A Differential Mobility Analyzer/Tandem Differential Mobility Analyzer (DMA/TDMA) was used to measure size distributions, hygroscopicity, and volatility during the May 2003 Aerosol Intensive Operational Period at the Central Facility of the Atmospheric Radiation Measurement Southern Great Plains site. Hygroscopic growth factor distributions for particles at eight dry diameters ranging from 0.012 µm to 0.600 µm were measured. These measurements, along with backtrajectory clustering, were used to infer aerosol composition and evolution. The hygroscopic growth of the smallest and largest particles analyzed was typically less than that of particles with dry diameters of about 0.100 µm. Condensation of secondary organic aerosol on nucleation mode particles may be responsible for the minimal growth observed at the smallest sizes. Growth factor distributions of the largest particles typically contained a non-hygroscopic mode believed to be composed of dust. A model was developed to characterize the hygroscopic properties of particles within a size distribution mode through analysis of the fixed-size hygroscopic growth measurements. This model was used to examine three cases in which the sampled aerosol evolved over a period of hours or days. Additionally, size and hygroscopicity information were combined to model the aerosol as a population of multi-component particles. With this model, the aerosol hygroscopic growth factor f(RH), relating the submicron scattering at high RH to that at low RH, is predicted. The f(RH) values predicted when the hygroscopic fraction of the aerosol is assumed to be metastable agree better with measurements than do those predicted under the assumption of crystalline aerosol. Agreement decreases at RH greater than 65%. This multi-component aerosol model is used to derive cloud condensation nuclei (CCN) spectra for comparison with spectra measured directly with two Desert Research Institute (DRI) CCN spectrometers. Among the 1490 pairs of DMA/TDMA-predicted and DRI-measured CCN concentrations at various critical supersaturations from 0.02-1.05%, the sample number-weighted mean R2 value is 0.74. CCN concentrations are slightly overpredicted at both the lowest (0.02-0.04%) and highest (0.80-1.05%) supersaturations measured. Overall, this multi-component aerosol model based on size distributions and size-resolved hygroscopicity yields reasonable predictions of the humidity-dependent optical properties and CCN spectra of the aerosol.

A Differential Mobility Analyzer/Tandem Differential Mobility Analyzer (DMA/TDMA) was used to measure size distributions, hygroscopicity, and volatility during the May 2003 Aerosol Intensive Operational Period at the Central Facility of the Atmospheric Radiation Measurement Southern Great Plains site. Hygroscopic growth factor distributions for particles at eight dry diameters ranging from 0.012 µm to 0.600 µm were measured. These measurements, along with backtrajectory clustering, were used to infer aerosol composition and evolution. The hygroscopic growth of the smallest and largest particles analyzed was typically less than that of particles with dry diameters of about 0.100 µm. Condensation of secondary organic aerosol on nucleation mode particles may be responsible for the minimal growth observed at the smallest sizes. Growth factor distributions of the largest particles typically contained a non-hygroscopic mode believed to be composed of dust. A model was developed to characterize the hygroscopic properties of particles within a size distribution mode through analysis of the fixed-size hygroscopic growth measurements. This model was used to examine three cases in which the sampled aerosol evolved over a period of hours or days. Additionally, size and hygroscopicity information were combined to model the aerosol as a population of multi-component particles. With this model, the aerosol hygroscopic growth factor f(RH), relating the submicron scattering at high RH to that at low RH, is predicted. The f(RH) values predicted when the hygroscopic fraction of the aerosol is assumed to be metastable agree better with measurements than do those predicted under the assumption of crystalline aerosol. Agreement decreases at RH greater than 65%. This multi-component aerosol model is used to derive cloud condensation nuclei (CCN) spectra for comparison with spectra measured directly with two Desert Research Institute (DRI) CCN spectrometers. Among the 1490 pairs of DMA/TDMA-predicted and DRI-measured CCN concentrations at various critical supersaturations from 0.02-1.05%, the sample number-weighted mean R2 value is 0.74. CCN concentrations are slightly overpredicted at both the lowest (0.02-0.04%) and highest (0.80-1.05%) supersaturations measured. Overall, this multi-component aerosol model based on size distributions and size-resolved hygroscopicity yields reasonable predictions of the humidity-dependent optical properties and CCN spectra of the aerosol.

Understanding the interaction between atmospheric aerosol and water vapour is key in assessing the impacts of anthropogenic influences on the earth's radiative budget, both directly through scattering and absorbing incident solar radiation, and indirectly through changing cloud properties, with considerable uncertainty in the magnitude of the estimated forcings of the latter. Although aerosol particle water uptake is well defined for inorganic compounds, the effects of the aerosol organic fraction on cloud droplet formation and cloud condensation nuclei (CCN) properties are relatively poorly characterised, due to the large number of organic compounds present in atmosphere and their highly complex influences on properties such as water solubility and surface tension.This thesis presents extensive field measurements of CCN/aerosol hygroscopicity from three different environments, together with a novel error model, which has been developed to propagate instrumental uncertainties from measurements in the sub- and supersaturated regimes through to commonly used data products used in large-scale models. This study illustrates that a single hygroscopicity framework is not able to reconcile the measurements within errors, for different measurement environments. The sensitivity of this type of reconciliation study was assessed using several different scenarios, making different assumptions in each case; sensitivity tests using a 'typical' regional aerosol particle water uptake or number-size distribution, demonstrate that it is not possible to apply a constant correction to data to guarantee reconciliation, that the best reconciliation was achieved for size-resolved high-temporal water uptake and aerosol number-size distribution data, and that the application of single-parameter hygroscopicity models requires further examination. It is concluded that high-temporal size-resolved measurements of sub- and supersaturated particle water uptake are fundamental to providing a thorough characterisation of the interaction between atmospheric aerosol and water vapour, and are essential in order to achieve the best possible predictive capability from large-scale models.

O objetivo deste trabalho foi estudar o papel dos aerossóis em modificar o desenvolvimento das nuvens e da precipitação. Esta tem sido uma das mais intrigantes questões no estudo das mudanças climáticas. Medidas da concentração de núcleos de condensação de nuvens (CCN) e distribuições de gotículas de nuvem durante o Experimento de Grande Escala da Biosfera-Atmosfera na Amazônia (LBA) revelaram características distintas entre condições atmosféricas limpas e poluídas. As medidas foram conduzidas no Sudoeste da Região Amazônica durante os meses de setembro e outubro de 2002, focando a transição do final da estação seca para o início da estação chuvosa. Durante a transição, a análise da concentração de CCN dentro da camada limite revelou um decréscimo geral, de valores acima de 1200 cm-3 para menos de 300 cm-3. A comparação entre áreas limpas e poluídas mostrou concentrações de CCN cerca de 5 vezes maiores em áreas poluídas. As diferenças não foram tão grandes nos níveis acima da camada limite. As medidas também mostraram um ciclo diurno acompanhando a atividade de queima de biomassa. Distribuições de tamanho de gotículas medidas em duas regiões com concentrações de aerossóis extremamente diferentes foram analisadas. Em condições poluídas pela queima de biomassa foi encontrada alta concentração de gotículas, com diâmetro médio e conteúdo de água de nuvem aumentando muito pouco com a altura, em comparação com regiões limpas. A função gama foi usada para ajustar as distribuições de gotículas e o parâmetro de forma da função foi usado como critério para definir adequadamente a melhor representação das distribuições de gotículas. De acordo com os valores encontrados, distribuições gama estreitas (parâmetro de forma em torno de 5) são mais bem indicadas para representar condições poluídas enquanto que aquelas mais largas se ajustam melhor em condições limpas (parâmetro de forma em torno de 2). Com base nesses resultados, experimentos numéricos foram conduzidos com o Brazilian Regional Atmospheric Modeling System (BRAMS) para investigar os efeitos da concentração de CCN e do parâmetro de forma das distribuições de gotículas no desenvolvimento da precipitação em nuvens convectivas tropicais. Os resultados mostraram uma grande sensibilidade devido às mudanças nesses parâmetros. Altas concentrações de CCN e distribuições de gotículas estreitas (parâmetros de forma maiores), típicas de dias poluídos, produziram baixos valores médios para água líquida integrada na coluna e precipitação acumulada na superfície. Por outro lado, tendência oposta a este efeito foi encontrada em condições limpas (baixos valores para ambos, a concentração de CCN e o parâmetro de forma). O parâmetro de forma se mostrou ser mais importante que a concentração de CCN. Os efeitos da concentração de CCN e do parâmetro de forma também influenciaram a distribuição espacial dos campos de nuvem e precipitação. Embora o valor médio desses campos tenha diminuído em condições poluídas, o valor máximo aumentou. Como conseqüência da menor dispersão nas nuvens em condições poluídas, mais radiação solar esteve disponível na superfície. Isto é oposto aos resultados dos modelos globais que mostram redução na radiação solar como conseqüência do segundo efeito indireto dos aerossóis. Da mesma forma, este estudo encontrou que as diferenças são reduzidas quando é incluído o efeito direto dos aerossóis em absorver ou refletir a radiação solar. Sobretudo, os resultados sugerem que um maior número de modelos com tratamento explícito dos processos microfísicos de nuvem são necessários. Esses modelos permitem comparações, podendo mostrar o melhor tratamento numérico a ser usado na representação dos efeitos dos aerossóis no processo de precipitação como um todo. Estes resultados são importantes porque melhoram a compreensão de como o clima será afetado como conseqüência das mudanças futuras. / The objective of this work was to study the role of aerosols in modifying clouds and precipitation. This is one of the most difficult aspects in the study of climate changes. Field measurements of cloud condensation nuclei (CCN) and cloud size distributions performed during the Large Scale Biosphere-Atmosphere Experiment in Amazonia (LBA) campaign revealed distinct characteristics between clean and polluted atmospheric conditions. Measurements were conducted over the southwestern Amazon region during September-October 2002 focusing the transition from dry to wet seasons. During this period, analysis of CCN concentrations in the boundary layer revealed a general decreasing trend from mean values higher than 1200 cm-3 to values lower than 300 cm-3. The comparison between clean and polluted areas showed CCN concentrations 5 times higher than in polluted areas. These differences were not so strong above the boundary layer. Measurements also showed a diurnal cycle following the biomass burning activity. Cloud droplet size distributions at two regions with extremely different aerosols loading were also analyzed. During biomass-burning conditions, at high concentrations of cloud droplets, the mean diameter and liquid water content increased very little with altitude when compared with unpolluted conditions. A gamma distribution was used to fit the measured droplet spectra and the shape parameter was used as a criterion to define the best choice of spectra representation. According to the found values, narrow gamma distributions optimally fit polluted conditions (shape parameter around 5), while broad distributions are best fits for unpolluted conditions (shape parameter around 2). Based on these results, numerical experiments were carried out using the Brazilian Regional Atmospheric Modeling System (BRAMS) to investigate the effects of CCN concentrations and shape parameters of droplet spectra on the development of precipitation in tropical convective clouds. The results showed large sensitivity due to changes in these parameters. It was observed that high CCN concentrations and narrower cloud droplet distributions (high values for shape parameter), typical of the polluted days, produced low mean values of liquid water path and accumulated surface precipitation. On the other hand, an opposite trend to this effect was found under clean conditions (low CCN concentration and shape parameter values). Shape parameter showed to be much more important than CCN concentration. The effects of CCN concentration and shape parameter also influenced the spatial distribution of cloud and precipitation fields. Although mean values of these fields decreased under polluted conditions, maximum values were increased. Consequently, the less dispersion in clouds under polluted conditions, the more surface solar radiation was found. This is opposite to the results of global climate models, which predict reduction in solar radiation as a consequence of the second aerosol indirect effect. Also, it was found that the differences were reduced when the aerosols direct effect to absorb or reflect solar radiation is included. Moreover, the results suggest that additional models with explicit microphysics process treatment are necessary in order to allow further comparisons, which could show the best numerical treatment to be used in representing the aerosol effects on precipitation process. The importance of these results is to improve the understanding of future climate changes.

This work tests the validity of using a commercial cloud condensation nuclei (CCN) counter (CCNc) on the Facility for Airborne Atmospheric Measurements (FAAM) research aircraft. The CCNc was suitable for aircraft work with sta- ble and repeatable supersaturation, temperature and pressure relationships. The sample architecture of the aircraft fitted CCNc was found to transmit particles with acceptable losses in the diameter range of interest as was a pressure control device designed for airborne work. Rosemount inlets, used to sample aerosol, were found to be sensitive to particle density resulting in disparate aerosol being sam- pled with different efficiencies. In dust dominated aerosol inlet efficiency peaks at 10.24 at an optical diameter of 2.91 μm, with a minimum inlet efficiency between 1.78 and 1.51 at 0.28μm. In less dense aerosol inlets sample representatively below 0.6 μm and comparably below 1.0 μm. The thorough testing of the CCNc, associated sampling architecture and mea- surement strategies, enabled vertical and horizontal CCN to be investigated along with other aerosol and cloud microphysical properties in the Southern Equato- rial Pacific (SEP). The primary source of particulates was the South American continent, with sulphate dominating composition. There were strong gradients in aerosol and gas phase chemistry concentration with distance from the coast and in the cloud microphysics measurements where highest droplet numbers and smallest diameters were close to the coast. These data represent an important validatory and parameterisation data set for models of all scales. CCN data were used to calculate the aerosol hygroscopicity parameter, the mean project value, κ, was 0.21 ± 0.18 . There was no evident variation in hygroscopicity with distance from the Chilean coastline suggesting a single dominant source and a well mixed boundary layer up to 907km to the west. CCN measurements were also com- pared to predictions from multiple models of different composition and mixing state assumptions. The best CCN closure used an external mixture of inorganic and organic aerosol components, with a modelled to observed ratio of 1.37 ± 0.32. It was hypothesised that this large ratio and the relatively low bulk hy- groscopicity was influenced by an external mixture. Incorporating this external mixture is imperative if CCN are to be accurately modelled and any subsequent cloud processes accurately captured.

O objetivo deste trabalho foi estudar o papel dos aerossóis em modificar o desenvolvimento das nuvens e da precipitação. Esta tem sido uma das mais intrigantes questões no estudo das mudanças climáticas. Medidas da concentração de núcleos de condensação de nuvens (CCN) e distribuições de gotículas de nuvem durante o Experimento de Grande Escala da Biosfera-Atmosfera na Amazônia (LBA) revelaram características distintas entre condições atmosféricas limpas e poluídas. As medidas foram conduzidas no Sudoeste da Região Amazônica durante os meses de setembro e outubro de 2002, focando a transição do final da estação seca para o início da estação chuvosa. Durante a transição, a análise da concentração de CCN dentro da camada limite revelou um decréscimo geral, de valores acima de 1200 cm-3 para menos de 300 cm-3. A comparação entre áreas limpas e poluídas mostrou concentrações de CCN cerca de 5 vezes maiores em áreas poluídas. As diferenças não foram tão grandes nos níveis acima da camada limite. As medidas também mostraram um ciclo diurno acompanhando a atividade de queima de biomassa. Distribuições de tamanho de gotículas medidas em duas regiões com concentrações de aerossóis extremamente diferentes foram analisadas. Em condições poluídas pela queima de biomassa foi encontrada alta concentração de gotículas, com diâmetro médio e conteúdo de água de nuvem aumentando muito pouco com a altura, em comparação com regiões limpas. A função gama foi usada para ajustar as distribuições de gotículas e o parâmetro de forma da função foi usado como critério para definir adequadamente a melhor representação das distribuições de gotículas. De acordo com os valores encontrados, distribuições gama estreitas (parâmetro de forma em torno de 5) são mais bem indicadas para representar condições poluídas enquanto que aquelas mais largas se ajustam melhor em condições limpas (parâmetro de forma em torno de 2). Com base nesses resultados, experimentos numéricos foram conduzidos com o Brazilian Regional Atmospheric Modeling System (BRAMS) para investigar os efeitos da concentração de CCN e do parâmetro de forma das distribuições de gotículas no desenvolvimento da precipitação em nuvens convectivas tropicais. Os resultados mostraram uma grande sensibilidade devido às mudanças nesses parâmetros. Altas concentrações de CCN e distribuições de gotículas estreitas (parâmetros de forma maiores), típicas de dias poluídos, produziram baixos valores médios para água líquida integrada na coluna e precipitação acumulada na superfície. Por outro lado, tendência oposta a este efeito foi encontrada em condições limpas (baixos valores para ambos, a concentração de CCN e o parâmetro de forma). O parâmetro de forma se mostrou ser mais importante que a concentração de CCN. Os efeitos da concentração de CCN e do parâmetro de forma também influenciaram a distribuição espacial dos campos de nuvem e precipitação. Embora o valor médio desses campos tenha diminuído em condições poluídas, o valor máximo aumentou. Como conseqüência da menor dispersão nas nuvens em condições poluídas, mais radiação solar esteve disponível na superfície. Isto é oposto aos resultados dos modelos globais que mostram redução na radiação solar como conseqüência do segundo efeito indireto dos aerossóis. Da mesma forma, este estudo encontrou que as diferenças são reduzidas quando é incluído o efeito direto dos aerossóis em absorver ou refletir a radiação solar. Sobretudo, os resultados sugerem que um maior número de modelos com tratamento explícito dos processos microfísicos de nuvem são necessários. Esses modelos permitem comparações, podendo mostrar o melhor tratamento numérico a ser usado na representação dos efeitos dos aerossóis no processo de precipitação como um todo. Estes resultados são importantes porque melhoram a compreensão de como o clima será afetado como conseqüência das mudanças futuras. / The objective of this work was to study the role of aerosols in modifying clouds and precipitation. This is one of the most difficult aspects in the study of climate changes. Field measurements of cloud condensation nuclei (CCN) and cloud size distributions performed during the Large Scale Biosphere-Atmosphere Experiment in Amazonia (LBA) campaign revealed distinct characteristics between clean and polluted atmospheric conditions. Measurements were conducted over the southwestern Amazon region during September-October 2002 focusing the transition from dry to wet seasons. During this period, analysis of CCN concentrations in the boundary layer revealed a general decreasing trend from mean values higher than 1200 cm-3 to values lower than 300 cm-3. The comparison between clean and polluted areas showed CCN concentrations 5 times higher than in polluted areas. These differences were not so strong above the boundary layer. Measurements also showed a diurnal cycle following the biomass burning activity. Cloud droplet size distributions at two regions with extremely different aerosols loading were also analyzed. During biomass-burning conditions, at high concentrations of cloud droplets, the mean diameter and liquid water content increased very little with altitude when compared with unpolluted conditions. A gamma distribution was used to fit the measured droplet spectra and the shape parameter was used as a criterion to define the best choice of spectra representation. According to the found values, narrow gamma distributions optimally fit polluted conditions (shape parameter around 5), while broad distributions are best fits for unpolluted conditions (shape parameter around 2). Based on these results, numerical experiments were carried out using the Brazilian Regional Atmospheric Modeling System (BRAMS) to investigate the effects of CCN concentrations and shape parameters of droplet spectra on the development of precipitation in tropical convective clouds. The results showed large sensitivity due to changes in these parameters. It was observed that high CCN concentrations and narrower cloud droplet distributions (high values for shape parameter), typical of the polluted days, produced low mean values of liquid water path and accumulated surface precipitation. On the other hand, an opposite trend to this effect was found under clean conditions (low CCN concentration and shape parameter values). Shape parameter showed to be much more important than CCN concentration. The effects of CCN concentration and shape parameter also influenced the spatial distribution of cloud and precipitation fields. Although mean values of these fields decreased under polluted conditions, maximum values were increased. Consequently, the less dispersion in clouds under polluted conditions, the more surface solar radiation was found. This is opposite to the results of global climate models, which predict reduction in solar radiation as a consequence of the second aerosol indirect effect. Also, it was found that the differences were reduced when the aerosols direct effect to absorb or reflect solar radiation is included. Moreover, the results suggest that additional models with explicit microphysics process treatment are necessary in order to allow further comparisons, which could show the best numerical treatment to be used in representing the aerosol effects on precipitation process. The importance of these results is to improve the understanding of future climate changes.

Près de la moitié des patients atteints de sclérodermie systémique (ScS) présentent des troubles de la pigmentation cutanée. La mélanogenèse est sous la dépendance, outre les facteurs épidermiques, de facteurs dermiques produits par les fibroblastes et les cellules endothéliales. Parmi ces facteurs se trouve NOV (CCN3) (protéine appartenant à la même famille que CTGF (CCN2), protéine pro-fibrotique augmentée dans la ScS) qui aurait un rôle anti-fibrotique. Nous souhaitons ainsi disséquer le lien entre la composante fibrotique dermique et la pigmentation épidermique. Pour cela, des biopsies cutanées ont été réalisées chez 21 patients ScS, en zone lésionnelle (scléreuse avec ou sans trouble de pigmentation) et non lésionnelle pour 12 d’entre eux. Ces biopsies ont été séparées en 3 fragments qui ont été soit fixés pour analyses histologiques et immunohistochimiques, soit congelés à -80°C pour analyse protéomique ou transcriptomique, soit dissociés pour isoler les cellules cutanées afin de les analyser en protéomique ou transcriptomique. Des témoins de peau et des cellules saines sont utilisées en contrôle. Nous avons dégagé deux types de troubles pigmentaires : une hyperpigmentation s’apparentant à un photo-vieillissement, et une dépigmentation péri-folliculaire apparaissant de manière précoce. Les niveaux d’expression de CCN2 et CCN3 varient chez les patients en fonction des données cliniques, aussi bien au niveau protéique qu’au niveau immunohistochimique. S’il existe des différences en fonction de l’atteinte pigmentaire, il semble que dans les fibroblastes sclérodermiques, la balance CCN2/CCN3 soit déséquilibrée tant au niveau de la zone lésionnelle que cliniquement non lésionnelle, suggérant que CCN2 et 3 pourraient être dérégulés intrinsèquement ou à des stades précoces. Ce travail pourrait aboutir à l’identification d’un phénotype précoce basé sur l’atteinte pigmentaire, et au développement d’une thérapie basée sur la rééquilibration du ratio CCN2/CCN3. / Systemic Sclerosis (SSc) is a rare but potentially deadly connective tissue disease. Its pathophysiology remains partly unknown but combines auto-immunity, small and large vessels involvement and fibrosis of the connective tissue, affecting all organs. Skin features are considered as diagnostic and prognosis markers and include for some patients the presence of pigmentary disorders. In this work, we looked into pigmentary disorders in SSc and their relationship with the pathophysiology of the disease. First, we analyzed the presence of pigmentary disorders among a local cohort of 239 patients as well as their association with systemic involvement in the disease. We have found that diffuse hyperpigmentation was associated with an increased risk of vascular involvement in SSc, particularly digital ulcers. Then, we investigated the molecular basis behind this association. Proteins of the CCN (CYR61 / CTGF / NOV) family are multimodular proteins secreted in the extra-cellular matrix, where they take part in numerous biological processes, such as cell proliferation, adhesion, collagen secretion. Within this family, CCN3 (also called NOV) is a promising candidate, being implicated both in angiogenesis and epidermal homeostasis. We studied CCN3 expression in the skin of SSc patients presenting or not pigmentary disorders, as compared to healthy controls. We found that CCN3 expression was particularly decreased in the dermal vessels in situ, as well as in endothelial cells in vitro. CCN3 inhibition in endothelial cells resulted in altered angiogenesis in vitro, through a decrease in cell migration. We also studied CCN3 expression in SSc epidermis. SSc patients presenting hyperpigmentation exhibited decreased CCN3 in their melanocytes as well as increased CCN3 in their keratinocytes, compared to patients without pigmentary disorders. Overall, CCN3 represents a promising therapeutic lead for SSc patients with vascular involvement, which could bespotted early thanks to the presence of hyperpigmentation.

The indirect effect of atmospheric aerosol on climate remains a large source of uncertainty in anthropogenic climate change prediction. An important fraction of this uncertainty arises from the impacts of organic aerosol on cloud droplet formation. Conventional thinking says that organic aerosol hygroscopicity, typically represented by the hygroscopicity parameter κ, increases with oxidation, most commonly represented by the oxygen to carbon ratio of the aerosol, O:C. Furthermore, these quantities are expected to increase as aerosol volatility decreases. Results indicate that the link between organic aerosol hygroscopicity and oxidation is not always straightforward, and in some cases, the average carbon oxidation state OSc appears to be a better indicator of oxidation than the oxygen to carbon ratio, O:C. In chamber and ambient studies, the least volatile fraction of the aerosol also appeared to be the least hygroscopic, contradictory to current thinking; however, in both cases, thermally-denuded aerosol showed greater oxidation, in terms of OSc, than non-denuded aerosol. When these findings are placed in the context of numerous published studies from a variety of different environment, the overall trend of increasing organic hygroscopicity with O:C still holds. This is also true for volatilized aerosol, though the magnitude of organic hygroscopicity is generally lower than that of non-denuded aerosol.

Le but de ce travail de thèse est d'améliorer la compréhension des interactions aérosols -nuages. Pour ce faire, nous avons dû traiter des sujets aussi larges et divers que le développement de moyens instrumentaux, l'analyse statistique et la modélisation. Ainsi, nous avons été amenés à installer et à développer un échantillonneur d'air nuageux. Il permet maintenant un échantillonnage en nuages en continu à l'observatoire du sommet du puy de Dôme. Il s'en est suivi deux campagnes de mesures durant les hivers 2000 et 2001 aboutissant à la collecte de plus de 600000 échantillons. Grâce à ce large panel de conditions météorologiques et d'origines de masses d'air, nous avons pu quantifier un des points clés de l'étude des relations aérosol - nuage. Nous avons pu obtenir une relation entre la concentration totale de particules d'aérosol et, d'une part la concentration de gouttelettes de nuages, et d'autre part le rayon effectif du nuage pour un contenu en eau liquide du nuage constant. De plus, l'utilisation d'un modèle d'activation des gouttelettes de nuage appelé ExMix nous a permis d'avoir une meilleure compréhension de l'évolution de l'incorporation des particules dans le nuage. Ainsi, nous avons pu comparer ces variations avec le contenu en eau qui augmente ou avec le rayon effectif du nuage pour un contenu en eau constant des sorties du modèle à celles mesurées. Toutefois, cela a montré le manque important d'une mesure physico-chimique de l'aérosol avec une fréquence de mesure élevée permettant par exemple une meilleure prise en compte de la phase organique de l'aérosol. C'est pourquoi, un analyseur de la volatilité et de la granulométrie des aérosols a été développé, construit et testé durant la dernière partie de ce travail de thèse.

This dissertation describes the use of measured aerosol size distributions and size-resolved hygroscopic growth to examine the physical and chemical properties of several particle classes. The primary objective of this work was to investigate the optical and cloud forming properties of a range of ambient aerosol types measured in a number of different locations. The tool used for most of these analyses is a differential mobility analyzer / tandem differential mobility analyzer (DMA / TDMA) system developed in our research group. To collect the data described in two of the chapters of this dissertation, an aircraft-based version of the DMA / TDMA was deployed to Japan and California. The data described in two other chapters were conveniently collected during a period when the aerosol of interest came to us. The unique aspect of this analysis is the use of these data to isolate the size distributions of distinct aerosol types in order to quantify their optical and cloud forming properties. I used collected data during the Asian Aerosol Characterization Experiment (ACE-Asia) to examine the composition and homogeneity of a complex aerosol generated in the deserts and urban regions of China and other Asian countries. An aircraft-based TDMA was used for the first time during this campaign to examine the size-resolved hygroscopic properties of the aerosol. The Asian Dust Above Monterey (ADAM-2003) study was designed both to evaluate the degree to which models can predict the long-range transport of Asian dust, and to examine the physical and optical properties of that aged dust upon reaching the California coast. Aerosol size distributions and hygroscopic growth were measured in College Station, Texas to investigate the cloud nucleating and optical properties of a biomass burning aerosol generated from fires on the Yucatan Peninsula. Measured aerosol size distributions and size-resolved hygroscopicity and volatility were used to infer critical supersaturation distributions of the distinct particle types that were observed during this period. The predicted cloud condensation nuclei concentrations were used in a cloud model to determine the impact of the different aerosol types on the expected cloud droplet concentration. RH-dependent aerosol extinction coefficients were also calculated.