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Investigations into the impact of transported particles on air pollution and climate using aerosol time-of-flight mass spectrometry


Atmospheric aerosols have a significant impact on human health and climate, yet the full scope of these influences are only beginning to be discovered and characterized. To understand these impacts, detailed in-situ measurements of the physical, chemical, and optical properties of aerosols are necessary. Aerosol time-of-flight mass spectrometry (ATOFMS) provides the ability to measure chemical, physical, and optical properties of single particles in real-time. This dissertation uses ATOFMS to explore both the properties and evolution of particles as they are transported over local to global distances. The results of numerous field studies are utilized to explore the changes to these particles as they travel through the atmosphere from their source to eventual deposition. Local to regional scale transport of particles was observed from a number of perspectives in this dissertation. Particles regionally transported from the Ports of Los Angeles and Long Beach to San Diego were identified chemically as ship and truck emissions and shown to overwhelm local sources during peak transport conditions. Ship emissions were studied in detail at the Port of Los Angeles by characterizing individual ship plumes at a site adjacent to the main channel. Mobile laboratory measurements demonstrated the variation in particle concentrations and composition on a local-to-regional level. On the intercontinental-to-global scale, Asian dust was observed in precipitation samples collected in the Sierra Nevada Mountains during orographic precipitation. The incorporation of the long range-transported dust might enhance precipitation, which may alter California's precipitation patterns and water supply. The outflow of particles from Asia to North America were measured on a remote island off Korea, and the sources and aging of particles in Chinese urban, Chinese dust, and Korean air masses were compared to marine air masses. Lastly, ATOFMS studies from sites across North America, Asia, Europe, and Africa were compared to determine similarities and differences in size-resolved chemical mixing state of particles across numerous types of sampling sites, with the objective being to provide information for global climate models to more accurately represent particles. Taken together these results provide an increased understanding of particle chemistry and transport on the scale of meters-to-continents

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