Detection in the summer polar stratosphere of pollution plume from East Asia and North America by balloon-borne in situ CO measurements

The SPIRALE and SWIR balloon-borne instruments were launched in the Arctic polar region (near Kiruna, Sweden, 67.9° N-21.1° E) during summer on 7 and 24 August 2009 and on 14 August 2009, respectively. The SPIRALE instrument performed in situ measurements of several trace gases including CO and O₃ at altitudes between 9 and 34 km, with very high vertical resolution (∼ 5 m). The SWIR-balloon instrument measured total and partial column of several species including CO. The CO stratospheric profile from SPIRALE for 7 August 2009 shows some specific structures with large concentrations in the low levels (potential temperatures between 320 and 380 K, i.e. 10-14 km height). These structures are not present in the CO vertical profile of SPIRALE for 24 August 2009, for which the volume mixing ratios are typical from polar latitudes (∼ 30 ppb). CO total columns retrieved from the IASI-MetOp satellite sounder for the three dates of flights are used to understand this CO variability. SPIRALE and SWIR CO partial columns between 9 and 34 km are compared, allowing us to confirm that the enhancement of CO is localised in the stratosphere. The measurements are also investigated in terms of CO:O₃ correlations and using several modelling approaches (trajectory calculations, potential vorticity fields, results of chemistry transport model) in order to characterize the origin of the air masses sampled. The emission sources are qualified in terms of source type (fires, urban pollution) using NH₃ and CO measurements from IASI-MetOp and fires detection from MODIS on board the TERRA/AQUA satellite. The results give strong evidence that the unusual abundance of CO on 7 August is due to surface pollution plumes from East Asia and North America transporting to the upper troposphere and then entering the lower stratosphere by isentropic advection. This study strengthens evidence that the composition of low polar stratosphere in summer may be affected by anthropogenic surface emissions through long-range transport.