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Mémoire géologique sur le Bassin d'Amiens, et en partienlier sur les Cantons Littoraux de la Somme
(1834)
We present simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS) for the Arctic winter 2002/2003. We integrated a Lagrangian denitrification scheme into the three-dimensional version of CLaMS that calculates the growth and sedimentation of nitric acid trihydrate (NAT) particles along individual particle trajectories. From those, we derive the HNO3 downward flux resulting from different particle nucleation assumptions. The simulation results show a clear vertical redistribution of total inorganic nitrogen ( ), with a maximum vortex average permanent removal of over 5ppb in late December between 500 and 550K and a corresponding increase of of over 2ppb below about 450K. The simulated vertical redistribution of is compared with balloon observations by MkIV and in-situ observations from the high altitude aircraft Geophysica. Assuming a globally uniform NAT particle nucleation rate of 7.8x10-6cm-3h-1 in the model, the observed denitrification is well reproduced.
In the investigated winter 2002/2003, the denitrification has only moderate impact (≤14%) on the simulated vortex average ozone loss of about 1.1ppm near the 460K level. At higher altitudes, above 600K potential temperature, the simulations show significant ozone depletion through -catalytic cycles due to the unusual early exposure of vortex air to sunlight.
Viertaljahresbericht der Kaiserlichen Hauptwetterwarte von Deutsch-Ostafrika. 1913, 2. Vierteljahr
(1913)
Beilage in: Deutsch-Ostafrikanische Zeitung. April 1913
In weiten Teilen zentraleuropäischer Mittelgebirge wird das anstehende Gestein durch periglaziäre Lagen verhüllt. Diese polygenetisch entwickelten Lockergesteinsdecken sind Schichten im geologisch-sedimentologischen Sinne und das Ausgangsmaterial der Bodenbildung. Ihre Substrateigenschaften, die durch pedogenetische Prozesse lediglich modifiziert werden, beeinflussen maßgeblich die ökologischen Standortbedingungen. Bisher waren nur sehr wenige Informationen zum Aufbau des oberflächennahen Untergrundes und der Böden des hessischen Spessarts vorhanden. Deswegen wurden im Rahmen dieser Arbeit in fünf Untersuchungsgebieten die Verbreitung und Eigenschaften der periglaziären Lagen und Böden mit Hilfe von umfangreichen Geländeuntersuchungen, Laboranalysen und mikromorphologischen Analysen erfasst. Die Ergebnisse belegen die Koppelung verschiedener Bodentypen mit bestimmten Schichtungskombinationen periglaziärer Lagen. Mit Hilfe von Dünnschliffanalysen wird die Wirksamkeit unterschiedlicher bodenbildender Prozesse in den Substraten näher beleuchtet. In lösslehmreichen, lithologisch dreigeteilten Lockergesteinsdecken sind Parabraunerden entwickelt. Die Untersuchung der Bodendünnschliffe offenbart jedoch, dass ein Teil der Tongehaltsdifferenz auf Sedimenteigenschaften der Deckschichten zurückzuführen ist: In der Mittellage finden sich Reste einer Paläobodenbildung in Form von Toncutanbruchstücken und tonigen Aggregaten. Teilweise wurde dieses Material auch bei der Formung der Hauptlage aufgearbeitet und als tonige Aggregate in die schluffige Matrix inkorporiert. Rezente Lessivierungsprozesse maskieren lediglich den schichtungsbedingten Tongehaltsunterschied und damit auch den Einfluss der Paläobodenreste auf die heutige Profilgestalt. In den höher gelegenen Gebieten des Gebirges stellen Braunerden aus Hauptlage über Basislage den am weitesten verbreiteten Bodentyp. Der Lösslehmanteil in der Hauptlage ist gegenüber den Profilen am Westrand des Spessarts deutlich geringer, lösslehmreiche Mittellagen kommen kaum vor. Mikromorphologische Analysen bestätigen Geländebefunde, nach denen sich die Verbraunung auf die lösslehmhaltigen Sedimente (Hauptlage, in die Basislage eingemischtes Hauptlagenmaterial) beschränkt. Lessivierungsprozesse dagegen sind nicht an bestimmte Schichten oder Substrate gebunden: Toneinspülungen sind in allen periglaziären Lagen nachweisbar und die Verlagerung findet schichtübergreifend statt. Sehr viele Bodenprofile zeigen Podsolierungstendenzen, trotzdem bleibt der Braunerdecharakter der Profile bestimmend. Stärkere Podsolierung beschränkt sich auf durch den Menschen in der Vergangenheit stark veränderte Substrate. Weitere Fragestellungen für die Dünnschliffuntersuchungen waren die qualitative Bewertung der Überformungsintensität periglaziärer Lagen durch bioturbate Prozesse sowie die Identifikation von Solumsedimenten, die granulometrisch kaum vom liegenden Hauptlagenmaterial zu unterscheiden sind.
Das Ziel dieser Studie ist es, die Möglichkeiten und Grenzen von hochauflösenden Klimaprojektionen in orographisch beeinflussten Gebieten an den Beispielen der europäischen Alpen und des Himalajas zu prüfen. Insbesondere wird die Fragestellung untersucht, ob beobachtete regionale Muster in den höher aufgelösten Daten besser wiedergegeben werden als in den antreibenden großskaligen Daten. Dazu werden regionale Klimasimulationen des COSMO-CLM Modells und Daten von zwei statistischen Regionalisierungsmethoden mit ERA40 Reanalysen sowie Daten des globalen Atmosphäre-Ozean Modells ECHAM5/MPIOM für verschiedene Parameter des Klimasystems verglichen. Ein Vergleich mit den Reanalysen anhand täglicher Niederschlagsstatistiken ergibt, dass die COSMO-CLM Niederschlagsdaten auf der 0.5° Skala vergleichbar sind mit ERA40 Niederschlägen und mit statistisch regionalisierten ERA40 Niederschlägen. Eine zusätzliche Fehlerkorrektur der COSMO-CLM Niederschläge liefert gute Ergebnisse. Dabei sind jedoch etwa 500 Regentage notwendig, um eine robuste Fehlerabschätzung zu gewährleisten. Für das südasiatische Gebiet ist eine realistische Wiedergabe des indischen Sommermonsuns (ISM) in den Modellen von hoher Relevanz. Betrachtet man nur die Mittelwerte und zeitlichen Variabilitäten von verschiedenen Indizes des ISM, so liefert das COSMO-CLM keinen Mehrwert im Vergleich zu den antreibenden Daten. Allerdings werden die räumlichen Strukturen von Niederschlag und vertikaler Windscherung, sowie die zeitliche Korrelation der modellierten Indizes gegenüber dem ECHAM5/MPIOM Modell verbessert. Die durchgeführten COSMO-CLM Projektionen für die Jahre 1960 bis 2100 zeigen negative Trends des ISM für die SRES Szenarien A2, A1B und B1. Die negativsten Trends sind dabei im Szenario A2 zu finden, gefolgt von A1B und B1. Fast keine Trends zeigen sich im commitment Szenario. Trotz großen zeitlichen Variabilitäten sind die Abnahmen in Niederschlagsmengen, ausgehender langwelliger Strahlung und Windscherung statistisch signifikant in großen Regionen des Simulationsgebietes. Für Nordwest-Indien weisen die Projektionen teilweise einen Rückgang der Monsunniederschläge von über 70% in 100 Jahren auf. Der Rückgang der Windscherung ist hauptsächlich auf Veränderungen in der oberen Troposphäre bei 200 hPa zurück zu führen. Während in den COSMO-CLM Projektionen alle Indizes des ISM synchrone Negativtrends aufweisen, sind die Trends für den Monsunregen über Indien im globalen ECHAM5/MPIOM Model positiv. Gemäß den Definitionen der verschiedenen Indizes, sind jedoch synchrone Trends wahrscheinlicher und das COSMO-CLM liefert zu den globalen ISM Projektionen ebenfalls einen Mehrwert. Insgesamt zeigen die Ergebnisse dieser Studie, dass das COSMO-CLM wertvolle regionale Zusatzinformationen zu den globalen Modellen in den beiden untersuchten Regionen liefert. Für die Einzugsgebiete der oberen Donau und des oberen Brahmaputra liefern die COSMO-CLM Projektionen einen signifikanten Anstieg der Temperatur für alle Jahreszeiten der Jahre 1960 bis 2100. Die Werte sind generell höher im Brahmaputragebiet, mit den größten Trends in der Region des tibetanischen Plateaus. Im Niederschlag zeigen die saisonalen Anteile ebenfalls klare Trends, beispielsweise eine Zunahme des Frühjahrsniederschlags im Einzugsgebiet der oberen Donau. Die größten Trends werden wiederum in der Region des tibetanischen Plateaus projiziert mit einem Anstieg von bis zu 50% in der Länge der Trockenperioden zwischen Juni und September und einem gleichzeitigen Anstieg von etwa 10% für die maximale Niederschlagsmenge an fünf aufeinander folgenden Tagen. Für die Region Assam in Indien, zeigen die Projektionen zudem eine Zunahme von 25% in der Anzahl der aufeinander folgenden trockenen Tage während der Monsunzeit
In this thesis, laboratory investigations have been conducted to investigate several processes occurring during the melt segregation (crystal settling and compaction processes), as well as during emplacement of plutons. With the help of three different sets of centrifuge experiments rates of these three magmatic processes have been evaluated. In the first series of the centrifuge experiments, the diapiric ascent of buoyant material from two source layers at different depths was studied. Through five models, the hypothesis of ascending diapirs was tested and it was demonstrated whether a rising diapir ascends straight upward or if its ascent might be deviated by another buoyant, softer – and consequently easier to travel through – layer which is located within the overburden strata. We were interested under which conditions they can be formed. For this purpose we placed perturbations on top of both the buoyant layers; either with a set-off of both the protrusions (for three of these experiments), or with both protrusion sitting directly on top of each other (for one of the experiments). In the first experiment, we omitted the perturbations, to test which pathways diapirs take which grow from natural Rayleigh-Taylor instabilities. Three others experiments differed in the viscosity contrast between the overburden and the buoyant material. Through the experimental runs, the effects of different overburden viscosities and perturbation positions on the number of the diapirs were observed. The modeling results show that two diapirs rising from the offset perturbations do not take the same pathway through the overburden layer. Rather, each diapir takes a different pathway, with the deeper diapir piercing through its overburden while rising, regardless if it was a buoyant layer or denser overburden layers. However, when the two perturbations were situated directly above each other in the different PDMS layers, this resulted in the formation of one big diapir rather than several smaller ones, and the overburden layer was less deformed than with offset perturbations. Diapiric structures as those derived from the models without perturbation and where the perturbation are offset occur within Great Kavir Basin (Iran), where numerous salt diapirs grew from several salt horizons, which show a similar spatial distribution. The resulting structure observed in the model where the two perturbations situated directly above each other, is close to what is observed in composite batholiths such as the Flasergranitoid Zone within the Bergsträßer Odenwald Crystalline Complex (Germany). The second series of models were aimed to study crystal settling within a magma. For this purpose experiments with an artificial magma of 30 vol% olivine in 70 vol% basaltic melt were conducted to elucidate the formation mechanisms and time scales of gravitational cumulates. Through the experiments, two physical processes have been observed: (i) purely mechanical compaction, and (ii) chemical compaction induced by dissolution and re-precipitation of settled crystals. The results reveals that the mechanical settling of the dense olivine suspension occurs at about 1/6 the speed of simple Stokes settling, and a sedimentation exponent n of 4.1 is found. Evidences of chemical compaction induced by dissolution and re-precipitation of settled crystals have been highlighted by a detailed analysis of the fine structure of olivine grain boundaries. This last has revealed (1) the presence of Ca, which is characteristic only for MORB-melt, at the interface of two adjacent Ol-grains even when no melt is present; (2) a not fully crystallized boundary layer between two adjacent olivine grains. The crystal size distribution curves and the grain size growth exponent n ~3.6 indicate that diffusion controlled Ostwald ripening is the dominant crystal growth mechanism in concentrated magmatic suspensions. Finally, the formation times in natural olivine adcumulates have been calculated. The last series of centrifuge experiments deals with the crystal-melt settling-floating mechanism in a system composed of natural two pyroxene gabbro. The results have revealed a vertical evolution of the major and trace elements in the melt phase. Then, a numerical modelling of the sedimentation process of the crystals has been made in order to describe the compaction evolution with time. In comparing the numerical simulation with the centrifuge modelling, the stratification of the compacted layer in the runs is reproduced in numerical models. Moreover, on the base of the numerical and centrifuge modelling, a sedimentation exponent describing a deviation of settling in concentrated suspensions from Stokes sedimentation has been evaluated. Finally, the numerical simulation is applied to the Muskox intrusion to estimate the formation time and the melt fraction evolution in using the hindered sedimentation model calculations.
IFLS-Journal. Nr. 4, 2003
(2003)
IFLS-Journal. Nr. 3, 2003
(2003)
IFLS-Journal. Nr. 2, 2002
(2002)
IFLS-Journal. Nr. 1, 2002
(2002)
In this study, I investigate the crustal and upper mantle velocity structure beneath the Rwenzori Mountains in western Uganda. This mountain range is situated within the western branch of the East African Rift and reaches altitudes of more than 5000 m. I use four different approaches that belong to the travel-time tomography method. The first approach is based on the isotropic tomographic inversion of local data, which contain information about 2053 earthquakes recorded by a network of up to 35 stations covering an area of 140×90 km2. The LOTOS-09 algorithm described here is used to realize this approach. The second approach is based on the anisotropic tomographic inversion of the same local dataset. This method employs the tomographic code ANITA, developed with my participation, which provides 3D anisotropic P and isotropic S velocity distributions based on P and S travel-times from local seismicity. For the P anisotropic model, four parameters for each parameterization cell are determined. This represents an orthorhombic anisotropy with one vertically-oriented predefined direction. Three of the parameters describe slowness variations along three horizontal orientations with azimuths of 0°, 60° and 120°, and one is a perturbation along the vertical axis. The third approach is based on tomographic inversion of the teleseismic data, which contain information about the traveltimes of P-waves coming from 284 teleseismic events recorded by the seismic network stations. The TELELOTOS code, which is my own modification of the LOTOS-09 algorithm, is used in this approach. The TELELOTOS code is designed to iteratively invert the local and/or teleseismic datasets. Finally, I present the results of the new tomographic approach, which is based on the simultaneous inversion of the joint local and teleseismic data. The simultaneous use of these datasets for the tomographic inversion has several advantages. In this case, the velocity structure in the study area can be resolved as deep as in the teleseismic approach. At the same time, in the upper part of the study volume, the resolution of the obtained models is as good as in the local tomography. The TELELOTOS algorithm is used to perform the joint tomographic inversion. Special attention is paid in this work to synthetic testing. A number of different synthetic and real data tests are performed to estimate the resolution ability and robustness of the obtained models. In particular, synthetic tests have shown that the results of the anisotropic tomographic inversion of the local data have to be considered as unsatisfactory. For all approaches used in this study, I present synthetic models that reproduce the same pattern of anomalies as that obtained by inverting the real data. These models are used to interpret the results and estimate the real amplitudes of the obtained anomalies. The obtained models exhibit a relatively strong negative P anomaly (up to -10%) beneath the Rwenzori Mountains. Low velocities are found in the northeastern part of the array at shallower depths and are most likely related to sedimentary deposits, while higher velocities are found beneath the eastern rift shoulder and are thought to be related to old cratonic crust. The presence of low velocities in the northwestern part of the array may be caused by a magmatic intrusion beneath the Buranga hot springs. Relatively low velocities were observed within the lower crust and upper mantle in the western and southern parts of the study area (beneath the rift valley and the entire length of the Rwenzori range). The higher amplitude of the low-velocity anomaly in the south can be related to the thinner lithosphere in the southern part of the Albertine rift. In the center of the study area, a small negative anomaly is observed, with the intensity increasing with depth. This anomaly is presumably related to a fluids rising up from a plume branch in the deeper part of the mantle. According to the interpretation of the local earthquake distribution, the Rwenzori Mountains are located between two rift valleys with flanks marked by normal faults. The Rwenzori block is bounded by thrust faults that are probably due to compression.
Flusssysteme im mediterranen Raum reagieren besonders sensitiv auf Veränderungen von Umweltbedingungen, z.B. durch Neotektonik, Klimaänderungen und Landnutzung. Geowissenschaftler der Goethe-Universität Frankfurt untersuchen in diesem Zusammenhang das Einzugsgebiet des Rio Palancia (Spanien), um über die Erstellung einer Sediment-Massenbilanzierung die Entwicklungsgeschichte des Systems zu erforschen. Zur Identifizierung und Quantifizierung verschiedener Sediment-Ablagerungstypen wurde das Georadarverfahren (GPR) eingesetzt. Ziel dieser Arbeit ist es, am Beispiel fluvialer Lockersedimente das Zustandekommen von Radargrammen noch besser zu verstehen und möglichst viel Information über den Untergrund aus einem Radargramm zu extrahieren. An 30 Standorten wurden GPR-Messungen durchgeführt und mit Geoelektrik und Rammkernsondierungen kombiniert. Die Einführung einer Bearbeitungs- und Auswertesystematik gewährleistet die Vergleichbarkeit von Radardaten unterschiedlicher Standorte. Als Besonderheit werden die Radargramme jeweils auf zwei verschiedene Arten bearbeitet und dargestellt, um sowohl Strukturen herauszuarbeiten als auch die – zumindest relative – Amplitudencharakteristik zu erhalten. Erst dadurch wird eine Auswertung mithilfe der erweiterten Radarstratigraphie-Methode möglich. Diese setzt sich aus der klassischen Radarstratigraphie und der neu entwickelten Reflexionsanalyse zusammen. Dabei werden systematisch Radar-Schichtflächen, Radareinheiten und Radarfazies ermittelt und anschließend die Amplitudengröße, die Polarität und die Breite der Reflexionen betrachtet. Die Radarstratigraphie liefert objektive Erkenntnisse über Form und Verlauf von Untergrundstrukturen, während mithilfe der Reflexionsanalyse Aussagen zu relativen Änderungen von Wassergehalt, Korngrößenverteilung und elektrischer Leitfähigkeit möglich sind. Mithilfe der Radarstratigraphie wurde die Radarantwort verschiedener Sediment-Ablagerungstypen im Untersuchungsgebiet verglichen. Die Radargramme zeigen unterschiedliche Zusammensetzungen von Radarfazies. Eine Unterscheidung und räumliche Abgrenzung verschiedener Ablagerungstypen mit GPR ist somit durchführbar. Die Dielektrizität des Mediums bestimmt, zusammen mit der elektrischen Leitfähigkeit, die Geschwindigkeit und Dämpfung der elektromagnetischen Welle sowie die Reflexionskoeffizienten. Um das Zustandekommen von Radargrammen im Detail nachvollziehen zu können, ist es notwendig, die Dielektrizitätskoeffizienten (DK) der untersuchten Sedimente zum Zeitpunkt der Messung zu kennen und die Abhängigkeit des DK von petrophysikalischen Parametern zu verstehen. Deshalb wurden Proben aus den Rammkernsondierungen entnommen. Im Labor wurden der Real- und Imaginärteil des DK im Radarfrequenzbereich (mit Schwerpunkt auf 200 MHz) in Abhängigkeit von Wassergehalt, Trockendichte, Korngrößenverteilung und Kalkgehalt mithilfe der Plattenkondensatormethode bestimmt. Der DK ist in erster Linie vom Wassergehalt abhängig. Es konnte eine für die Sedimente im Untersuchungsgebiet charakteristische Wassergehalts-DK-Beziehung ermittelt werden. Die resultierende Kurve ist gegenüber entsprechenden in der Fachliteratur zu findenden Beziehungen verschoben, was vermutlich auf die hohen Kalkgehalte der Proben zurückzuführen ist. Für trockene Sedimente wurde eine Korrelation des DK mit der Trockendichte festgestellt. Bei der Bestimmung der Absorptionskoeffizienten fiel auf, dass Proben mit hohem Tonanteil selbst bei geringen Wassergehalten außerordentlich hohe Dämpfungskoeffizienten aufweisen können. Die charakteristische Wassergehalts-DK-Beziehung wurde für Modellierungen von Radardaten genutzt, die dann mit Messdaten verglichen wurden. Über die Modellierung einer einzelnen Radarspur konnte die spezielle Charakteristik der entsprechenden gemessenen Spur erklärt werden, die durch den Einfluss einer dünnen Schicht zustande kommt, deren Mächtigkeit an der Grenze der theoretischen Auflösung für die verwendete Radarfrequenz liegt. Auf Basis der Erkenntnisse aus der erweiterten Radarstratigraphie an einem Radargramm auf fluvialen Lockersedimenten war es zudem möglich, ein komplettes Radargramm zu simulieren. Es gibt das gemessene Radargramm vereinfacht, aber in guter Übereinstimmung wieder. Die Georadarmethode erwies sich als sehr gut geeignet für die Untersuchung, Identifizierung und Quantifizierung fluvialer Sedimente im Palancia-Einzugsgebiet. Die im Rahmen dieser Doktorarbeit entwickelte erweiterte Radarstratigraphie-Methode stellt ein systematisches und weitgehend objektives Verfahren zur Auswertung von Radargrammen dar, das sich auch auf andere Untersuchungsgebiete übertragen lassen sollte. Durch Laboruntersuchungen wurde der Einfluss petrophysikalischer Parameter auf den DK bestimmt. Über die Modellierungen konnten die Ergebnisse großskaliger Geländemessungen mit denen kleinskaliger Labormessungen verknüpft werden. Die insgesamt gewonnenen Erkenntnisse tragen zu einem besseren Verständnis von Radargrammen bei.
The TTL is the transition layer between the tropical troposphere and stratosphere, and is the main region where tropospheric air enters the stratosphere. In this thesis different transport processes are studied by using in situ measurements of tracers. Long-lived tracers were measured with the High Altitude Gas Analyzer (HAGAR) on board the M55 Geophysica aircraft. The instrument was developed by the University of Frankfurt and measures the long-lived tracers CO2, N2O, CFC-12, CFC-11, H-1211, SF6, CH4 and H2 with two gas chromatographic channels and a CO2 sensor (LICOR). The measurements are supported by CO and O3 measurements of other instruments. Two campaigns were conducted to obtain measurements in the TTL: SCOUT-O3 (November/December 2005 in Darwin, Australia) and AMMA-SCOUT-O3 (August 2006 in Ouagadougou, Burkina Faso). After a general introduction of the thesis in chapters one and two, the third chapter describes the findings during this last campaign. Five local flights are analyzed to study the different transport processes that occur in the tropical tropopause layer above West-Africa: deep convection up to the level of main convective outflow, vertical mixing after overshooting of air in deep convection, horizontal inmixing from the extratropical lower stratosphere, and horizontal transport across the subtropical barrier. Main findings are that the TTL over West-Africa is mostly influenced by remote convection. The subtropical barrier is not a strong barrier but more a region of transition between the extratropical and the tropical stratosphere. Chapter 4 presents the results obtained during the SCOUT-O3 campaign. From the eight local flights the last four flights (051129, 051130a, 051130b, 051205) show enhanced values of ozone, CO and CO2 between 355 and 380 K potential temperature in comparison with the first four flights (051116, 051119, 051123, 051125). Horizontal inmixing from the extra-tropical stratosphere and influence of the local convective system Hector cannot explain the enhanced values of the two flights on 30 November Therefore, other possible explanations for these enhanced CO, CO2 and ozone levels are proposed. The first explanation is vertical mixing in the vicinity of the jet stream. However, the jet cannot explain the differences between the flights on 30 November and the flights on 29 November and 5 December. Another possible explanation is influence of polluted boundary layer air masses from the Indonesian region. Especially air sampled during the flights on November 30 crossed large parts of northern Indonesia between 8 and 10 days before the measurements. Convective uplift of biomass burning and other pollution plumes can transport CO and ozone precursors into the upper troposphere, where they can significantly enhance the ozone production. The last chapter deals with the vertical ascent rate in the TTL and uses measurements of both the SCOUT-O3 and AMMA-SCOUT-O3 campaign as well as data from previous aircraft campaigns (TROCCINOX and APE-THESEO). Time scales and residence times for mean vertical transport in the background TTL are estimated for different seasons and over different geographic regions using in situ observations of CO2 and long-lived tracers. The vertical transport time scales are constrained using the seasonal variation of CO2 in the tropical troposphere as a “tracer clock” for vertical ascent. Two methods are applied to calculate the residence time in the layer between 360 and 390 K potential temperature. The first method uses the slope of the CO2 index, the second method fits the CO2 index directly to the measurements assuming a constant ascent rate. The first method yields residence times for Australia,West Africa, and Brazil of the same order, 35-45 days to 380 K and 50 days to 390 K (where no value can be derived for Australia as the slope is changing approximately one month before the campaign). For APE-THESEO, the method does not yield reasonable results. The best estimates using the second method show moderate residence times between 360 and 390 K of 60±25 days SCOUT-O3 (NH autumn) and 43±8 days for AMMA/SCOUT-O3 (NH summer). These results agree well with the results calculated using the first method. For APE-THESEO and TROCCINOX the best fits yield shorter residence times of 23±7 and 40±10 days, respectively, both during winter. These results correspond well to the expectations based on the seasonal variation of the Brewer-Dobson circulation.
Im Rahmen dieser Dissertation wurde die spätpleistozäne und holozäne Landschaftsentwicklung im Umfeld der im Tal des Wadis Chuera in Nordsyrien liegenden bronzezeitlichen Siedlung Tell Chuera untersucht. Durch die Kombination von hochgenauen Vermessungen, Satellitenbildauswertungen und Untersuchungen der Wadisedimente konnten mehrere flussgeschichtliche Entwicklungsphasen erarbeitet und in einen chronostratigraphischen Rahmen eingeordnet werden. Über ein grobsandig-kiesiges System eines verzweigten Flusses wurden mindestens bis ins Obere Pleistozän mächtige Kieslagen im Untersuchungsgebiet sedimentiert. Innerhalb einer fossilen Rinne abgelagerte lössähnliche Sedimente, welche die Kiesfolgen partiell überlagern, konnten relativchronologisch ins Obere Pleistozän gestellt werden und dokumentieren vermutlich eine trockene Phase. Durch die mit scharfer Diskordanz über den Kiesen abgelagerten pelitischen Hochflutsedimente wird ein abrupter flussdynamischer Umbruch von dem eines ursprünglich verzweigten Flusses zu dem eines mäandrierenden Flusses mit Hochflutsedimentation nachgewiesen. IRSL-Datierungen stellen den Beginn der Ablagerung der Hochflutsedimente ins letzte Glazial. Der größte Teil der Sedimente wurde jedoch im frühen und mittleren Holozän (ca. 9 und 5 kaBP) abgelagert, so dass zu Beginn der Hauptsiedlungsphase am Tell Chuera (3. Jahrtausend v.Chr.) die Oberfläche der Überschwemmungsebene ihr heutiges Niveau nahezu erreicht hatte. Bis dahin führten großflächige Überschwemmungen zur Hochflutsedimentation in der Aue. Ein erneuter Wechsel der fluvialen Geomorphodynamik und der Sedimentationsverhältnisse zeigt sich darin, dass die letzten ca. 5000 Jahre keine nennenswerte Sedimentation in der Hochflutebene zu verzeichnen war. Es kam zu einer bis heute stattfindenden, lateralen Verlagerung der Mäander des Wadis und damit der Aufarbeitung von Teilen der Kiese und Hochflutsedimente. Siedlungsspuren im Wadiverlauf weisen auf eine Periodizität des Abflusses des Wadis Chuera zwischen etwa 4.7 und 4.2 kaBP hin. Die Theorie einer verstärkten Akkumulation von Kolluvien der Rahmenhöhen im Wadital als direkte Folge eines steigenden Siedlungsdrucks während der Hauptsiedlungsphase konnte widerlegt werden. Vielmehr handelt es sich bei den vermeintlichen Kolluvien um fluvial aufgearbeitete Hochflutsedimente. Anthropogene Eingriffe in den Landschaftshaushalt lassen sich in Form von Kalkkrustensteinbrüchen und einem komplexen Wegenetz nachweisen.
Am 7. September 1981 wurde der Raum Bellersen von einem heftigen Unwetter mit Gewitter und sintflutartigen Regenfällen heimgesucht. Das Unwetter richtete einen nicht unbeträchtlichen Schaden im Dorf und in der Feldmark an. Es bot aber auch Gelegenheit, den Einfluß solcher relativ seltener und daher episodisch zu bezeichnenden extremen Niederschlagsereignisse auf die Formung der Erdoberfläche zu erkennen. An dieser Stelle soll an einem Einzelbeispiel gezeigt werden, wie sich die Oberflächenformen im Talgrund von Trockentälern weiterentwickeln können. Genaue quantitative Angaben über den gefallenen Niederschlag lassen sich leider nicht machen, da für das angesprochene Einzugsgebiet keine Messungen vorliegen.
An eclogite barometer has profound importance in the study of upper mantle processes and potential application to diamond prospecting. Studies on the partitioning of Li between clinopyroxene (cpx) and garnet (grt) in natural samples have shown that this particular element is very sensitive to changes in pressure and could be calibrated as the barometer demanded for bimineralic eclogites. Experiments were performed from 4 to 13 GPa and 1100 to 1400°C in the CMAS (CaO, MgO, Al2O3, SiO2) system with Li added as Li3PO4 to quantify this pressure dependence into a barometer expressed in the following equation: P= (0.00255*T-lnKd)/0.2351 where P is in GPa, T is in °C and Kd is defined as the partition coefficient of Li (in ppm) between clinopyroxene and garnet. The experimental pressures are reproduced to ± 0.38 GPa (1σ) by this equation. This barometer is strictly applicable only to CMAS. Experiments at 1300°C, 8-12 GPa showed that Henry’s Law is fulfilled for Li partitioning between cpx and grt in the concentration range of approximately 0.01 – 1 wt% Li. Direct application of the equation to experiments in natural systems performed at 1300°C from 4 GPa to 13 GPa consistently overestimates pressures by approximately 2 GPa. Our previous experiments in the system CaO-MgO-Al2O3-SiO2 + Li3PO4 showed that the partitioning of Li between garnet and clinopyroxene is pressure dependent in eclogitic bulk compositions. This supports experimentally the hypothesis of Seitz et al. (2003), based on the analysis of Li in eclogitic xenoliths and inclusions in diamond, that the partitioning of this particular element between clinopyroxene and garnet is very sensitive to changes in pressure and could be calibrated as a barometer for bimineralic eclogites. In order to calibrate this pressure dependence into a barometer, experiments were performed in natural systems using starting materials sourced from a well preserved eclogitic xenolith from the Roberts Victor kimberlite pipe (South Africa) to extrapolate our findings in CMAS to natural systems. Sixteen multianvil experiments were performed from 4-13 GPa and 1100-1500°C. Our findings reinforced the general trend we observed in the CMAS system, that KdLi cpx-grt for Li decreases with increasing P, and that at P ≥ 12 GPa, garnet is able to incorporate more Li than clinopyroxene. Multiple linear regression was applied to our experimental results to create the barometer: P = (0.000963*T – ln KdLi cpx-grt + 1.581) / 0.252 Where P is pressure in GPa, T is temperature in °C and KdLi cpx-grt is defined as the partitioning coefficient of Li obtained by dividing the concentration of Li in cpx by the concentration of Li in garnet. This barometer reproduces the experimental conditions to ± 0.2 GPa. It is applicable to eclogitic xenoliths, to garnet pyroxenites and to peridotitic and eclogitic inclusions in diamond. Application of the barometer to diamond bearing xenoliths results in pressures in the diamond stability field. Clinopyroxene is easily corrupted in xenoliths and also preferentially takes in Li during short lived metasomatic processes. Care must be taken therefore to analyse primary, unaltered clinopyroxene. Our preliminary application to natural samples shows that the barometer can be applied beyond the experimental range to pressures down to 3 GPa. Seventeen eclogitic xenoliths were chosen from a sample set of greater than 200 for their fresh microscopic and macroscopic appearance and were analyzed for Li content in coexisting garnet (grt) and clinopyroxene (cpx). These samples can be subdivided into two groups on the basis of Mg in cpx (cpfu: cations per formula unit, based on 6 oxygens): Group 1 with Mg > 0.75, and Group 2 with Mg < 0.75. Group 1 xenoliths show lower Li contents in both grt and cpx compared to Group 2. The Li barom ter calibrated in Hanrahan et al. (2009b)/Chapter 3 was applied to these samples as well as available literature data to obtain pressures of provenance - Group 2 xenoliths often provide pressures that appear unrealistic for eclogitic xenoliths. In light of observed crystal chemical relations in the natural samples, a new fitting procedure was applied to the experimental data presented in Chapter 3. This new fit appears to be more realistic than the previous fit, although a strong relationship with Mg# remains present, suggesting that Li-barometry is, at present, only applicable to Mg-rich eclogites. Inclusions in diamond, with the exception of eclogitic inclusions of coexisting majorite and cpx, often yield pressures that are inconsistent with the pressures required for diamond formation. Although an interesting observation when comparing all of the data is that inclusions in diamond have significantly higher average Li concentrations compared to xenoliths, which suggests that Li is highly present in the fluids from which diamonds form in the mantle, an observation which was previously made for the deep mantle as a result of high Li in ferropericlase inclusions in diamond (Seitz et al. 2003).
During a 4-week run in October–November 2006, a pilot experiment was performed at the CERN Proton Synchrotron in preparation for the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment, whose aim is to study the possible influence of cosmic rays on clouds. The purpose of the pilot experiment was firstly to carry out exploratory measurements of the effect of ionising particle radiation on aerosol formation from trace H2SO4 vapour and secondly to provide technical input for the CLOUD design. A total of 44 nucleation bursts were produced and recorded, with formation rates of particles above the 3 nm detection threshold of between 0.1 and 100 cm -3 s -1, and growth rates between 2 and 37 nm h -1. The corresponding H2O concentrations were typically around 106 cm -3 or less. The experimentally-measured formation rates and htwosofour concentrations are comparable to those found in the atmosphere, supporting the idea that sulphuric acid is involved in the nucleation of atmospheric aerosols. However, sulphuric acid alone is not able to explain the observed rapid growth rates, which suggests the presence of additional trace vapours in the aerosol chamber, whose identity is unknown. By analysing the charged fraction, a few of the aerosol bursts appear to have a contribution from ion-induced nucleation and ion-ion recombination to form neutral clusters. Some indications were also found for the accelerator beam timing and intensity to influence the aerosol particle formation rate at the highest experimental SO2 concentrations of 6 ppb, although none was found at lower concentrations. Overall, the exploratory measurements provide suggestive evidence for ion-induced nucleation or ion-ion recombination as sources of aerosol particles. However in order to quantify the conditions under which ion processes become significant, improvements are needed in controlling the experimental variables and in the reproducibility of the experiments. Finally, concerning technical aspects, the most important lessons for the CLOUD design include the stringent requirement of internal cleanliness of the aerosol chamber, as well as maintenance of extremely stable temperatures (variations below 0.1 °C)
In order to quantitatively analyse the chemical and dynamical evolution of the polar vortex it has proven extremely useful to work with coordinate systems that follow the vortex flow. We propose here a two-dimensional quasi-Lagrangian coordinate system {X i, delta X i}, based on the mixing ratio of a long-lived stratospheric trace gas i, and its systematic use with i = N2O, in order to describe the structure of a well-developed Antarctic polar vortex. In the coordinate system {X i, delta X i} the mixing ratio X i is the vertical coordinate and delta X i = X i(theta) - X i vort(theta) is the meridional coordinate (X i vort(theta) being a vertical reference profile in the vortex core). The quasi-Lagrangian coordinates {X i, delta X i} persist for much longer time than standard isentropic coordinates, potential temperature theta and equivalent latitude Phi e, do not require explicit reference to geographic space, and can be derived directly from high-resolution in situ measurements. They are therefore well-suited for studying the evolution of the Antarctic polar vortex throughout the polar winter with respect to the relevant chemical and microphysical processes. By using the introduced coordinate system {X N2O, delta X N2O} we analyze the well-developed Antarctic vortex investigated during the APE-GAIA (Airborne Polar Experiment – Geophysica Aircraft in Antarctica – 1999) campaign (Carli et al., 2000). A criterion, which uses the local in-situ measurements of X i=X i(theta) and attributes the inner vortex edge to a rapid change (delta-step) in the meridional profile of the mixing ratio X i, is developed to determine the (Antarctic) inner vortex edge. In turn, we suggest that the outer vortex edge of a well-developed Antarctic vortex can be attributed to the position of a local minimum of the X H2O gradient in the polar vortex area. For a well-developed Antarctic vortex, the delta X N2O-parametrization of tracer-tracer relationships allows to distinguish the tracer inter-relationships in the vortex core, vortex boundary region and surf zone and to examine their meridional variation throughout these regions. This is illustrated by analyzing the tracer-tracer relationships X i : X N2O obtained from the in-situ data of the APE-GAIA campaign for i = CFC-11, CFC-12, H-1211 and SF6. A number of solitary anomalous points in the CFC-11 : N2O correlation, observed in the Antarctic vortex core, are interpreted in terms of small-scale cross-isentropic dispersion.
Östlich des Rwenzori Gebirges im Westen Ugandas wurden magnetotellurische Messungen durchgeführt. An 23 Stationen wurden Übertragungsfunktionen und Phasen Tensor Elemente zwischen den gemessenen magnetischen- und tellurischen Feldern im Periodenbereich von 10s bis 10000s geschätzt. Die Übertragungsfunktionen deuten eine komplexe drei dimensionale Leitfähigkeitsstruktur innerhalb der Kruste an, insbesondere in der Verbindungszone zwischen dem Rwenzori Gebirge und der östlichen Riftschulter. In dieser Arbeit wird eine alternative Darstellung der Phasen Tensor Ellipsen als Balken eingeführt. Für Perioden größer 100s zeigen die maximalen Phasen der Phasen Tensor Balken aller Stationen einheitlich in SSW-NNE und die Phasen Tensor Invarianten f min und f max weisen eine Differenz von mindestens 20° auf. Dieses auffällige Verhalten und die kleinen vertikalen magnetischen Feldr im gleich Periodenbereich kann mit einer anisotropen Leitfähigkeit in einer Tiefenbereich zwischen 30-50km mit der gut leitenden Richtung senkrecht zur Riftachse erklärt werden. Die Anisotropie könnte ihren Ursprung in orientierten Olivien Kristallen im oberen Mantel haben, wobei die Orientierungsrichtung mit der Delamination der Unterkruste unter den Rwenzoris zusammen hängen kann. Eine gut leitende Zone süd-östlich der Rwenzoris wurde in 15km Tiefe gefunden, die mit einer seismischen low velocity zone übereinstimmt und partielle Schmelzen innerhalb der Kruste andeutet. An allen Stationen steigt die minimale Phase bei der Periode 200s über 45° und zeigt einen Anstieg der elektrischen Leitfähigkeit unterhalb der Lithosphäre an.
Die Magnesitlagerstätte Beli Kamen, die so nachdem Berge im Dorfe Strezovce, unweit von Novo Brdo, benannt wurde, war der Gegenstand unserer Untersuchungen fünf volle Jahre hindurch - von Juni 1956 bis Juli 1961. In der ersten Phase dieses Zeitabschnittes war es unsere Aufgabe, alle Untersuchungsarbeiten in diesem bisher ungenügend bearbeiteten Objekte, von dem seitens unserer Wirtschaft und unserer Forscher viel erwartet wurde - anzusetzen und durchzuführen. Die Ergebnisse dieser Arbeiten wurden in unserem Elaborat (1959), mit einer ausführlichen Dokumentation über die allgemeine Charakteristik und praktischen Wert der untersuchten Magnesitmasse dargestellt. In der zweiten Phase - in Zusammenhang mit der Planung und Finansieurng wissenschaftlicher Arbeiten seitens des Rates für wissenschaftliche Arbeit, V. R. Serbien, und seitens des Geologischen Forschungsinstitutes, V. R. Serbien, wurden die Untersuchungen über die Frage des Auftretens des Magnesit in der Lagerstätte Beli Kamen fortgesetzt, wobei das Untersuchungsgebiet bedeutend erweitert und eingehender erfasst wurde. Unumgänglich nötige nachträgliche Begehungen und neue Untersuchungen wurden von der Tatsache diktiert, dass eine wissenschaftliche Bearbeitung solcher Lagerstätten, insbesondere deren Entstehung, bedeutend zahlreichere Angaben forderte, als es alle durchgeführten, von praktischen Standpunkt aus ansomsten zufriedenstellende und umfangreiche Untersuchungsarbeiten boten. So musste in der zweiten Phase, von 1958 bis 1961 mehrmals das Terrain begangen werden und dabei stiessen wir auf neue Probleme, allmählich das Untersuchungsgebiet immer mehr erweiternd. Ausserdem war es nötig, gleichzeitig die umfangreiche Probensammlung, die nicht nur Magnesit, sondern auch verschiedenartiges taubes Material enthielt, laboratorisch zu bearbeiten. Die Ergebnisse dieser vervollständigten, vor allem wissenschfatlichen Behandlung der Magnesitlagerstätte Beli Kamen und deren Nebengesteine, sowie natürlich auch jene aus dem erwähnten Elaborat (1959), werden nun in dieser Studie dargestellt. Wir sind der Ansicht, dass viele Einzelheiten dieser Studie, die wie vorliegend geordnet ist und in den Hauptzügen ausreichend bearbeitet ist, von besonderem InLeresse für die Fachwelt sein wird, um so mehr, da sich dieselbe tatsächlich auf eine ganz besonderes, in der Welt seltenes Magnesitvorkommen handelt. Von den insgesamt gewonnen Ergebnissen der wissenschaftlichen Bearbeitung der Lagerstätte Beli Kamen wollen wir nur die allgemeinsten und ausgeprägtesten hervorheben.
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.
Atmospheric observation-based global SF6 emissions - comparison of top-down and bottom-up estimates
(2009)
Emissions of sulphur hexafluoride (SF6), one of the strongest greenhouse gases on a per molecule basis, are targeted to be collectively reduced under the Kyoto Protocol. Because of its long atmospheric lifetime (≈3000 years), the accumulation of SF6 in the atmosphere is a direct measure of its global emissions. Examination of our extended data set of globally distributed high-precision SF6 observations shows an increase in SF6 abundance from near zero in the 1970s to a global mean of 6.7 ppt by the end of 2008. In-depth evaluation of our long-term data records shows that the global source of SF6 decreased after 1995, most likely due to SF6 emission reductions in industrialised countries, but increased again after 1998. By subtracting those emissions reported by Annex I countries to the United Nations Framework Convention of Climatic Change (UNFCCC) from our observation-inferred SF6 source leaves a surprisingly large gap of more than 70–80% of non-reported SF6 emissions in the last decade.
Emissions of sulphur hexafluoride (SF6), one of the strongest greenhouse gases on a per molecule basis, are targeted to be collectively reduced under the Kyoto Protocol. Because of its long atmospheric lifetime (estimated as 800 to 3200 years), the accumulation of SF6 in the atmosphere is a direct measure of its global emissions. Examination of our extended data set of globally distributed high-precision SF6 observations shows an increase in SF6 abundance from near zero in the 1970s to a global mean of 6.7 ppt by the end of 2008. In-depth evaluation of our long-term data records shows that the global source of SF6 decreased after 1995, most likely due to SF6 emission reductions in industrialised countries, but increased again after 1998. By subtracting those emissions reported by Annex I countries to the United Nations Framework Convention of Climatic Change (UNFCCC) from our observation-inferred SF6 source leaves a surprisingly large gap of more than 70–80% of non-reported SF6 emissions in the last decade. This suggests a strong under-estimation of emissions in Annex I countries and underlines the urgent need for independent atmospheric verification of greenhouse gases emissions accounting.
Samples of freshly fallen snow were collected at the high alpine research station Jungfraujoch, Switzerland, during the Cloud and Aerosol Characterization Experiments (CLACE) 5 in February and March 2006. Sampling was carried out on the Sphinx platform. Headspace-solid-phase-dynamic extraction (HS-SPDE) combined with gas chromatography/mass spectrometry (GC/MS) was used to quantify C6–C10 n-aldehydes in the snow samples. The most abundant n-aldehyde was n-hexanal (median concentration 1.324 micro g L -1) followed by n-nonanal, n-decanal, n-octanal and n-heptanal (median concentrations 1.239, 0.863, 0.460, and 0.304 micro g L -1, respectively). A wide range of concentrations was found among individual snow samples, even for samples taken at the same time. Higher median concentrations of all n-aldehydes were observed when air masses reached Jungfraujoch from the north-northwest in comparison to air masses arriving from the southeast-southwest. Results suggest that the n-aldehydes detected most likely are of direct and indirect biogenic origin, and that they entered the snow through the particle phase.
Both, gas and particle scavenging contribute to the transport of organic compounds by ice crystals in the troposphere. To simulate these processes an experimental setup was developed to form airborne ice crystals under atmospheric conditions. Experiments were performed in a wall independent reactor (WIR) installed in a walk-in cold chamber maintained constantly at -20°C. Aerosol particles were added to the carrier gas of ambient air by an aerosol generator to allow heterogeneous ice formation. Temperature variations and hydrodynamic conditions of the WIR were investigated to determine the conditions for ice crystal formation and crystal growth by vapour deposition. In detail, the dependence of temperature variations from flow rate and temperature of the physical wall as well as temperature variations with an increasing reactor depth were studied. The conditions to provide a stable aerosol concentration in the carrier gas flow were also studied. The temperature distribution inside the reactor was strongly dependent on flow rate and physical wall temperature. At an inlet temperature of -20°C, a flow rate of 30 L•min exp -1 and a physical wall temperature of +5°C turned out to provide ideal conditions for ice formation. At these conditions a sharp and stable laminar down draft "jet stream" of cold air in the centre of the reactor was produced. Temperatures measured at the chamber outlet were kept well below the freezing point in the whole reactor depth of 1.0 m. Thus, melting did not affect ice formation and crystal growth. The maximum residence time for airborne ice crystals was calculated to at 40 s. Ice crystal growth rates increased also with increasing reactor depth. The maximum ice crystal growth rate was calculated at 2.82 mg• exp -1. Further, the removal efficiency of the cleaning device for aerosol particles was 99.8% after 10 min. A reliable particle supply was attained after a preliminary lead time of 15 min. Thus, the minimum lead time was determined at 25 min. Several test runs revealed that the WIR is suitable to perform experiments with airborne ice crystals.
Within the present study the occurrence and fate of the organophosphorus flame retardants and plasticizers tris(2-chloroethyl) phosphate (TCEP), tris(2-chloro-1-methylethyl) phosphate (TCPP), tris(1,3-dichloro-2-propyl) phosphate (TDCP), tris(2-butoxyethyl) phosphate (TBEP), tri-iso-butyl phosphate (TiBP), and tri-n-butyl phosphate (TnBP) in precipitation, lake water, surface runoff and groundwater from urban and remote areas in Germany was investigated between June 2007 and October 2009. 255 samples of precipitation, 210 samples of lentic surface water and 72 samples of groundwater were analyzed for the six organophosphates (OPs) by solid phase extraction followed by gas chromatography-mass spectrometry. The research focused on aspects concerning (1) the atmospheric washout of OPs by precipitation, (2) the temporal variation of OP concentrations in precipitation and in lentic surface waters as well as (3) the pollution of groundwater by OPs. The results of the study emphasize the importance of precipitation as an all-season entry-pathway for OPs in the aquatic environment, particularly in densely populated urban environments with high traffic volume and abundant usage of flame-protected products. No seasonal trends were observed for all analytes in precipitation at the urban sampling site. TCPP dominated in all precipitation and storm water holding tank (SWHT) water samples with maximum levels exceeding 1 µg/L. An accumulation of OPs deposited in SWHTs was observed with concentrations often exceeding those observed in wet precipitation. Median concentrations of TCPP (880 ng/L), TDCP (13 ng/L), and TBEP (77 ng/L) at the urban SWHT were more than twice as high as those measured at the urban precipitation sampling site (403 ng/L, 5 ng/L, 21 ng/L) located close to the SWHT. OP levels in more remote lakes were often below or close to the limits of quantitation (LOQ). Nevertheless, TCPP was the substance with the highest median concentration in rural volcanic lakes (7–18 ng/L) indicating an atmospheric transport of the compound. At urban lakes the median OP concentrations were in the range of 23–61 ng/L (TCEP), 85–126 ng/L (TCPP), <LOQ–53 ng/L (TBEP), 8–10 ng/L (TiBP), and 17–32 ng/L (TnBP). In laboratory experiments, TBEP, TiBP, and TnBP were photochemically degraded in spiked lake water samples upon exposure to sunlight. In the SWHT a seasonal trend with decreasing concentrations in summer/autumn was evident for TiBP and TnBP but not for the chlorinated OPs. The decreasing concentrations can be explained by in-lake photodegradation. Results have also shown that the occurrence of OPs in groundwater is depending on the anthropogenic impact during groundwater recharge/natural replenishment. Infiltration of precipitation was found to be no important entry-pathway for OPs into aquifers at rural sites. Highest OP concentrations (>0.1 µg/L) were determined in groundwater polluted by percolating leachate from contaminated sites or groundwater recharged via bank filtration of OP-loaded recipients. Concentrations of TCEP, TCPP, TiBP and TnBP in groundwater decreased rapidly (89–97%) during bank filtration with increasing distance from the recipient due to adsorption processes and/or biotransformation. Although TCEP and TCPP are stable within the aquifer, they are not suitable as conservative organic tracers in groundwater.
Nucleation experiments starting from the reaction of OH radicals with SO2 have been performed in the IfT-LFT flow tube under atmospheric conditions at 293±0.5 K for a relative humidity of 13–61%. The presence of different additives (H2, CO, 1,3,5-trimethylbenzene) for adjusting the OH radical concentration and resulting OH levels in the range (4–300) ×105 molecule cm -3 did not influence the nucleation process itself. The number of detected particles as well as the threshold H2SO4 concentration needed for nucleation was found to be strongly dependent on the counting efficiency of the used counting devices. High-sensitivity particle counters allowed the measurement of freshly nucleated particles with diameters down to about 1.5 nm. A parameterization of the experimental data was developed using power law equations for H2SO4 and H2O vapour. The exponent for H2SO4 from different measurement series was in the range of 1.7–2.1 being in good agreement with those arising from analysis of nucleation events in the atmosphere. For increasing relative humidity, an increase of the particle number was observed. The exponent for H2O vapour was found to be 3.1 representing an upper limit. Addition of 1.2×1011 molecule cm -3 or 1.2×1012 molecule cm -3 of NH3 (range of atmospheric NH3 peak concentrations) revealed that NH3 has a measureable, promoting effect on the nucleation rate under these conditions. The promoting effect was found to be more pronounced for relatively dry conditions, i.e. a rise of the particle number by 1–2 orders of magnitude at RH = 13% and only by a factor of 2–5 at RH = 47% (NH3 addition: 1.2×1012 molecule cm -3). Using the amine tert-butylamine instead of NH3, the enhancing impact of the base for nucleation and particle growth appears to be stronger. Tert-butylamine addition of about 1010 molecule cm -3 at RH = 13% enhances particle formation by about two orders of magnitude, while for NH3 only a small or negligible effect on nucleation in this range of concentration appeared. This suggests that amines can strongly influence atmospheric H2SO4-H2O nucleation and are probably promising candidates for explaining existing discrepancies between theory and observations.
We report the first measurements of 1,1,1,2,3,3,3-heptafluoropropane (HFC-227ea), a substitute for ozone depleting compounds, in remote regions of the atmosphere and present evidence for its rapid growth. Observed mixing ratios ranged from below 0.01 ppt in deep firn air to 0.59 ppt in the northern mid-latitudinal upper troposphere. Firn air samples collected in Greenland were used to reconstruct a history of atmospheric abundance. Year-on-year increases were deduced, with acceleration in the growth rate from 0.026 ppt per year in 2000 to 0.057 ppt per year in 2007. Upper tropospheric air samples provide evidence for a continuing growth until late 2009. Fur- thermore we calculated a stratospheric lifetime of 370 years from measurements of air samples collected on board high altitude aircraft and balloons. Emission estimates were determined from the reconstructed atmospheric trend and suggest that current "bottom-up" estimates of global emissions for 2005 are too high by more than a factor of three.
We report the first measurements of 1,1,1,2,3,3,3-heptafluoropropane (HFC-227ea), a substitute for ozone depleting compounds, in air samples originating from remote regions of the atmosphere and present evidence for its accelerating growth. Observed mixing ratios ranged from below 0.01 ppt in deep firn air to 0.59 ppt in the current northern mid-latitudinal upper troposphere. Firn air samples collected in Greenland were used to reconstruct a history of atmospheric abundance. Year-on-year increases were deduced, with acceleration in the growth rate from 0.029 ppt per year in 2000 to 0.056 ppt per year in 2007. Upper tropospheric air samples provide evidence for a continuing growth until late 2009. Furthermore we calculated a stratospheric lifetime of 370 years from measurements of air samples collected on board high altitude aircraft and balloons. Emission estimates were determined from the reconstructed atmospheric trend and suggest that current "bottom-up" estimates of global emissions for 2005 are too high by a factor of three.
A comprehensive evaluation of seasonal backward trajectories initialized in the northern hemisphere lowermost stratosphere (LMS) has been performed to investigate the factors that determine the temporal and spatial structure of troposphere-to-stratosphere-transport (TST) and it’s impact on the LMS. In particular we explain the fundamental role of the transit time since last TST (tTST) for the chemical composition of the LMS. According to our results the structure of the LMS can be characterized by a layer with tTST<40 days forming a narrow band around the local tropopause. This layer extends about 30K above the local dynamical tropopause, corresponding to the extratropical tropopause transition layer (ExTL) as identified by CO. The LMS beyond this layer shows a relatively well defined separation as marked by an aprupt transition to longer tTST indicating less frequent mixing and a smaller fraction of tropospheric air. Thus the LMS constitutes a region of two well defined regimes of tropospheric influence. These can be characterized mainly by different transport times from the troposphere and different fractions of tropospheric air. Carbon monoxide (CO) mirrors this structure of tTST due to it’s finite lifetime on the order of three months. Water vapour isopleths, on the other hand, do not uniquely indicate TST and are independent of tTST, but are determined by the Lagrangian Cold Point (LCP) of air parcels. Most of the backward trajectories from the LMS experienced their LCP in the tropics and sub-tropics, and TST often occurs 20 days after trajectories have encountered their LCP. Therefore, ExTL properties deduced from CO and H2O provide totally different informations on transport and particular TST for the LMS.
Two different single particle mass spectrometers were operated in parallel at the Swiss High Alpine Research Station Jungfraujoch (JFJ, 3580 m a.s.l.) during the Cloud and Aerosol Characterization Experiment (CLACE 6) in February and March 2007. During mixed phase cloud events ice crystals from 5–20 micro m were separated from larger ice aggregates, non-activated, interstitial aerosol particles and supercooled droplets using an Ice-Counterflow Virtual Impactor (Ice-CVI). During one cloud period supercooled droplets were additionally sampled and analyzed by changing the Ice-CVI setup. The small ice particles and droplets were evaporated by injection into dry air inside the Ice-CVI. The resulting ice and droplet residues (IR and DR) were analyzed for size and composition by the two single particle mass spectrometers: a custom-built Single Particle Laser-Ablation Time-of-Flight Mass Spectrometer (SPLAT) and a commercial Aerosol Time-of-Flight Mass Spectrometer (ATOFMS, TSI Model 3800). During CLACE 6 the SPLAT instrument characterized 355 individual IR that produced a mass spectrum for at least one polarity and the ATOFMS measured 152 IR. The mass spectra were binned in classes, based on the combination of dominating substances, such as mineral dust, sulfate, potassium and elemental carbon or organic material. The derived chemical information from the ice residues is compared to the JFJ ambient aerosol that was sampled while the measurement station was out of clouds (several thousand particles analyzed by SPLAT and ATOFMS) and to the composition of the residues of supercooled cloud droplets (SPLAT: 162 cloud droplet residues analyzed, ATOFMS: 1094). The measurements showed that mineral dust was strongly enhanced in the ice particle residues. Close to all of the SPLAT spectra from ice residues did contain signatures from mineral compounds, albeit connected with varying amounts of soluble compounds. Similarly, close to all of the ATOFMS IR spectra show a mineral or metallic component. Pure sulfate and nitrate containing particles were depleted in the ice residues. Sulfate and nitrate was found to dominate the droplet residues (~90% of the particles). The results from the two different single particle mass spectrometers were generally in agreement. Differences in the results originate from several causes, such as the different wavelength of the desorption and ionisation lasers and different size-dependent particle detection efficiencies.
The likely manifestations of climate change like flood hazards are prominent topics in public communication. This can be shown by media analysis and questionnaire data. However, in the case of flood risks an information gap remains resulting in misinformed citizens who probably will not perform the necessary protective actions when an emergency occurs. This paper examines more closely a newly developed approach to flood risk communication that takes the heterogeneity of citizens into account and aims to close this gap. The heterogeneity is analysed on the meso level regarding differences in residential situation as well as on the micro level with respect to risk perception and protective actions. Using the city of Bremen as a case study, empirical data from n=831 respondents were used to identify Action Types representing different states of readiness for protective actions in view of flood risks. These subpopulations can be provided with specific information to meet their heterogeneous needs for risk communication. A prototype of a computer-based information system is described that can produce and pass on such tailored information. However, such an approach to risk communication has to be complemented by meso level analysis which takes the social diversity of subpopulations into account. Social vulnerability is the crucial concept for understanding the distribution of resources and capacities among different social groups. We therefore recommend putting forums and organisations into place that can mediate between the state and its citizens.
Atmospheric new particle formation is a general phenomenon observed over coniferous forests. So far nucleation is described as a function of gaseous sulfuric acid concentration only, which is unable to explain the observed seasonality of nucleation events at different measurement sites. Here we introduce a new nucleation parameter including ozone and water vapor concentrations as well as UV-B radiation as a proxy for OH radical formation. Applying this new parameter to field studies conducted at Finnish and German measurement sites it is found capable to predict the occurrence of nucleation events and their seasonal and annual variation indicating a significant role of organics. Extrapolation to possible future conditions of ozone, water vapor and organic concentrations leads to a significant potential increase in nucleation event number.
Atmospheric new particle formation is a general phenomenon observed over coniferous forests. So far nucleation is either parameterised as a function of gaseous sulphuric acid concentration only, which is unable to explain the observed seasonality of nucleation events at different measurement sites, or as a function of sulphuric acid and organic molecules. Here we introduce different nucleation parameters based on the interaction of sulphuric acid and terpene oxidation products and elucidate the individual importance. They include basic trace gas and meteorological measurements such as ozone and water vapour concentrations, temperature (for terpene emission) and UV B radiation as a proxy for OH radical formation. We apply these new parameters to field studies conducted at conducted at Finnish and German measurement sites and compare these to nucleation observations on a daily and annual scale. General agreement was found, although the specific compounds responsible for the nucleation process remain speculative. This can be interpreted as follows: During cooler seasons the emission of biogenic terpenes and the OH availability limits the new particle formation while towards warmer seasons the ratio of ozone and water vapour concentration seems to dominate the general behaviour. Therefore, organics seem to support ambient nucleation besides sulphuric acid or an OH-related compound. Using these nucleation parameters to extrapolate the current conditions to prognosed future concentrations of ozone, water vapour and organic concentrations leads to a significant potential increase in the nucleation event number.
A new, two-channel instrument for simultaneous NO3 and N2O5 monitoring was used to make the first comprehensive set of nocturnal NOx measurements (NO, NO2, NO3 and N2O5) at the Taunus Observatory, a rural mountain site (Kleiner Feldberg) in South-western Germany. In May 2008, NO3 and N2O5 mixing ratios were well above the instrumental detection limit (a few ppt) on all nights of the campaign and were characterised by large variability. The concentrations of NO3, N2O5 and NO2 were consistent with the equilibrium constant, K2, defining the rates of formation and thermal dissociation of N2O5. A steady-state lifetime analysis is consistent with the loss of nocturnal NOx being dominated by the reaction of NO3 with volatile organic compounds in this forested region, with N2O5 uptake to aerosols of secondary importance. Analysis of a limited dataset obtained at high relative humidity indicated that the loss of N2O5 by reaction with water vapour is less efficient (>factor 3) than derived using laboratory kinetic data. The fraction of NOx present as NO3 and N2O5 reached ~20% on some nights, with night-time losses of NOx competing with daytime losses.
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.
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.
River flow regimes, including long-term average flows, seasonality, low flows, high flows and other types of flow variability, play an important role for freshwater ecosystems. Thus, climate change affects freshwater ecosystems not only by increased temperatures but also by altered river flow regimes. However, with one exception, transferable quantitative relations between flow alterations and ecological responses have not yet been derived. While discharge decreases are generally considered to be detrimental for ecosystems, the effect of future discharge increases is unclear. As a first step towards a global-scale analysis of climate change impacts on freshwater ecosystems, we quantified the impact of climate change on five ecologically relevant river flow indicators, using the global water model WaterGAP 2.1g to simulate monthly time series of river discharge with a spatial resolution of 0.5 degrees. Four climate change scenarios based on two global climate models and two greenhouse gas emissions scenarios were evaluated. We compared the impact of climate change by the 2050s to the impact of water withdrawals and dams on natural flow regimes that had occurred by 2002. Climate change was computed to alter seasonal flow regimes significantly (i.e. by more than 10%) on 90% of the global land area (excluding Greenland and Antarctica), as compared to only one quarter of the land area that had suffered from significant seasonal flow regime alterations due to dams and water withdrawals. Due to climate change, the timing of the maximum mean monthly river discharge will be shifted by at least one month on one third on the global land area, more often towards earlier months (mainly due to earlier snowmelt). Dams and withdrawals had caused comparable shifts on less than 5% of the land area only. Long-term average annual river discharge is predicted to significantly increase on one half of the land area, and to significantly decrease on one quarter. Dams and withdrawals had led to significant decreases on one sixth of the land area, and nowhere to increases. Thus, by the 2050s, climate change may have impacted ecologically relevant river flow characteristics more strongly than dams and water withdrawals have up to now. The only exception refers to the decrease of the statistical low flow Q90, with significant decreases both by past water withdrawals and future climate change on one quarter of the land area. However, dam impacts are likely underestimated by our study. Considering long-term average river discharge, only a few regions, including Spain, Italy, Iraq, Southern India, Western China, the Australian Murray Darling Basin and the High Plains Aquifer in the USA, all of them with extensive irrigation, are expected to be less affected by climate change than by past anthropogenic flow alterations. In some of these regions, climate change will exacerbate the discharge reductions, while in others climate change provides opportunities for reducing past reductions. Emissions scenario B2 leads to only slightly reduced alterations of river flow regimes as compared to scenario A2 even though emissions are much smaller. The differences in alterations resulting from the two applied climate models are larger than those resulting from the two emissions scenarios. Based on general knowledge about ecosystem responses to flow alterations and data related to flow alterations by dams and water withdrawals, we expect that the computed climate change induced river flow alterations will impact freshwater ecosystems more strongly than past anthropogenic alterations.
This paper investigates the potential impact of secondary information on rainfall mapping applying Ordinary Kriging. Secondary information tested is a natural area indicator, which is a combination of topographic features and weather conditions. Cross validation shows that secondary information only marginally improves the final mapping, indicating that a one-day accumulation time is possibly too short.
Development of a Bioaerosol single particle detector (BIO IN) for the Fast Ice Nucleus CHamber FINCH
(2010)
In this work we present the setup and first tests of our new BIO IN detector. This detector was constructed to classify atmospheric ice nuclei (IN) for their biological content. It is designed to be coupled to the Fast Ice Nucleus CHamber FINCH. If one particle acts as an ice nucleus, it will be at least partly covered with ice at the end of the development section of the FINCH chamber. The device combines an auto-fluorescence detector and a circular depolarization detector for simultaneous detection of biological material and discrimination between water droplets, ice crystals and non activated large aerosol particles. The excitation of biological material with UV light and analysis of auto-fluorescence is a common principle used for flow cytometry, fluorescence microscopy, spectroscopy and imaging. The detection of auto-fluorescence of airborne single particles demands some more experimental effort. However, expensive commercial sensors are available for special purposes, e.g. size distribution measurements. But these sensors will not fit the specifications needed for the FINCH IN counter (e.g. high sample flow of up 10 LPM). The newly developed -low cost- BIO IN sensor uses a single high-power UV LED for the electronic excitation instead of much more expensive UV lasers. Other key advantages of the new sensor are the low weight, compact size, and the little effect on the aerosol sample, which allows it to be coupled with other instruments for further analysis. The instrument will be flown on one of the first missions of the new German research aircraft "HALO" (High Altitude and LOng range).