Upper tropospheric pollutants observed by MIPAS: geographic and seasonal variations

Abstract

Abstract. We present a global climatology of upper tropospheric hydrogen cyanide (HCN), carbon monoxide (CO), acetylene (C₂H₂), ethane (C₂H₆), peroxyacetyl nitrate (PAN) and formic acid (HCOOH), obtained from MIPAS/Envisat observations between 2002 and 2012. At northern mid- and high latitudes the biomass burning tracer HCN as well as CO, PAN and HCOOH exhibit maxima during spring and/or summer and minima during winter. On the contrary, maximum northern extra-tropical C₂H₂ and C₂H₆ amounts were measured during winter and spring and minimum values during summer and fall. In the tropics and subtropics, enhanced amounts of all pollutants were observed during all seasons, especially widespread and up to southern mid-latitudes during austral spring. Other characteristic features are eastward transport of anthropogenic C₂H₆ and of biogenic HCOOH from Central and North America in boreal summer, accumulation of pollutants in the Asian Monsoon Anticyclone and enhanced C₂H₂ over South-East Asia in boreal winter. Clear indication of biogenic release of HCOOH was also found above tropical South America and Africa. A global correlation analysis of the other pollutants with HCN corroborates common release by biomass burning as source of the widespread southern hemispheric pollution during austral spring. Further, high correlation with HCN points to biomass burning as major source of tropical and subtropical C₂H₂ and PAN during most of the year. In the northern extra-tropics there are generally low correlations with HCN during spring and early summer, indicating the influence of anthropogenic and biogenic sources. However, in August there are stronger correlations above Siberia and boreal North America, which points to common release by boreal fires. This is confirmed by the respective enhancement ratios (ERs). The ERs measured above North-East Africa fit well to the emission ratios of the dominant local fire type (savanna burning) for C₂H₂, while those for CO, C₂H₆ and HCOOH rather indicate tropical forest fires or additional anthropogenic or biogenic sources. The southern hemispheric ΔC₂H₆/ΔHCN ERs obtained during August to October are in good agreement with the emission ratio for savanna fires. The same applies for ΔC₂H₂/ΔHCN in August and for ΔHCN/ΔCO as well as for ΔHCOOH/ΔHCN in October.