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Upwind sources of NO x and SO2 play a crucial role in the amount of O3 and aerosols in the lower troposphere in the Mid-Atlantic US. This paper describes a novel method of clustering trace gas and aerosol profiles allowing for the quantification of the relationship between point sources and pollution levels. This improves our understanding of pollution origins and has the potential for prediction of episodes of poor air quality. A hierarchical clustering method was used to classify distinct chemical and meteorological events from over 200 aircraft vertical profiles in the lower troposphere. Profile measurements included O3, SO2, CO and particle scattering from June to August 1997–2003, in the Mid-Atlantic US (mostly in Maryland, Pennsylvania and Virginia). The clustering technique could discriminate distinct profile shapes including measurements made during the 2002 Canadian forest fires. Forty-eight-hour back trajectories were run for each profile and the integrated NO x and SO2 point source emissions encountered by each trajectory were calculated using data from the EPA Clean Air Market Division''s emissions database. There was a strong correlation between integrated NO x emissions and O3 profiles, indicating that O3 profiles are strongly influenced by and can be predicted with point source emissions. There is a prevalent concentration of SO2 over the eastern US with mixing ratios decreasing smoothly from about 3.5ppb near the surface to 0.2ppb at 2400m. [Copyright &y& Elsevier]

In community time series studies on the effect of particulate air pollution on mortality, particulate air pollution data are often available from multiple monitors. Published studies have combined the data from the multiple monitors using a simple or trimmed average. In this paper, I describe an alternative method for combining the particulate air pollution data available from multiple monitors. Using time series data from Cook County, Illinois the proposed method yields more meaningful biologically plausible particulate air pollution mortality effect estimates without loss of statistical accuracy and reduces the full set of monitors to a smaller set without loss of information. The proposed monitor combination may be more highly correlated with the average population exposure to particulate air pollution than a simple or trimmed average of the monitors. [Copyright &y& Elsevier]

Engineering estimates of methane emissions from natural gas production have led to varied projections of national emissions. This work reports direct measurements of methane emissions at 190 onshore natural gas sites in the United States (150 production sites, 27 well completion flowbacks, 9 well unloadings, and 4 workovers). For well completion flowbacks, which clear fractured wells of liquid to allow gas production, methane emissions ranged from 0.01 Mg to 17 Mg (mean = 1.7 Mg; 95% confidence bounds of 0.67-3.3 Mg), compared with an average of 81 Mg per event in the 2011 EPA national emission inventory from April 2013. Emission factors for pneumatic pumps and controllers as well as equipment leaks were both comparable to and higher than estimates in the national inventory. Overall, if emission factors from this work for completion flowbacks, equipment leaks, and pneumatic pumps and controllers are assumed to be representative of national populations and are used to estimate national emissions, total annual emissions from these source categories are calculated to be 957 Gg of methane (with sampling and measurement uncertainties estimated at ±200 Gg). The estimate for comparable source categories in the EPA national inventory is ~1,200 Gg. Additional measurements of unloadings and workovers are needed to produce national emission estimates for these source categories. The 957 Gg in emissions for completion flowbacks, pneumatics, and equipment leaks, coupled with EPA national inventory estimates for other categories, leads to an estimated 2,300 Gg of methane emissions from natural gas production (0.42% of gross gas production). [ABSTRACT FROM AUTHOR]

Field blanks (bQF) and backup filters (quartz-fiber behind quartz-fiber filter; QBQ) have been adopted by US long-term air quality monitoring networks to estimate PM2.5 organic carbon (OC) sampling artifacts. This study documents bQF and QBQ carbon levels for the: 1) Interagency Monitoring of Protected Visual Environments (IMPROVE); 2) Speciation Trends Network (STN; part of the Chemical Speciation Network [CSN]); and 3) Southeastern Aerosol Research and Characterization (SEARCH) networks and examines the similarities/differences associated with network-specific sampling protocols. A higher IMPROVE sample volume and smaller filter deposit area results in PM2.5 areal density (μg/cm2 on filter) 3-11 times those of STN/CSN and SEARCH samples for the same ambient PM2.5 concentrations, thus reducing the relative contribution of sampling artifacts from passive OC adsorption. A relatively short (1-15 min) passive exposure period of STN/CSN and SEARCH bQF OC (0.8-1 μg/cm2) underestimates positive and negative OC artifacts resulting from passive adsorption or evaporation of semi-volatile organic compounds on quartz-fiber filters. This is supported by low STN/CSN and SEARCH bQF levels and lack of temporal or spatial variability among the sites within the networks. With a much longer period, ∼7 days of ambient passive exposure, average IMPROVE bQF and QBQ OC are comparable (2.4±0.5 and 3.1±0.8 μg/cm2, respectively) and more than twice levels found in the STN/CSN and SEARCH networks. Sampling artifacts in STN/CSN were estimated from collocated IMPROVE samples based on linear regression. At six of the eight collocated sites in this study, STN/CSN bQFs underestimated OC artifacts by 11-34%. Using a preceding organic denuder in the SEARCH network minimized passive adsorption on QBQ, but OC on QBQ may not be attributed entirely to the negative sampling artifact (e.g., evaporated or volatilized OC from the front filter deposits after sample collection). [ABSTRACT FROM AUTHOR]

A study of air quality was performed using a compact, aircraft aerosol lidar designed in the Science Directorate at NASA Langley Research Center and Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical depth (AOD) retrievals. Five flights of lidar measurements conducted in the Hampton–Norfolk–Virginia Beach, Virginia, region showed complex regional aerosol distributions. Comparisons with MODIS AOD at 10 km × 10 km and 5 km × 5 km resolutions show good agreement, with correlation R2 values of 0.82 and 0.88, respectively. Linear regressions of particulate matter with a diameter of less than 2.5 μm (PM2.5) and AOD within the ranges of 5–40 μg m-3 and 0.05–0.7, respectively, result in R2 values of ∼0.64 and ∼0.82 for MODIS and the Compact Aerosol Lidar, respectively. The linear regressions reflect approximately 51 μg m-3 to 1 AOD. These relationships are in agreement with previous findings for air pollution aerosols in the eastern United States and in northern Italy. However, large vertical variation is seen case by case, with planetary boundary layer heights ranging between 0.7 and 2 km and uncertainties ranging between 0.1 and 0.4 km. The results of the case studies suggest that AOD can be used as an indicator of surface measurements of PM2.5 but with larger uncertainties associated with small aerosol loading (AOD < 0.3). [ABSTRACT FROM AUTHOR]

Valley cold pools (VCPs), which are trapped, cold layers of air at the bottoms of basins or valleys, pose a significant problem for forecasters because they can lead to several forms of difficult-to-forecast and hazardous weather such as fog, freezing rain, or poor air quality. Numerical models have historically failed to routinely provide accurate guidance on the formation and demise of VCPs, making the forecast problem more challenging. In some case studies of persistent wintertime VCPs, there is a connection between the movement of upper-level waves and the timing of VCP formation and decay. Herein, a 3-yr climatology of persistent wintertime VCPs for five valleys and basins in the western United States is performed to see how often VCP formation and decay coincides with synoptic-scale (∼200–2000 km) wave motions. Valley cold pools are found to form most frequently as an upper-level ridge approaches the western United States and in response to strong midlevel warming. The VCPs usually last as long as the ridge is over the area and usually only end when a trough, and its associated midlevel cooling, move over the western United States. In fact, VCP strength appears to be almost entirely dictated by midlevel temperature changes, which suggests large-scale forcing is dominant for this type of VCP most of the time. [ABSTRACT FROM AUTHOR]

During the New England Air Quality Study (NEAQS) in the summer of 2004, airborne measurements were made of the major inorganic ions and the water-soluble organic carbon (WSOC) of the submicron (PM1.0) aerosol. These and ancillary data are used to describe the overall aerosol chemical characteristics encountered during the study. Fine particle mass was estimated from particle volume and a calculated density based on measured particle composition. Fine particle organic matter (OM) was estimated from WSOC and a mass balance analysis. The aerosol over the northeastern United States (U.S.) and Canada was predominantly sulfate and associated ammonium, and organic components, although in unique plumes additional ionic components were also periodically above detection limits. In power generation regions, and especially in the Ohio River Valley region, the aerosol tended to be predominantly sulfate (~ 60%µgµg-1) and apparently acidic, based on an excess of measured anions compared to cations. In all other regions where sulfate concentrations were lower and a smaller fraction of overall mass, the cations and anions were balanced suggesting a more neutral aerosol. In contrast, the WSOC and estimated OM were more spatially uniform and the fraction of OM relative to PM mass was largely influenced by sources of sulfate. The study median OM mass fraction was 40%. Throughout the study region, sulfate and organic aerosol mass were highest near the surface and decreased rapidly with increasing altitude. The relative fraction of organic mass to sulfate was similar throughout all altitudes within the boundary layer (altitude less than 2.5 km), but was significantly higher at altitude layers in the free troposphere (above 2.5 km). A number of distinct biomass burning plumes from fires in Alaska and the Yukon were periodically intercepted, mostly at altitudes between 3 and 4 km. These plumes were associated with highest aerosol concentrations of the study and were largely comprised of organic aerosol components (~60%). [ABSTRACT FROM AUTHOR]

Concentrations of ozone exceeding regulatory standards are regularly observed along the coasts of New Hampshire and Maine in summer. These events are primarily caused by the transport of pollutants from urban areas in Massachusetts and farther south and west. Pollutant transport is most efficient over the ocean. The coastline makes transport processes complex because it makes the structure of the atmospheric boundary layer complex. During pollution episodes, the air over land in daytime is warmer than the sea surface, so air transported from land over water becomes statically stable and the formerly well-mixed boundary layer separates into possibly several layers, each transported in a different direction. This study examines several of the atmospheric boundary layer processes involved in pollutant transport. A three-dimensional model [the Coupled Ocean–Atmosphere Mesoscale Prediction System (COAMPS)] run on grids of 2.5 and 7.5 km is used to examine the winds, thermodynamic structure, and structure of tracer plumes emitted from Boston, Massachusetts, and New York City, New York, in two different real cases—one dominated by large-scale transport (22–23 July 2002) and one with important mesoscale effects (11–14 August 2002). The model simulations are compared with measurements taken during the 2002 New England Air Quality Study. The model simulates the basic structure of the two different episodes well. The boundary layer stability over the cold water is weaker in the model than in reality. The tracer allows for easy visualization of the pollutant transport. [ABSTRACT FROM AUTHOR]