Among various factors that influence the long-range transport of pollutants in the free troposphere (FT), the prevailing atmospheric weather states probably play the most important role in governing characteristics and efficacy of such transport. The weather states, such as a particular wind pattern, cyclonic or anticyclonic conditions, and their degree of persistency determine the spatio-temporal distribution and the final fate of the pollutants. This is especially true in the case of Nordic countries, where baroclinic disturbances and associated weather fronts primarily regulate local meteorology, in contrast to the lower latitudes where a convective paradigm plays a similarly important role. Furthermore, the long-range transport of pollutants in the FT has significant contribution to the total column burden over the Nordic countries. However, there is insufficient knowledge on the large-scale co-variability of pollutants in the FT and atmospheric weather states based solely on observational data over this region. The present study attempts to quantify and understand this statistical co-variability while providing relevant meteorological background. To that end, we select eight weather states that predominantly occur over the Nordic countries and three periods of their persistency (3 days, 5 days, and 7 days), thus providing in total 24 cases to investigate sensitivity of free tropospheric carbon monoxide, an ideal tracer for studying pollutant transport, to these selected weather states. The eight states include four dominant wind directions (namely, NW, NE, SE and SW), cyclonic and anticyclonic conditions, and the enhanced positive and negative phases of the North Atlantic Oscillation (NAO). For our sensitivity analysis, we use recently released Version 6 retrievals of CO at 500 hPa from the Atmospheric Infrared Sounder (AIRS) onboard Aqua satellite covering the 11-year period from September 2002 through August 2013 and winds from the ECMWF's ERA-Interim project to classify weather states for the same 11-year period. We show that, among the various weather states studied here, southeasterly winds lead to highest observed CO anomalies (up to +8%) over the Nordic countries while transporting pollution from the central and eastern parts of Europe. The second (up to +4%) and third highest (up to +2.5%) CO anomalies are observed when winds are northwesterly (facilitating inter-continental transport from polluted North American regions) and during the enhanced positive phase of the NAO respectively. Higher than normal CO anomalies are observed during anticyclonic conditions (up to +1%) compared to cyclonic conditions. The cleanest conditions are observed when winds are northeasterly and during the enhanced negative phases of the NAO, when relatively clean Arctic air masses are transported over the Nordic regions in the both cases. In the case of nearly all weather states, the CO anomalies consistently continue to increase or decrease as the degree of persistency of a weather state is increased. The results of this sensitivity study further provide an observational basis for the process-oriented evaluation of chemistry transport models, especially with regard to the representation of large-scale coupling of chemistry and local weather states and its role in the long-range transport of pollutants in such models.
2014. Vol. 14, no 21, 11545-11555 p.