Atmospheric aerosols can influence society and the environment in many ways including altering the planet's energy budget, the hydrologic cycle, and public health. However, the Fourth Assessment Report of the Intergovernmental Panel on Climate Change indicates that the anthropogenic radiative forcing associated with aerosol effects on clouds has the highest uncertainty in the future climate predictions. This thesis focuses on the nature of the organic fraction of ambient particles and how particles interact with clouds using a combination of tools including aircraft and ground measurements, models, and satellite data. Fine aerosol particles typically contain between 20 - 90% organic matter by mass and a major component of this fraction includes water soluble organic carbon (WSOC). Consequently, water-soluble organic species can strongly influence aerosol water-uptake and optical properties. However, the chemical composition of this fraction is not well-understood. PILS-TOC was used to characterize WSOC in ambient aerosol in Los Angeles, California. The spatial distribution of WSOC was found to be influenced by (i) a wide range of aerosol sources within this urban metropolitan area, (ii) transport of pollutants by the characteristic daytime sea breeze trajectory, (iii) topography, and (iv) secondary production during transport. Meteorology is linked with the strength of many of these various processes. Many methods and instruments have been used to study aerosol-cloud interactions. Each observational platform is characterized by different temporal/spatial resolutions and operational principles, and thus there are disagreements between different studies for the magnitude of mathematical constructs used to represent the strength of aerosol-cloud interactions. This work points to the sensitivity of the magnitude of aerosol-cloud interactions to cloud lifetime and spatial resolution of measurements and model simulations. Failure to account for above-cloud aerosol layers and wet scavenging are also shown to cause biases in the magnitude of aerosol-cloud interaction metrics. Air mass source origin and meteorology are also shown to be important factors that influence aerosol-cloud interactions. The results from this work contribute towards a better understanding of atmospheric aerosols and are meant to improve parameterizations that can be embedded in models that treat aerosol affects on clouds, precipitation, air quality, and public health.

Les aérosols atmosphériques sont omniprésents dans l'air et jouent un rôle important à la fois à l'échelle globale, par leur action sur le bilan radiatif de la Terre, et à l'échelle locale, par leur impact sur la santé publique dans les zones fortement polluées. La matière organique est l'un des constituants principaux de l'aérosol ; la complexité et l'hétérogénéité de cette fraction ont jusqu'à présent constitué des difficultés majeures à leur intégration dans les études d'impact sanitaire ou climatique. 10 à 30% de la masse de cette fraction est constituée de « Humic Like Substances ». L'objectif de la thèse est de développer une méthode fiable et efficace d'extraction et d'analyse des HULIS (HUmic LIke Substances) issus de l'aérosol atmosphérique, et de déterminer leurs distributions spatiales et temporelles, leurs sources majeures et leurs structures chimiques grâce à 250 échantillons collectés sur six sites urbains. L'identification des deux sources majeures des HULIS sur l'aérosol, à savoir les sources secondaires (photo-oxydation en phase aqueuse dans certains cas) en été et les sources primaires liées à la combustion de biomasse en hiver, et ce, indépendamment du lieu géographique est démontrée. Une différence significative de la structure chimique des HULIS provenant de ces deux sources majeures est observée : ils regroupent des composés plus aliphatiques et moins aromatiques en été qu'en hiver, et leur teneur en groupements carboxyliques augmente de l'hiver à l'été.

900 archived FRM filters from 15 sites over the southeast during 2007 were analyzed for PM2.5 chemical composition and physical properties. Secondary components (i.e. sulfate aerosol and SOA) were the major contributors to the PM2.5 mass over the southeast, whereas the contribution from biomass burning varied with season and was negligible (2%) during summer. Excluding biomass burning influence, FRM WSOC was spatially homogeneous throughout the region, similar to sulfate, yet WSOC was moderately enhanced in locations of greater predicted isoprene emissions in summer. On smaller spatial scale, a substantial urban/rural gradient of WSOC was found through comparisons of online WSOC measurements at one urban/rural pair (Atlanta/Yorkville) in August 2008, indicating important contribution from anthropogenic emissions. A comparative study between Atlanta and LA reveals a number of contrasting features between two cities. WSOC gas-particle partitioning, investigated through the fraction of total WSOC in the particle phase, Fp, exhibited differing relationships with ambient RH and organic aerosols. In Atlanta, both particle water and organic aerosol (OA) can serve as an absorbing phase. In contrast, in LA the aerosol water was not an important absorbing phase, instead, Fp was correlated with OA mass. Fresh LA WSOC had a consistent brown color and a bulk absorption per soluble carbon mass at 365 nm that was 4 to 6 times higher than freshly-formed Atlanta soluble organic carbon. Interpreting soluble brown carbon as a property of freshly-formed anthropogenic SOA, the difference in absorption per carbon mass between the two cities suggests most WSOC formed within Atlanta is not from an anthropogenic process similar to LA.

This thesis focuses on the volatile and hygroscopic properties of mixed aerosol species. In particular, the influence organic species of varying solubility have upon seed aerosols. Aerosol studies were conducted at the Paul Scherrer Institut Laboratory for Atmospheric Chemistry (PSI-LAC, Villigen, Switzerland) and at the Queensland University of Technology International Laboratory for Air Quality and Health (QUT-ILAQH, Brisbane, Australia). The primary measurement tool employed in this program was the Volatilisation and Hygroscopicity Tandem Differential Mobility Analyser (VHTDMA - Johnson et al. 2004). This system was initially developed at QUT within the ILAQH and was completely re-developed as part of this project (see Section 1.4 for a description of this process). The new VHTDMA was deployed to the PSI-LAC where an analysis of the volatile and hygroscopic properties of ammonium sulphate seeds coated with organic species formed from the photo-oxidation of á-pinene was conducted. This investigation was driven by a desire to understand the influence of atmospherically prevalent organics upon water uptake by material with cloud forming capabilities. Of particular note from this campaign were observed influences of partially soluble organic coatings upon inorganic ammonium sulphate seeds above and below their deliquescence relative humidity (DRH). Above the DRH of the seed increasing the volume fraction of the organic component was shown to reduce the water uptake of the mixed particle. Below the DRH the organic was shown to activate the water uptake of the seed. This was the first time this effect had been observed for á-pinene derived SOA. In contrast with the simulated aerosols generated at the PSI-LAC a case study of the volatile and hygroscopic properties of diesel emissions was undertaken. During this stage of the project ternary nucleation was shown, for the first time, to be one of the processes involved in formation of diesel particulate matter. Furthermore, these particles were shown to be coated with a volatile hydrophobic material which prevented the water uptake of the highly hygroscopic material below. This result was a first and indicated that previous studies into the hygroscopicity of diesel emission had erroneously reported the particles to be hydrophobic. Both of these results contradict the previously upheld Zdanovksii-Stokes-Robinson (ZSR) additive rule for water uptake by mixed species. This is an important contribution as it adds to the weight of evidence that limits the validity of this rule.

abstract: N-Nitrosodimethylamine (NDMA), a probable human carcinogen, has been found in clouds and fogs at concentration up to 500 ng/L and in drinking water as disinfection by-product. NDMA exposure to the general public is not well understood because of knowledge gaps in terms of occurrence, formation and fate both in air and water. The goal of this dissertation was to contribute to closing these knowledge gaps on potential human NDMA exposure through contributions to atmospheric measurements and fate as well as aqueous formation processes. Novel, sensitive methods of measuring NDMA in air were developed based on Solid Phase Extraction (SPE) and Solid Phase Microextraction (SPME) coupled to Gas Chromatography-Mass Spectrometry (GC-MS). The two measuring techniques were evaluated in laboratory experiments. SPE-GC-MS was applicable in ambient air sampling and NDMA in ambient air was found in the 0.1-13.0 ng/m3 range. NDMA photolysis, the main degradation atmospheric pathway, was studied in the atmospheric aqueous phase. Water soluble organic carbon (WSOC) was found to have more impact than inorganic species on NDMA photolysis by competing with NDMA for photons and therefore could substantially increase the NDMA lifetime in the atmosphere. The optical properties of atmospheric WSOC were investigated in aerosol, fog and cloud samples and showed WSOC from atmospheric aerosols has a higher mass absorption efficiency (MAE) than organic matter in fog and cloud water, resulting from a different composition, especially in regards of volatile species, that are not very absorbing but abundant in fogs and clouds. NDMA formation kinetics during chloramination were studied in aqueous samples including wastewater, surface water and ground water, at two monochloramine concentrations. A simple second order NDMA formation model was developed using measured NDMA and monochloramine concentrations at select reaction times. The model fitted the NDMA formation well (R2 >0.88) in all water matrices. The proposed model was then optimized and applied to fit the data of NDMA formation from natural organic matter (NOM) and model precursors in previously studies. By determining the rate constants, the model was able to describe the effect of water conditions such as DOC and pH on NDMA formation. / Dissertation/Thesis / Doctoral Dissertation Chemistry 2016

Characterization and Source Apportionment of Ambient PM2.5 in Atlanta, Georgia: On-Road Emission, Biomass Burning and SOA Impact Bo Yan 260 Pages Directed by Drs. Armistead G. Russell and Mei Zheng Various airborne PM2.5 samples were collected in the metropolitan Atlanta and surrounding areas, which are directly impacted or dominated by on-road mobile and other typical urban emissions, regional transport sources, prescribed burning plumes, wildfire plumes, as well as secondary sources with anthropogenic and biogenic nature in origin. Detailed PM2.5 chemical speciation was conducted including over one hundred of GC/MS-quantified organic compounds, organic carbon (OC), water-soluble organic carbon (WSOC), elemental carbon (EC), ionic species, and tens of trace metals. Day-night, seasonal and spatial variations of PM2.5 characterization were also studied. Contributions of PM2.5 major sources were identified quantitatively through the receptor source apportionment models. These modeling results, especially on-road mobile source contributions and secondary organic carbon (SOC) were assessed by multiple approaches. Furthermore, new season- and location-specific source profiles were developed in this research to reflect real-world and representative local emission characterizations of on-road mobile sources, aged prescribed burning plumes, and wildfire plumes. Secondary organic aerosol (SOA), a major component of PM2.5 in the summer, was also explored for sources and contributions.

Introduktion Arbetsrelaterad känsla av sammanhang (eng. WSOC) kan användas som en indikator för arbetstrivsel och bygger på hur anställda ser på sitt arbete utifrån hanterbarhet, begriplighet och meningsfullhet. Kunskapsläget gällande hur WSOC påverkar anställdas vilja att stanna hos sin arbetsgivare är begränsat. Syfte Syftet var att undersöka hur WSOC relaterar till anställdas intention att stanna kvar hos sin arbetsgivare. Metod Syfte och frågeställningar besvarades genom en kvantitativ analys baserad på en enkätundersökning bland 450 personer i den svenska Marinen. De statistiska test som genomförts är oberoende t-test och envägs-ANOVA. Resultat De som ser sig stanna kvar hos sin arbetsgivare om tre år eller inte har funderat på att lämna det senaste året har signifikant högre WSOC än de som inte ser sig stanna kvar eller har övervägt att sluta. Starkare WSOC tyder på en högre intention för värnpliktiga att ta anställning och för GSS/K att söka officersutbildning. Resultatet tyder även på ett samband mellan WSOC och balansen mellan arbete och privatliv. Slutsats Resultatet tyder på ett samband mellan ett högre WSOC och en vilja att stanna hos sin arbetsgivare. Med vetskapen om hur personalen uppfattar sin känsla av sammanhang på arbetet kan en arbetsgivare vidta åtgärder för att öka behållandegraden och även som i Försvarsmaktens fall, öka rekryteringsgraden till myndigheten. Nyckelord Arbetsrelaterad känsla av sammanhang, behålla personal, rekrytering, Försvarsmakten, balans mellan arbete och privatliv. / Introduction Work related sense of coherence (WSOC) can be used as an indicator of well-being at work and is based on how employees view their work in terms of manageability, comprehensibility and meaningfulness. Research on how WSOC affects employees’ willingness to stay with their employer is as of now limited. Aim The aim of the study was to investigate how WSOC relates to employees' intention to remain with their employer. Method The aim and sub-questions were answered through a quantitative analysis based on a survey among 450 employees in the Swedish Navy. The statistical tests carried out are independent t- test and one-way ANOVA. Results People who see themselves staying with their employer for the next three years or those who have not considered leaving in the past year have a significantly stronger WSOC than those who do not see themselves staying or have considered leaving. Stronger WSOC furthermore indicated a higher intention for conscripts to take up employment and for employed sailors to enroll for officer training. The results also indicate a relationship between WSOC and work- life balance. Conclusion The results indicated a relationship between a stronger WSOC and a willingness to stay with one's employer. With the knowledge of how the employees perceives their sense of coherence at work, an employer can take measures to increase the retention rate and also, as in the case of the Armed Forces, increase the recruitment rate. Key words Work related sense of coherence (WSOC), retention, recruitment, Armed forces, work-life balance.