Atmospheric & Oceanic Science
Permanent URI for this communityhttp://hdl.handle.net/1903/2264
Formerly known as the Department of Meteorology.
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Item EXAMINATION OF TROPOSPHERIC OZONE AND ITS PRECURSORS WITHIN AN AIR QUALITY MODEL AND IMPLICATIONS FOR AIR QUALITY AND CLIMATE(2021) Hembeck, Linda; Salawitch, Ross J; Canty, Timothy P; Atmospheric and Oceanic Sciences; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Elevated levels of tropospheric ozone (O3) caused by emissions of NOx and VOCs negatively impact human health, crops, and ecosystems. Even if precursor emissions are reduced below current levels, predicted higher temperatures due to increased greenhouse gas emissions could impede resulting air quality benefits. Air quality models simulate the complex relationships that form O3 and are used to guide policy decisions directed at improving O3. The body of this work encompasses three projects related to improvements in the representation of O3 and precursors in air quality models. First, I examine the role of O3 and its precursors in air quality and climate change by evaluating ozone production efficiency (OPE) and O3 precursors within models. I modified a chemical mechanism and the emissions of NOx to accurately represent NOx, the reactivity of NOx with peroxy radicals, HCHO, isoprene, as well as organic and inorganic NOy reservoir species. Implementation of these modifications increased confidence in model simulations. Results indicate accepted inventories overestimated NOx emissions but underestimate total VOC reactivity and OPE. Second, I examined the dependence of surface O3 on temperature (climate penalty factor (CPF)) throughout a period of 11 years within an air quality model and measurements. Future increases in temperature could offset benefits from future reductions in the emission of O3 precursors. Determining and understanding the CPF is critical to formulating effective strategies to reduce future exceedances. I have demonstrated that the model can reproduce O3 sensitivity to temperature reasonably well. By controlling emissions specifically of NOx mankind has reduced its vulnerability. Third, I compare satellite-observed and modeled ammonia (NH3) under varying chemical environments over East Asia. Regulation of O3 precursor concentrations in the atmosphere has an indirect effect on NH3 concentrations. Air quality policy to reduce NOx and through that also nitric acid (HNO3) in the atmosphere can result in an increase in the concentration of NH3 because of its neutralizing ability. Therefore, a less acidic atmosphere sequesters less NH3. This preliminary work exposes different areas that need to be addressed to gain greater insight into NH3 emissions and chemistry.Item RELATIONSHIP BETWEEN COLUMN DENSITY AND SURFACE MIXING RATIO FOR O3 AND NO2: IMPLICATIONS FOR SATELLITE OBSERVATIONS AND THE IMPACTS OF VERTICAL MIXING(2016) Flynn, Clare Marie; Pickering, Kenneth E; Atmospheric and Oceanic Sciences; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Satellites have great potential for diagnosis of surface air quality conditions, though reduced sensitivity of satellite instrumentation to the lower troposphere currently impedes their applicability. One objective of the NASA DISCOVER-AQ project is to provide information relevant to improving our ability to relate satellite-observed columns to surface conditions for key trace gases and aerosols. In support of DISCOVER-AQ, this dissertation investigates the degree of correlation between O3 and NO2 column abundance and surface mixing ratio during the four DISCOVER-AQ deployments; characterize the variability of the aircraft in situ and model-simulated O3 and NO2 profiles; and use the WRF-Chem model to further investigate the role of boundary layer mixing in the column-surface connection for the Maryland 2011 deployment, and determine which of the available boundary layer schemes best captures the observations. Simple linear regression analyses suggest that O3 partial column observations from future satellite instruments with sufficient sensitivity to the lower troposphere may be most meaningful for surface air quality under the conditions associated with the Maryland 2011 campaign, which included generally deep, convective boundary layers, the least wind shear of all four deployments, and few geographical influences on local meteorology, with exception of bay breezes. Hierarchical clustering analysis of the in situ O3 and NO2 profiles indicate that the degree of vertical mixing (defined by temperature lapse rate) associated with each cluster exerted an important influence on the shapes of the median cluster profiles for O3, as well as impacted the column vs. surface correlations for many clusters for both O3 and NO2. However, comparisons to the CMAQ model suggest that, among other errors, vertical mixing is overestimated, causing too great a column-surface connection within the model. Finally, the WRF-Chem model, a meteorology model with coupled chemistry, is used to further investigate the impact of vertical mixing on the O3 and NO2 column-surface connection, for an ozone pollution event that occurred on July 26-29, 2011. Five PBL schemes were tested, with no one scheme producing a clear, consistent “best” comparison with the observations for PBLH and pollutant profiles; however, despite improvements, the ACM2 scheme continues to overestimate vertical mixing.Item Lifetime and distribution of ozone and related pollutants in the eastern United States(2015) Goldberg, Daniel L.; Dickerson, Russell R; Salawitch, Ross J; Atmospheric and Oceanic Sciences; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Most major cities in the eastern United States have air quality deemed unhealthy by the EPA under a set of regulations known as the National Ambient Air Quality Standards (NAAQS). The worst air quality in Maryland is measured in Edgewood, MD, a small community located along the Chesapeake Bay and generally downwind of Baltimore during hot, summertime days. Direct measurements and numerical simulations were used to investigate how meteorology and chemistry conspire to create adverse levels of photochemical smog especially at this coastal location. Ozone (O3) and oxidized reactive nitrogen (NOy), a family of ozone precursors, were measured over the Chesapeake Bay during a ten day experiment in July 2011 to better understand the formation of ozone over the Bay and its impact on coastal communities such as Edgewood. Ozone over the Bay during the afternoon was 10% to 20% higher than the closest upwind ground sites. A combination of complex boundary layer dynamics, deposition rates, and unaccounted marine emissions play an integral role in the regional maximum of ozone over the Bay. The CAMx regional air quality model was assessed and enhanced through comparison with data from NASA’s 2011 DISCOVER-AQ field campaign. Comparisons show a model overestimate of NOy by +86.2% and a model underestimate of formaldehyde (HCHO) by –28.3%. I present a revised model framework that better captures these observations and the response of ozone to reductions of precursor emissions. Incremental controls on electricity generating stations will produce greater benefits for surface ozone while additional controls on mobile sources may yield less benefit because cars emit less pollution than expected. Model results also indicate that as ozone concentrations improve with decreasing anthropogenic emissions, the photochemical lifetime of tropospheric ozone increases. The lifetime of ozone lengthens because the two primary gas-phase sinks for odd oxygen (Ox ≈ NO2 + O3) – attack by hydroperoxyl radicals (HO2) on ozone and formation of nitrate – weaken with decreasing pollutant emissions. This unintended consequence of air quality regulation causes pollutants to persist longer in the atmosphere, and indicates that pollutant transport between states and countries will likely play a greater role in the future.Item IMPACTS OF FAIR-WEATHER CUMULUS CLOUDS, BAY BREEZES, AND LAND USE ON URBAN AIR QUALITY AND CLIMATE(2011) Loughner, Christopher Paul; Allen, Dale J; Dickerson, Russell R; Atmospheric and Oceanic Sciences; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Fair-weather cumulus clouds, bay breezes, and land use influence air quality and climate. The impacts of urban land surface changes and model resolution on fair-weather cumulus clouds, bay breezes, air quality, and climate are examined. As model resolution increases, more pollutants are transported aloft through fair-weather cumulus clouds causing an increase in the rate of sulfur dioxide conversion to sulfate aerosols and an increase in boundary layer venting. As model resolution increases, a larger temperature gradient develops along the shoreline of the Chesapeake Bay causing the bay breeze to form sooner, push farther inland, and loft more pollutants upward. This stronger bay breeze results in low-level convergence, a buildup of near surface ozone over land and a decrease in the land-to-sea flux of ozone and ozone precursors. Also, an examination of the sensitivity of sulfur dioxide to sulfate conversion to different model cloud parameters shows the importance of accurately simulating clouds to obtain accurate sulfate concentrations. To analyze the impact of urbanization on the atmosphere, an urban tree parameterization is developed for the Weather Research and Forecasting model coupled with an urban canopy model (WRF-UCM) to determine how urban trees can dampen the urban heat island (UHI). Adding vegetation decreases the (subgrid-scale) surface air temperature due to tree shading and evapotranspiration. The impact of building height on the UHI shows that shorter urban buildings have higher daytime surface temperatures due to less shading and lower nighttime temperatures due to less longwave radiative trapping in urban street canyons. The WRF-UCM with urban trees is utilized with an air quality model to investigate how urban vegetation changes impact air quality. Cooling due to planting urban trees is expected to improve air quality. However, for one case study that does not include anthropogenic emissions reductions due to cooling from increased vegetation, adding trees in the model results in higher ground level ozone concentrations due to a shallower planetary boundary layer and more pollutants converging near a stronger bay breeze near Baltimore, MD. Future work incorporating changes in anthropogenic emissions with changes in urban vegetation will help quantify how urban trees impact air quality.Item Assimilation of trace gas retrievals with the Local Ensemble Transform Kalman Filter(2009) Kuhl, David Derieg; Kalnay, Eugenia; Szunyogh, Istvan; Atmospheric and Oceanic Sciences; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Over the 50 year history of Numerical Weather Prediction (NWP), the focus has been on the modeling and prediction of meteorological parameters such as surface pressure, temperature, wind, and precipitation. However, due to concerns over pollution and to recent advancements in satellite technologies, an increasing number of NWP systems have been upgraded to include capabilities to analyze and predict the concentration of trace gases. This dissertation explores some of the specific issues that have to be addressed for an efficient modeling of the concentration of the trace gases. These issues include modeling the effects of convective mixing on the concentration of the trace gases and the multivariate assimilation of space-based observations of the concentration of the trace gases. In this dissertation, we assimilate observations of the concentration of trace gases with an implementation of the Local Ensemble Transform Kalman Filter (LETKF) data assimilation system on the National Centers for Environmental Prediction (NCEP) Global Forecast System (GFS) NWP model. We use a modified version of the NCEP GFS model that was operational in 2004 at resolution T62/L28. We modify the model by adding parameterization for the process of convective mixing of the trace gases. We consider two specific trace gases: ozone (O3) and carbon monoxide (CO). We incorporate these gases into the model by using 3-dimensional time-dependent O3 and CO production-loss values from the Real-time Air Quality Modeling System (RAQMS) global chemical model. The O3 observations we assimilate are from the Solar Backscatter UltraViolet generation 2 (SBUV/2) satellite instrument (version 8) flown on the NOAA 16 and 17 satellites. The CO observations we assimilate are from the Measurements Of Pollution In The Troposphere (MOPITT) instrument (version 3) flown on the NASA TERRA satellite. We also develop a new observation operator for the assimilation of retrievals with the LETKF. We carry out numerical experiment for the period between 000UTC 1 July 2004 to 000UTC 15 August in the summer of 2004. The analysis and forecast impact of the assimilation of trace gas observations on the meteorological fields is assessed by comparing the analyses and forecasts to the high resolution operational NCEP GFS analyses and to radiosonde observations. The analysis and forecast impact on the trace gas fields is assessed by comparing the analyzed and predicted fields to observations collected during the Intercontinental Chemical Transport Experiment (INTEX-A) field mission. The INTEX-A field mission was conducted to characterize composition of pollution over North America, thus providing us with ozonesonde and aircraft based verification data. We find that adding the process of convective mixing to the parameterization package of the model and the assimilation of observations of the trace gases improves the analysis and forecast of the concentration of the trace gases. In particular, our system is more accurate in quantifying the concentration of O3 in the troposphere than the original NCEP GFS. Also, our system is competitive with the state-of-the-art RAQMS atmospheric chemical model in analyzing the concentration of O3 and CO throughout the full atmospheric model column. The assimilation of O3 and CO observations has a mixed impact on the analysis and forecast of the meteorological fields. We find that most of the negative impact on the meteorological fields can be eliminated, without much reduction to the positive impact on the trace gas fields, by inflating the prescribed variance of the trace gas observations. The appendices of this dissertation reproduces two papers on related research. The first paper covers the northward front movement and rising surface temperatures in the great planes. The second paper covers the assessment of predictability with a Local Ensemble Kalman Filter.