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Unprecedented growth of East Asian economies has led to increases of anthropogenic pollutants in the regional atmosphere. This pollutant burden is transported into the global atmosphere and is a significant source of intercontinental and transboundary anthropogenic pollution. This work analyzes pollution transport into the western Pacific associated with the dispersion of East Asian pollution during Northern Hemisphere winter. To examine transport characteristics, we use chemical and dynamical data sets obtained during the CONvective TRansport of Active Species in the Tropics (CONTRAST) field campaign, conducted from Guam during January–February 2014. We identify that the evolution of shear lines from decaying cold fronts and their southward advancement facilitates polluted air transport into low latitudes of the Western Pacific Ocean. Observations from two cases of shear line passage are analyzed. The result shows that this transport process significantly elevates anthropogenic trace gases in the marine boundary layer and lowermost free troposphere up to 3–4 km. Results of our analysis show that chemical influence of the shear line on the background tropical marine atmosphere varies as a function of pollution source, intensity, shear line strength, and the speed of advancement, as well as local background conditions. To quantify the contribution of shear-line-related transport, we introduce an index, the Anthropogenic Enhancement Factor (AEF), defined as a fractional change in mixing ratio of a gas brought about by the advancing front. This index shows that the most significant enhancements are for species with photochemical lifetimes comparable to their transport times from source regions.

We use isoprene and related field measurements from three different ocean data sets together with remotely sensed satellite data to model global marine isoprene emissions. We show that using monthly mean satellite-derived chl a concentrations to parameterize isoprene with a constant chl a normalized isoprene production rate underpredicts the measured oceanic isoprene concentration by a mean factor of 19±12. Improving the model by using phytoplankton functional type dependent production values and by decreasing the bacterial degradation rate of isoprene in the water column results in only a slight underestimation (factor 1.7±1.2). We calculate global isoprene emissions of 0.21TgC for 2014 using this improved model, which is twice the value calculated using the original model. Nonetheless, the sea-to-air fluxes have to be at least 1 order of magnitude higher to account for measured atmospheric isoprene mixing ratios. These findings suggest that there is at least one missing oceanic source of isoprene and, possibly, other unknown factors in the ocean or atmosphere influencing the atmospheric values. The discrepancy between calculated fluxes and atmospheric observations must be reconciled in order to fully understand the importance of marine-derived isoprene as a precursor to remote marine boundary layer particle formation.

In California, emission control strategies have been implemented to reduce air pollutants. Here we estimate the changes in nitrogen oxides (NOx = NO + NO2) emissions in 2005-2010 using a state-of-the-art four-dimensional variational approach. We separately and jointly assimilate surface NO2 concentrations and tropospheric NO2 columns observed by Ozone Monitoring Instrument (OMI) into the regional-scale Sulfur Transport and dEposition Model (STEM) chemical transport model on a 12 × 12 km2 horizontal resolution grid in May 2010. The assimilation generates grid-scale top-down emission estimates, and the updated chemistry fields are evaluated with independent aircraft measurements during the NOAA California Nexus (CalNex) field experiment. The emission estimates constrained only by NO2 columns, only by surface NO2, and by both indicate statewide reductions of 26%, 29%, and 30% from ~0.3 Tg N/yr in the base year of 2005, respectively. The spatial distributions of the emission changes differ in these cases, which can be attributed to many factors including the differences in the observation sampling strategies and their uncertainties, as well as those in the sensitivities of column and surface NO2 with respect to NOx emissions. The updates in California's NOx emissions reduced the mean error in modeled surface ozone in the Western U.S., even though the uncertainties in some urban areas increased due to their NOx-saturated chemical regime. The statewide reductions in NOx emissions indicated from our observationally constrained emission estimates are also reflected in several independently developed inventories: ~30% in the California Air Resources Board bottom-up inventory, ~4% in the 2008 National Emission Inventory, and ~20% in the annual mean top-down estimates by Lamsal et al. using the global Goddard Earth Observing System (GEOS)-Chem model and OMI NO2 columns. Despite the grid-scale differences among all top-down and bottom-up inventories, they all indicate stronger emission reductions in the urban regions. This study shows the potential of using space-/ground-based monitoring data and advanced data assimilation approach to timely and independently update NOx emission estimates on a monthly scale and at a fine grid resolution. The well-evaluated results here suggest that these approaches can be applied more broadly.

A large fraction of atmospheric aerosols are derived from organic compounds with various volatilities. A National Oceanic and Atmospheric Administration (NOAA) WP-3D research aircraft made airborne measurements of the gaseous and aerosol composition of air over the Deepwater Horizon (DWH) oil spill in the Gulf of Mexico that occurred from April to August 2010. A narrow plume of hydrocarbons was observed downwind of DWH that is attributed to the evaporation of fresh oil on the sea surface. A much wider plume with high concentrations of organic aerosol (>25 micrograms per cubic meter) was attributed to the formation of secondary organic aerosol (SOA) from unmeasured, less volatile hydrocarbons that were emitted from a wider area around DWH. These observations provide direct and compelling evidence for the importance of formation of SOA from less volatile hydrocarbons.

Volatile organic compounds (VOCs) were measured at the South Pole (SP) from late Austral spring to mid-summer 2000 as part of the Investigation of Sulfur Chemistry in the Antarctic Troposphere Program (ISCAT-2000). This paper focuses on VOCs that are directly emitted from the ocean, specifically dimethyl sulfide (DMS), methyl nitrate (CH3ONO2), methyl iodide (CH 3I) and bromoform (CHBr3). A partial seasonal cycle of these gases was also recorded during the year following ISCAT-2000. During the summer, the SP periodically receives relatively fresh marine air containing short-lived oceanic trace gases, such as DMS (τ≈1 day). However, DMS was not detected at the SP until January even though DMS emissions from the Southern Ocean typically start peaking in November and elevated levels of other ocean-derived VOCs, including CH3ONO2 and CHBr 3, were observed in mid-November. We speculate that in November and December most of the DMS is oxidized before it reaches the SP: a strong correlation between CH3ONO2 and methane sulfonate (MSA), an oxidation product of DMS, supports this hypothesis. Based on a limited number of samples taken over the course of one year, CH3ONO2 apparently accumulates to a quasi-steady-state level over the SP in winter, most likely due to continuing emissions of the compound coupled with a lower rate of photochemical destruction. Oceanic emissions were concluded to be the dominant source of alkyl nitrates at the SP; this is in sharp contrast to northern high latitudes where total alkyl nitrate mixing ratios are dominated by urban sources. © 2004 Elsevier Ltd. All rights reserved.