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Characterization of ambient aerosol composition and formation mechanisms and development of quantification methodologies utilizing ATOFMS


Aerosols are solid or liquid particles suspended in the air. They are generated from a range of natural and anthropogenic sources. Aerosols also experience various reactions such as photo-oxidation and aqueous-phase processing, which constantly change their physical and chemical properties. Therefore, in order to determine the emission inventory, it is important to study aerosol reactions and transformation mechanisms in ambient atmosphere. The research described in this dissertation aimed to characterize temporal, spatial, and seasonal variations on ambient aerosol chemical compositions and formation mechanisms. The results contribute to the understanding of air pollution, climate change, and human health problems, and to devising necessary strategies and policies to resolve these problems. The main experimental technique utilized in the current work is Aerosol time-of- flight mass spectrometry (ATOFMS). It measures the size and chemical composition of individual particles in real- time, and can thus provide high time resolution information on aerosol mixing states, reaction mechanisms, and sources. Continuous ATOFMS measurements have been conducted to study the ambient aerosol properties in several highly polluted regions of California, including the Fresno and Angiola area and the Riverside area. The results provide important insights on the characteristics, distinct diurnal temporal trends, and seasonal variations of aerosols in both urban and rural locations. The second focus of this dissertation is on the quantification capability of ATOFMS, which had been limited by several factors including the size-dependent particle transmission loss and shot-to-shot variability of the desorption/ ionization laser. It is demonstrated that, by scaling the ATOFMS measurements using the results from an aerodynamic particle sizer (APS) or a micro-orifice uniform deposit impactor (MOUDI) measurements, it is possible to obtain high temporal resolution mass concentrations from ATOFMS that are in very good agreements with standard beta attenuation monitor mass concentrations. This development substantially improves the quantitative capability of ATOFMS, and will be useful in future application of ATOFMS to study aerosol source apportionment

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