Thesis advisor: Paul Davidovits / Aerosol particles are an important component of the Earth-Atmosphere system because of their influence on the radiation budget both directly (through absorption and scattering) and indirectly (through cloud condensation nuclei (CCN) activity). The magnitude of the raditaive forcing attributed to the direct and indirect aerosol effects is highly uncertain, leading to large uncertainties in projections of global climate change. Real-time measurements of aerosol properties are a critical step toward constraining the uncertainties in current global climate modeling and understanding the influence that anthropogenic activities have on the climate. The objective of the work presented in this thesis is to gain a more complete understanding of the atmospheric transformations of aerosol particles and how such transformations influence the direct and indirect radiative effects of the particles. The work focuses on real-time measurements of aerosol particles made with the Aerodyne Aerosol Mass Spectrometer (AMS) developed in collaboration with the Boston College research group. A key feature of the work described is the development of a lightscattering module for the AMS. Here we present the first results obtained with the integrated light scattering – AMS system. The unique and powerful capabilities of this new instrument combination are demonstrated through laboratory experiments and field deployments. Results from two field studies are presented: (1) The Northeast Air Quality Study (NEAQS), in the summer of 2004, conducted at Chebogue Point, Nova Scotia and (2) The Megacity Initiative: Local and Global Research Observations (MILAGRO) field campaign conducted in and around Mexico City, Mexico in March of 2006. Both field studies were designed to study the transformations that occur within pollution plumes as they are transported throughout the atmosphere. During the NEAQS campaign, the pollution plume from the Northeastern United States was intercepted as it was transported towards Europe. In this study, particles were highly processed prior to sampling, with residence times of a few days in the atmosphere. The MILAGRO campaign focused on the evolution of the Mexico City plume as it was transported north. During this study, regional and locally emitted particles were measured with residence times varying from minutes to days in the atmosphere. In both studies, the light scattering – AMS system provided detailed information about the density and composition of single particles, leading to important insights into how atmospheric processing transforms the particle properties. In Mexico City, the light scattering-AMS system was used for the first time as a true single particle mass spectrometer and revealed specific details about the atmospheric processing of primary particles from combustion sources.To quantify the radiative effects of the particles on climate, the processing and ultimate fate of primary emissions (often containing black carbon or soot) must be understood. To provide a solid basis for the interpretation of the data obtained during the field studies, experiments were conducted with a well characterized soot generation-sampling system developed by the Boston College research group. The laboratory soot source was combined with the light scattering – AMS system and a Cloud Condensation Nuclei Counter (CCNC) to measure the change in cloud-forming activity of soot particles as they are processed in the atmosphere. Because of the importance of black carbon in the atmosphere, several instruments have been developed to measure black carbon. In July of 2008, an intercomparison study of 18 instruments was conducted in the Boston College laboratory, with soot particles produced and processed to mimic a wide range of atmospherically-relevant conditions. Transformations in the physical, chemical, and optical properties of soot particles were monitored with the combined suite of aerosol instrumentation. Results from the intercomparison study not only calibrated the different instruments used in the study, but also provided critical details about how atmospheric processing influences the radiative effects of primary combustion particles. / Thesis (PhD) — Boston College, 2008. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Chemistry.

Primary marine aerosol particles containing biogenic polymer microgels play a potential role for cloud formation in the pristine high Arctic summer. One of the major sources of the polymer gels in Arctic aerosol was suggested to be the surface water and more specifically, the surface microlayer (SML) of the open leads within the perennial sea ice as a result of bubble bursting at the air-sea interface.  Phytoplankton and/or ice algae are believed to be the main origins of the polymer gels. In this thesis, we examine the chemical composition of biogenic polymers, with focus on polysaccharides, in seawater and airborne aerosol particles collected during the Arctic Summer Cloud Ocean Study (ASCOS) in the summer of 2008. The main results and findings include: A novel method using liquid chromatography coupling with tandem mass spectrometry was developed and applied for identification and quantification of polysaccharides. The enrichment of polysaccharides in the SML was shown to be a common feature of the Arctic open leads. Rising bubbles and surface coagulation of polymers are the likely mechanism for the accumulation of polysaccharides at the SML. The size dependencies of airborne polysaccharides on the travel-time since the last contact with the open sea are indicative of a submicron microgel source within the pack ice.  The similarity of polysaccharides composition observed between the ambient aerosol particles and those generated by in situ bubbling experiments confines the microgel source to the open leads. The demonstrated occurrence of polysaccharides in surface sea waters and in air, with surface-active and hygroscopic properties, has shown their potential to serve as cloud condensation nuclei and subsequently promote cloud-drop activation in the pristine high Arctic. Presumably this possibility may renew interest in the complex but fascinating interactions between marine biology, aerosol, clouds and climate. / At the time of doctoral defence, the following paper was unpublished and had a status as follows: Paper 4: Manuscript

This study focuses on the analysis of atmospheric particles sampled from two different field campaigns: the field study at a cattle feeding facility in the summer from 2005 to 2008 and the Indirect and Semi-Direct Aerosol Campaign (ISDAC) in 2008. A ground site field study at a representative large cattle feeding facility in the Texas Panhandle was conducted to characterize the particle size distributions, hygroscopicity, and chemical composition of agricultural aerosols. Here, a first comprehensive dataset is reported for these physical and chemical properties of agricultural aerosols appropriate for use in a site-specific emission inventory. The emission rate and transport of the aerosols are also discussed. In addition, mixing ratios of total and gaseous ammonia were measured at the same field in 2007 and 2008. Measurements such as these provide a means to determine whether the fugitive dust emitted from a typical large feedlot represents a health concern for employees of the feeding operation and the nearby community. Detailed chemical composition of aircraft-sampled particles collected during ISDAC was studied. Filter samples were collected under a variety of conditions in and out of mixed phase and ice clouds in the Arctic. Specifically, particles were sampled from a mixed-phase cloud during a period of observed high concentrations of ice nuclei (IN), a biomass plume, and under relatively clean ambient conditions. Composition of particles was studied on a particle-by-particle basis using several microspectroscopy techniques. Based on the elemental composition analysis, more magnesium was found in Arctic cloud residues relative to ambient air. Likewise, based on the carbon speciation analysis, high IN samples contained coated inorganics, carbonate, and black or brown carbon particles. In the samples collected during a flight through a biomass burning plume, water-soluble organic carbon was the dominant overall composition. Due to their hygroscopic nature, these organics may preferably act as cloud condensation nuclei (CCN) rather than IN. Other ambient samples contained relatively higher fractions of organic and inorganic mixtures and less purely water-soluble organics than found in the biomass particles. The most likely source of inorganics would be sea salt. When present, sea salt may further enhance ice nucleation.

Recent research has shown that secondary organic aerosols (SOA) are major contributors to ultrafine particle growth to climatically relevant sizes, increasing global cloud condensation nuclei (CCN) concentrations within the continental boundary layer (BL). This thesis contains two separate studies investigating SOA characteristics and the implications of SOA on global climate. The first study investigates two critical, but uncertain, characteristics of SOA: (1) the amount of SOA available to condense and (2) the volatility or condensational behavior of SOA. The second study investigates the effect of biological volatile organic compound (BVOC) emission changes on SOA formation from preindustrial to present day, and the effect on CCN concentrations using BVOC emission estimates over the last millennium.

Aerosols have significant impacts on earth's climate and hydrological cycle. They can directly reflect the amount of incoming solar radiation into space; by acting as cloud condensation nuclei (CCN), they can indirectly impact climate by affecting cloud albedo. Our current assessment of the interactions of aerosols and clouds is uncertain and parameters used to estimate cloud droplet formation in global climate models are not well constrained. Organic aerosols attribute much of the uncertainty in these estimates and are known to affect the ability of aerosol to form cloud droplets (CCN Activity) by i) providing solute, thus reducing the equilibrium water vapor pressure of the droplet and ii) acting as surfactants capable of depressing surface tension, and potentially, growth kinetics. My thesis dissertation investigates various organic aerosol species (e.g., marine, urban, biomass burning, Humic-like Substances). An emphasis is placed on the water soluble components and secondary organic aerosols (SOA). In addition the sampled organic aerosols are acquired via different media; directly from in-situ ambient studies (TEXAQS 2006) environmental chamber experiments, regenerated from filters, and cloud water samples. Novel experimental methods and analyses to determine surface tension, molar volumes, and droplet growth rates are presented from nominal volumes of sample. These key parameters for cloud droplet formation incorporated into climate models will constrain aerosol-cloud interactions and provide a more accurate assessment for climate prediction.

A change in atmospheric aerosol particles, especially cloud condensation nuclei (CCN) and ice-nucleating particles (INPs), is bound to impact cloud properties, precipitation and cloud radiative effects. In this thesis, two field campaigns were carried out in two representative locations, i.e. the anthropogenic polluted environment at Cyprus and the marine-dust intersect environment at Cabo Verde (a.k.a. Cape Verde) to understand the role of CCN and INPs over the tropical and subtropical regions in the northern hemisphere. On-line aerosol physical measurements were performed and samples from different environ- mental compartments were examined with respect to INPs: the oceanic sea surface microlayer (SML), underlying water (ULW), cloud water and atmospheric filters. Both measurement sites differ in aerosol properties, such as particle number size distribution, CCN and INP concentrations and CCN-derived particle hygroscopicity, due to different environment backgrounds and air mass origins. Aerosol particles at Cyprus were dominated by anthropogenic pollution, with small contributions of sea spray aerosol (SSA) and mineral dust. Particle aging process were observed through changes in CCN-derived particle hygroscopicity. New particle formation events with subsequent growth of the particles into the CCN size range were observed. INPs mainly originated from long-range transport. And anthropogenic pollution were found to be inefficient INPs at temperature range >−25 ◦C. However, aerosol particles at Cabo Verde featured a marine background with intrusions of dust. Dust and marine aerosols featured clearly different PNSDs. CCN number concentration at a supersaturation of 0.30% during the strongest observed dust periods was about 2.5 times higher than during marine periods. However, the CCN-derived hygroscopicity for marine and dust periods shows no significant difference. INPs at Cabo Verde were mainly in the supermicron size range, with a large contribution of biological particles. When comparing atmospheric INP number concentration to those found in seawater, it can be concluded that SSA only contributed a minor fraction to the atmospheric INP population.:1 Introduction 2 Methodology 3 Results and Discussion 4 Summary and Conclusions 5 Outlook Appendix Bibliography / Veränderungen im atmosphärischen Aerosol, speziell bei Wolkenkondensationskernen (CCN) und eisnukleierenden Partikeln (INPs), haben Auswirkungen auf Wolkeneigenschaften wie Niederschlagsbildung und Strahlung. Für die hier vorgelegte Arbeit wurden zwei Feldmesskampagnen durchgeführt, im anthropogen verschmutzten Zypern und auf Cabo Verde (alias Kap Verde), einer Schnittstelle zwischen Meer und Wüste. Ziel war es, die Rolle von CCN und INPs in den tropischen und subtropischen Regionen der nördlichen Hemisphäre besser zu verstehen. Es wurden aerosol-physikalische online Messungen durchgeführt und verschiedene Proben auf INPs hin untersucht: die Meeresoberflächen-Mikroschicht (SML), das darunter liegende Wasser (ULW), das Wolkenwasser und atmosphärische Filter. Die beiden verschiedenen Orte an denen die Messkampagnen stattfanden unterscheiden sich in den Aerosoleigenschaften wie z.B. Partikelanzahlgrößenverteilung (PNSD), CCN- und INP-Konzentration und der von CCN abgeleiteten Partikelhygroskopizität. Grund hierfür sind Unterschiede in der Umgebung und der Luftmassenherkunft. Die Aerosolpartikel auf Zypern wurden von anthropogener Verschmutzung dominiert, mit kleinen Beiträgen von Partikeln aus Meeres-Gischt (SSA) und Mineralstaub. Partikelalterung ging einher mit einer Veränderung der Hygroskopizität der CCN. Partikelneubildung wurde beobachtet, mit anschließendem Wachstum der Partikel bis in den CCN-Größenbereich. INPs stammen hauptsächlich aus Ferntransport, und Partikel aus anthropogener Verschmutzung waren ineffiziente INPs im Temperaturbereich >−25 ◦C. Das Aerosol in Cabo Verde speiste sich sowohl aus marinen Quellen als auch aus Wüstenstaub. Staub und marines Aerosol wiesen sehr verschiedene PNSDs auf. Die CCN-Anzahlkonzentration bei 0,30% Übersättigung war während der stärksten Staubperioden etwa 2,5 Mal höher als während der marinen Perioden. Die aus CCN abgeleitete Hygroskopizität zeigte jedoch keinen signifikanten Unterschied für marine und Staubperioden. Die INPs in Cabo Verde waren zum Großteil größer als ein Mikrometer, und waren zum Großteil biogenen Ursprungs. Aus dem Vergleich der atmosphärischen INP-Anzahlkonzentration mit der im Meerwasser gefundenen kann man schließen, dass SSA nur einen geringen Anteil zur atmosphärischen INP-Population beitrug.:1 Introduction 2 Methodology 3 Results and Discussion 4 Summary and Conclusions 5 Outlook Appendix Bibliography

Despite large efforts and decades of research, the scientific understanding of how aerosols impact climate by modulating microphysical cloud properties is still low and associated radiative forcing estimates (RFaci ) vary with a wide spread. But since anthropogenically forced aerosol-cloud interactions (ACI) are considered to oppose parts of the global warming, it is crucial to know their contribution to the total radiative forcing in order to improve climate predictions. To obtain a better understanding and quantification of ACI and the associated radiative effect it as been suggested to use concurrent measurements and observationally constrained model simulations. In this dissertation a joint satellite-reanalysis approach is introduced, bridging the gap between climate models and satellite observations in a bottom-up approach. This methodology involves an observationally constrained aerosol model, refined and concurrent multi-component satellite retrievals, a state-of-the-art aerosol activation parameteriza- tion as well as radiative transfer model. This methodology is shown here to be useful for a quantitative as well as qualitative analysis of ACI and for estimating RFaci . As a result, a 10-year long climatology of cloud condensation nuclei (CCN) (particles from which cloud droplets form) is produced and evaluated. It is the first of its kind providing 3-D CCN concentrations of global coverage for various supersaturations and aerosol species and offering the opportunity to be used for evaluation in models and ACI studies. Further, the distribution and variability of the resulting cloud droplet numbers and their susceptibility to changes in aerosols is explored and compared to previous estimates. In this context, an analysis by cloud regime has been proven useful. Last but not least, the computation and analysis of the present-day regime-based RFaci represents the final conclusion of the bottom-up methodology. Overall, this thesis provides a comprehensive assessment of interactions and uncertainties related to aerosols, clouds and radiation in regimes of liquid water clouds and helps to improve the level of scientific understanding.

Abstract Aerosol-cloud and aerosol-radiation interactions depend on several factors such as the physico-chemical properties, geographical and temporal variability, and vertical distribution of atmospheric aerosols. Of particular importance are cloud condensation nuclei (CCN) and black carbon (BC) particles as a subset of the atmospheric aerosol population. CCN are a prerequisite for cloud droplet formation, and variations in CCN loading can modify cloud properties. BC can efficiently absorb solar radiation, induce local heating and inhibit cloud formation. In order to determine the effects of CCN and BC on clouds, precipitation, radiation and the Earth’s energy budget, atmospheric loading and spatio-temporal distribution of aerosols are highly relevant. Thus this dissertation addresses and helps to elucidate the spatio-temporal variation and co-variability of CCN and BC with extensive field measurement data from aircraft and ground-based measurements. The data analyses focus on anthropogenic pollution, wildfire emissions and volcanic aerosols. In the Anthropocene, the distribution and abundance of atmospheric aerosols have changed drastically. Major sources of anthropogenic particulate pollution are the combustion of fossil fuels and biofuels as well as emissions from open biomass burning. The ubiquitous presence of anthropogenic air pollution, especially over continental regions in the Northern Hemisphere, hampers the assessment of anthropogenic influence on aerosol and climate due to a lack of unperturbed reference measurements. The abrupt reduction in human activities during the first COVID-19 lockdown created unprecedented atmospheric conditions that allowed us to investigate and quantify changes in the tropospheric composition in response to changes in anthropogenic emissions. The results reflect a strong and immediate influence of human activities on air quality, the role of BC as a major air pollutant in the Anthropocene, and close links between the atmospheric burdens of CCN and BC. Measurement data from five aircraft missions in polluted environments reveal characteristic relationships between CCN and BC in urban haze from Europe and East Asia, highly aged biomass burning smoke over the tropical Atlantic and the Amazon rainforest, and lightly aged biomass burning smoke over Europe, Brazil, and Asia. Over Europe and Asia, the vertical distribution of CCN in the lower troposphere up to altitudes about 5 km is highly sensitive to regional anthropogenic emissions. Over the tropical Atlantic ocean, the vertical distribution is strongly influenced by the longrange transport of mineral dust and biomass burning smoke, but volcanic eruptions also contribute to the aerosol load.

Aerosol-cloud interactions are the most uncertain component of the anthropogenic radiative forcing. A substantial part of this uncertainty comes from the limitations of currently used spaceborne CCN proxies that (i) are column integrated and do not guarantee vertical co-location of aerosols and clouds, (ii) have retrieval issues over land, and (iii) do not account for aerosol hygroscopicity. A possible solution to overcome these limitations is to use height-resolved measurements of the spaceborne lidar aboard the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) satellite. This thesis presents a novel CCN retrieval algorithm based on Optical Modelling of CALIPSO Aerosol Microphysics (OMCAM) that is designed particularly for CALIPSO lidar measurements, along with its validation with airborne and surface in-situ measurements. \noindent OMCAM uses a set of normalized size distributions from the CALIPSO aerosol model and modifies them to reproduce the CALIPSO measured aerosol extinction coefficient. It then uses the modified size distribution and aerosol type-specific CCN parameterizations to estimate the number concentration of CCN (nCCN) at different supersaturations. The algorithm accounts for aerosol hygroscopicity by using the kappa parametrization. Sensitivity studies suggest that the uncertainty associated with the output nCCN may range between a factor of 2 and 3. OMCAM-estimated aerosol number concentrations (ANCs) and nCCN are validated using temporally and spatially co-located in-situ measurements. In the first part of validation, the airborne observations collected during the Atmospheric Tomography (ATom) mission are used. It is found that the OMCAM estimates of ANCs are in good agreement with the in-situ measurements with a correlation coefficient of 0.82, an RMSE of 247.2 cm-3, and a bias of 44.4 cm-3. The agreement holds for all aerosol types, except for marine aerosols, in which the OMCAM estimates are about an order of magnitude smaller than the in-situ measurements. An update of the marine model in OMCAM improve the agreement significantly. In the second part of validation, the OMCAM-estimated ANC and nCCN are compared to measurements from seven surface in-situ stations covering a variety of aerosol environments. The OMCAM-estimated monthly nCCN are found to be in reasonable agreement with the in-situ measurements with a 39 % normalized mean bias and 71 % normalized mean error. Combining the validation studies, the algorithm outputs are found to be consistent with the co-located in-situ measurements at different altitude ranges over both land and ocean. Such an agreement has not yet been achieved for spaceborne-derived CCN concentrations and demonstrates the potential of using CALIPSO lidar measurements for inferring global 3D climatologies of CCN concentrations related to different aerosol types.:1 Introduction . . . . . . . . . . . . . . . 1 1.1 Background: Aerosols in the climate system . . . . . . . . . . . . . . . . . 1 1.1.1 Aerosol-induced effective radiative forcing . . . . . . . . . . . . . . 3 1.1.2 Significance of aerosol-cloud interactions . . . . . . . . . . . . . . . 3 1.2 Observation-based ACI studies . . . . . . . . . . . . . . . . . . . . . . . . 4 1.2.1 In-situ studies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5 1.2.2 Spaceborne studies . . . . . . . . . . . . . . . . . . . . . . . . . . . 5 1.3 Spaceborne CCN proxies and their limitations . . . . . . . . . . . . . . . . 8 1.4 CCN concentrations from lidars . . . . . . . . . . . . . . . . . . . . . . . . 10 1.5 Objective: CCN from spaceborne lidar . . . . . . . . . . . . . . . . . . . . 11 2 Paper 1: Estimating cloud condensation nuclei concentrations from CALIPSO lidar measurements . . . . . . . . . . . . . . . 15 2.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16 2.2 Data and retrievals . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18 2.2.1 CALIPSO . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18 2.2.2 MOPSMAP . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19 2.2.3 POLIPHON . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19 2.3 Methodology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20 2.3.1 Aerosol size distribution . . . . . . . . . . . . . . . . . . . . . . . . 20 2.3.2 Aerosol hygroscopicity . . . . . . . . . . . . . . . . . . . . . . . . . 23 2.3.3 CCN parameterizations . . . . . . . . . . . . . . . . . . . . . . . . 23 2.3.4 Application of OMCAM to CALIPSO retrieval . . . . . . . . . . . 23 2.4 Results . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24 2.4.1 Sensitivity analysis . . . . . . . . . . . . . . . . . . . . . . . . . . . 24 2.4.2 Comparison with POLIPHON . . . . . . . . . . . . . . . . . . . . . 30 2.4.3 Case study . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32 2.5 Summary and conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . 35 3 Paper 2: Evaluation of aerosol number concentrations from CALIPSO with ATom airborne in situ measurements . . . . . . . . . . . . . . . 39 3.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 40 3.2 Data, retrievals, and methods . . . . . . . . . . . . . . . . . . . . . . . . . 42 3.2.1 ATom 3.2.2 CALIOP . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 43 3.2.3 Aerosol number concentration from CALIOP . . . . . . . . . . . . 44 3.2.4 Data matching and comparison . . . . . . . . . . . . . . . . . . . . 48 3.3 Results . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 52 3.3.1 Example cases . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 52 3.3.2 General findings . . . . . . . . . . . . . . . . . . . . . . . . . . . . 55 3.4 Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 59 3.5 Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 61 3.6 Appendix . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 63 4 Paper 3: Assessment of CALIOP-derived CCN concentrations by in situ surface measurements . . . . . . . . . . . . . . . 65 4.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 66 4.2 Data and methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 68 4.2.1 In situ observations . . . . . . . . . . . . . . . . . . . . . . . . . . . 68 4.2.2 CALIOP . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 69 4.2.3 Comparison Methodology . . . . . . . . . . . . . . . . . . . . . . . 71 4.3 Comparison of CCN Concentrations . . . . . . . . . . . . . . . . . . . . . . 73 4.4 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 76 5 Summary and conclusions . . . . . . . . . . . . . . . 79 6 Outlook . . . . . . . . . . . . . . . 83 References . . . . . . . . . . . . . . . 88 List of Abbreviations . . . . . . . . . . . . . . . 107 List of Variables . . . . . . . . . . . . . . . 109 List of Figures . . . . . . . . . . . . . . . 111 List of Tables . . . . . . . . . . . . . . . 113 A List of Publications . . . . . . . . . . . . . . . 115 B Acknowledgements . . . . . . . . . . . . . . . 117

It is well known that atmospheric aerosols provide the sites for forming cloud droplets, and can affect the Earth's radiation budget through their interactions with clouds. The ability of aerosols to act as cloud condensation nuclei is a strong function of their chemical composition and size. The compositional complexity of aerosol prohibits their explicit treatment in atmospheric models of aerosol-cloud interactions. Nevertheless, the cumulative impact of organics on CCN activity is still required, as carbonaceous material can constitute up to 90% of the total aerosol, 10-70% of which is water soluble. Therefore it is necessary to characterize the water soluble organic carbon fraction by CCN activation, droplet growth kinetics, and surface tension measurements. In this thesis, we investigate the water soluble properties, such as surface tension, solubility, and molecular weight, of laboratory and ambient aerosols and their effect on CCN formation. A mechanism called Curvature Enhanced Solubility is proposed and shown to explain the apparent increased solubility of organics. A new method, called Köhler Theory Analysis, which is completely new, fast, and uses minimal amount of sample was developed to infer the molar volume (or molar mass) of organics. Due to the success of the technique in predicting the molar volume of laboratory samples, it was applied to aerosols collected in Mexico City. Additionally the surface tension, CCN activity, and droplet growth kinetics of these urban polluted aerosols were investigated. Studies performed for the water soluble components showed that the aerosols in Mexico City have surfactants present, can readily become CCN, and have growth similar to ammonium sulfate. Finally, aerosols from three different polluted sources, urban, bovine, and ship emissions, were collected and characterized. The data assembled was used to predict CCN concentrations and access our understanding of the system. From these analyses, it was evident that knowledge of the chemical composition and mixing state of the aerosol is necessary to achieve agreement between observations and predictions. The data obtained in this thesis can be introduced and used as constraints in aerosol-cloud interaction parameterizations developed for global climate models, which could lead to improvements in the indirect effect of aerosols.