No description available.

A field-deployable instrument has been developed that isolates from an ambient aerosol population only those particles that have critical supersaturations, Sc, within a narrow, user-specified, range. This Differential Critical Supersaturation Separator (DScS) is designed to supply one or more particle size and/or composition analyzers to permit the direct examination of the factors that influence the activation properties of ambient aerosols. The DScS consists of two coupled parallel plate continuous flow thermal gradient diffusion cloud chambers housed within a single enclosure. Descriptions of instrument operation, construction and calibration data collected, when pure ammonium sulfate aerosols were injected into the DScS for operation at 0.15%< Sc<0.175%, 0.30%< Sc<0.35%, and 0.60% < Sc<0.70%, are included. Following instrument development, the DScS was deployed during March 2006 for the Megacities Impact on Regional And Global Environment (MIRAGE) field campaign in Mexico City, Mexico. Throughout the MIRAGE field campaign a Differential Mobility Analyzer/Tandem Differential Mobility Analyzer (DMA/TDMA) system measured aerosol size distributions and size-resolved hygroscopicity of DScS separated aerosol. The dry diameter (Dp*) of particles sampled in the TDMA system as well as the known Sc prescribed in the DScS were combined in a modified version of Köhler Theory to make predictions of particle hygroscopicity. These predictions frequently overestimated the measurements. Further analysis of DScS separated aerosols compares the known particle Sc to a predicted particle Sc, providing insight into particle activation efficiency. Overall, the sampled aerosol exhibited properties that indicate they were more efficient at activation than Köhler Theory would predict.

A field-deployable instrument has been developed that isolates from an ambient aerosol population only those particles that have critical supersaturations, Sc, within a narrow, user-specified, range. This Differential Critical Supersaturation Separator (DScS) is designed to supply one or more particle size and/or composition analyzers to permit the direct examination of the factors that influence the activation properties of ambient aerosols. The DScS consists of two coupled parallel plate continuous flow thermal gradient diffusion cloud chambers housed within a single enclosure. Descriptions of instrument operation, construction and calibration data collected, when pure ammonium sulfate aerosols were injected into the DScS for operation at 0.15%< Sc<0.175%, 0.30%< Sc<0.35%, and 0.60% < Sc<0.70%, are included. Following instrument development, the DScS was deployed during March 2006 for the Megacities Impact on Regional And Global Environment (MIRAGE) field campaign in Mexico City, Mexico. Throughout the MIRAGE field campaign a Differential Mobility Analyzer/Tandem Differential Mobility Analyzer (DMA/TDMA) system measured aerosol size distributions and size-resolved hygroscopicity of DScS separated aerosol. The dry diameter (Dp*) of particles sampled in the TDMA system as well as the known Sc prescribed in the DScS were combined in a modified version of Köhler Theory to make predictions of particle hygroscopicity. These predictions frequently overestimated the measurements. Further analysis of DScS separated aerosols compares the known particle Sc to a predicted particle Sc, providing insight into particle activation efficiency. Overall, the sampled aerosol exhibited properties that indicate they were more efficient at activation than Köhler Theory would predict.

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.

A Differential Mobility Analyzer/Tandem Differential Mobility Analyzer (DMA/TDMA) system was used to measure simultaneously the size distribution and hygroscopicity of the ambient aerosol population. The system was operated aboard the National Center for Atmospheric Research/National Science Foundation (NCAR/NSF) C-130 during the 2006 Megacity Initiative: Local and Global Research Observations (MILAGRO) field campaign followed by the 2006 Intercontinental Chemical Transport Experiment – Phase B (INTEX-B) field campaign. The research flights for the MILAGRO campaign were conducted within the Mexico City basin and the region to the northeast within the pollution plume. The aerosol within the basin is dominated by organics with an average measured kappa value of 0.21 /- 0.18, 0.13 /- 0.09, 0.09 /- 0.06, 0.14 /- 0.07, and 0.17 /- 0.04 for dry particle diameters of 0.025, 0.050, 0.100, 0.200, and 0.300 mu m, respectively. As the aerosols are transported away from the Mexico City Basin, secondary organic aerosol formation through oxidation and condensation of sulfate on the aerosols surface rapidly increases the solubility of the aerosol. The most pronounced change occurs for a 0.100 mu m diameter aerosol where, after 6 hours of transport, the average kappa value increased by a factor of 3 to a kappaof 0.29 /- 0.13. The rapid increase in solubility increases the fraction of the aerosol size distribution that could be activated within a cloud. The research flights for the INTEX-B field campaign investigated the evolution of the physicochemical properties of the Asian aerosol plume after 3 to 7 days of transport. The Asian aerosol within the free troposphere exhibited a bimodal growth distribution roughly 50 percent of the time. The more soluble mode of the growth distribution contributed between 67-80 percent of the overall growth distribution and had an average kappabetween 0.40 and 0.53 for dry particle diameters of 0.025, 0.050, 0.100, and 0.300 mu m. The secondary mode was insoluble with an average kappabetween 0.01 and 0.05 for all dry particle diameters. Cloud condensation nuclei closure was attained at a supersaturation of 0.2 percent for all particles within the free troposphere by either assuming a pure ammonium bisulfate composition or a binary composition of ammonium bisulfate and an insoluble organic.

Numerous factors play a role in the development and maintenance of North Atlantic tropical cyclones as they originate and cross the Main Development Region. These factors include sea-surface temperatures (SSTs), relative humidity, vertical wind shear, etc. One key player in many of these factors is the Saharan Air Layer (SAL) which has been a source for study for nearly five decades. The interplay between dust loading within the SAL and the development of African Easterly Waves (AEWs) has been repeatedly noted in many of the studies in this field. The cumulative indirect effect of the dust on AEWs however remains unknown (Evan et al., 2006a). On a case by case basis, the SAL has been shown to negatively influence the development of AEWs, i.e. entrainment of dry air into the low to mid-levels, enhanced vertical wind shear and suppression of convection within the storm (Dunion & Velden, 2004). Positive influences on AEW development have also been attributed to the SAL, namely its enhancement of the African Easterly Jet (AEJ) which in turn helps produce positive vorticity along its southern edge that AEWs tap into for energy (Karyampudi & Pierce, 2002). Further study is indeed warranted to try to fully understand whether or not the SAL has a positive or negative influence on the development of AEWs. A polarized view may be inadequate, as the SAL’s role could very well be positive, negative or somewhere in between depending on the storm characteristics and environmental conditions present at that unique time. This study looked into the role dust loading has on the mixing between the SAL and the moist marine boundary layer directly beneath the base of the SAL, which can range from 500 – 1500m and revealed a dynamic and varying relationship. It also demonstrated, through a decrease in cloud top temperatures, that dust levels are associated with the convective strength of AEWs by acting as cloud condensation nuclei (CCNs). However this association can be nullified through other parameters unique to each individual storm; SSTs, vertical wind shear, dry-air entrainment, etc.

No description available.

Atmospheric aerosols are known to exert a significant influence on the Earth's climate system; however, the magnitude of this influence is highly uncertain because of the complex interaction between aerosols and water vapor to form clouds. Toward reducing this uncertainty, this dissertation outlines a series of laboratory and in-situ field measurements, instrument technique development, and model simulations designed to characterize the ability of aerosols to act as cloud condensation nuclei (CCN) and form cloud droplets. Specifically, we empirically quantify the mixing state and thermodynamic properties of organic aerosols (e.g., hygroscopicity and droplet condensational uptake coefficient) measured in polluted and non-polluted environments including Alaska, California, and Georgia. It is shown that organic aerosols comprise a substantial portion of the aerosol mass and are often water soluble. CCN measurements are compared to predictions from theory in order to determine the error associated with simplified composition and mixing state assumptions employed by current large-scale models, and these errors are used to constrain the uncertainty of global and regional cloud droplet number and albedo using a recently-developed cloud droplet parameterization adjoint coupled with the GMI chemical transport model. These sensitivities are important because they describe the main determinants of climate forcing. We also present two novel techniques for fast measurements of CCN concentrations with high size, supersaturation, and temporal resolution that substantially improve the state of the art by several orders of magnitude. Ultimately, this work represents a step toward better understanding how atmospheric aerosols influence cloud properties and Earth's climate.

Atmospheric particles can affect climate directly, by scattering solar radiation, or indirectly, by acting as the seed upon which cloud droplets form. These clouds can then cool the earth's surface by reflecting incoming sunlight. In order to constrain the large uncertainties in predicting the ultimate effect of aerosol on climate, the sources of atmospheric particles and their subsequent ability to turn into cloud droplets needs to be better understood. This thesis addresses two parts of this issue: the sources of Arctic aerosol and the hygroscopicity of continental organic aerosol. Small particles were observed in Baffin Bay during September 2008 that coincided with high atmospheric and ocean surface dimethyl sulphide (DMS) concentrations suggesting that the aerosol formed from oceanic sources. An aerosol microphysics box model confirmed that local DMS could have produced the observed particles. In addition, the particle chemical composition was measured using aerosol mass spectrometry in the central Arctic Ocean in August 2008 and particles were found to be 43% organic and 46% sulphate. Factor analysis further apportioned the aerosol mass to marine biogenic and continental sources 33% and 36% of the time, respectively, with the source of the remaining mass unidentified. The second part of the study parameterises the hygroscopicity of the ambient organic aerosol fraction (κorg) at Egbert, Ontario and Whistler, British Columbia. This was done using two methods: 1) by assuming that the oxygenated organic component was hygroscopic and that the unoxygenated organic component was non-hygroscopic, κ of the oxygenated component was found to be 0.22 ± 0.04, and 2) by assuming that κorg varied linearly with the atomic oxygen to atomic carbon ratio, it could be parameterised as κorg = (0.29 ± 0.05) × (O/C). Calculations predict that knowing κorg is important in urban, semi-urban, and remote locations whenever the inorganic mass fraction is low.

Atmospheric particles can affect climate directly, by scattering solar radiation, or indirectly, by acting as the seed upon which cloud droplets form. These clouds can then cool the earth's surface by reflecting incoming sunlight. In order to constrain the large uncertainties in predicting the ultimate effect of aerosol on climate, the sources of atmospheric particles and their subsequent ability to turn into cloud droplets needs to be better understood. This thesis addresses two parts of this issue: the sources of Arctic aerosol and the hygroscopicity of continental organic aerosol. Small particles were observed in Baffin Bay during September 2008 that coincided with high atmospheric and ocean surface dimethyl sulphide (DMS) concentrations suggesting that the aerosol formed from oceanic sources. An aerosol microphysics box model confirmed that local DMS could have produced the observed particles. In addition, the particle chemical composition was measured using aerosol mass spectrometry in the central Arctic Ocean in August 2008 and particles were found to be 43% organic and 46% sulphate. Factor analysis further apportioned the aerosol mass to marine biogenic and continental sources 33% and 36% of the time, respectively, with the source of the remaining mass unidentified. The second part of the study parameterises the hygroscopicity of the ambient organic aerosol fraction (κorg) at Egbert, Ontario and Whistler, British Columbia. This was done using two methods: 1) by assuming that the oxygenated organic component was hygroscopic and that the unoxygenated organic component was non-hygroscopic, κ of the oxygenated component was found to be 0.22 ± 0.04, and 2) by assuming that κorg varied linearly with the atomic oxygen to atomic carbon ratio, it could be parameterised as κorg = (0.29 ± 0.05) × (O/C). Calculations predict that knowing κorg is important in urban, semi-urban, and remote locations whenever the inorganic mass fraction is low.