Atmosphärische Aerosolpartikel können durch ein breites Spektrum an natürlichen oder anthropogenen Emissionen mit unterschiedlich hohen Konzentrationen in die Atmosphäre freigesetzt werden. Sie beeinflussen den Strahlungshaushalt und damit auch das Klima der Erde und können außerdem durch ihre Präsenz in der Atmosphäre Wechselwirkungen mit Mensch und Natur, also dem gesamten Ökosystem haben. Seit dem Jahr 2010 gelten in der EU Grenzwerte für die PM10 Tagesmittelkonzentration, die jedoch bereits wenige Monate nach Beginn der Gültigkeit an vielen Messstationen überschritten wurden. Das Ziel der vorliegenden Arbeit war eine objektive Bewertung der Herkunft und des Zustandes der an einem Messort ankommenden Luftmasse und der damit verbundenen Schadstoffniveaus. Im ersten Teil der Arbeit wurden PM10 Messdaten aus fünf Jahren in und um Leipzig sowie analog in fünf verschiedenen Regionen deutschlandweit in Bezug auf PM10 Grenzwertüberschreitungen untersucht. Es wurden Rückwärtstrajektorien für eine Clusteranalyse verwendet, mit der spezifische Wetterlagen unterschieden wurden und diesen dann die einzelnen Messtage mit den zugehörigen Schadstoffkonzentrationen zugeordnet wurden. Hierbei wurde deutlich, dass durch entsprechende meteorologische Bedingungen sowohl lokal als auch regional emittierte Schadstoffe in Bodennähe akkumulieren oder aber auch räumlich verteilt werden können. Außerdem wurde in dieser Arbeit eine Modellvalidierung vorgestellt. Es wurde das Modellsystem COSMO-MUSCAT/ext-M7 verwendet, dessen Ergebnisse mit Beobachtungsdaten verglichen wurden. Als erstes wurde die Beschreibung der meteorologischen Bedingungen, dann die räumliche Verteilung von PM10, die chemische Partikelzusammensetzung sowie physikalische Aerosolparameter wie Partikelanzahl, -volumen und -durchmesser verglichen. Die Ergebnisse deuten darauf hin, dass nach wie vor Probleme bei der Beschreibung der mikrophysikalischen Aerosoleigenschaften bestehen. Die Größenordnungen der verglichenen Parameter können vom Modell abgebildet werden, dennoch müssen Modellergebnisse nach wie vor mit Vorsicht interpretiert werden, insbesondere hinsichtlich von Prozessen, bei denen die Partikelanzahl eine Rolle spielen.

Trace gases and aerosols, or suspended liquid and solid material in the atmosphere, have significant climatological and societal impacts; consequently, accurate representation of their contribution to atmospheric composition is vital to predicting climate change and informing policy actions. Sensitivity analysis allows scientists and environmental decision makers alike to ascertain the role a specific component of the very complex system that is the atmosphere of the Earth. Anthropogenic and natural emissions of gases and aerosol are transported by winds and interact with sunlight, allowing significant transformation before these species reach the end of their atmospheric life on land or in water. The adjoint-based sensitivity method assesses the relative importance of each emissions source to selected results of interest, including aerosol and cloud droplet concentration. In this work, the adjoint of a comprehensive inorganic aerosol thermodynamic equilibrium model was produced to improve the representativeness of regional and global chemical transport modeling. Furthermore, a global chemical transport model adjoint equipped with the adjoint of a cloud droplet activation parameterization was used to explore the footprint of emissions contributing to current and potential future cloud droplet concentrations, which impact the radiative balance of the earth. In future work, these sensitivity relationships can be exploited in optimization frameworks for assimilation of observations of the system, such as satellite-based or in situ measurements of aerosol or precursor trace gas concentrations.

The feedbacks among aerosols, clouds, and radiation are important components for understanding Earth's climate system and quantifying human-induced climate change, yet the magnitude of these feedbacks remain highly uncertain. Since every cloud droplet in the atmosphere begins with water condensing on a pre-existing aerosol particle, characterizing the ability of aerosols to uptake water vapor and form cloud condensation nuclei (CCN) are key to understanding the microphysics behind cloud formation, as well as assess the impact aerosols have on the Earth system. Through a combination of controlled laboratory experiments and field measurements, this thesis characterizes the ability of atmospheric aerosols to uptake water vapor and become CCN at controlled levels of water vapor supersaturation. The origin of the particle water uptake, termed hygroscopicity, is also explored, being from either the presence of deliquescent soluble material and/or adsorption onto insoluble surfaces. The data collected and presented is comprehensive and includes (1) ground samples of volcanic ash, collected from six recent eruptions re-suspended in the laboratory for analysis, (2) laboratory chamber and flow-tube studies on the oxidation and uptake of surface active organic compounds, and (3) in-situ aircraft measurements of aerosols from the Arctic background, Canadian boreal forests, fresh and aged biomass burning, anthropogenic industrial pollution, and from within tropical cyclones in the Atlantic basin. Having a more thorough understanding of aerosol water uptake will enable more accurate representation of cloud droplet number concentrations in global models, which can have important implications on reducing the uncertainty of aerosol-cloud-climate interactions, as well as additional uncertainties in aerosol transport, atmospheric lifetime, and impact on storm dynamics.

This thesis characterizes properties of ambient secondary organic aerosol (SOA), an important and abundant component of particulate matter. The findings presented in this thesis are significant because they represent the results from ambient measurements, which are relatively scarce, and because they report on properties of SOA that, until now, were highly uncertain. The analyses utilized the fraction of particulate organic carbon that was soluble in water (WSOCp) to approximate SOA concentrations in two largely different urban environments, Mexico City and Atlanta. In Mexico City, measurements of atmospheric gases and fine particle chemistry were made at a site ~ 30 km down wind of the city center. Using box model analyses and a comparison to ammonium nitrate aerosol, a species whose thermodynamic properties are generally understood, the morning formation and mid-day evaporation of SOA are investigated. In Atlanta, simultaneous measurements of WSOCp and water-soluble organic carbon in the gas phase (WSOCg) were carried out for an entire summer to investigate the sources and partitioning of WSOC. The results suggest that both WSOCp and WSOCg were secondary and biogenic, except possibly in several strong biomass burning events. The gas/particle partitioning of WSOC in Atlanta was investigated through the parameter, Fp, which represented the fraction of WSOC in the particle phase. Factors that appear to influence WSOC partitioning in Atlanta include ambient relative humidity and the WSOCp mass concentration. There was also a relationship between the NOx concentration and Fp, though this was not likely related to the partitioning process. Temperature did not appear to impact Fp, though this may have been due to positive relationships WSOCp and WSOCg each exhibited with temperature. Neither the total Organic Carbon aerosol mass concentration nor the ozone concentration impacted WSOC partitioning.

Thesis (Ph. D.)--Ohio State University, 2008. / Title from first page of PDF file. Includes bibliographical references (p. 151-167).

Thesis (Ph.D)--Earth and Atmospheric Sciences, Georgia Institute of Technology, 2009. / Committee Chair: Fu, Rong; Committee Member: Dickinson, Robert E.; Committee Member: Nenes, Athanasios; Committee Member: Webster,Peter J.; Committee Member: Yu, Hongbin. Part of the SMARTech Electronic Thesis and Dissertation Collection.

Thesis (Ph. D.)--University of California, San Diego, 2000. / Vita. Includes bibliographical references.

Thesis (Ph.D.)--York University, 2005. Graduate Programme in Earth and Space Science. / Typescript. Includes bibliographical references (leaves 181-196). Also available on the Internet. MODE OF ACCESS via web browser by entering the following URL: http://wwwlib.umi.com/cr/yorku/fullcit?pNR11647

Doctorat en Sciences / info:eu-repo/semantics/nonPublished

Atmospheric aerosols play an important role in various atmospheric issues (effect to the radiation budget of the atmosphere, visibility reduction, smog production, destruction of stratospheric ozone, …). Epidemiological studies proved a correlation between increased mortality and high concentration of ambient particulate matter. Over the past decade, a growing attention has been focused on the organic compounds that are constituents of aerosol particles. Although organic compounds comprise often up to 60% of the total aerosol mass, their composition, concentration and formation mechanisms are not well understood. Diploma thesis will deal with the study of chemical composition of organic compounds bound to atmospheric aerosols with focus on polyaromatic hydrocarbons and sugars. Atmospheric aerosols will be sampled on filters and filter extracts will be analysed for content of studied organic compounds by means of GC, GC-MS or LC, respectively. Development and optimalization of extraction methods (PSE, …) and detection of compounds of interest. Concentration of studied organic compounds in aerosol size fractions PM 10, PM 2.5 and PM 1 will be compared.