction decreased from 0.6 to 0.1 when the particle diameter increased from 2 to 50 nm. The results provide information on the composition of nucleated aerosol particles during their growth in the presence of various combinations of sulphuric acid, ammonia, dimethylamine and organic oxidation products.
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.