UMD Theses and Dissertations
Permanent URI for this collectionhttp://hdl.handle.net/1903/3
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Item MEASUREMENTS OF AEROSOL PHYSICOCHEMICAL PROPERTIES(2022) Razafindrambinina, Patricia Nirina; Asa-Awuku, Akua A; Chemistry; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Tiny liquid or solid particles suspended in the air with sizes ranging between several nanometers to several microns, collectively referred to as aerosol particles, are ubiquitous in the atmosphere and have been shown to affect a planet’s radiative budget. Aerosol particles have the ability to directly reflect and absorb solar radiation leading to a cooling or heating the planet’s surface, respectively (aerosol direct effect). Aerosol particles can also indirectly affect the net radiative forcing through water uptake and cloud formation prior to reflecting and absorbing solar radiation (aerosol indirect effect). In my dissertation, I utilize lab-based measurements to measure the optical properties of mineral dust and Martian dust simulants, and quantify the water uptake and cloud condensation nuclei activity of secondary organic aerosols (SOA), and water-soluble organic compounds in various mixing states and relative humidities. This body of work provides directly-measured values that may reduce uncertainties in climate prediction when used as inputs in future climate and air quality models.Item PROBING ATMOSPHERIC AEROSOL AND GAS PROPERTIES WITH PHOTOACOUSTIC SPECTROSCOPY(2011) Bueno, Pedro Antonio; Zachariah, Michael R; Dickerson, Russell R; Chemistry; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Absorption by atmospheric aerosols is the wild card for global climate change. Issues regarding atmospheric gases and aerosols have been at the forefront and the work presented within is directed at those issues. Specifically, work has been performed in order to help understand the issue of absorption in the atmosphere and whether this contributes towards positive forcing or warming of the atmosphere. In the process of conducting this research a custom, first-principles photoacoustic spectrometer was improved, calibrated and used extensively in order to obtain knowledge of the interaction of light with atmospherically relevant gases and make the first measurements of absorbing aerosols. The absorption cross-section of uncoated and coated soot was measured and quantified and found to be consistent with other work where amplifications on the order of nearly 100% were observed with uncertainty levels much lower than previously reported. Soot was also found to be optically thin where the total mass of the soot contributes to the absorption. Consequential to the soot work, the photoacoustic spectrometer developed to measure the absorption was utilized as a high precision greenhouse gas sensor. The photoacoustic spectrometer was found to produce results on the absorption of CO2 to within 3% of the theoretically predicted line profile Moreover, the photoacoustic spectrometer was used to determine measurable coating thicknesses of less than 10 nanometers on 100 nm soot particles.Item An analysis of convective transport, Lightning NO.sub.x production, and chemistry in midlatitude and subtropical thunderstorms(2006-10-18) Ott, Lesley Elaine; Dickerson, Russell R.; Atmospheric and Oceanic Sciences; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)The impact of lightning NO.sub.x production and convective transport on tropospheric chemistry was studied in four thunderstorms observed during field projects using a 3-dimensional (3-D) cloud-scale chemical transport model (CSCTM). The dynamical evolution of each storm was simulated using a cloud-resolving model, and the output used to drive the off-line CSCTM which includes a parameterized source of lightning NO.sub.x based on observed cloud-to-ground (CG) and intracloud (IC) flash rates. Simulated mixing ratios of tracer species were compared to anvil aircraft observations to evaluate convective transport in the model. The production of NO per CG flash (P.sub.CG) was estimated based on mean observed peak current, and production per IC flash (P.sub.IC) was scaled to P.sub.CG. Different values of P.sub.IC/P.sub.CG were assumed and the results compared with in-cloud aircraft measurements to estimate the ratio most appropriate for each storm. The impact of lightning NO.sub.x on ozone and other species was examined during the storm in the CSCTM and following each storm in the convective plume using a chemistry-only version of the model which includes diffusion but without advection, and assumes clear-sky photolysis rates. New lightning parameterizations were implemented in the CSCTM. One parameterization uses flash length data, rather than flash rates, as input, and production per meter of flash channel length is estimated. A second parameterization simulates indivdual lightning flashes rather than distributing lightning NOx uniformly among a large number of gridcells to better reproduce the variability of observations. The results suggest that PIC is likely on the order of PCG and not significantly less as has been assumed in many global modeling studies. Mean values of PCG=500 moles NO and PIC=425 moles NO have been estimated from these simulations of midlatitude and subtropical continental thunderstorms. Based on the estimates of production per flash, and an assumed ratio of the number of IC to CG flashes and global flash rate, a global annual lightning NO source of 8.6 Tg N yr-1 is estimated. Based on these simulations, vertical profiles of lightning NOx mass for subtropical and midlatitude continental regimes have been computed for use in global and regional chemical transport models.Item Investigating Uncertainties in Trace Gas Emissions from Boreal Forest Fires Using MOPITT Measurements of Carbon Monoxide and a Global Chemical Transport Model(2005-08-02) Hyer, Edward Joseph; Kasischke, Eric S; Geography; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Boreal forest fires are a significant contributor to atmospheric composition in the high northern hemisphere, and are highly variable both spatially and temporally. This study uses a new emissions model [Kasischke et al., 2005] to generate input to the University of Maryland Chemical Transport Model [Allen et al., 1996], with the goal of examining and constraining the key uncertainties in current understanding of boreal forest fire behavior. Model outputs are compared with data from the MOPITT instrument as well as in situ measurements of CO. A case study of CO transport during the summer of 2000 is used to examine several key uncertainties in the emissions estimates, describing how current levels of uncertainty affect atmospheric composition and applying atmospheric measurements can be applied to constrain uncertainty. Source magnitudes determined by inverse methods were shown to be highly sensitive to the assumed injection properties. For the boreal forest in 2000, the best agreement with observations was obtained with a pressure-weighted profile of injection throughout the tropospheric column, but detailed examination of the results makes clear that any uniform parameterization of injection will be a significant source of error when applied globally. Comparison of simulated CO distributions from daily, weekly, and monthly aggregate emissions sources demonstrated that while model data sources produced a valid representation of emissions at weekly resolution, the atmospheric distribution outside the source region has very little sensitivity to temporal variability at scales finer than 30 days. Different estimates of burned area produced large differences in simulated patterns of atmospheric CO. The GBA-2000 global product and the data sources used by Kasischke et al. [2005] gave better agreement with atmospheric observations compared to the GLOBSCAR product. Comparison of different estimates of fuel consumption indicated that atmospheric measurements of CO have limited sensitivity to spatial variability in fuels, but that current fuels maps can improve agreement with atmospheric measurements. These results provide a clear indication of how atmospheric measurements can be used to test hypotheses generated by emissions models.