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An optical microscope coupled to a flow cell was used to investigate ice nucleation on five atmospherically relevant mineral dusts at temperatures ranging from 233 to 247 K. Kaolinite and muscovite particles were found to be efficient ice nuclei in the deposition mode, requiring relative humidities with respect to ice (RHi) below 112% in order to initiate ice crystal formation. Quartz and calcite particles, by contrast, were poor ice nuclei, requiring relative humidities close to water saturation before ice crystals would form. Montmorillonite particles were efficient ice nuclei at temperatures below 241 K, but poor ice nuclei at higher temperatures. In several cases, there was a lack of quantitative agreement between these data and previously published work. This can be explained by several factors including mineral source, particle size, observation time and surface area available for nucleation. Heterogeneous nucleation rates (Jhet) were calculated from the onset data. Jhet values ranged from 60 to 1100 cm-²s-¹ for the five minerals studied. These values were then used to calculate contact angles (θ) for each mineral according to classical nucleation theory. The contact angles measured for kaolinite and muscovite ranged from 6 to 12º; for quartz and calcite the contact angles were much higher, ranging from 25 to 27º. The contact angles measured for montmorillonite were less than 15º at temperatures below 241 K, and above 20º at higher temperatures. The reported Jhet and θ values may allow for a more direct comparison between laboratory studies and can be used when modeling ice cloud formation in the atmosphere. The roles of H₂SO₄ and (NH4)₂SO₄ coatings on the ice nucleating properties of kaolinite were also investigated. Onset data was collected for H₂SO₄ coated and (NH4)₂SO₄ coated kaolinite particles at temperatures ranging from 233 to 247 K. In contrast to uncoated kaolinite particles, which were effective ice nuclei, H₂SO₄ coated particles were found to be poor ice nuclei, requiring relative humidities close to water saturation before nucleating ice at all temperatures studied. (NH4)₂SO₄ coated particles were poor ice nuclei at 245 K, but effective ice nuclei at 236 K. / Science, Faculty of / Chemistry, Department of / Graduate

A remote aerosol sampler, capable of up to 3 weeks continuous sampling has been developed. It consists of an Anderson 2000 Inc. mini-sampler or personnel monitor requiring an air flow of 1.4 e/min, a flow meter, a vacuum meter, a bleed valve, a dry gas volume meter, and a pump. The pump is a Brailsford Model TD-4X2, and operates on a 24 volt D.C. power supply. The sampler consists of four impaction stages with a 0.4 μ Nuclepore backup filter. Particulates are removed from the plates in an ultrasonic cleaner with hexane solvent. The suspended particulates are collected on a 0.4 μ Nuclepore filter. Elemental analysis of the aerosol is accomplished by the method of charged particle X-ray fluorescence. The results of two samples taken in Utah County, Utah, are tabulated. Elemental composition is reported as ppm of particulate, as a ratio relation to stage 1, and as a ratio relation to iron. High values are reported for iron and lead, with most of the lead being collected in the filter.

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The chemical and optical properties of particulate organic compounds remain unclear, which leaves large uncertainties in the estimation of global radiative transfer balance. Gas and find particle (PM2.5) phase formic acid concentrations were measured with online instrumentation during separate one-month studies in the summer of 2010 in Los Angeles (LA), CA, and Atlanta, GA, and the gas-particle partitioning behavior was investigated and compared with that of water-soluble organic compounds (WSOC). The diurnal profiles clearly indicated that the photochemistry production serves as a strong source for the formation of organics, while the correlation between the gas and particle phase suggested that another partitioning route, the aqueous reactions, is also very important. Later, the optical properties of light-absorbing organic compounds were examined. Little is known about the optical importance of light absorbing particulate organic compounds (brown carbon), especially its extent and absorption relative to black carbon throughout the tropospheric column. Mie theory was applied to size-resolved spectrophotometric absorption measurements of methanol and water-extracts from cascade impactor substrates collected at three surface sites around Atlanta, GA, including both urban and rural. These results were applied to similar measurements of brown carbon in extracts from aircraft bulk filter samples collected over central USA. At the surface sites predicted light absorption by brown carbon relative to total absorption (brown carbon plus pure black carbon) was about 10% and 30% at 350 nm, versus 1 and 11% at 450 nm, for water and methanol extracts, respectively. The relative contribution of brown carbon was greater in the free troposphere and significantly increased with altitude. Although this approach has limitations, it demonstrates the ubiquity and significant potential contribution of brown carbon.

This thesis characterizes the ambient fine organic carbon aerosol and investigates its sources through the development and deployment of new measurement techniques. The focus is on organic compounds that are soluble in water (WSOC), which comprise a large fraction of the organic aerosol, yet little has been known about its chemical nature. A method was developed for quantitative on-line measurements of WSOC by using a Particle-into-Liquid Sampler (PILS) to capture ambient particles into a flow of purified water, which is then forced through a liquid filter and the carbonaceous content quantified by a Total Organic Carbon (TOC) analyzer. This system allows for a continuous 6 minute (ground-based) or 3 s integrated measurement (airborne) with a limit of detection of 0.1 microgramsC/m3 and uncertainty of 10%. Furthermore, a new quantitative method was developed to group speciate the WSOC. In the first step, WSOC is separated by use of XAD-8 resin into its hydrophilic (WSOCxp) and hydrophobic (WSOCxr) fractions. This separation can be performed on-line by coupling the XAD-8 column with the PILS-TOC or off-line on WSOC extracted from integrated filter samples. If off-line, a second step involving size-exclusion chromatography (SEC) is used to chromatographically separate by organic functional groups the WSOCxp and recovered hydrophobic fraction (WSOCxrr). During this step, the WSOCxp is further separated into aliphatic acids with less than four carbons, neutrals, and bases. The WSOCxrr can be separated into acids and neutrals. Results showing the capabilities of the PILS-TOC both on the ground at the St. Louis Midwest Supersite and when airborne during the New England Air Quality Study/Intercontinental Transport and Chemical Transformation 2004 mission conducted in the northeastern U.S. will be presented. Ambient results from urban sites where a PILS-TOC was coupled with a XAD-8 column will be discussed. Data from the two-step speciation performed on samples collected from urban Atlanta summer and winter, and biomass burning in rural Georgia in a region of prescribed burning are presented. Finally, WSOC measurements obtained in Atlanta and its surrounding regions from both the speciation measurements and PILS-TOC will be used to investigate the sources of WSOC in the southeastern U.S.

This thesis is based on measurements of aerosol optical and microphysical properties made at inland, coastal and island locations in India. Aerosol vertical distribution measurements have also been made both using surface based and aircraft borne instruments. In addition to these, satellite based measurements (MODIS and OMI) have also been used to estimate regional aerosol radiative forcing over the oceanic regions around India. The measurements at an inland, continental, urban location reveals the large effect of anthropogenic activities on aerosol characteristics at surface and the atmospheric vertical column. A clear seasonality is observed in aerosol optical and microphysical properties as a consequence of modulation by anthropogenic activities and the effect of meteorological parameters like rainfall, winds and boundary layer dynamics. The variability observed at different time scales (from diurnal, weekly, monthly to annual) reveals the importance of anthropogenic and natural processes in modulating the aerosol loading. The estimates of aerosol radiative forcing at surface were as high as ~ 40W m-2. A large discrepancy was observed between the observed and modeled aerosol forcing efficiency (forcing per unit optical depth) at surface. These discrepancies are due to the inadequate representation of aerosol mixing state in models. In addition, the large difference found in the observed forcing between winter and summer could also be influenced due to the presence of elevated aerosols during the summer. Measurements made over coastal and central India shows that a large fraction (75-85%) of aerosol column optical depth was contributed by aerosols located above 1 km. The horizontal gradients were sharp with e-1 scaling distance as small as ~250 km in the well-mixed regions mostly under the influence of local source effects. However, above the atmospheric boundary layer, the gradients were much shallower (~800 to 1200 km). In addition, a large fraction (60-75%) of aerosol was found located above clouds leading to enhanced aerosol absorption. Large spatial gradient in aerosol optical depth and hence radiative impacts between the coastal landmass and the adjacent oceans within a short distance of <300 km (even at an altitude of 3 km) during summer and pre-monsoon is of importance to regional climate. Observations at Minicoy, a remote island in southern Arabian Sea to study the characteristics of transported aerosols reveals variability at daily, weekly, monthly and seasonal time scales associated with changes in precipitation and air mass characteristics. The daily mean Black Carbon (BC) mass mixing ratio varied between as low as ~ 0.2 to 9.0%. The resultant average aerosol atmospheric forcing for the observation period was ~15 W m-2. Trajectory based cluster analysis has shown six distinct advection/transport pathways influencing aerosol characteristics over southern Arabian Sea. The Indo-Gangetic Plain, northern Arabian Sea and west Asia are identified to be the most important source regions having a major impact on aerosols loading over the southern Arabian Sea. The cluster analysis, concentration weighted trajectory (CWT) analysis and the MODIS retrievals show an asymmetry in aerosol characteristics between the Arabian Sea and the Bay of Bengal, with the Arabian Sea characterized by large loading by natural aerosols (eg., dust and sea salt) and the Bay of Bengal characterized by anthropogenic loading (eg., BC). The low value of the BC mass mixing ratio measured at the island (mostly ~ 1 to 1.6%), has major implications for regional radiative forcing. The annually averaged net aerosol atmospheric forcing was as low as ~1.7 W m-2 with highest forcing corresponding to IGP cluster. The single scattering albedo (SSA) which is an important parameter in the estimation of aerosol radiative forcing was retrieved by utilizing a joint OMI-MODIS retrieval methodology. The SSA over the oceanic regions around India shows that the largest absorption (SSA < 0.9) occurs during winter. The largest gradients in AOD and SSA were observed over Arabian Sea during the summer as a result of large dust emissions. The largest forcing observed also was confined to the northern Arabian Sea (~ 37 W m-2) as a result of high aerosol column loading and dust transport. The observed annual mean forcing at Minicoy were comparable to that estimated using satellite measurements, but were much lower than those observed during INDOEX.

Aerosol are solid or liquid particles suspended in the atmosphere ranging in size from 10 3 to 102 m. Aerosol influence both the regional and global climate of the earth by its direct and indirect effect. Role of atmospheric aerosols on the radiative forcing of atmosphere is a matter of serious research for past few decades and still it remains highly uncertain as acknowledged by Intergovernmental Panel on Climate Change. Heterogeneous nature of aerosol both spatially and temporally makes it more complex in estimating radiative forcing compared to that of greenhouse gases. Compounding to the existing difficulty in determining the climate effects, changing aerosol concentration and nature of the aerosol further increases the complexity in determining its effects in both regional and global climate. Increasing aerosol loading is emerging to be an issue of major concern over several regions. The first step towards achieving this goal is by determining the trends in the physical and optical properties of aerosol over the globe. Main objective of the thesis is the determination of the recent trends in aerosol loading over the globe and then to focus specifically on the properties of aerosol over an urban site in southern India. Specific objectives are (a) to determine the trend in aerosol physical and optical properties over the globe using AERONET surface observations (b) to characterize the chemical properties of water soluble inorganic aerosol over an urban site in Southern India, Bangalore (c) to have a better estimation of aerosol radiative forcing over Bangalore with measured aerosol chemical concentration, black carbon concentration and aerosol optical depth (AOD). To quantify the recent trends in aerosol loading over the globe, we have used the surface observations from AERONET and the study provided the first step in giving a global picture of the recent trends in the fundamental optical and physical property of aerosol. Trend analysis showed a significant spatial inhomogenity, and Asian continent clearly showed an increasing trend in AOD compared to other continents. Solar village (24.9oN, 46.4oE) of Saudi Arabia showed a maximum with a value of 0.04/yr and Bac -Giang (21oN, 106oE) of Vietnam showed the minimum value of -0.04/yr. North American study region included 18 sites in which eastern US (E.US) exhibited a decreasing trend while the scenario in western US (W.US) is different with more of sites with increasing AOD trend. Single scattering albedo (SSA) trend in W. US showed a decreasing trend irrespective of the AOD trend. Study sites in South America include Cordoba -CETT (31.5oNS, 64.5 oN W) Alta Floresta (9.8oS, 56.1 o W), Riobranco (9.9oNS, 67.8o W) and Soa Poulo (23.5oS, 46.7o W).Except Riobranco which has a positive trend in AOD, all other sites exhibited a statistically signi cant negative trend. Over Australia, there is an inclination towards increasing AOD in sites and all the three sites in Australia exhibit a statistically significant increasing trend in SSA. According to the recent trends in AOD over African region, there exists a significant decrease in AOD compared to that reported for few years earlier, showing the high temporal in homogeneity and need for continuous observation of aerosol over the regions. European study region included 15 stations, among them only 3 sites showed an increasing trend in AOD, remaining 12 sites showed a significant decreasing trend in aerosol loading over the period of study. SSA was also observed to be decreasing over most of the European sites, even with a decreasing AOD over most of the sites. A Comparison study carried out to determine the relation of population growth rate and aerosol loading, and it revealed that the increasing AOD trend not always coincided with the sites having high population growth rate. Having determined the trends in AOD and other aerosol parameters over the globe and seeing an alarmingly increasing trend over most of the Asian sites, especially over Indian region, we have then focused over work on the aerosol properties of one of the rapidly growing urban location in southern India, Bangalore. While physical properties of aerosol have been extensively studied over Bangalore, chemical characteristics are still an unexplored area. Extensive information on aerosol chemical composition is not available over Indian region except for a few locations based on campaign mode. Even available data is of very coarse temporal resolution, since hours or full day sampling is needed to gather enough samples for chemical analysis. High temporal resolution data of aerosol chemical characteristics, especially for all season is completely lacking over Indian subcontinent. Among aerosol, water soluble aerosol form an important component in particulate matter, since it can change its size, composition, can easily mix with other aerosols and can act as cloud condensation nuclei, based on its hygroscopic nature. Present study provided the rst time results from a high temporal resolution water soluble inorganic aerosol chemical data over Indian region, which is first step towards estimating aerosol climate impacts more accurately. Water soluble inorganic aerosol ions over Bangalore namely, sulphate, nitrate, chloride, potassium, calcium, magnesium, sodium and ammonium are measured using Particle Into Liquid Sampler Ion Chromatograph (PILS-IC). PILS is an online sampling technique for quantitatively measuring the chemical concentration of ion in water soluble aerosol particles. PILS IC used in the present study is developed in Georgia Institute of Technology. Instrument samples ambient air at a flow rate of 16.7Lmin 1. Particles below PM 2.5 micron are collected for the analysis using cyclone impactor. Two annular glass denuders are used to remove inorganic gases which else will interfere with the aerosol ion concentration. Ambient air which is deprived of the inorganic gases is then mixed with steam vapours at 150oC, eventually high supersaturated atmosphere is produced with rapid adiabatic mixing of steam and ambient air. High supersaturated air allows droplets to grow enough to be collected by inertial impaction onto a quartz impactor plate. Entire PILS condensation unit is kept at a slight tilt of 15o, to remove all condensate through drain tube connected to the end of the PILS condensate body. Condensed liquid sample is collected from the impaction chamber and known concentration LiF is allowed to mix with the collected sample at a constant rate. LiF known as carrier liquid is added to know the dilution occurring to the collected sample. Sample with carrier liquid is then collected to a debubbler and is supplied to the IC through peristaltic tubings for determining the ion chemical concentration. Seasonal variation of mass concentration of water soluble aerosol species and the influence of long range transport is carried out using HYSPILT back trajectory analysis. Marine air mass from Arabian Sea dominated the air parcel reaching the site for both SW monsoon and summer. Continental air mass dominated the site during both NE monsoon and winter with slight contribution from marine atmosphere. Source characteristics of sulphate, potassium, calcium and magnesium ions are carried out based on sea salt (ss) and non sea salt (nss) origin and it is observed that the nss contribution is dominant over the site for all these ions except magnesium where ss component comparatively dominates the source. SO24 and NO3 form the dominant anions while NH+4 makes the dominant cation species. Monthly variation of the ratio of ammonium to nss -sulphate is carried out to determine the possible cation -anion relation existing between these two major ions. During later winter and summer months ammonium bi sulphate is found to be the existing chemical form and ammonium sulphate during other seasons. High temporal resolution data enabled us to study the diurnal variation of aerosol ions and it is influenced by various mechanisms from boundary layer to local emissions. Optical properties of aerosols depend upon the size and the relative abun-dance of each components. It is usual practice to assume default aerosol chemical composition in radiative transfer models due to unavailability of data, which can lead to errors in forcing estimates. Incorporating realistic aerosol chemical composition in models is essential to reduce the uncertainty in aerosol radiative forcing. Hence we have included measured aerosol chemical compositions, black carbon and AOD to improve the determination of radiative forcing of aerosol. OPAC and SBDART models were used for estimating the aerosol radiative forcing over Bangalore. We have used mainly four components namely, soot, water soluble, sea salt and dust. Except dust all are other components are measured over the site and formed a constrain for the calculation. Dust concentration was altered so that the OPAC AOD matched the measured AOD within 5%. Mineral dust shows the highest contribution in AOD among the four components, however water soluble and soot even being less is mass concentration compared to mineral dust, has significant impact on the AOD. This clearly indicate the influence of both water soluble and soot aerosol over the regional climate of the site. Sea Salt exhibited low AOD compared to other three constituents. The results presented in the thesis highlights the importance of varying trends in the aerosol properties and its effects on a global picture and speci - cally over an urban site in Indian region , we explored the temporal variations of water soluble inorganic aerosol ions and its effects on regional climate. Hence the thesis addressed some of the unexplored areas in aerosol science. This study also suggests the need of continuous observation of aerosol over both spatial and temporal scale, which is essential to estimate their effects on earth's climate.

Air quality degradation is emerging to be an issue of major concern in India. Recent investigations have shown that anthropogenic aerosols have significant impact on climate as well as on health. In fourth assessment report of IPCC, it has been mentioned that radiative effects of anthropogenic aerosols constitute one of the major uncertainties in assessing aerosol-induced climate impact. In addition to climate impacts, aerosol causes respiratory and cardiovascular diseases, air quality degradation, acidification of aquatic and terrestrial ecosystems. Characterization of anthropogenic aerosol fraction (defined as the fraction of anthropogenic aerosols to composite aerosols) is an appealing topic of research in current scenario. The first step towards achieving this goal is to separate natural aerosol from composite aerosols, which is a complex task. The main objective of this thesis work is the assessment of air quality and anthropogenic aerosol fraction over India using observations (ground-based as well as satellite-based) and chemistry-transport model. Specifically objectives are (a) assessment of air quality and anthropogenic aerosol fraction over Indian region (b) develop a method to derive natural aerosol properties over land and oceans using multi-satellite data analysis, which is first step towards separating natural aerosol effects from its anthropogenic counter parts and (c) evaluate performance of CHIMERE chemistry-transport model for Indian region and validate its suitability to air quality studies over India. In this thesis, different approaches have been followed such as ground-based observations, multi-satellite data analysis and CHIMERE transport model. We have used multi-year observations of particulate mass (PM) concentration, aerosol black carbon (BC) mass concentration and aerosol optical depth (AOD) from a network of observatories to make an assessment of ambient air quality over India. First, we have developed a method to estimate dust and sea-salt optical depth using multi-satellite data analysis. This enabled the determination of anthropogenic aerosol fraction over land and ocean and we have validated this method by comparing against observations. Surprisingly, even over desert locations in India and Saudi Arabia, the anthropogenic fraction were unexpectedly high (~0.3 to 0.4) and the regionally averaged anthropogenic fraction over India was 0.620.06 (for the year 2004). The CHIMERE chemistry-transport model was used to simulate PM, BC and AOD over India and are compared with measurements. Evaluation of CHIMERE output shows that diurnal and seasonal trends are captured reasonably well by the model. It was found that absolute magnitudes differ substantially during monsoon months. Model simulations are also used to estimate anthropogenic fraction over Indian region and are compared with observations. Implications of the results are discussed. Mineral dust constitutes the single largest contributor of natural aerosols over continents. The first step towards separating natural aerosol radiative impact from its anthropogenic counterparts over continents is to gather information on dust aerosols. The infrared (IR) radiance (10.5–12.5 mm) acquired from the Kalpana satellite (8-km resolution) was used to retrieve regional characteristics of dust aerosols over the Afro-Asian region during the winter of 2004, coinciding with a national aerosol campaign. Here, we used aerosol-induced IR radiance depression as an index of dust load. The regional distribution of dust over various arid and semi-arid regions of India and adjacent continents has been estimated, and these data in conjunction with regional maps of column aerosol optical depth (AOD) are used to infer anthropogenic aerosol fraction. Surprisingly, even over desert locations in India and Saudi Arabia, the anthropogenic fraction were relatively high (0.3 to 0.4) and the regionally averaged anthropogenic fraction over India was 0.62 ±0.06. Sea-salt constitutes the single largest contributor of natural aerosols over oceans. We derive sea-salt aerosol distribution using a method utilizing multi-satellite data analysis. This information was used in conjunction with dust aerosols retrieval to calculate anthropogenic fraction over land and ocean. First, we derived a relation between MODIS AOD and NCEP wind speed at the sea-surface. An exponential increase in AOD as a function of wind speed was observed from mid of southern ocean to northern Arabian Sea. Latitudinal variation of wind independent component of optical depth (τ0) and wind index (b) was used to estimate the sea-salt optical depth over Arabian Sea. The value of τ0 showed an exponential increase as we move towards north from 35°S while b showed linear increase. The derived relations for the τ0 and b have been used to derive the sea-salt AOD distribution over oceanic regions in the domain (Eq-30°N; 30°E-110°E). Then we subtract the natural aerosol contribution from composite AOD data from MISR to obtain anthropogenic aerosol fraction. Over Indian region, high anthropogenic fraction was observed over northern belt specifically Indo-Gangetic Plains (IGP). Annually averaged anthropogenic fraction over Indian domain (4N-29.5N; 67E-88.5E) is ~0.43. Further, we have investigated the impact of sea-surface winds on sea-salt radiative effect in visible and infrared region with the help of SBDART radiative transfer model. The SBDART simulations have shown that at 15 m s-1, sea-salt induced shortwave cooling at the sea-surface was -86 W m-2. Derivation of anthropogenic aerosol fraction over whole Indian domain has demonstrated the importance of anthropogenic aerosols. This observation motivated us to examine the air quality over Bangalore, a fast growing city in India. We have analyzed data from ground based measurements of particulate matter, observations from satellites and also model simulations. Comparison with national threshold indicates that more than 50% of observations were above the residential threshold. To represent the air quality of Bangalore we have calculated the air quality index (AQI) for air pollutants. Coarse spatial and temporal resolution of observational data is one major shortcoming in such analysis. Therefore, satellite observations are alternative to quantify the air quality over large area. We have used MODIS AOD and RSPM to develop an empirical relation between these two parameters. A reasonably good agreement was observed between measured RSPM and RSPM derived using satellite data (by applying empirical relation). The CHIMERE chemistry-transport model was used to simulate PM, BC and AOD over India and are compared with measurements. Evaluation of CHIMERE output shows that diurnal and seasonal trends are captured reasonably well by the model. It was found that absolute magnitudes differ substantially during pre-monsoon and monsoon months. Model simulations are also used to estimate anthropogenic fraction over Indian region and are compared with observations. Implications of the results and future scope are discussed. The validation of model results suggests that CHIMERE model is suitable for simulating air quality over India with reasonable accuracy. This would in turn help us to address the impacts of air pollution on regional climate and help policy makers in order to reduce the air pollution. In summary, we have developed a new method to infer natural aerosol (sea-salt and dust) properties using multi-satellite data analysis. This technique has been applied to derive anthropogenic aerosol fraction over Indian region. Surprisingly, even over desert locations in India and Saudi Arabia, the anthropogenic fraction were relatively high (0.3 to 0.4) and regionally averaged anthropogenic fraction over India was 0.62±0.06 in 2004. This study indicates that multi-satellite observations can provide a powerful tool in monitoring air quality. We have noticed that anthropogenic fraction was 0.62 in 2004 and reduced to 0.43 in 2008. Major anthropogenic aerosol over India is BC and decreasing trend in BC could be one of the reasons for the decrease in anthropogenic fraction from 2004 to 2008. The CHIMERE chemistry-transport model was used to simulate PM, BC and AOD over India and are compared with measurements. Evaluation of CHIMERE output shows that diurnal and seasonal trends are captured reasonably well by the model. It was found that absolute magnitudes differ substantially during pre-monsoon and monsoon months. Presence of elevated aerosol layers during these seasons could be one of the sources for such discrepancy. Model simulations of anthropogenic fraction over Indian region are compared with observations and found good agreement. Results from this thesis moves us one step forward to reduce the uncertainties involved in anthropogenic aerosol fraction, its spatial and temporal distributions and regional distribution of OC/BC ratio, which are most important parameters in order to assess the climate forcing by anthropogenic aerosols.