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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.

Aircraft measurements, including non-methane hydrocarbons (NMHCs), long-lived halocarbons, carbon monoxide (CO), and ozone (O3) collected on board the NASA DC-8 during the Deep Convection, Clouds, and Chemistry (DC3) field campaign (May – June 2012), were used to investigate interactions and mixing between stratospheric intrusions and polluted air masses. Stratospherically influenced air masses were detected using a suite of long-lived halocarbons, including chlorofluorocarbons (CFCs) and HCFCs, as a tracer for stratospheric air. A large number of stratospherically influenced samples were found to have reduced levels of O3 and elevated levels of CO (both relative to background stratospheric air), indicative of mixing with anthropogenically influenced air. Using n-butane and propane as further tracers of anthropogenically influenced air, we show that this type of mixing was present both at low altitudes and in the upper troposphere (UT). At low altitudes, this mixing resulted in O3 enhancements consistent with those reported at surface sites during deep stratospheric intrusions, while in the UT, two case studies were performed to identify the process by which this mixing occurs. In the first case study, stratospheric air was found to be mixed with aged outflow from a convective storm, while in the second case study, stratospheric air was found to have mixed with outflow from an active storm occurring in the vicinity of a stratospheric intrusion. From these analyses, we conclude that deep convective events may facilitate the mixing between stratospheric air and polluted boundary layer air in the UT. Throughout the entire DC3 study region, this mixing was found to be prevalent: 72% of all samples that involve stratosphere-troposphere mixing show influence of polluted air. Applying a simple chemical kinetics analysis to these data, we show that during DC3, the instantaneous production of hydroxyl radical (OH) in these mixed stratospheric-polluted air masses was 11 ± 8 times higher than that of stratospheric air, and 4.2 ± 1.8 times higher than that of background upper tropospheric air.

Emission of bromine from sea-salt aerosol, frost flowers, ice leads, and snow results in the nearly complete removal of surface ozone during Arctic spring. Regions of enhanced total column BrO observed by satellites have traditionally been associated with these emissions. However, airborne measurements of BrO and O3 within the convective boundary layer (CBL) during the ARCTAS and ARCPAC field campaigns at times bear little relation to enhanced column BrO. We show that the locations of numerous satellite BrO "hotspots" during Arctic spring are consistent with observations of total column ozone and tropopause height, suggesting a stratospheric origin to these regions of elevated BrO. Tropospheric enhancements of BrO large enough to affect the column abundance are also observed, with important contributions originating from above the CBL. Closure of the budget for total column BrO, albeit with significant uncertainty, is achieved by summing observed tropospheric partial columns with calculated stratospheric partial columns provided that natural, short-lived biogenic bromocarbons supply between 5 and 10 ppt of bromine to the Arctic lowermost stratosphere. Proper understanding of bromine and its effects on atmospheric composition requires accurate treatment of geographic variations in column BrO originating from both the stratosphere and troposphere. Copyright 2010 by the American Geophysical Union.

Emission of bromine from sea-salt aerosol, frost flowers, ice leads, and snow results in the nearly complete removal of surface ozone during Arctic spring. Regions of enhanced total column BrO observed by satellites have traditionally been associated with these emissions. However, airborne measurements of BrO and O3 within the convective boundary layer (CBL) during the ARCTAS and ARCPAC field campaigns at times bear little relation to enhanced column BrO. We show that the locations of numerous satellite BrO "hotspots" during Arctic spring are consistent with observations of total column ozone and tropopause height, suggesting a stratospheric origin to these regions of elevated BrO. Tropospheric enhancements of BrO large enough to affect the column abundance are also observed, with important contributions originating from above the CBL. Closure of the budget for total column BrO, albeit with significant uncertainty, is achieved by summing observed tropospheric partial columns with calculated stratospheric partial columns provided that natural, short-lived biogenic bromocarbons supply between 5 and 10 ppt of bromine to the Arctic lowermost stratosphere. Proper understanding of bromine and its effects on atmospheric composition requires accurate treatment of geographic variations in column BrO originating from both the stratosphere and troposphere. Copyright 2010 by the American Geophysical Union.