Sources and sinks of selected trace gases in the tropospheric boundary layer of the eastern United States
This dissertation describes three major research projects with the common goal of characterizing sources and sinks of trace gases of strong relevance to regional air quality and global climate issues. In the first study, volatile organic compound (VOC) measurements collected at a marine and continental site in northern New England were compared and examined for evidence of regional VOC sources. Biogenic VOCs, including isoprene, monoterpenes, and oxygenated VOCs, were significant components of the total reactivity at both locations. However, very different VOC distributions were observed for each site. The impact of local anthropogenic hydrocarbon sources such as liquefied petroleum gas (LPG) leakage was also evident at both sites. During the campaign, a propane flux of 9 (+/-2) x 109 molecules cm-2 s-1 was calculated for the continental site. In the second study, three hydrocarbon sources were investigated for their potential contributions to the summertime atmospheric toluene enhancements observed at a rural location in southern New Hampshire. These sources included: (1) warm season fuel evaporation emissions, (2) local industrial emissions, and (3) local vegetative emissions. The estimated contribution of fuel evaporation emissions (16-30 pptv d-1) could not fully account for observed summertime toluene enhancements (20-50 pptv d-1). Vegetation enclosure measurements suggested biogenic toluene emissions (5 and 12 pptv d-1 for alfalfa and pine trees) made significant contributions to summertime enhancements. Industrial toluene emissions, estimated at 7 pptv d-1, most likely occurred year round rather than seasonally. Finally, controls over carbonyl sulfide (COS) uptake in a temperate loblolly pine forest grown under ambient and elevated CO2 were examined in the third study. Vegetative consumption dominated net ecosystem COS uptake (10 to 40 pmol m-2 s-1) under both CO2 regimes. Environmental controls over vegetation stomatal conductance and photosynthetic capacity were the major factors influencing COS uptake rates. The loblolly pines exhibited substantial COS consumption overnight (50% of daytime rates) that was independent of CO2 assimilation. This suggests current estimates of the global vegetative COS sink, which assume that COS and CO2 are consumed simultaneously, may need to be reevaluated.
Atmospheric Sciences, Environmental Sciences
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