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This study investigated the elemental composition of PM10 collected in a polar environment (Ny-Alesund, Norwegian Arctic), to identify its sources and to understand the effects of short- and long-range transport processes. Natural (crustal and marine) and anthropogenic Arctic PM sources were identified, and specific emission sources were recognised by means of Principal Component Analysis and Hierarchical Cluster Analysis: airborne pollution deriving from ship fuels, local vehicle (non-exhaust) and continental emissions (e.g. incinerators or industries) were the main sources of anthropogenic elements. The results obtained so far from samples collected during four successive spring-summer sampling campaigns (2010–2013) show a remarkable seasonal trend for most of the investigated elements. For both geogenic and anthropogenic elements, concentrations are generally higher in March and April, when the ground is almost entirely covered by snow and ice, suggesting that long-range transport processes might be taking place. On the other hand, the concentrations of anthropogenic metals related to ship emissions (i.e. Co, Ni and V) peak in late spring and summer, when the marine traffic in the fjord is generally higher. For most of the analytes, the four campaigns were not significantly different; therefore, in the studied period, the composition of PM10 in Ny-Alesund did not vary remarkably. Finally, the behaviour of Rare Earth Elements was discussed in terms of parent material mineralogy.

A long-term study of the chemical composition of Arctic aerosol has been carried out at the Gruvebadet Observatory located in Ny-Ålesund since 2010. The PM10 aerosol has been collected continuously every year on a daily/2-day basis, each covering at least the spring and summer months, and the ionic content was evaluated using simultaneously three IC-systems. In order to determine the contribution of different sources (sea spray, crustal, biogenic and anthropogenic) to the total sulphate budget, specific markers and characteristic marker-to-sulphate ratios were used (Na+, Ca2+ and methanesulphonate). The obtained data set was then compared with the one from the Zeppelin Observatory, also located in Ny-Ålesund. The anthropogenic fraction resulted to be the major component, reaching the highest value in March and April during the Haze period, followed by the sea salt, biogenic and crustal ones. The comparison between the two datasets confirms the seasonal trend of these fractions even though some differences in magnitude were observed, likely due to discrepancies in the timing and resolution of sampling campaigns. The temporal profile of the anthropogenic fraction, evaluated in both sites, showed no evident continuous trend from 2010 to 2019, although the 2017-19 period revealed higher concentration with respect to the previous years. Focusing on single months, two opposite trends in the sulphate budget along 10 years were observed for March against April and September. Whereas a decrease was observed in March, April and September showed an increase in the monthly mean concentration values. Finally, the correlation between the non-sea salt non-crustal sulphate fraction and ammonium was evaluated. An increase in the ammonia neutralizing effect, resulting in a decrease in aerosol acidity, was observed at GVB, from the 2010 to 2017, then stabilized. Conversely, a decrease in the concentration of ammonia was found in ZEP since 2015, leading to an increase of the nssSO42-/NH4+ ratio in the same period.

A prolonged and exceptionally intense air mass advection event transporting biomass burning aerosols generated in Alaska affected Ny-Ålesund in the mid of July 2015. This paper reports the morphochemical characteristics and mixing state of individual aerosol particles collected during the event. To this aim aerosol samples were collected on nucleopore polycarbonate membrane filters using a DEKATI 12-stage low volume impactor and analyzed by scanning electron microscopy (SEM) techniques. Results of SEM investigations depict a complex aerosol characterized by an external mixing between a main part of carbonaceous organic particles (tar balls and organic particles), lower ammonium sulfate and minor potassium chloride and mineral dust amounts. The carbonaceous particles are spherical to slightly elongated and the organic particles show an internal mixing of low density organics and/or ammonium sulfate upon denser nuclei. Most particles are in the accumulation mode size range although the size and the morphology of the chloride and the sulfate salts evidence the growth of these species both in the air and upon the sampling membranes. Individual particle analyses were complemented by aerosol size distribution (Aerodynamic Particle Sizer, Scanning Mobility Particle Sizer) and optical (Particle Soot Absorption Photometer, nephelometer) measurements at ground level in order to retrieve the optical and radiative properties of the aerosol in the atmosphere and to predict the fate and behaviour of particles upon deposition at ground level. Individual particle analyses were also compared with bulk chemical analyses on daily sampling filters and back-trajectory analyses of the air mass movement in order to enucleate distinct sources of the aerosol during the long range transport.

This paper presents the results of measurements of aerosol physical and chemical properties during iAREA2014 campaign that took place on Svalbard between 15th of Mar and 4th of May 2014. With respect to field area, the experiment consisted of two sites: NyeAlesund (78�550N, 11�560E) and Longyearbyen (78�130N, 15�330E) with further integration of Aerosol Robotic Network (AERONET) station in Hornsund (77�000N, 15�330E). The subject of this study is to investigate the inesitu, passive and active remote sensing observations as well as numerical simulations to describe the temporal variability of aerosol singleescattering properties during spring season on Spitsbergen. The retrieval of the data indicates several event days with enhanced singleescattering properties due to the existence of sulphate and additional seaesalt load in the atmosphere which is possibly caused by relatively high wind speed. Optical results were confirmed by numerical simulations made by the GEMeAQ model and by chemical observations that indicated up to 45% contribution of the seaesalt to a PM10 total aerosol mass concentration. An agreement between the in-situ optical and microphysical properties was found, namely: the positive correlation between aerosol scattering coefficient measured by the nephelometer and effective radius obtained from laser aerosol spectrometer as well as negative correlation between aerosol scattering coefficient and the Angstrom exponent indicated that slightly larger particles dominated during special events. The inesitu surface observations do not show any significant enhancement of the absorption coefficient as well as the black carbon concentration which might occur during spring. All of extensive singleescattering properties indicate a diurnal cycle in Longyearbyen, where 21:00e5:00 data stays at the background level, however increasing during the day by the factor of 3e4. It is considered to be highly connected with local emissions originating in combustion, traffic and harbour activities. On the other hand, no daily fluctuations in NyeAlesund are observed. Mean values in NyeAlesund are equal to 8.2, 0.8 Mm�1 and 103 ng/m3 for scattering, absorption coefficients and black carbon concentration; however in Longyearbyen (only data from 21:00e05:00 UTC) they reach 7.9, 0.6 Mm�1 as well as 83 ng/ m3 respectively. Overall, the spring 2014 was considerably clean and seaesalt was the major aerosol component

This study examines the relationships linking methanesulfonic acid (MSA, arising from the atmospheric oxidation of the biogenic dimethylsulfide, DMS) in atmospheric aerosol, satellite-derived chlorophyll a (Chl-a), and oceanic primary production (PP), also as a function of sea ice melting (SIM) and extension of the ice free area in the marginal ice zone (IF-MIZ) in the Arctic. MSA was determined in PM10 samples collected over the period 2010-2012 at two Arctic sites, Ny Ålesund (78.9°N, 11.9°E), Svalbard islands, and Thule Air Base (76.5°N, 68.8°W), Greenland. PP is calculated by means of a bio-optical, physiologically based, semi-analytical model in the potential source areas located in the surrounding oceanic regions (Barents and Greenland Seas for Ny Ålesund, and Baffin Bay for Thule). Chl-a peaks in May in the Barents sea and in the Baffin Bay, and has maxima in June in the Greenland sea; PP follows the same seasonal pattern of Chl-a, although the differences in absolute values of PP in the three seas during the blooms are less marked than for Chl-a. MSA shows a better correlation with PP than with Chl-a, besides, the source intensity (expressed by PP) is able to explain more than 30% of the MSA variability at the two sites; the other factors explaining the MSA variability are taxonomic differences in the phytoplanktonic assemblages, and transport processes from the DMS source areas to the sampling sites. The taxonomic differences are also evident from the slopes of the correlation plots between MSA and PP: similar slopes (in the range 34.2-36.2 ng m-3of MSA/(gC m-2 d-1)) are found for the correlation between MSA at Ny Ålesund and PP in Barents Sea, and between MSA at Thule and PP in the Baffin Bay; conversely, the slope of the correlation between MSA at Ny Ålesund and PP in the Greenland Sea in summer is smaller (16.7 ng m-3of MSA/(gC m-2 d-1)). This is due to the fact that DMS emission from the Barents Sea and Baffin Bay is mainly related to the MIZ diatoms, which are prolific DMS producers, whereas in the Greenland Sea the DMS peak is related to an offshore pelagic bloom where low-DMS producer species are present. The sea ice dynamic plays a key role in determining MSA concentration in the Arctic, and a good correlation between MSA and SIM (slope = 39 ng m-3 of MSA/106 km2 SIM) and between MSA and IF-MIZ (slope = 56 ng m-3 of MSA/106 km2 IF-MIZ) is found for the cases attributable to bloomings of diatoms in the MIZ. Such relationships are calculated by combining the data sets from the two sites and suggest that PP is related to sea ice melting and to the extension of marginal sea ice areas, and that these factors are the main drivers for MSA concentrations at the considered Arctic sites. © 2016 The Authors.

The aim of the present work was to investigate the likely toxicological impact of atmospheric PM10 particles by comparing different effect-based methodologies, namely the Vibrio fischeri bioluminescence inhibition bioassay to evaluate ecotoxicity, the SOS Chromotest assay to estimate genotoxicity, and the Dithiothreitol (DTT) and Ascorbic Acid (AA) acellular assays to assess oxidative potential. The chemical composition was characterized for about 30 species, to assess the potential health impact of specific chemical components. Atmospheric particles were collected from spring to summer at a coastal site of the Central Mediterranean, away from large sources of local pollution. The Toxicity Unit (TU) index, used to assess the ecotoxicity, showed that 33% of the samples were toxic. The Induction Factor (IF), generally used to assess particle's genotoxicity, varied from 0.3 to 1.5 that represents the threshold value for genotoxicity. The oxidative potential (OP) determined by the DTT and AA assay varied within the 4.9–34.5 and 4.8–140.6 nmol min−1 range, respectively. DTT-OP and TU values were significantly correlated with OC, EC, and nss-K+, likely because the DTT and Vibrio fischeri responses were mainly associated with species from combustion sources. The IF factor was significantly correlated with some metals (Al, Ba, La, P, Sr, and Ti) likely from traffic sources and did not show any significant correlation with TU and OP values. Overall, paper's results proved the episodic occurrence of ecotoxicity and genotoxicity levels in PM10 particles sampled directly from their natural environment and away from strong pollution sources, highlighting the role mainly of carbonaceous compounds and heavy metals. The impact of spurious correlations between DTT- and AA-OPV and chemical species concentration has also been addressed.

From November 2004 to December 2007, size-segregated aerosol samples were collected all-year-round at Dome C (East Antarctica) by using PM10 and PM2.5 samplers, and multi-stage impactors. The data set obtained from the chemical analysis provided the longest and the most time-resolved record of sea spray aerosol (sea salt Na+) in inner Antarctica. Sea spray showed a sharp seasonal pattern. The highest values measured in winter (Apr–Nov) were about ten times larger than in summer (Dec–Mar). For the first time, a size-distribution seasonal pattern was also shown: in winter, sea spray particles are mainly sub-micrometric, while their summer size-mode is around 1–2 μm. Meteorological analysis on a synoptic scale allowed the definition of atmospheric conditions leading sea spray to Dome C. An extreme-value approach along with specific environmental based criteria was taken to yield stronger fingerprints linking atmospheric circulation (means and anomalies) to extreme sea spray events. Air mass back-trajectory analyses for some high sea spray events allowed the identification of two major air mass pathways, reflecting different size distributions: micrometric fractions for transport from the closer Indian-Pacific sector, and sub-micrometric particles for longer trajectories over the Antarctic Plateau. The seasonal pattern of the SO 4 2 − /Na+ ratio enabled the identification of few events depleted in sulphate, with respect to the seawater composition. By using methanesulphonic acid (MSA) profile to evaluate the biogenic SO 4 2 − contribution, a more reliable sea salt sulphate was calculated. In this way, few events (mainly in April and in September) were identified originating probably from the “frost flower” source. A comparison with daily-collected superficial snow samples revealed that there is a temporal shift between aerosol and snow sea spray trends. This feature could imply a more complex deposition processes of sea spray, involving significant contribution of wet and diamond dust deposition, but further work has to be carried out to rule out the effect of wind re-distribution and to have more statistic significance.

A year-round study, which was conducted from November 2004 to November 2007, of atmospheric oxidised sulphur compounds (methanesulphonic acid (MSA) and sulphate) was carried out in the east Antarctic Plateau at Dome C (75° 06′ S, 123° 20′ E, 3220 m a.s.l. and 1100 km away from the nearest coast). The two sulphur-derived species exhibit a seasonal cycle characterised by maxima in the summer from November to March. Size-segregated sampling performed with Andersen 8-stage impactors revealed that SO 4 2− and MSA have different size distributions in early summer (November) in comparison with mid-late summer (February). In November, the size distribution exhibited two distinct modes, the accumulation (0.4–0.7 μm) and the micrometric mode (1.1–2.1 μm), which is in contrast to February when only the accumulation mode was observed. The two modes exhibited different speciation; in the finest mode, sulphate and methanesulphonate were present primarily in the acidic form, whereas they were present primarily as sodium or ammonium salts in the micrometric mode. The different size distributions and speciation patterns in the two months are related to different transport pathways from oceanic areas to the central Antarctic Plateau. In the early summer months, air masses came primarily from the Indian Ocean and lingered for a long time over the Antarctic continent. The transport of sulphur compounds is related to sea spray aerosols and the resulting condensation of H 2 SO 4 and MSA over sea salt particles to form sodium salts. In contrast, a rapid transport of H 2 SO 4 and MSA formed above the boundary layer over oceanic areas leads to higher concentrations of the acidic species in the fine fraction of aerosols reaching Dome C in February relative to other summer months.

Methylene Blue Active Substances (MBAS) and Linear Alkylbenzene Sulphonates (LAS) concentrations, together with organic carbon and ions were measured in atmospheric coastal aerosols in the NW Mediterranean Basin. Previous studies have suggested that the presence of surfactants in coastal aerosols may result in vegetation damage without specifically detecting or quantifying these surfactants. Coastal aerosols were collected at a remote site (Porquerolles Island-Var, France) and at a more anthropised site (San Rossore National Park-Tuscany, Italy). The chemical data were interpreted according to a comprehensive local meteorological analysis aiming to decipher the airborne source and transport processes of these classes of compounds. The LAS concentration (anthropogenic surfactants) was measured in the samples using LC-MS/MS, a specific analytical method. The values were compared with the MBAS concentration, determined by a non-specific analytical method. At Porquerolles, the MBAS concentration (103 ± 93 ng m −3 ) in the summer samples was significantly higher than in the winter samples. In contrast, LAS concentrations were rarely greater than in the blank filters. At San Rossore, the mean annual MBAS concentration (887 ± 473 ng m −3 in PM10) contributed about 10% to the total atmospheric particulate organic matter. LAS mean concentration in these same aerosol samples was 11.5 ± 10.5 ng m −3 . A similar MBAS (529 ± 454 ng m −3 ) – LAS (7.1 ± 4.1 ng m −3 LAS) ratio of ∼75 was measured in the fine (PM2.5) aerosol fraction. No linear correlation was found between MBAS and LAS concentrations. At San Rossore site the variation of LAS concentrations was studied on a daily basis over a year. The LAS concentrations in the coarse fraction (PM10–2.5) were higher during strong sea storm conditions, characterized by strong air flow coming from the sea sector. These events, occurring with more intensity in winter, promoted the formation of primary marine aerosols containing LAS from the sea surface microlayer. In contrast to LAS, MBAS concentrations in the coarse fraction peaked in summer. Therefore, different sources are suggested for the two classes of compounds. In summer, increased MBAS concentration could be an indicator of phytoplanktonic blows enriching the sea surface microlayer with biogenic surfactants. In winter, some spikes in MBAS concentrations in the coarse fraction could be related to LAS concentrations and sea storm events. Moreover, in the fine fraction MBAS have a large concentration maxima in winter, corresponding to air masses coming from polluted continental areas. It is concluded that MBAS concentration in the fine or the coarse fraction is not an appropriate surrogate measurement of LAS concentration in aerosols because of the significant contribution from other sources to the MBAS concentration.