On the seasonal variation in observed size distributions in northern Europe and their changes with decreasing anthropogenic emissions in Europe: climatology and trend analysis based on 17 years of data from Aspvreten, Sweden

摘要

Size-resolved aerosol trends were investigated based on a 17-year data set (2000–2017) from the rural background site Aspvreten located in southern Sweden (58.8°N, 17.4°E). Cluster analysis of the size distributions was performed to aid in the interpretation of the data. The results confirm previous findings of decreasing aerosol mass and number during the last decades as a result of reduced anthropogenic emissions in Europe. We show that both particle modal number concentration and size have substantially been reduced during the last 17 years. Negative trends in particle number concentration of about 10cm?3yr?1 are present for nuclei, Aitken, and accumulation modes. In total, integral particle number concentration has decreased by 30%, from 1860 to ca. 1300cm?3. The reduction in modal number concentration is accompanied by a decrease in modal size, and this decrease is largest for the accumulation mode (2nmyr?1 or about 17% for the whole period). These reductions have resulted in a decrease in submicron particle mass (390nm) by more than 50% over the period 2000–2017. These decreases are similar to observations found at other stations in northern Europe. Although all size classes show a downward trend as annual averages, we also show that observed trends are not evenly distributed over the year and that a rather complex picture emerges where both sign and magnitude of trends vary with season and size. The strongest negative trends are present during spring (accumulation mode) and autumn (Aitken mode). The strongest positive trends are present during summer months (Aitken mode). The combined trajectory and data analyses do not present evidence for an increase in new particle formation formed locally, although some evidence of increased new particle formation some distance away from the receptor is present. Observed aerosol size distribution data, together with an adiabatic cloud parcel model, were further used to estimate the change in cloud droplet concentration for various assumptions of updraught velocities and aerosol chemical composition. The results indicate a substantial increase in the atmospheric brightening effect due to a reduction in cloud reflectivity corresponding to 10%–12% reduction in cloud albedo over the period 2000–2017.