Abstract
Abstract. A case study of atmospheric aerosol measurements exploring the impact of the vertical distribution of aerosol chemical composition upon the radiative budget in North-Western Europe is presented. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) on both an airborne platform and a ground-based site at Cabauw in the Netherlands. The examined period in May 2008 was characterised by enhanced pollution loadings in North-Western Europe and was dominated by ammonium nitrate and Organic Matter (OM). Both ammonium nitrate and OM were observed to increase with altitude in the atmospheric boundary layer. This is primarily attributed to partitioning of semi-volatile gas phase species to the particle phase at reduced temperature and enhanced relative humidity. Increased ammonium nitrate concentrations in particular were found to strongly increase the ambient scattering potential of the aerosol burden, which was a consequence of the large amount of associated water as well as the enhanced mass. During particularly polluted conditions, increases in aerosol optical depth of 50–100% were estimated to occur due to the observed increase in secondary aerosol mass and associated water uptake. Furthermore, the single scattering albedo was also shown to increase with height in the boundary layer. These enhancements combined to increase the negative direct aerosol radiative forcing by close to a factor of two at the median percentile level. Such increases have major ramifications for regional climate predictions as semi-volatile components are often not included in aerosol models. The results presented here provide an ideal opportunity to test regional and global representations of both the aerosol vertical distribution and subsequent impacts in North-Western Europe. North-Western Europe can be viewed as an analogue for the possible future air quality over other polluted regions of the Northern Hemisphere, where substantial reductions in sulphur dioxide emissions have yet to occur. Anticipated reductions in sulphur dioxide in polluted regions will result in an increase in the availability of ammonia to form ammonium nitrate as opposed to ammonium sulphate. This will be most important where intensive agricultural practises occur. Our observations over North-Western Europe, a region where sulphur dioxide emissions have already been reduced, indicate that failure to include the semi-volatile behaviour of ammonium nitrate will result in significant errors in predicted aerosol direct radiative forcing. Such errors will be particularly significant on regional scales.
Highlights
The radiative impact of anthropogenic aerosols is often most keenly felt upon regional scales due to its shorter life-time compared to greenhouse gases (e.g. Charlson et al, 1992)
The results show that the observed increase in particle mass with altitude in the boundary layer was predominately driven by ammonium nitrate
A case study comparing the aerosol chemical composition measured from two platforms operating during highly polluted conditions in North-Western Europe has been presented
Summary
The radiative impact of anthropogenic aerosols is often most keenly felt upon regional scales due to its shorter life-time compared to greenhouse gases (e.g. Charlson et al, 1992). Charlson et al, 1992). This is evident over industrialized regions of the Northern Hemisphere such as North America, Europe and Asian countries such as India and China. Forster et al, 2007) Such assessments are traditionally undertaken via employment of global or regional scale models. These often produce wildly differing results due to the complexity of representing atmospheric aerosol (Kinne et al, 2006; Textor et al, 2006). One such complexity is the representation of semi-volatile compounds
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