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Mobile source emissions are a major contributor to global and local air pollution. Governments and regulatory agencies have been increasing the stringency of regulations in the transportation sector for the last ten years to help curb transportation sector air pollution. The need for regulations has been emphasized by scientific research on the impacts from ambient pollution, especially research on the effect of particulate matter on human health. The particulate emissions from diesel vehicles, diesel particulate matter (DPM) is considered a known or probable carcinogen in various countries and increased exposure to DPM is linked to increased cardiovascular health problems in humans. The toxicity of vehicle emissions and diesel particulate emissions in particular, in conjunction with an increased awareness of potential petroleum fuel shortages, international conflict over petroleum fuel sources and climate change science, have all contributed to the increase of biodiesel use as an additive to or replacement for petroleum fuel. The goal of this research is to determine how this increased use of biodiesel in the particular emission testing setup impacts urban air quality. To determine if biodiesel use contributes to a health or climate benefit, both the size range and general composition were investigated using a comprehensive comparison of the particulate component of the emissions in real time. The emissions from various biodiesel and diesel mixtures from a common diesel passenger vehicle were measured with a cavity ring-down transmissometer (CRDT) coupled with a condensation particle counter, a SMPS, a nephelometer, NOx, CO, CO2, and O3 measurements. From these data, key emission factors for several biodiesel and diesel fuel mixtures were developed. This approach reduces sampling artifacts and allows for the determination of optical properties, particle number concentration, and size distributions, along with several important gas phase species' concentrations. Findings indicate that biodiesel additions to diesel fuel do not necessarily have an air quality benefit for particulate emissions in this emission testing scenario. The often cited linear decrease in particulate emissions with increasing biodiesel content was not observed. Mixtures with half diesel and half biodiesel tended to have the highest particulate emissions in all size ranges. Mixtures with more than 50% biodiesel had slightly lower calculated mass for light absorbing carbon, but this reduction in mass is most likely a result of a shift in the size of the emission particles to a smaller size range, not a reduction in the total number of particles. Evaluation of the extensive optical properties from this experimental set-up indicates that biodiesel additions to diesel fuel has an impact on emission particle extinction in both visible and near-IR wavelengths. The B99 mixture had the smallest emission factor for extinction at 532 nm and at 1064 nm. For the extinction at 532 nm, the trend was not linear and the emission factor peaked at the B50 mixture. Results from intensive properties indicate that emissions from B5 and B25 mixtures have Ångström exponents close to 1, typical for black carbon emissions. The mixtures with a larger fraction of biodiesel have Ångström exponent values closer to 2, indicating more absorbing organic matter and/or smaller particle size in the emissions. Additional experimental testing should be completed to determine the application of these results and emission factors to other diesel vehicles or types of diesel and biodiesel fuel mixtures.
The optical properties of carbonaceous aerosols were investigated to understand the impact source emissions and ambient particulate matter (PM) have on atmospheric radiative forcing. Black carbon (BC) is a strong absorber of visible light and contributes highly to atmospheric radiative forcing, therefore it is important to link BC properties to combustion emission sources. Brown carbon (BrC) is poorly understood and may be an important contributor to both positive and negative radiative forcing. The research investigates these primary knowledge gaps. The optical properties of carbonaceous aerosols were investigated to understand the impact source emissions and ambient particulate matter (PM) have on atmospheric radiative forcing. Black carbon (BC) is a strong absorber of visible light and contributes highly to atmospheric radiative forcing, therefore it is important to link BC properties to combustion emission sources. Brown carbon (BrC) is poorly understood and may be an important contributor to both positive and negative radiative forcing. The research investigates these primary knowledge gaps. Multiple methods were developed and applied to quantify the mass absorption cross-section (MAC) at multiple wavelengths of source and ambient samples. The MAC of BC was determined to be approximately 7.5 m2g−1 at 520nm. However, the MAC was highly variable with OC fraction and wavelength. The BrC MAC was similar for all sources, with the highest absorption in the UV at 370nm; the MAC quickly decreases at larger wavelengths. In the UV, the light absorption by BrC could exceed BC contribution by over 100 times, but only when the OC fraction is large (>90%) as compared to the total carbon. BrC was investigated by measuring the light absorption of solvent extracted fractions in water, dichloromethane, and methanol. Source emissions exhibited greater light absorption in methanol extractions as compared to water and DCM extracts. The BrC MAC was 2.4 to 3.7 m2g−1 at 370nm in methanol. Ambient samples showed similar MACs for the water and methanol extracts. Dichloromethane extracts did not have a significant light absorption characteristics for ambient samples. BrC and BC were measured in Beijing, China. Both were reduced significantly when restrictive air pollution controls were put in place. The industrial regions south and east of Beijing were the highest contributors to ambient BrC and BC. The controls reduced BrC more than BC as compared to observations during the regions heating period. Using the color characteristics of ambient PM, a model was developed to estimate elemental and organic carbon (EC/OC). The method will allow fast and cost effective quantification of PM composition in combination with large climate and health studies, especially in the developing world.
Measurements of aerosol extinction coefficient at 632 nm were made aboard the NSF C-130 aircraft to study aerosol optical properties under fresh and aged air masses and the impacts of various emission source to aerosol extinction. 2) The oxidation of 1-methylnaphthalene, phenol, toluene, longifolene, and [Alpha]-pinene hydrocarbon precursors in smog chamber studies.
Aerosols, or particulate matter (PM), can affect climate through scattering and absorption of radiation and influence the radiative properties, precipitation efficiency, thickness, and lifetime of clouds. Aerosols are one of the greatest sources of uncertainty in climate model predictions of radiative forcing. To fully understand the sources of uncertainty contributing to the radiative properties of aerosols, measurements of PM mass, composition, and size distribution are needed globally and seasonally. To add to the current understanding of the seasonal and temporal variations in aerosol composition and chemistry, this study has focused on the quantification, speciation, and characterization of atmospheric PM in urban and rural regions of the United States (US) for short and long periods of time. In the first two chapters, we focus on 1 month of aerosol and gas-phase measurements taken in Fresno, CA, an urban and agricultural area, during the National Aeronautics and Space Administration's (NASA) field study called DISCOVER-AQ. This air quality measurement supersite included a plethora of highly detailed chemical measurements of aerosols and gases, which were made at the same time as similar aircraft column measurements of aerosols and gases. The goal of DISCOVER-AQ is to improve the interpretation of satellite observations to approximate surface conditions relating to air quality, which can be achieved by making concurrent ground- and aircraft-based measurements of aerosols and gases. We begin in chapter 2 by exploring the urban aerosol and gas-phase dataset from the NASA DISCOVER-AQ study in California. Specifically, we discuss the chemical composition and mass concentration of water-soluble PM2.5 that were measured using a particle-into-liquid sampler with ion chromatography (PILS-IC) in Fresno, California from January 13–February 10, 2013. This data was analyzed for ionic inorganic species, organic acids and amines. Gas-phase species including HNO3 and NH3 were collected with annular denuders and analyzed using ion chromatography. Using the thermodynamic E-AIM model, inorganic particle water mass concentration and pH were calculated for the first time in this area. Organic particle water mass concentration was calculated from [kappa]-Köhler theory. In chapter 3 further analysis of the aerosol- and gas-phase data measured during DISCOVER-AQ was performed to determine the effectiveness of a local residential wood burning curtailment program in improving air quality. Using aerosol speciation and concentration measurements from the 2013 winter DISCOVER-AQ study in Fresno, CA, we investigate the impact of residential wood burning restrictions on fine particulate mass concentration and composition. Key species associated with biomass burning in this region include K+, acetonitrile, black carbon, and biomass burning organic aerosol (BBOA), which represents primary organic aerosol associated with residential wood burning. Reductions in acetonitrile associated with wood burning restrictions even at night were not observed and most likely associated with stagnant conditions during curtailment periods that led to the buildup of this long-lived gas. In chapter 4 we transition to the rural aerosol dataset from the DOE SGP site. We discuss the chemical composition and mass concentration of non-refractory submicron aerosols (NR-PM1) that were measured with an aerosol chemical speciation monitor (ACSM) at the DOE SGP site from November 2010 through June 2012. Positive matrix factorization (PMF) was performed on the measured organic aerosol (OA) mass spectral matrix using a newly developed rolling window technique to derive factors associated with distinct sources, evolution processes, and physiochemical properties. The rolling window approach captured the dynamic variations of the chemical properties of the OA factors over time. Three OA factors were obtained including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a BBOA factor. Sources of NR-PM1 species at the SGP site were determined from back trajectory analyses. NR-PM1 mass concentration was dominated by organics for the majority of the study with the exception of winter, when NH4N33 increased due to transport of precursor species from surrounding urban and agricultural regions and also due to cooler temperatures. Chapter 5 is a continuation of chapter 4, where we will explore the use of the multilinear engine (ME-2) as a factor analysis technique, which is an algorithm used for solving the bilinear model called positive matrix factorization (PMF). The importance of ME-2 and its potential application on the long-term aerosol chemical speciation monitor (ACSM) data collected from the Department of Energy (DOE) Southern Great Plains (SPG) site will be discussed. ME-2 was performed on 19 months of OA mass spectral data obtained from the ACSM at the SGP site. Evaluation of ME-2 results are presented, followed by comparison of ME-2 factor results with corresponding OACOMP factor results reported in chapter 4. We show that ME-2 can determine a biomass burning organic aerosol (BBOA) factor during periods when OACOMP cannot. (Abstract shortened by ProQuest.)
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.
This dissertation describes the use of measured aerosol size distributions and size-resolved hygroscopic growth to examine the physical and chemical properties of several particle classes. The primary objective of this work was to investigate the optical and cloud forming properties of a range of ambient aerosol types measured in a number of different locations. The tool used for most of these analyses is a differential mobility analyzer / tandem differential mobility analyzer (DMA / TDMA) system developed in our research group. To collect the data described in two of the chapters of this dissertation, an aircraft-based version of the DMA / TDMA was deployed to Japan and California. The data described in two other chapters were conveniently collected during a period when the aerosol of interest came to us. The unique aspect of this analysis is the use of these data to isolate the size distributions of distinct aerosol types in order to quantify their optical and cloud forming properties. I used collected data during the Asian Aerosol Characterization Experiment (ACE-Asia) to examine the composition and homogeneity of a complex aerosol generated in the deserts and urban regions of China and other Asian countries. An aircraft-based TDMA was used for the first time during this campaign to examine the size-resolved hygroscopic properties of the aerosol. The Asian Dust Above Monterey (ADAM-2003) study was designed both to evaluate the degree to which models can predict the long-range transport of Asian dust, and to examine the physical and optical properties of that aged dust upon reaching the California coast. Aerosol size distributions and hygroscopic growth were measured in College Station, Texas to investigate the cloud nucleating and optical properties of a biomass burning aerosol generated from fires on the Yucatan Peninsula. Measured aerosol size distributions and size-resolved hygroscopicity and volatility were used to infer critical supersaturation distributions of the distinct particle types that were observed during this period. The predicted cloud condensation nuclei concentrations were used in a cloud model to determine the impact of the different aerosol types on the expected cloud droplet concentration. RH-dependent aerosol extinction coefficients were also calculated.
Scientists have been observing a change in the climate since the beginning of the 20th century that cannot be attributed to any of the natural influences of the past. Natural and anthropogenic substances and processes perturb the Earth's energy budget, contributing to climate change. In particular, aerosols (particles suspended in air) have long been recognized to be important in processes throughout the atmosphere that affect climate. They directly influence the radiative balance of the Earth's atmosphere, affect cloud formation and properties, and are also key air pollutants that contribute to a variety of respiratory and cardiovascular diseases. Despite their importance, aerosol particles are less well-characterized than greenhouse gases with respect to their sources, temporal and spatial concentration distribution, and physical and chemical properties. This uncertainty is mainly caused by the variable and insufficiently understood sources, formation and transformation processes, and complex composition of atmospheric particles. Instruments that can precisely and accurately measure and characterize the aerosol physical and chemical properties are in great demand. Atmospheric relative humidity (RH) has a crucial impact on the particles' optical properties; the RH dependence of the particle extinction coefficient is an important parameter for radiative forcing and thus climate change modeling. In this work a Humidity-Controlled Cavity Ring-Down (HC-CRD) aerosol optical instrument is described and its ability to measure RH dependent extinction coefficients and related hygroscopicity parameters is characterized.
Aerosol Science and Technology: History and Reviews captures an exciting slice of history in the evolution of aerosol science. It presents in-depth biographies of four leading international aerosol researchers and highlights pivotal research institutions in New York, Minnesota, and Austria. One collection of chapters reflects on the legacy of the Pasadena smog experiment, while another presents a fascinating overview of military applications and nuclear aerosols. Finally, prominent researchers offer detailed reviews of aerosol measurement, processes, experiments, and technology that changed the face of aerosol science. This volume is the third in a series and is supported by the American Association for Aerosol Research (AAAR) History Working Group, whose goal is to produce archival books from its symposiums on the history of aerosol science to ensure a lasting record. It is based on papers presented at the Third Aerosol History Symposium on September 8 and 9, 2006, in St. Paul, Minnesota, USA.
Scores of talented and dedicated people serve the forensic science community, performing vitally important work. However, they are often constrained by lack of adequate resources, sound policies, and national support. It is clear that change and advancements, both systematic and scientific, are needed in a number of forensic science disciplines to ensure the reliability of work, establish enforceable standards, and promote best practices with consistent application. Strengthening Forensic Science in the United States: A Path Forward provides a detailed plan for addressing these needs and suggests the creation of a new government entity, the National Institute of Forensic Science, to establish and enforce standards within the forensic science community. The benefits of improving and regulating the forensic science disciplines are clear: assisting law enforcement officials, enhancing homeland security, and reducing the risk of wrongful conviction and exoneration. Strengthening Forensic Science in the United States gives a full account of what is needed to advance the forensic science disciplines, including upgrading of systems and organizational structures, better training, widespread adoption of uniform and enforceable best practices, and mandatory certification and accreditation programs. While this book provides an essential call-to-action for congress and policy makers, it also serves as a vital tool for law enforcement agencies, criminal prosecutors and attorneys, and forensic science educators.
The first part of this book reviews the basics of atmospheric chemistry, radiation transport, and optical spectroscopy before detailing the principles underlying DOAS. The second part describes the design and application of DOAS instruments as well as the evaluation and interpretation of spectra. The recent expansion of DOAS application to the imaging of trace gas distributions by ground, aircraft, and satellite-based instruments is also covered.