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- ItemChanges in the production rate of secondary aerosol particles in Central Europe in view of decreasing SO2 emissions between 1996 and 2006(München : European Geopyhsical Union, 2010) Hamed, A.; Birmili, W.; Joutsensaari, J.; Mikkonen, S.; Asmi, A.; Wehner, B.; Spindler, G.; Jaatinen, A.; Wiedensohler, A.; Korhonen, H.; Lehtinen, K.E.J.; Laaksonen, A.In anthropogenically influenced atmospheres, sulphur dioxide (SO2) is the main precursor of gaseous sulphuric acid (H2SO4), which in turn is a main precursor for atmospheric particle nucleation. As a result of socio-economic changes, East Germany has seen a dramatic decrease in anthropogenic SO2 emissions between 1989 and present, as documented by routine air quality measurements in many locations. We have attempted to evaluate the influence of changing SO2 concentrations on the frequency and intensity of new particle formation (NPF) using two different data sets (1996–1997; 2003–2006) of experimental particle number size distributions (diameter range 3–750 nm) from the atmospheric research station Melpitz near Leipzig, Germany. Between the two periods SO2 concentrations decreased by 65% on average, while the frequency of NPF events dropped by 45%. Meanwhile, the average formation rate of 3 nm particles decreased by 68% on average. The trends were statistically significant and therefore suggest a connection between the availability of anthropogenic SO2 and freshly formed new particles. In contrast to the decrease in new particle formation, we found an increase in the mean growth rate of freshly nucleated particles (+22%), suggesting that particle nucleation and subsequent growth into larger sizes are delineated with respect to their precursor species. Using three basic parameters, the condensation sink for H2SO4, the SO2 concentration, and the global radiation intensity, we were able to define the characteristic range of atmospheric conditions under which particle formation events take place at the Melpitz site. While the decrease in the concentrations and formation rates of the new particles was rather evident, no similar decrease was found with respect to the generation of cloud condensation nuclei (CCN; particle diameter >100 nm) as a result of atmospheric nucleation events. On the contrary, the production of CCN following nucleation events appears to have increased by tens of percents. Our aerosol dynamics model simulations suggest that such an increase can be caused by the increased particle growth rate.
- ItemA method for detecting the presence of organic fraction in nucleation mode sized particles(München : European Geopyhsical Union, 2005) Vaattovaara, P.; Räsänen, M.; Kühn, T.; Joutsensaari, J.; Laaksonen, A.New particle formation and growth has a very important role in many climate processes. However, the overall knowlegde of the chemical composition of atmospheric nucleation mode (particle diameter, d<20 nm) and the lower end of Aitken mode particles (d≤50 nm) is still insufficient. In this work, we have applied the UFO-TDMA (ultrafine organic tandem differential mobility analyzer) method to shed light on the presence of an organic fraction in the nucleation mode size class in different atmospheric environments. The basic principle of the organic fraction detection is based on our laboratory UFO-TDMA measurements with organic and inorganic compounds. Our laboratory measurements indicate that the usefulness of the UFO-TDMA in the field experiments would arise especially from the fact that atmospherically the most relevant inorganic compounds do not grow in subsaturated ethanol vapor, when particle size is 10 nm in diameter and saturation ratio is about 86% or below it. Furthermore, internally mixed particles composed of ammonium bisulfate and sulfuric acid with sulfuric acid mass fraction ≤33% show no growth at 85% saturation ratio. In contrast, 10 nm particles composed of various oxidized organic compounds of atmospheric relevance are able to grow in those conditions. These discoveries indicate that it is possible to detect the presence of organics in atmospheric nucleation mode sized particles using the UFO-TDMA method. In the future, the UFO-TDMA is expected to be an important aid to describe the composition of atmospheric newly-formed particles.
- ItemMeteorological and trace gas factors affecting the number concentration of atmospheric Aitken (DP Combining double low line 50 nm) particles in the continental boundary layer: Parameterization using a multivariate mixed effects model(München : European Geopyhsical Union, 2011) Mikkonen, S.; Korhonen, H.; Romakkaniemi, S.; Smith, J.N.; Joutsensaari, J.; Lehtinen, K.E.J.; Hamed, A.; Breider, T.J.; Birmili, W.; Spindler, G.; Plass-Duelmer, C.; Facchini, M.C.; Laaksonen, A.Measurements of aerosol size distribution and different gas and meteorological parameters, made in three polluted sites in Central and Southern Europe: Po Valley, Italy, Melpitz and Hohenpeissenberg in Germany, were analysed for this study to examine which of the meteorological and trace gas variables affect the number concentration of Aitken (Dp= 50 nm) particles. The aim of our study was to predict the number concentration of 50 nm particles by a combination of in-situ meteorological and gas phase parameters. The statistical model needs to describe, amongst others, the factors affecting the growth of newly formed aerosol particles (below 10 nm) to 50 nm size, but also sources of direct particle emissions in that size range. As the analysis method we used multivariate nonlinear mixed effects model. Hourly averages of gas and meteorological parameters measured at the stations were used as predictor variables; the best predictive model was attained with a combination of relative humidity, new particle formation event probability, temperature, condensation sink and concentrations of SO2, NO2 and ozone. The seasonal variation was also taken into account in the mixed model structure. Model simulations with the Global Model of Aerosol Processes (GLOMAP) indicate that the parameterization can be used as a part of a larger atmospheric model to predict the concentration of climatically active particles. As an additional benefit, the introduced model framework is, in theory, applicable for any kind of measured aerosol parameter.