Browsing by Author "Usenko, Sascha"
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Item Apportioned primary and secondary organic aerosol during pollution events of DISCOVER-AQ Houston(Elsevier, 2021) Yoon, Subin; Ortiz, Stephanie M.; Clark, Adelaide E.; Barrett, Tate E.; Usenko, Sascha; Duvall, Rachelle M.; Ruiz, Lea Hildebrandt; Bean, Jeffrey K.; Faxon, Cameron B.; Flynn, James H.; Lefer, Barry L.; Leong, Yu Jun; Griffin, Robert J.; Sheesley, Rebecca J.Understanding the drivers for high ozone (O3) and atmospheric particulate matter (PM) concentrations is a pressing issue in urban air quality, as this understanding informs decisions for control and mitigation of these key pollutants. The Houston, TX metropolitan area is an ideal location for studying the intersection between O3 and atmospheric secondary organic carbon (SOC) production due to the diversity of source types (urban, industrial, and biogenic) and the on- and off-shore cycling of air masses over Galveston Bay, TX. Detailed characterization of filter-based samples collected during Deriving Information on Surface Conditions from Column and VERtically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) Houston field experiment in September 2013 were used to investigate sources and composition of organic carbon (OC) and potential relationships between daily maximum 8 h average O3 and PM. The current study employed a novel combination of chemical mass balance modeling defining primary (i.e. POC) versus secondary (i.e. SOC) organic carbon and radiocarbon (14C) for apportionment of contemporary and fossil carbon. The apportioned sources include contemporary POC (biomass burning [BB], vegetative detritus), fossil POC (motor vehicle exhaust), biogenic SOC and fossil SOC. The filter-based results were then compared with real-time measurements by aerosol mass spectrometry. With these methods, a consistent urban background of contemporary carbon and motor vehicle exhaust was observed in the Houston metropolitan area. Real-time and filter-based characterization both showed that carbonaceous aerosols in Houston was highly impacted by SOC or oxidized OC, with much higher contributions from biogenic than fossil sources. However, fossil SOC concentration and fractional contribution had a stronger correlation with daily maximum 8 h average O3, peaking during high PM and O3 events. The results indicate that point source emissions processed by on- and off-shore wind cycles likely contribute to peak events for both PM and O3 in the greater Houston metropolitan area.Item Captive Aerosol Growth and Evolution (CAGE) chamber system to investigate particle growth due to secondary aerosol formation(Copernicus Publications, 2021) Sirmollo, Candice L.; Collins, Don R.; McCormick, Jordan M.; Milan, Cassandra F.; Erickson, Matthew H.; Flynn, James H.; Sheesley, Rebecca J.; Usenko, Sascha; Wallace, Henry W.; Bui, Alexander A.T.; Griffin, Robert J.; Tezak, Matthew; Kinahan, Sean M.; Santarpia, Joshua L.Environmental chambers are a commonly used tool for studying the production and processing of aerosols in the atmosphere. Most are located indoors and most are filled with air having prescribed concentrations of a small number of reactive gas species. Here we describe portable chambers that are used outdoors and filled with mostly ambient air. Each all-Teflon® 1 m3 Captive Aerosol Growth and Evolution (CAGE) chamber has a cylindrical shape that rotates along its horizontal axis. A gas-permeable membrane allows exchange of gas-phase species between the chamber and surrounding ambient air with an exchange time constant of approximately 0.5 h. The membrane is non-permeable to particles, and those that are injected into or nucleate in the chamber are exposed to the ambient-mirroring environment until being sampled or lost to the walls. The chamber and surrounding enclosure are made of materials that are highly transmitting across the solar ultraviolet and visible wavelength spectrum. Steps taken in the design and operation of the chambers to maximize particle lifetime resulted in averages of 6.0, 8.2, and 3.9 h for ∼ 0.06, ∼ 0.3, and ∼ 2.5 µm diameter particles, respectively. Two of the newly developed CAGE chamber systems were characterized using data acquired during a 2-month field study in 2016 in a forested area north of Houston, TX, USA. Estimations of measured and unmeasured gas-phase species and of secondary aerosol production in the chambers were made using a zero-dimensional model that treats chemical reactions in the chamber and the continuous exchange of gases with the surrounding air. Concentrations of NO, NO2, NOy, O3, and several organic compounds measured in the chamber were found to be in close agreement with those calculated from the model, with all having near 1.0 best fit slopes and high r2 values. The growth rates of particles in the chambers were quantified by tracking the narrow modes that resulted from injection of monodisperse particles and from occasional new particle formation bursts. Size distributions in the two chambers were measured intermittently 24 h d−1. A bimodal diel particle growth rate pattern was observed, with maxima of about 6 nm h−1 in the late morning and early evening and minima of less than 1 nm h−1 shortly before sunrise and sunset. A pattern change was observed for hourly averaged growth rates between late summer and early fall.Item Composition and Sources of Particulate Matter Measured near Houston, TX: Anthropogenic-Biogenic Interactions(MDPI, 2016) Bean, Jeffrey K.; Faxon, Cameron B.; Leong, Yu Jun; Wallace, Henry William; Cevik, Basak Karakurt; Ortiz, Stephanie; Canagaratna, Manjula R.; Usenko, Sascha; Sheesley, Rebecca J.; Griffin, Robert J.; Ruiz, Lea HildebrandtParticulate matter was measured in Conroe, Texas (~60 km north of downtown Houston, Texas) during the September 2013 DISCOVER-AQ campaign to determine the sources of particulate matter in the region. The measurement site is influenced by high biogenic emission rates as well as transport of anthropogenic pollutants from the Houston metropolitan area and is therefore an ideal location to study anthropogenic-biogenic interactions. Data from an Aerosol Chemical Speciation Monitor (ACSM) suggest that on average 64 percent of non-refractory PM1 was organic material, including a high fraction (27%–41%) of organic nitrates. There was little diurnal variation in the concentrations of ammonium sulfate; however, concentrations of organic and organic nitrate aerosol were consistently higher at night than during the day. Potential explanations for the higher organic aerosol loadings at night include changing boundary layer height, increased partitioning to the particle phase at lower temperatures, and differences between daytime and nighttime chemical processes such as nitrate radical chemistry. Positive matrix factorization was applied to the organic aerosol mass spectra measured by the ACSM and three factors were resolved—two factors representing oxygenated organic aerosol and one factor representing hydrocarbon-like organic aerosol. The factors suggest that the measured aerosol was well mixed and highly processed, consistent with the distance from the site to major aerosol sources, as well as the high photochemical activity.Item The impacts of regional shipping emissions on the chemical characteristics of coastal submicron aerosols near Houston, TX(Copernicus Publications, 2018) Schulze, Benjamin C.; Wallace, Henry W.; Bui, Alexander T.; Flynn, James H.; Erickson, Matt H.; Alvarez, Sergio; Dai, Qili; Usenko, Sascha; Sheesley, Rebecca J.; Griffin, Robert J.The air quality of the Texas Gulf Coast region historically has been influenced heavily by regional shipping emissions. However, the effects of the recently established North American Emissions Control Area on aerosol concentrations and properties in this region are presently unknown. In order to better understand the current sources and processing mechanisms influencing coastal aerosol near Houston, a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed for 3 weeks at a coastal location during May–June 2016. Total mass loadings of organic and inorganic non-refractory aerosol components during onshore flow periods were similar to those published before establishment of the regulations. Based on estimated methanesulfonic acid (MSA) mass loadings and published biogenic MSA/non-sea-salt sulfate (nss-SO4) ratios, an average of over 75% of the observed nss-SO4 was from anthropogenic sources, predominantly shipping emissions. Mass spectral analysis indicated that for periods with similar backward-trajectory-averaged meteorological conditions, air masses influenced by shipping emissions had an increased mass fraction of ions related to carboxylic acids and larger oxygen-to-carbon ratios than those that avoided shipping lanes, suggesting that shipping emissions increase marine organic aerosol (OA) oxidation state. Amine fragment mass loadings were correlated positively with anthropogenic nss-SO4 during onshore flow, implying anthropogenic–biogenic interaction in marine OA production. Model calculations also suggest that advection of shipping-derived aerosol may enhance inland aqueous-phase secondary OA production. These results imply a continuing role of shipping emissions on aerosol properties over the Gulf of Mexico and suggest that further regulation of shipping fuel sulfur content will reduce coastal submicron aerosol mass loadings near Houston.Item Urban core-downwind differences and relationships related to ozone production in a major urban area in Texas(Elsevier, 2021) Guo, Fangzhou; Bui, Alexander A.T.; Schulze, Benjamin C.; Yoon, Subin; Shrestha, Sujan; Wallace, Henry W.; Sakai, Yuta; Actkinson, Blake W.; Erickson, Matthew H.; Alvarez, Sergio; Sheesley, Rebecca; Usenko, Sascha; Flynn, James; Griffin, Robert J.San Antonio, the second-most populous city in Texas and the seventh-most populous city in the United States (US), has been designated a marginal non-attainment area by the US Environmental Protection Agency with respect to the 2015 ozone (O3) National Ambient Air Quality Standard. While stationary air quality monitoring sites are operated in the region by the Texas Commission on Environmental Quality (TCEQ), there are limited in situ field measurements for O3 and its precursors in the urban core. To better understand O3 dynamics in San Antonio, a suite of meteorological and gas instruments was deployed during May 2017. We incorporate field measurements from two campaign sites and one TCEQ stationary monitoring site into a zero-dimensional O3 model to characterize the local formation and destruction rates of O3, hydroxyl radical (OH) reactivity of volatile organic compounds (VOCs), O3 production efficiency, and O3 formation regime in the urban core and directly downwind of San Antonio. Upwind/downwind differences indicate the importance of photochemical processing of VOCs with carbon-carbon double bonds. San Antonio was mostly in a nitrogen oxide (NOX)-sensitive regime throughout the daytime during the campaign period, with O3 formation peaking at noon in the city center and early afternoon at the downwind region. Formaldehyde (HCHO), isoprene, and alkenes dominated VOC reactivity, with alkenes and isoprene from San Antonio's core (upwind) likely contributing to the downwind formation of HCHO and enhancing its OH reactivity. However, their direct impact on downwind O3 production was not observed. Model results suggest further strengthening NOX emission controls to decrease O3 formation in San Antonio.