Michael G. Barna

Directional Biases in Back Trajectories Caused by Model and Input Data

Abstract Back trajectory analyses are often used for source attribution estimates in visibility and other air quality studies. Several models and gridded meteorological datasets are readily available for generation of trajectories. The Big Bend Regional Aerosol and Visibility Observational (BRAVO) tracer study of July to October 1999 provided an opportunity to evaluate trajectory methods and input data against tracer concentrations, particulate data, and other source attribution techniques. Results showed evidence of systematic biases between the results of different back trajectory model and meteorological input data combinations at Big Bend National Park during the BRAVO. Most of the differences were because of the choice of meteorological data used as input to the trajectory models. Different back trajectories also resulted from the choice of trajectory model, primarily because of the different mechanisms used for vertical placement of the trajectories. No single model or single meteorological data set was found to be superior to the others, although rawinsonde data alone are too sparse in this region to be used as the only input data, and some combinations of model and input data could not be used to reproduce known attributions of tracers and simulated sulfate.

Regional Impacts of Oil and Gas Development on Ozone Formation in the Western United States

Abstract The Intermountain West is currently experiencing increased growth in oil and gas production, which has the potential to affect the visibility and air quality of various Class I areas in the region. The following work presents an analysis of these impacts using the Comprehensive Air Quality Model with extensions (CAMx). CAMx is a state-of-the-science, “one-atmosphere” Eulerian photochemical dispersion model that has been widely used in the assessment of gaseous and particulate air pollution (ozone, fine [PM2.5], and coarse [PM10] particulate matter). Meteorology and emissions inventories developed by the Western Regional Air Partnership Regional Modeling Center for regional haze analysis and planning are used to establish an ozone baseline simulation for the year 2002. The predicted range of values for ozone in the national parks and other Class I areas in the western United States is then evaluated with available observations from the Clean Air Status and Trends Network (CASTNET). This evaluation demonstrates the model’s suitability for subsequent planning, sensitivity, and emissions control strategy modeling. Once the ozone baseline simulation has been established, an analysis of the model results is performed to investigate the regional impacts of oil and gas development on the ozone concentrations that affect the air quality of Class I areas. Results indicate that the maximum 8-hr ozone enhancement from oil and gas (9.6 parts per billion [ppb]) could affect southwestern Colorado and northwestern New Mexico. Class I areas in this region that are likely to be impacted by increased ozone include Mesa Verde National Park and Weminuche Wilderness Area in Colorado and San Pedro Parks Wilderness Area, Bandelier Wilderness Area, Pecos Wilderness Area, and Wheeler Peak Wilderness Area in New Mexico.

Aerosol species concentrations and source apportionment of ammonia at Rocky Mountain National Park

Changes in ecosystem function at Rocky Mountain National Park (RMNP) are occurring because of emissions of nitrogen and sulfate species along the Front Range of the Colorado Rocky Mountains, as well as sources farther east and west. The nitrogen compounds include both oxidized and reduced nitrogen. A year-long monitoring program of various oxidized and reduced nitrogen species was initiated to better understand their origins as well as the complex chemistry occurring during transport from source to receptor. Specifically, the goals of the study were to characterize the atmospheric concentrations of nitrogen species in gaseous, particulate, and aqueous phases (precipitation and clouds) along the east and west sides of the Continental Divide; identify the relative contributions to atmospheric nitrogen species in RMNP from within and outside of the state of Colorado; identify the relative contributions to atmospheric nitrogen species in RMNP from emission sources along the Colorado Front Range versus other areas within Colorado; and identify the relative contributions to atmospheric nitrogen species from mobile sources, agricultural activities, and large and small point sources within the state of Colorado. Measured ammonia concentrations are combined with modeled releases of conservative tracers from ammonia source regions around the United States to apportion ammonia to its respective sources, using receptor modeling tools. Implications: Increased deposition of nitrogen in RMNP has been demonstrated to contribute to a number of important ecosystem changes. The rate of deposition of nitrogen compounds in RMNP has crossed a crucial threshold called the “critical load.” This means that changes are occurring to park ecosystems and that these changes may soon reach a point where they are difficult or impossible to reverse. Several key issues need attention to develop an effective strategy for protecting park resources from adverse impacts of elevated nitrogen deposition. These include determining the importance of previously unquantified nitrogen inputs within the park and identification of important nitrogen sources and transport pathways.

Reconciliation and Interpretation of Big Bend National Park Particulate Sulfur Source Apportionment: Results from the Big Bend Regional Aerosol and Visibility Observational Study—Part I

Abstract The Big Bend Regional Aerosol and Visibility Observational (BRAVO) study was an intensive monitoring study from July through October 1999 followed by extensive assessments to determine the causes and sources of haze in Big Bend National Park, located in Southwestern Texas. Particulate sulfate compounds are the largest contributor of haze at Big Bend, and chemical transport models (CTMs) and receptor models were used to apportion the sulfate concentrations at Big Bend to North American source regions and the Carbón power plants, located 225 km southeast of Big Bend in Mexico. Initial source attribution methods had contributions that varied by a factor of ≥2. The evaluation and comparison of methods identified opposing biases between the CTMs and receptor models, indicating that the ensemble of results bounds the true source attribution results. The reconciliation of these differences led to the development of a hybrid receptor model merging the CTM results and air quality data, which allowed a nearly daily source apportionment of the sulfate at Big Bend during the BRAVO study. The best estimates from the reconciliation process resulted in sulfur dioxide (SO2) emissions from U.S. and Mexican sources contributing ~55% and 38%, respectively, of sulfate at Big Bend. The distribution among U.S. source regions was Texas, 16%; the Eastern United States, 30%; and the Western United States, 9%. The Carbón facilities contributed 19%, making them the largest single contributing facility. Sources in Mexico contributed to the sulfate at Big Bend on most days, whereas contributions from Texas and Eastern U.S. sources were episodic, with their largest contributions during Big Bend sulfate episodes. On the 20% of the days with the highest sulfate concentrations, U.S. and Mexican sources contributed ˜71% and 26% of the sulfate, respectively. However, on the 20% of days with the lowest sulfate concentrations, Mexico contributed 48% compared with 40% for the United States.

Rocky Mountain National Park reduced nitrogen source apportionment

Excess wet and dry deposition of nitrogen-containing compounds are a concern at a number of national parks. The Rocky Mountain Atmospheric Nitrogen and Sulfur Study Part II (RoMANS II) campaign was conducted from November 2008 to November 2009 to characterize the composition of reactive nitrogen and sulfur deposited in Rocky Mountain National Park (RMNP). RoMANS II identified reduced nitrogen as the major contributor to reactive nitrogen deposition in RMNP, making up over 50% of the total. Motivated by this finding, the particulate source apportionment technology within the Comprehensive Air Quality Model with extensions was used here to estimate source apportionment of reduced nitrogen concentrations at RMNP. Source apportionment results suggest that approximately 40% of reduced nitrogen deposition to RMNP comes from ammonia sources within Colorado. However, the model evaluation also suggests that this number could be underrepresenting ammonia sources in eastern Colorado due to the difficulty of capturing upslope airflow on the eastern side of the Continental Divide with meteorological models. Emissions from California, the western model boundary, and the Snake River Valley in Idaho, the next three most influential sources, contribute approximately 15%, 8%, and 7%, respectively, to total reduced nitrogen measured in RMNP. Within Colorado, about 61%, 26%, and 13% of the total Colorado contribution comes from sources to the east of the Continental Divide, sources to the west of the Continental Divide, and from the park itself.

Meteorological and Back Trajectory Modeling for the Rocky Mountain Atmospheric Nitrogen and Sulfur Study II

The Rocky Mountain Atmospheric Nitrogen and Sulfur (RoMANS II) study with field operations during November 2008 through November 2009 was designed to evaluate the composition and sources of reactive nitrogen in Rocky Mountain National Park, Colorado, USA. As part of RoMANS II, a mesoscale meteorological model was utilized to provide input for back trajectory and chemical transport models. Evaluation of the models ability to capture important transport patterns in this region of complex terrain is discussed. Previous source-receptor studies of nitrogen in this region are also reviewed. Finally, results of several back trajectory analyses for RoMANS II are presented. The trajectory mass balance (TrMB) model, a receptor-based linear regression technique, was used to estimate mean source attributions of airborne ammonia concentrations during RoMANS II. Though ammonia concentrations are usually higher when there is transport from the east, the TrMB model estimates that, on average, areas to the west contribute a larger mean fraction of the ammonia. Possible reasons for this are discussed and include the greater frequency of westerly versus easterly winds, the possibility that ammonia is transported long distances as ammonium nitrate, and the difficulty of correctly modeling the transport winds in this area.

Origin of Fine Particulate Carbon in the Rural United States

Carbonaceous compounds are a significant component of fine particulate matter and haze in national parks and wilderness areas where visibility is protected, i.e., class I areas (CIAs). The Regional Haze Rule set the goal of returning visibility in CIAs on the most anthropogenically impaired days to natural by 2064. To achieve this goal, we need to understand contributions of natural and anthropogenic sources to the total fine particulate carbon (TC). A Lagrangian chemical transport model was used to simulate the 2006-2008 contributions from various source types to measured TC in CIAs and other rural lands. These initial results were incorporated into a hybrid model to reduce systematic biases. During summer months, fires and vegetation-derived secondary organic carbon together often accounted for >75% of TC. Smaller contributions, <20%, from area and mobile sources also occurred. During the winter, contributions from area and mobile sources increased, with area sources accounting for half or more of the TC in many regions. The area emissions were likely primarily from residential and industrial wood combustion. Different fire seasons were evident, with the largest contributions during the summer when wildfires occur and smaller contributions during the spring and fall when prescribed and agricultural fires regularly occur.

Reconciliation and Interpretation of the Big Bend National Park Light Extinction Source Apportionment: Results from the Big Bend Regional Aerosol and Visibility Observational Study—Part II

Abstract The recently completed Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study focused on particulate sulfate source attribution for a 4‐month period from July through October 1999. A companion paper in this issue by Schichtel et al. describes the methods evaluation and results reconciliation of the BRAVO Study sul-fate attribution approaches. This paper summarizes the BRAVO Study extinction budget assessment and interprets the attribution results in the context of annual and multiyear causes of haze by drawing on long‐term aerosol monitoring data and regional transport climatology, as well as results from other investigations. Particulate sulfates, organic carbon, and coarse mass are responsible for most of the haze at Big Bend National Park, whereas fine particles composed of light‐absorbing carbon, fine soils, and nitrates are relatively minor contributors. Spring and late summer through fall are the two periods of high-haze levels at Big Bend. Particulate sulfate and carbonaceous compounds contribute in a similar magnitude to the spring haze period, whereas sulfates are the primary cause of haze during the late summer and fall period. Atmospheric transport patterns to Big Bend vary throughout the year, resulting in a seasonal cycle of different upwind source regions contributing to its haze levels. Important sources and source regions for haze at Big Bend include biomass smoke from Mexico and Central America in the spring and African dust during the summer. Sources of sulfur dioxide (SO2) emissions in Mexico, Texas, and in the Eastern United States all contribute to Big Bend haze in varying amounts over different times of the year, with a higher contribution from Mexican sources in the spring and early summer, and a higher contribution from U.S. sources during late summer and fall. Some multiple‐day haze episodes result from the influence of several source regions, whereas others are primarily because of emissions from a single source region.

Modeling to Evaluate Contribution of Oil and Gas Emissions to Air Pollution

ABSTRACT Oil and gas production in the Western United States has increased considerably over the past 10 years. While many of the still limited oil and gas impact assessments have focused on potential human health impacts, the typically remote locations of production in the Intermountain West suggests that the impacts of oil and gas production on national parks and wilderness areas (Class I and II areas) could also be important. To evaluate this, we utilize the Comprehensive Air quality Model with Extensions (CAMx) with a year-long modeling episode representing the best available representation of 2011 meteorology and emissions for the Western United States. The model inputs for the 2011 episodes were generated as part of the Three State Air Quality Study (3SAQS). The study includes a detailed assessment of oil and gas (O&G) emissions in Western States. The year-long modeling episode was run both with and without emissions from O&G production. The difference between these two runs provides an estimate of the contribution of the O&G production to air quality. These data were used to assess the contribution of O&G to the 8 hour average ozone concentrations, daily and annual fine particulate concentrations, annual nitrogen deposition totals and visibility in the modeling domain. We present the results for the Class I and II areas in the Western United States. Modeling results suggest that emissions from O&G activity are having a negative impact on air quality and ecosystem health in our National Parks and Class I areas. Implications: In this research, we use a modeling framework developed for oil and gas evaluation in the western United States to determine the modeled impacts of emissions associated with oil and gas production on air pollution metrics. We show that oil and gas production may have a significant negative impact on air quality and ecosystem health in some national parks and other Class I areas in the western United States. Our findings are of particular interest to federal land managers as well as regulators in states heavy in oil and gas production as they consider control strategies to reduce the impact of development.

Source regions contributing to excess reactive nitrogen deposition in the Greater Yellowstone Area (GYA) of the United States

10 Research has shown that excess reactive nitrogen (Nr) deposition in the Greater Yellowstone Area (GYA) of the United States has passed critical load thresholds and is adversely affecting sensitive ecosystems in this area. To better understand the sources causing excess Nr deposition, the Comprehensive Air Quality Model with extensions (CAMx), using Western Air Quality Study (WAQS) emission and meteorology inputs, was used to simulate Nr deposition in the GYA. CAMx’s Particulate Source Apportionment Technology (PSAT) was employed to estimate contributions from agriculture (AG), oil and gas (OG), fire (Fire), and other (Other) source sectors from 27 regions, including the model boundary conditions (BC) representative of international contributions, to the simulated Nr for 2011. 15 Emissions from the AG and Other source sectors are predominantly from reduced N and oxidized N compounds, respectively. The model evaluation revealed a systematic underestimation in ammonia (NH3) concentrations by 65% and overestimation in nitric acid concentrations by 108%. The measured inorganic N wet deposition at National Trend Network sites in the GYA was overestimated by 31–49%, due at least partially to an overestimation of precipitation. Source apportionment results showed that the AG sector was the single largest contributor to the GYA total Nr deposition, contributing 34% on an annual basis. Seventyfour percent of the AG contributions originated from the Idaho Snake River valley, with Wyoming, California, and northern Utah contributing another 7%, 5%, 20 and 4% respectively. Contributions from the OG sector were small at about 1% over the GYA, except in the southern Wind River Mountain Range during winter where they accounted for more than 10%, with 46% of these contributions coming from OG activities in Wyoming. Wild and prescribed fires contributed 18% of the total Nr deposition, with fires within the GYA having the highest impact. The five largest source area contributions to the annual total Nr deposition in the GYA were 1) the Snake River valley (38% with AG 68%, OG 2%, Fire 15%, and Other 16%); 2) BC (21%); 3) Wyoming (12% with AG 19%, OG 5%, Fire 38%, and Other 39%); 4) California (7% with AG 26%, OG 1%, Fire 14%, and Other 59%); and 5) northern Utah (6% with AG 25%, OG 2%, Fire 10%, and 25 Other 63%). These results suggest that Nr deposition over the GYA, especially in the western region, was above the critical loads for sensitive ecosystems, and Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-372 Manuscript under review for journal Atmos. Chem. Phys. Discussion started: 27 April 2018 c