Synthesis of the Southeast Atmosphere Studies: Investigating Fundamental Atmospheric Chemistry Questions

Carlton, Annmarie G.; Gouw, J. A. de; Jimenez, José L.; Ambrose, J. L.; Attwood, A. R.; Brown, Steven S.; Baker, Kirk R.; Brock, C. A.; Cohen, R. C.; Edgerton, Sylvia A.; Farkas, Caroline M.; Farmer, Delphine K.; Goldstein, Allen H.; Gratz, Lynne E.; Guenther, Alex; Hunt, S. W.; Jaeglé, Lyatt; Jaffe, Daniel A.; Mak, J. E.; McClure, Crystal D.; Nenes, Athanasios; Nguyen, T. K. V.; Pierce, Jeffrey R.; de, Suzane S.; Selin, Noelle E.; Shah, Viral; Shaw, Stephanie L.; Shepson, P. B.; Song, Shaojie; Stutz, J.; Surratt, Jason D.; Turpin, Barbara J.; Warneke, C.; Washenfelder, R. A.; Wennberg, P. O.; Zhou, X.

doi:10.1175/bams-d-16-0048.1

Cited by 78 publications

(115 citation statements)

References 122 publications

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“…High concentrations of water vapor were seen over the ocean, as well as along the Atlantic coastal plain. As expected, the areas of high concentrations for pollutants such as SO 2 , SO 2− 4 , and NO 2 were associated with urban regions in the southeast United States [42,43]. High ozone and sodium regions, on the other hand, were due to plumes transporting these species aloft.…”

Section: Resultssupporting

confidence: 61%

Pollution Transport Patterns Obtained Through Generalized Lagrangian Coherent Structures

2020

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Identifying atmospheric transport pathways is important to understand the effects of pollutants on weather, climate, and human health. The atmospheric wind field is variable in space and time and contains complex patterns due to turbulent mixing. In such a highly unsteady flow field, it can be challenging to predict material transport over a finite-time interval. Particle trajectories are often used to study how pollutants evolve in the atmosphere. Nevertheless, individual trajectories are sensitive to their initial conditions. Lagrangian Coherent Structures (LCSs) have been shown to form the template of fluid parcel motion in a fluid flow. LCSs can be characterized by special material surfaces that organize the parcel motion into ordered patterns. These key material surfaces form the core of fluid deformation patterns, such as saddle points, tangles, filaments, barriers, and pathways. Traditionally, the study of LCSs has looked at coherent structures derived from integrating the wind velocity field. It has been assumed that particles in the atmosphere will generally evolve with the wind. Recent work has begun to look at the motion of chemical species, such as water vapor, within atmospheric flows. By calculating the flux associated with each species, a new effective flux-based velocity field can be obtained for each species. This work analyzes generalized species-weighted coherent structures associated with various chemical species to find their patterns and pathways in the atmosphere, providing a new tool and language for the assessment of pollutant transport and patterns.

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Section: Resultssupporting

confidence: 61%

Pollution Transport Patterns Obtained Through Generalized Lagrangian Coherent Structures

2020

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“…The SOAS campaign also targeted observations of anthropogenic-biogenic interactions but at three sites (Centreville, AL; Birmingham, AL; and Look Rock, TN) in the substantially differing southeastern US environment during June and July 2013 (Carlton et al, 2016). Anthropogenic emissions, including NO x and SO 2 , have large influence on isoprene and monoterpene SOA in both rural and urban platforms (Budisulistiorini et al, 2015;Hu et al, 2015;Xu et al, 2015;Rattanavaraha et al, 2016).…”

Section: Observationsmentioning

confidence: 99%

Semivolatile POA and parameterized total combustion SOA in CMAQv5.2: impacts on source strength and partitioning

et al. 2017

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Abstract. Mounting evidence from field and laboratory observations coupled with atmospheric model analyses shows that primary combustion emissions of organic compounds dynamically partition between the vapor and particulate phases, especially as near-source emissions dilute and cool to ambient conditions. The most recent version of the Community Multiscale Air Quality model version 5.2 (CMAQv5.2) accounts for the semivolatile partitioning and gas-phase aging of these primary organic aerosol (POA) compounds consistent with experimentally derived parameterizations. We also include a new surrogate species, potential secondary organic aerosol from combustion emissions (pcSOA), which provides a representation of the secondary organic aerosol (SOA) from anthropogenic combustion sources that could be missing from current chemical transport model predictions. The reasons for this missing mass likely include the following: (1) unspeciated semivolatile and intermediate volatility organic compound (SVOC and IVOC, respectively) emissions missing from current inventories, (2) multigenerational aging of organic vapor products from known SOA precursors (e.g., toluene, alkanes), (3) underestimation of SOA yields due to vapor wall losses in smog chamber experiments, and (4) reversible organic compounds-water interactions and/or aqueous-phase processing of known organic vapor emissions. CMAQ predicts the spatially averaged contribution of pcSOA to OA surface concentrations in the continental United States to be 38.6 and 23.6 % in the 2011 winter and summer, respectively.Whereas many past modeling studies focused on a particular measurement campaign, season, location, or model configuration, we endeavor to evaluate the model and important uncertain parameters with a comprehensive set of United States-based model runs using multiple horizontal scales (4 and 12 km), gas-phase chemical mechanisms, July, 2011). Model improvements manifest better correlations (e.g., the correlation coefficient at Pasadena at night increases from 0.38 to 0.62) and reductions in underprediction during the photochemically active afternoon period (e.g., bias at Pasadena from −5.62 to −2.42 µg m −3 ). Daily averaged predictions of observations at routine-monitoring networks from simulations over the continental US (CONUS) in 2011 show modest improvement during winter, with mean biases reducing from 1.14 to 0.73 µg m −3 , but less change in the summer when the decreases from POA evaporation were similar to the magnitude of added SOA mass. Because the model-performance improvement realized by including the relatively simple pcSOA approach is similar to that of more-complicated parameterizations of OA formation and aging, we recommend caution when applying these morecomplicated approaches as they currently rely on numerous uncertain parameters.The pcSOA parameters optimized for performance at the southern and northern California sites lead to higher OA formation than is observed in the CONUS evaluation. This may be due to any of the following: variations in ...

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“…PAN is formed from both anthropogenic and biogenic hydrocarbon precursors. PPN, on the other hand, is formed primarily from anthropogenic hydrocarbons (AHCs) (e.g., propanal, propane, 1-butene), while MPAN is derived from methacrolein (MACR), an oxidation product of the mostly biogenic hydrocarbon (BHC) isoprene (e.g., Biesenthal and Shepson, 1997;Carter and Atkinson, 1996).…”

Section: Introductionmentioning

confidence: 99%

Importance of biogenic volatile organic compounds to acyl peroxy nitrates (APN) production in the southeastern US during SOAS 2013

et al. 2019

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Gas-phase atmospheric concentrations of peroxyacetyl nitrate (PAN), peroxypropionyl nitrate (PPN), and peroxymethacryloyl nitrate (MPAN) were measured on the ground using a gas chromatograph electron capture detector (GC-ECD) during the Southern Oxidants and Aerosols Study (SOAS) 2013 campaign (1 June to 15 July 2013) in Centreville, Alabama, in order to study biosphere-atmosphere interactions. Average levels of PAN, PPN, and MPAN were 169, 5, and 9 pptv, respectively, and the sum accounts for an average of 16 % of NO y during the daytime (10:00 to 16:00 local time). Higher concentrations were seen on average in air that came to the site from the urban NO x sources to the north. PAN levels were the lowest observed in ground measurements over the past two decades in the southeastern US. A multiple regression analysis indicates that biogenic volatile organic compounds (VOCs) account for 66 % of PAN formation during this study. Comparison of this value with a 0-D model simulation of peroxyacetyl radical production indicates that at least 50 % of PAN formation is due to isoprene oxidation. MPAN has a statistical correlation with isoprene hydroxynitrates (IN). Organic aerosol mass increases with gas-phase MPAN and IN concentrations, but the mass of organic nitrates in particles is largely unrelated to MPAN.

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Synthesis of the Southeast Atmosphere Studies: Investigating Fundamental Atmospheric Chemistry Questions

Cited by 78 publications

References 122 publications

Pollution Transport Patterns Obtained Through Generalized Lagrangian Coherent Structures

Pollution Transport Patterns Obtained Through Generalized Lagrangian Coherent Structures

Semivolatile POA and parameterized total combustion SOA in CMAQv5.2: impacts on source strength and partitioning

Importance of biogenic volatile organic compounds to acyl peroxy nitrates (APN) production in the southeastern US during SOAS 2013

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