During all eight flights conducted over the equatorial and tropical South Atlantic (27°–35°W, 2°N–11°S; September 9–22, 1989) in the course of the Chemical Instrumentation Test and Evaluation (CITE 3) experiment, we observed haze layers with elevated concentrations of aerosols, O 3 , CO, and other trace gases related to biomass burning emissions. They occurred at altitudes between 1000 and 5200 m and were usually only some 100–300 m thick. These layers extended horizontally over several 100 km and were marked by the presence of visible brownish haze. These layers strongly influenced the chemical characteristics of the atmosphere over this remote oceanic region. Air mass trajectories indicate that these layers originate in the biomass burning regions of Africa and South America and typically have aged at least 10 days since the time of emission. In the haze layers, O 3 and CO concentrations up to 90 and 210 ppb were observed, respectively. The two species were highly correlated. The ratio ΔO 3 /ΔCO (Δ, concentrations in plume minus background concentrations) is typically in the range 0.2–0.7, much higher than the ratios in the less aged plumes investigated previously in Amazonia. In most cases, aerosol (0.12–3 μm diameter) number concentrations were also elevated by up to 400 cm −3 in the layers; aerosol enrichments were also strongly correlated with elevated CO levels. Clear correlations between CO and NO x enrichments were not apparent due to the age of the plumes, in which most NO x would have already reacted away within 1–2 days. Only in some of the plumes could clear correlations between NO y and CO be identified; the absence of a general correlation between NO y and CO may be due to instrumental limitations and to variable sinks for NO y . The average enrichment of ΔNO y /ΔCO was quite high, consistent with the efficient production of ozone observed in the plumes. The chemical characteristics of the haze layers, together with remote sensing information and trajectory calculations, suggest that fire emissions (in Africa and/or South America) are the primary source of the haze layer components.
Abstract. In this study, we present a novel approach for assessing nearshore seepage atmospheric emissions through modeling of air quality station data, specifically a Gaussian plume inversion model. A total of 3 decades of air quality station meteorology and total hydrocarbon concentration, THC, data were analyzed to study emissions from the Coal Oil Point marine seep field offshore California. THC in the seep field directions was significantly elevated and Gaussian with respect to wind direction, θ. An inversion model of the seep field, θ-resolved anomaly, THC′(θ)-derived atmospheric emissions is given. The model inversion is for the far field, which was satisfied by gridding the sonar seepage and treating each grid cell as a separate Gaussian plume. This assumption was validated by offshore in situ data that showed major seep area plumes were Gaussian. Plume total carbon, TC (TC = THC + carbon dioxide, CO2, + carbon monoxide), 18 % was CO2 and 82 % was THC; 85 % of THC was CH4. These compositions were similar to the seabed composition, demonstrating efficient vertical plume transport of dissolved seep gases. Air samples also measured atmospheric alkane plume composition. The inversion model used observed winds and derived the 3-decade-average (1990–2021) field-wide atmospheric emissions of 83 400 ± 12 000 m3 THC d−1 (27 Gg THC yr−1 based on 19.6 g mol−1 for THC). Based on a 50 : 50 air-to-seawater partitioning, this implies seabed emissions of 167 000 m3 THC d−1. Based on atmospheric plume composition, C1–C6 alkane emissions were 19, 1.3, 2.5, 2.2, 1.1, and 0.15 Gg yr−1, respectively. The spatially averaged CH4 emissions over the ∼ 6.3 km2 of 25 × 25 m2 bins with sonar values above noise were 5.7 µM m−2 s−1. The approach can be extended to derive emissions from other dispersed sources such as landfills, industrial sites, or terrestrial seepage if source locations are constrained spatially.
