Jussi Paatero

Chemical composition of aerosol during particle formation events in boreal forest

Size-segregated chemical aerosol analysis of a total 5 integrated samples has been performed for the atmospheric aerosol during events of new particle formation. The experiments were conducted during the BIOFOR 3 measurement campaign at a boreal forest site in southern Finland in spring 1999. Aerosol samples collected by a cascade low-pressure impactor were taken selectively to distinguish particle formation event aerosol from non-event aerosol. The division into “event” and “non-event” cases was done “in situ” at field, based on the on-line submicron number size distribution. The results on the chemical ionic composition of the particles show only small differences between the event and non-event sample sets. The event samples show lower concentrations of total sulfate and ammonium as well as light dicarboxylic acids such as oxalate, malonate and succinate. In the event samples, nucleation mode particle MSA (methanesulphonic acid) was found to be present exceeding the concentrations found in the non-event samples, but at larger particle sizes the sample sets contained rather similar concentrations of MSA. The most significant difference between the event and non-event sets was found for dimethylammonium, ionic component of dimethylamine ((CH3)2NH), which seems to be present in the particle phase during the particle formation periods and/or during the subsequent particle growth. The absolute event sample dimethylamine concentrations were more than 30-fold greater than the non-event concentrations in the accumulation mode size range. On the other hand, the non-event back-up filter stage for sub-30 nm particles contained more dimethylamine than the event samples. This fractionation is probably a condensation artifact of the impactor sampling. A simple mass balance estimate is performed to evaluate the quality and consistency of the results for the overall mass concentration.

Effects of air masses and synoptic weather on aerosol formation in the continental boundary layer

Nucleation of near nm sized aerosol particles and subsequent growth to ~100 nm in 1–2 days has in recent years been frequently observed in the continental boundary layer at several European locations. In 1998–99, this was the focus of the BIOFOR experiment in Hyytiälä in the boreal Finnish forest. Nucleation occurred in arctic and to some extent in polar air masses, with a preference for maritime air in transition to continental air masses, and never in sub-tropical air. The air masses originated north of the BIOFOR experiment by paths from the southwest to northeast sector. The nucleation was also associated with cold air advection behind cold fronts, never warm air advection. This may relate to low pre-existing aerosol concentration, low cloudiness and large diurnal amplitudes in the continental boundary layer associated with cold air advection and clear skies. Arctic and polar air together with cold air advection did not always lead to nucleation. The most important limiting meteorological factors were cold front passages and high cloudiness, probably through reduced photochemistry and wet scavenging of precursor gases and new aerosol particles. The preference for nucleation to occur in arctic air masses, which seldom form in the summer, suggests a meteorological explanation for the annual cycle of nucleation, which has a minimum in summer. The connection to cold-air outbreaks suggests that the maximum in nucleation events during spring and autumn may be explained by the larger latitudinal temperature gradients and higher cyclone activity at that time of the year. Nucleation was observed on the same days over large parts (1000-km distance) of the same air mass. This suggests that the aerosol nucleation spans from the microphysical scale to the synoptic scale, perhaps connected through boundary layer and mesoscale processes.

Atmospheric aerosol over Finnish Arctic: source analysis by the multilinear engine and the potential source contribution function

Week-long samples of total suspended particles were collected between 1964 and 1978 from Kevo at the Finnish Arctic and analyzed for a number of chemical species. The chemical composition data was analyzed using a mixed 2-way/3-way model. The results of receptor modeling were connected with the back trajectory data in a Potential Source Contribution Function analysis to determine the likely source areas. Nine sources, namely silver emissions, coal/oil shale combustion, biomass burning, non-ferrous smelters (two sources), crustal elements from remote sources, excess silicon from local sources, sea salt particles and biogenic sulfur emissions from marine algae were found. Although the emissions from industrial areas in the Kola Peninsula had an effect on the concentration of anthropogenic pollutants at Kevo, the highest concentrations during winter were transported from the sources in the mid-latitudes. The yearly strength of the biogenic sulfur emissions showed no dependence on the Northern Hemisphere temperature anomaly and thus, a climatic feedback loop could not be confirmed.

Determination of the 241Pu Deposition in Finland after the Chernobyl Accident

Transuranium nuclides, including a considerable amount of Pu, were released in the Chernobyl explosion. Plutonium was separated from lichen and peat samples by coprecipitation and anion exchange. A portion of the separated Pu fraction was taken for measurement of Pu with a low-background liquid scintillation counter, Quantulus 1220, equipped with a pulse shape analyser. The detection limit for Pu was 0.007 Bq with a counting time of 600 minutes. The plutonium-241 concentrations of the peat samples varied between < 3 and 430 Bq m~ in Southern Finland. The radioactivity ratio of 241 Pu to 239.240^ i n t h e fallout from Chernobyl was 94.8. The fallout pattern of Pu resembles the patterns of other refractory nuclides, Zr and Ce. The concentrations in lichen samples collected from regions of heaviest deposition were comparable to those of the heaviest weapons test fallout in the early 1960s.

Composition of the Finnish Arctic aerosol: collection and analysis of historic filter samples

Abstract Week-long samples of total suspended particles have been collected between October 1964 and February 1978 from the Finnish Arctic. Neutron activation analysis, ion chromatography, and light-absorption techniques have been used to analyze the concentration of several heavy metals and other elements, major ions, methane sulfonate (MSA), and black carbon. Kevo is located near the Kola Peninsula and the effect of the industrial area can be seen. Compared to previous studies of Arctic aerosols carried out in North American Arctic, the Kevo results show higher concentration of anthropogenic pollutants and the seasonal variability for most constituents is weaker than the typical Arctic haze pattern. MSA, a marker of biogenic activity, has a clear seasonal cycle with a peak from April to August.

Tropospheric carbon dioxide concentrations at a northern boreal site in Finland: basic variations and source areas

Abstract Diurnal and annual variations of CO2, O3, SO2, black carbon and condensation nuclei and their source areas were studied by utilizing air parcel trajectories and tropospheric concentration measurements at a boreal GAW site in Pallas, Finland. The average growth trend of CO2 was about 2.5 ppm yr−1 according to a 4-yr measurement period starting in October 1996. The annual cycle of CO2 showed concentration difference of about 19 ppm between the summer minimum and winter maximum. The diurnal cycle was most pronounced during July and August. The variation between daily minimum and maximum was about 5 ppm. There was a diurnal cycle in aerosol concentrations during spring and summer. Diurnal variation in ozone concentrations was weak. According to trajectory analysis the site was equally affected by continental and marine air masses. During summer the contribution of continental air increased, although the southernmost influences decreased. During daytime in summer the source areas of CO2 were mainly located in the northern parts of the Central Europe, while during winter the sources were more evenly distributed. Ozone showed similar source areas during summer, while during winter, unlike CO2, high concentrations were observed in air arriving from the sea. Sulfur dioxide sources were more northern (Kola peninsula and further east) and CO2 sources west-weighted in comparison to sources of black carbon. Source areas of black carbon were similar to source areas of aerosols during winter. Aerosol source area distributions showed signs of marine sources during spring and summer.

Source areas of airborne 7Be and 210Pb measured in Northern Finland.

Daily aerosol samples were collected at Sodankylä, Northern Finland, from July 1995 to June 1997. The filter samples were analyzed for 7Be by semiconductor gamma spectrometry and for 210Pb by alpha counting of the in-grown 210Po. The concentrations were lognormally distributed with median concentrations of 2,500 and 160 &mgr;Bq m−3 for 7Be and 210Pb, respectively. The trajectory analysis performed showed that the highest 210Pb activity concentrations were associated with continental air masses originating in Central Russia. High 7Be activity concentrations were found in air masses from Central Russia and, during springtime, also in air masses coming from southwest. The latter cases were attributed to the transfer of stratospheric air masses into the troposphere along the polar front. Slightly elevated 7Be and 210Pb concentrations were found in air masses coming to Sodankylä from north-west between 70th and 80th latitudes. This was attributed to the long-range transport from continental North America.

Plutonium fallout in Southern Finland after the chernobyl accident

Abstract The plutonium concentrations of fuel peat samples from southern and central Finland were analyzed. The same samples had previously gone through gamma-spectrometric analysis, in which the detected nuclides could be divided into two groups by calculating correlations between activities: the volatile Cs-I group and the non-volatile Ce-Zr group. The plutonium of Chernobyl origin correlates rather well with the non-volatile group and not at all with the volatile group. The volatile group comprises the nuclides 137 Cs, 134 Cs, 131 I and 132 Te, and the non-volatile group 95 Zr, 141 Ce and Chernobyl-Pu.

Speciation of 129I in sea, lake and rain waters

Concentrations of the very long-lived fission product (129)I and stable iodine ((127)I) in the Baltic Sea and lake and rain waters from Finland, were measured as well as their occurrence as iodide (I(-)) and iodate (IO(3)(-)). The highest concentrations of both (127)I and (129)I occurred in sea water, on average 11.1 ± 4.3 μg/l and 3.9 ± 4.1 × 10(-9) at/l. In rain and lake waters the concentration of (129)I was more or less identical and almost one order of magnitude lower than in sea water. Based on these observations, and data from the literature, it is assumed that the source of (129)I in lakes is precipitation and the major source in the Baltic Sea is the inflow of sea water from the North Sea through the Danish Straits. The concentration of (129)I in the Baltic Sea has increased by a factor of six during ten years from 1999. In all studied water types the main chemical form of both iodine isotopes was iodide; in sea and lake waters by 92-96% and in rain water by 75-88%. Compared to (127)I the fraction of iodide was slightly higher in case of (129)I in all waters.

Americium and curium deposition in Finland from the Chernobyl accident

Summary 241Am and 244Cm were analysed from peat samples collected in Finland immediately after the Chernobyl accident. The separation method included co-precipitation, anion exchange and extraction chromatography. Activities of 241Am and 244Cm were measured by alpha spectrometry. The activity of Chernobyl-derived 241Am varied between 0.0115 and 9.32 Bq/m2 and that of 244Cm from < 0.002 to 1.97 Bq/m2 (reference date 1.5.1986). The origin of 241Am in Finland is predominantly from atmospheric nuclear tests. However, the geographical distribution of Chernobyl-americium is uneven and depending on a location even 100% of 241Am in peat originated from the Chernobyl accident. The deposition pattern of Chernobyl-derived 241Am and 244Cm resembles that of other refractory nuclides, such as 95Zr, 141Ce and 239,240Pu.