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.

Optimal estimation retrieval is a nonlinear regression scheme to determine the conditions statistically most-likely to produce a given measurement, weighted against any a priori knowledge. The technique is applied to three problems within the field of lidar data analysis. A retrieval of the aerosol backscatter and either the extinction or lidar ratio from two-channel Raman lidar data is developed using the lidar equations as a forward model. It produces profiles consistent with existing techniques at a resolution of 10-1000 m and uncertainty of 5-20%, dependent on the quality of data. It is effective even when applied to noisy, daytime data but performs poorly in the presence of cloud. Two of the most significant sources of uncertainty in that retrieval are the nonlinearity of the detectors and the instrument's calibration (known as the dead time and overlap function). Attempts to retrieve a nonlinear correction from a pair of lidar profiles, one attenuated by a neutral density filter, are not successful as uncertainties in the forward model eliminate any information content in the measurements. The technique of Whiteman et al. [1992] is found to be the most accurate. More successful is a retrieval of the overlap function of a Raman channel using a forward model combining an idealised extinction profile and an adaptation of the equations presented in Halldórsson and Langerholc [1978]. After refinement, the retrieval is shown to be at least as accurate, and often superior to, existing methods of calibration from routine measurements, presenting uncertainties of 5-15%. These techniques are then applied to observations of ash over southern England from the Eyjafjallajökull eruption of April 2010. Lidar ratios of 50-60 sr were observed when the plume first appeared, which reduced to 20-30 sr after several days within the planetary boundary layer, indicating an alteration of the particles over time.

We have studied gas flow and particle deposition in a realistic three-dimensional model of the bronchial tree, extending from the trachea to the segmental bronchi (7th airway generation for the most distal ones) using Computational Fluid Dynamics (CFD). The model is based on the morphometrical data of Horsfield et al. [J. Appl. Physiol., 31: 207-217, 1971] and on bronchoscopic and CT images, which give the spatial 3D-orientation of the curved ducts. It incorporates realistic angles of successive branching planes. Steady inspiratory flow varying between 50cm³/s and 500cm³/s was simulated as well as deposition of spherical aerosol particles (1 to 7 m diameter, 1g/cm³ density). Flow simulations indicated non-fully developed flows in the branches because of their relative short lengths. Velocity flow profiles in the segmental bronchi, taken one diameter downstream the bifurcation, were distorted compared with the flow in a simple curved tube, and wide patterns of secondary flow fields were observed. Both were due to the asymmetrical 3D configuration of the bifurcating network. Viscous pressure drop in the model was compared with results obtained by Pedley et al. [Respir Physiol, 9: 387-405, 1970], which are shown to be a good first approximation. Particle deposition increased with particle size and was minimal for approximately 200cm³/s inspiratory flow but it was highly heterogeneous for branches of the same generation.

Mining operations, including crushing, grinding, smelting, refining, and tailings management, are a significant source of airborne metal and metalloid contaminants such as As, Pb, Cd and other potentially toxic elements. Dust particles emitted from mining operations can accumulate in surrounding soils, natural waters and vegetation at relatively high concentrations through wind and water transport. Human exposure to the dust can occur through inhalation and, especially in the case of children, incidental dust ingestion, particularly during the early years when children are likely to exhibit pica. Furthermore, smelting operations release metals and metalloids in the form of fumes and ultra-fine particulate matter, which disperses more readily than coarser soil dusts. Of specific concern, these fine particulates can be transported to the lungs, allowing contaminants to be transferred into the blood stream. The main aim of this research is to assess the role of atmospheric aerosol and dust in the transport of metal and metalloid contaminants from mining operations to assess the deleterious impacts of these emissions to ecology and human health. In a field campaign, ambient particulates from five mining sites and four reference sites were examined utilizing micro-orifice deposit impactors (MOUDI), total suspended particulate (TSP) collectors, a scanning mobility particle sizer (SMPS), and Dusttrak optical particle counters for an understanding of the fate and transport of atmospheric aerosols. One of the major findings from size-resolved chemical characterization at three mining sites showed that the majority of the contaminant concentrations were found in the fine size fraction (<1 micrometer). Further, metal and metalloids (e.g. As, Cd, and Pb) around smelting activities are significantly enriched in both the coarse and fine size fraction when compared to reference sites. Additionally, with dust events being a growing concern because of predicted climate change and mine tailings being a significant source for dust, high wind conditions around mine tailings were studied for dust generation. Relative humidity was found to play an important predicting role in atmospheric dust concentration. More generally, findings indicate mining activities remain a serious threat to human health and ecology despite the regulations in place to protect from their pollution.

The freezing kinetics of binary nitric acid/water aerosols is of fundamental importance to the modelling of polar stratospheric clouds and the role they in ozone depletion over the Arctic/Antarctic regions. Cirrus clouds are also often composed of nitric acid solutions, hence an understanding of freezing process in these aerosols also aids in modelling the earth's radiation budget and global warming. This thesis explores the kinetic phase diagram of nitric acid/water aerosols with sizes ranging between 0. 2 and 1. 5 mm in radius and concentrations ranging between pure water and 0. 45 mole fraction HNO3. Although the kinetic phase diagram has now been studied between 0. 46 mole fraction HNO3 and pure water, more data is needed in the region between 0. 18 and 0. 25 mole fraction HNO3 to confirm the results reported. The project described in this thesis are a continuation of a project begun by Allan Bertram. The measurements involving aerosols with compositions greater than 0. 25 mole fraction HNO3 were carried out as part of Allan Bertram's Ph. D. thesis (see ref. 20) These data were later examined using a more comprehensive data analysis method (as presented in this thesis) in an effort to obtain a more complete understanding of this system.

Ahvaz, Iran ranks as the most polluted city of the world in terms of PM10 concentrations that lead to deleterious effects on its inhabitants. This study examines diurnal, weekly, monthly and annual fluctuations of PM10 between 2009 and 2014 in Ahvaz. Health effects of PM10 levels are also assessed using the World Health Organization AirQ software. Over the study period, the mean PM10 level in Ahvaz was 249.5 mu g m(-3), with maximum and minimum values in July (420.5 mu g m(-3)) and January (154.6 mu g m(-3)), respectively. The cumulative diurnal PM10 profile exhibits a dominant peak between 08:00-11:00 (local time) with the lowest levels in the afternoon hours. While weekend PM10 levels are not significantly reduced as compared to weekdays, an anthropogenic signature is instead observed diurnally on weekdays, which exhibit higher PM10 levels between 07:00-17:00 by an average amount of 14.2 mu g m(-3) as compared to weekend days. PMio has shown a steady mean-annual decline between 2009 (315.2 mu g m(-3)) and 2014 (143.5 mu g m(-3)). The AirQ model predicts that mortality was a health outcome for a total of 3777 individuals between 2009 and 2014 (i.e., 630 per year). The results of this study motivate more aggressive strategies in Ahvaz and similarly polluted desert cities to reduce the health effects of the enormous ambient aerosol concentrations. (C) 2016 Elsevier B.V. All rights reserved.

While most filters are made of pleated fibrous media, almost all existing theories of aerosol filtration are developed for flat media placed perpendicular to the air flow. Expressions developed for flat sheet media do not provide accurate information directly useful for designing a pleated filter, and therefore, most progress made in developing pleated filters is based on empiricism. This study is aimed at establishing an enabling knowledge that allows for a better design and optimization of pleated aerosol filters. This study is focused on developing a predictive simulation method that accounts for the influence of a filter’s micro-scale geometric parameters, such as fiber orientation, as well as its macro-scale features, like pleat shape, in predicting the transient pressure drop and collection efficiency with or without the effects of dust loading. The dual-scale simulation method developed in this work is believed to be the only feasible approach for design and optimization of pleated aerosol filters with the current academic-level computational power. Our study is divided into two major tasks of micro- and macro-scale modeling. Our micro-scale studies are comprised of a series of CFD simulations conducted in virtual 2-D or 3-D fibrous geometries that resemble the internal micro-structure of a fibrous medium. These simulations are intended to isolate the effects of each micro structural parameter and study its influence on the performance of the filter medium. In detail, it is intended to propose a method to predict the performance of micro-structures with fiber size distribution. Also, the effects of micro-structural fiber orientation were investigated. Moreover, we offered methodology to predict the performance of noncircular fibers using available analytical expressions for circular fibers. It is shown that the circumscribed circle for a trilobal shaped fiber gives the best prediction for collection efficiency. In macro-scale simulations, on the other hand, the filter medium is treated as a lumped porous material with its properties obtained via micro-scale simulations. Our results showed that more number of pleats helps better performance of pleated filters, however, if the pleat channel becomes blocked by dust cake then this effect is no longer valid.

The effects of aerosol in the atmosphere account for some of the largest uncertainties in estimates of the human impact on climate. These effects depend not only on the total mass of aerosol, but also its size distribution, mixing state and vertical profile. Previous studies have suggested that both the size distribution and mixing state of aerosol may be strongly influenced by repeated cycling through non-precipitating cloud. The extent of this process is assessed in the HadGEM3–UKCA model; although fewer cycles are seen for all aerosol than in previous studies, the figure varies considerably between aerosol types. The role of scavenging by precipitating cloud is also considered, and several approaches to increasing the physical realism of its representation are considered. In particular, coupling convective scavenging into the convective transport scheme is shown to provide significant benefits over an operator-split approach (which underestimates removal and allows excess aerosol to reach the upper troposphere and be transported to remote regions). To evaluate the alternative convective scavenging schemes, a method is developed for carrying out a pointwise evaluation against vertically-resolved in-situ observations from large-scale aircraft campaigns, based on nudging and flight-track sampling in the model. It is demonstrated that this approach can help to constrain the choice between different model configurations with a degree of statistical confidence. Finally, the processes controlling the vertical profile of aerosol are investigated using a series of model-based sensitivity tests, along with the extent to which these processes can account for the large diversity in vertical profiles seen amongst current models. For mass profiles and number profiles of large particles (greater than about 100nm dry diameter), removal and secondary production processes are shown to be most important; for number profiles of smaller particles, microphysical processes are shown to become increasingly dominant.

We examine three case studies during the Deep Convective Clouds and Chemistry (DC3) field experiment when storm inflow and outflow air were sampled for aerosol subsaturated hygroscopicity and the real part of refractive index (n) with a Differential Aerosol Sizing and Hygroscopicity Probe (DASH-SP) on the NASA DC-8. Relative to inflow aerosol particles, outflow particles were more hygroscopic (by 0.03 based on the estimated parameter) in one of the three storms examined. Two of three control flights with no storm convection reveal higher values, albeit by only 0.02, at high altitude (> 8km) versus < 4km. Entrainment modeling shows that measured values in the outflow of the three storm flights are higher than predicted values (by 0.03-0.11) based on knowledge of values from the inflow and clear air adjacent to the storms. This suggests that other process(es) contributed to hygroscopicity enhancements such as secondary aerosol formation via aqueous-phase chemistry. Values of n were higher in the outflow of two of the three storm flights, reaching as high as 1.54. More statistically significant differences were observed in control flights (no storms) where n decreased from 1.50-1.52 (< 4km) to 1.49-1.50 (> 8km). Chemical data show that enhanced hygroscopicity was coincident with lower organic mass fractions, higher sulfate mass fractions, and higher O:C ratios of organic aerosol. Refractive index did not correlate as well with available chemical data. Deep convection is shown to alter aerosol radiative properties, which has implications for aerosol effects on climate.

A poluição atmosférica é hoje uma questão que afeta as megacidades por todo o mundo. As partículas de aerossol participam do balanço radiativo, da formação de nuvens, da química atmosférica, e são prejudiciais à saúde da população exposta. A extensão e o rápido crescimento das megacidades têm levado à necessidade do desenvolvimento de ferramentas para o monitoramento da poluição do ar, urbana e regional, por sensoriamento remoto via satélites. Foram analisadas as propriedades ópticas dos aerossóis da região metropolitana de São Paulo com medidas obtidas por fotômetros da rede mundial AERONET (Aerosol Robotic Network) operada pela NASA. Foi desenvolvida uma nova metodologia para a determinação da espessura óptica das partículas de aerossol com alta resolução espacial de 1x1 km, sobre a região metropolitana de São Paulo, por satélite. Cinco modelos ópticos de aerossol, representativos da região, foram definidos como função do albedo simples. No comprimento de onda de 550 nm, os modelos possuem valores de albedo simples que variam de 0,83 a 0,93. Foram utilizadas medidas de radiâncias obtidas com o sensor MODIS (Moderate-Resolution Imaging Spectroradiometer), a bordo dos satélites Terra e Aqua da NASA. Extensos testes de sensibilidade foram realizados, analisando o papel do albedo simples, parâmetro de assimetria, refletância de superfície, vapor de água e outras propriedades na espessura óptica derivada. O algoritmo desenvolvido utiliza a propriedade de refletância crítica, que pode ser obtida pelo próprio sensor, para determinar o modelo de aerossol a ser empregado. Este procedimento permitiu a identificação mais precisa do modelo de aerossol, de forma dinâmica e interativa, reduzindo a incerteza na determinação da espessura óptica em alta resolução com o sensor MODIS. Os resultados de validação mostraram uma melhora significativa na comparação entre os produtos de espessura óptica obtidos com o sensor MODIS, quando comparado com as medidas de referência obtidas com radiômetros em superfície. Foram obtidos com esta metodologia mapas com a distribuição espacial de aerossóis com resolução de 1x1 km. Os estudos de casos também apresentaram a potencialidade do método em identificar o modelo de aerossol mais adequado, seja em eventos de poluição local, seja de transporte de poluentes de longa distância. Os modelos e procedimentos desenvolvidos podem ser aplicados a outras regiões urbanas, após as devidas validações. Como ferramenta complementar ao monitoramento ambiental de estações de superfície o produto apresentado pode-se tornar operacional e ser utilizado em rotina por órgãos de controle ambiental em megacidades, como, por exemplo, pela CETESB em São Paulo / Urban air pollution is a public concern in all megacities around the world. Aerosol particles are active participants in the atmospheric energy budget, cloud properties, atmospheric chemistry and have adverse effects on human health. The spatial extension and the high growth rate of the megacities show the need of the use of remote sensing technologies on urban air pollution monitoring. Optical properties of São Paulo aerosol particles were analyzed using global sun photometer measurements from the AERONET (Aerosol Robotic Network) operated by NASA. A new methodology was developed to retrieve aerosol optical thickness in 1x1 km resolution over São Paulo metropolitan area from satelites measurements. Five aerosol optical models representative of the region were defined as a function of the single scattering albedo. The single scattering albedo in 550 nm varied from 0,83 to 0,93 in the models. Radiances were used from MODIS (Moderate-Resolution Imaging Spectroradiometer) sensor on Terra and Aqua NASA platforms. Sensitivities studies have shown the importance of the single scattering albedo, assymmetry parameter, surface reflectance, water vapor and other properties in the aerosol optical thickness retrieval from space. The developed algorithm uses the critical reflectance aerosol property, that is obtainable from the sensor measurements, to identify the aerosol model to be used. This procedure allow a more precise and dynamic definition of the aerosol model, reducing the uncertainties in the aerosol optical thickness retrieved from the MODIS sensor. Validation results have shown a significant improvement in a comparison between aerosol optical thickness obtained from MODIS and from surface radiometers measurements. Aerosol optical thickness images with 1x1 km resolution were obtained with this methodology and shows that the increase in the resolution of the aerosol optical thickness provides a more effective monitoring of the aerosol distribution in São Paulo. The case studies have shown the potentiality of this methodology to identify an adequate aerosol model, for both local aerosol pollution and in the long distance transport of pollutants. The models and procedures developed in this work can be applied in other urban regions with the appropriate validation. The presented product can be operational and used as routine measurement by environmental agencies in megacities, as an example, for CETESB in São Paulo, as a complementary tool to the regular ground based particulate matter monitoring.