Publication Date:
2014-05-27
Description:
Measurements of atmospheric NOx (NOx = NO + NO2), peroxyacetyl nitrate (PAN), NOy and non-methane hydrocarbons (NMHC) were taken at the GEOSummit Station, Greenland (72.34° N, 38.29° W, 3212 m.a.s.l) from July 2008 to July 2010. The data set represents the first year-round concurrent record of these compounds sampled at a high latitude Arctic site in the free troposphere. Here, the study focused on the seasonal variability of these important ozone (O3) precursors in the Arctic free troposphere and the impact from transported anthropogenic and biomass burning emissions. Our analysis shows that PAN is the dominant NOy species in all seasons at Summit, varying from 49% to 78%, however, we find that odd NOy species (odd NOy = NOy − PAN-NOx) contribute a large amount to the total NOy speciation with monthly means of up to 95 pmol mol−1 in the winter and ∼40 pmol mol−1 in the summer, and that the level of odd NOy species at Summit during summer is greater than that of NOx. We hypothesize that the source of this odd NOy is most likely alkyl nitrates from transported pollution, and photochemically produced species such as HNO3 and HONO. FLEXPART retroplume analysis and tracers for anthropogenic and biomass burning emissions, were used to identify periods when the site was impacted by polluted air masses. Europe contributed the largest source of anthropogenic emissions during the winter and spring months, with up to 82% of the simulated anthropogenic black carbon originating from this region between December 2009 and March 2010, whereas, North America was the primary source of biomass burning emissions. Polluted air masses were typically aged, with median transport times to the site from the source region of 11 days for anthropogenic events in winter, and 14 days for BB plumes. Overall we find that the transport of polluted air masses to the high altitude Arctic typically resulted in high variability in levels of O3 and O3 precursors. During winter, plumes originating from mid-latitude regions and transported in the lower troposphere to Summit often result in lower O3 mole fractions than background levels. However, plumes transported at higher altitudes can result in positive enhancements in O3 levels. It is therefore likely that the air masses transported in the mid-troposphere were mixed with air from stratospheric origin. Similar enhancements in O3 and its precursors were also observed during periods when FLEXPART indicated that biomass burning emissions impacted Summit. The analysis of anthropogenic events over summer show that emissions of anthropogenic origin have a greater impact on O3 and precursor levels at Summit than biomass burning sources during the measurement period, with enhancements above background levels of up to 16 nmol mol−1 for O3 and 237 pmol mol−1 and 205 pmol mol−1, 28 pmol mol−1 and 1.0 nmol mol−1 for NOy, PAN, NOx and ethane, respectively.
Electronic ISSN:
1680-7375
Topics:
Geosciences
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