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Starting from 1952 C.E. more than 540 atmospheric nuclear weapons tests (NWT) were conducted in different locations of the Earth. This lead to the injection of about 2.8 t of 239Pu in the environment, roughly corresponding to a total 239Pu radioactivity of 6.5 PBq. A semiquantitative ICP-MS method was used to measure this isotope in an ice core drilled in Dome C (East Antarctica). The age scale for the ice core studied in this work was built by searching for well-known volcanic signatures and synchronising these sulfate spikes with established ice core chronologies. The reconstructed plutonium deposition history was compared with previously published NWT records, pointing out an overall agreement. The geographical location of the tests was found to be an important parameter strongly affecting the concentration of 239Pu on the Antarctic ice sheet. Despite the low yield of the tests conducted in the 1970s, we highlight their important role in the deposition of radioactivity in Antarctica due to the relative closeness of the testing sites. [Display omitted] • Nuclear Weapons Tests were responsible of a global dispersion of radioactivity. • Antarctic ice-cores preserve a detailed record of nuclear fallout. • An ICP-MS method was successfully used to measure 239Pu at fg g−1 level. • The nuclear fallout can represent an useful tool for the dating of an ice-core. [ABSTRACT FROM AUTHOR]

Two common types of wood (beech and fir) were burned in commercial pellet (11.1 kW) and wood (8.2 kW) stoves following a combustion cycle simulating the behavior of a real-world user. Ultrafine particulate matter (UFP, d p < 100 nm) was sampled with three parallel multistage impactors and analyzed for metals, main water soluble ions, anhydrosugars, total carbon, and PAH content. The measurement of the number concentration and size distribution was also performed by a fourth multistage impactor. UFP mass emission factors averaged to 424 mg/kg fuel for all the tested stove and wood type (fir, beech) combinations except for beech log burning in the wood stove (838 mg/kg fuel ). Compositional differences were observed for pellets and wood UFP samples, where high TC levels characterize the wood log combustion and potassium salts are dominant in every pellet sample. Crucial aspects determining the UFP composition in the wood stove experiments are critical situations in terms of available oxygen (a lack or an excess of combustion air) and high temperatures. Whereas for the automatically controlled pellets stove local situations (e.g., hindered air-fuel mixing due to heaps of pellets on the burner pot) determine the emission levels and composition. Wood samples contain more potentially carcinogenic PAHs with respect to pellets samples. Some diagnostic ratios related to PAH isomers and anhydrosugars compiled from experimental UFP data in the present study and compared to literature values proposed for the emission source discrimination for atmospheric aerosol, extend the evaluation usually limited to higher particle size fractions also to UFP. [ABSTRACT FROM AUTHOR]

Five snow pits and five firn cores were sampled during the 2003–2004 Italian Antarctic Campaign at Talos Dome (East Antarctica), where a deep ice core (TALDICE, TALos Dome Ice CorE, 1650 m depth) was drilled in 2005–2008 and analyzed for ionic content. Particular attention is spent in applying decontamination procedures to the firn cores, as core sections were stored for approximately 10 years before analysis. By considering the snow pit samples to be unperturbed, the comparison with firn core samples from the same location shows that ammonium, nitrate and MSA are affected by storage post-depositional losses. All the other measured ions are confirmed to be irreversibly deposited in the snow layer. The removal of the most external layers (few centimeters) from the firn core sections is proved to be an effective decontamination procedure. High-resolution profiles of seasonal markers (nitrate, sulfate and MSA) allow a reliable stratigraphic dating and a seasonal characterization of the samples. The calculated mean accumulation-rate values range from 70 to 85 mm w.e. year − 1 , in the period 2003–1973 with small differences between two sectors: 70–74 mm w.e. year − 1 in the NNE sector (spanning 2003–1996 years) and 81–92 mm w.e. year − 1 in the SSW sector (spanning 2003–1980 years). This evidence is interpreted as a coupled effect of wind-driven redistribution processes in accumulation/ablation areas. Statistical treatment applied to the concentration values of the snow pits and firn cores samples collected in different points reveals a larger temporal variability than spatial one both in terms of concentration of chemical markers and annual accumulation. The low spatial variability of the accumulation rate and chemical composition measured in the five sites demonstrates that the TALDICE ice core paleo-environmental and paleo-climatic stratigraphies can be considered as reliably representative for the Talos Dome area. [ABSTRACT FROM AUTHOR]

Recently, the increasing interest in the understanding of global climatic changes and on natural processes related to climate yielded the development and improvement of new analytical methods for the analysis of environmental samples. The determination of trace chemical species is a useful tool in paleoclimatology, and the techniques for the analysis of ice cores have evolved during the past few years from laborious measurements on discrete samples to continuous techniques allowing higher temporal resolution, higher sensitivity and, above all, higher throughput. Two fast ion chromatographic (FIC) methods are presented. The first method was able to measure Cl-, NO3- and SO42- in a melter-based continuous flow system separating the three analytes in just 1 min. The second method (called Ultra-FIC) was able to perform a single chromatographic analysis in just 30 s and the resulting sampling resolution was 1.0 cm with a typical melting rate of 4.0 cm min-1. Both methods combine the accuracy, precision, and low detection limits of ion chromatography with the enhanced speed and high depth resolution of continuous melting systems. Both methods have been tested and validated with the analysis of several hundred meters of different ice cores. In particular, the Ultra-FIC method was used to reconstruct the high-resolution SO42- profile of the last 10?000 years for the EDML ice core, allowing the counting of the annual layers, which represents a key point in dating these kind of natural archives. [ABSTRACT FROM AUTHOR]

Ice cores are widely used to reconstruct past changes of the climate system. For instance, the ice core record of numerous water-soluble and insoluble chemical species that are trapped in snow and ice offer the possibility to investigate past changes of various key compounds present in the atmosphere (i.e., aerosol, reactive gases). We developed a new method for the quantitative determination of fluoride in ice cores at sub-μg L-1 levels by coupling a flow injection analysis technique with a fast ion chromatography separation based on the "heart cut" column switching technology. Sensitivity, linear range (up to 60 μg L-1), reproducibility, and detection limit (0.02 μg L-1) were evaluated for the new method. This method was successfully applied to the analysis of fluoride at trace levels in more than 450 recent snow samples collected during the 1998-1999 International Trans-Antarctica Scientific Expedition traverse in East Antarctica at sites located between 170 and 850 km from the coastline. [ABSTRACT FROM AUTHOR]

Abstract: 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, 3220m a.s.l. and 1100km 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 SO4 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 (0.4–0.7μm) and the micrometric mode (1.1–2.1μm), 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 H2SO4 and MSA over sea salt particles to form sodium salts. In contrast, a rapid transport of H2SO4 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. [Copyright &y& Elsevier]

A detailed ionic component record was performed on EPICA Dome C ice core (East Antarctica) to a depth of 3180 musing Ion Chromatography and Fast Ion Chromatography (FIC). At depths greater than 2800 m, the sulfate profile shows intense, sharp spikes which are not expected due to the smoothing of sulfate peaks by diffusion processes. Moreover, these spikes show an "anomalous" chemical composition (e.g., unusually low acidity, high Mg2+ concentration and high Mg2+/Ca2+ ratio). These peaks and the surrounding layers also exhibit good Mg2+ vs SO42- and Cl- vs Na+ correlations through both glacial and interglacial periods. Furthermore, the high-resolution analysis of two horizontally contiguous ice sections showed that some fraction of the impurities are characterized by a heterogeneous distribution. Altogether, these results suggest the occurrence of long-term postdepositional processes involving a rearrangement of impurities via migration in the vein network, characterized by sulfuric acidity and leading to the formation of soluble particles of magnesium sulfate salts, along with ionic association of ions in the liquid films along boundaries. This evidence should be taken into consideration when inferring information on for rapid climatic and environmental changes from ice core chemical records at great depths. At Dome C, the depth threshold was found to be 2800 m. [ABSTRACT FROM AUTHOR]

Firn core methanesulphonic acid (MSA) stratigraphy from Talos Dome (East Antarctica) was compared with anomalies of the satellite-measured sea ice extent (1973–1995) in the Ross Sea and Wilkes Land oceanic sector. In spite of the sparseness of sea ice data, the MSA maxima fit with many positive sea ice anomalies in the Ross Sea. This evidence suggests that marine biogenic activity enhanced by large sea ice cover is an important, but not exclusive, factor in controlling MSA concentration in snow precipitation at Talos Dome. Other than source intensity, differences in regional atmospheric transport mechanisms affect the arrival of MSA-rich aerosol at Talos Dome. To clarify the role of transport processes in bringing biogenic aerosol to Talos Dome, a spectral analysis was applied to the MSA, SOI (South Oscillation Index), and SAM (Southern Annular Mode) record. Synchronicity or phase shift between the chemical signature and atmospheric circulation modes were tested. The variations in the MSA profile have a periodicity of 6.9, 4.9, 3.5, and 2.9 years. The 6.9 and 2.9 year periodicities show a strong positive correlation and are synchronous with corresponding SOI periodicity. This variability could be related to an increase in MSA source intensity (by dimethylsulphide from phytoplanktonic activity) linked to the sea ice extent in the Ross Sea area, but also to an increased strength in transport processes. Both of these factors are correlated with La Niña events (SOI positive values). Furthermore, SAM positive values are related to an increased sea ice extent in the Ross Sea sector and show two main periodicities 3.3 and 3.8 years. These periodicities determine the MSA variability at 3.5 years. However, the effect of intensification of the polar vortex and the consequent reduction in transport process intensity, which reduce the delivery of air masses enriched in MSA from oceanic areas to Talos Dome, make the effect of the SAM on the MSA concentration at Talos Dome less active than the SOI. In this way, snow deposition at the Talos Dome records larger MSA concentration by the combined effects of increased source emissions and more efficient transport processes. The MSA record from Talos Dome can therefore be considered a reliable proxy of sea ice extent when the effect of changes in transport processes in this region of Antarctica is considered. Over the previous 140 years, these conditions occur with a periodicity of 6.9 years. [Copyright &y& Elsevier]

Abstract: A method was developed for the quantitative determination of cations and anions in Antarctic ice cores at μgL−1 and sub-μgL−1 levels by ion chromatography (IC), after ultra-clean decontamination procedures. Strict manipulation and decontamination procedures were used in sub-sampling, in order to minimise sample contamination. Na+, NH4 +, K+, Mg2+ and Ca2+ were determined by 12-min isocratic elution (H2SO4 eluent). Contemporaneously, in a parallel device, F−, MSA (methanesulfonic acid), Cl−, NO3 − and SO4 2− were analysed in a single 12-min run with multiple-step elution using Na2CO3/NaHCO3 as eluent. Melted ice samples were pumped from their still-closed containers (polystyrene accuvettes with polyethylene caps), shared between the two ion chromatographic systems, online filtered (0.45μm Teflon membrane) and pre-concentrated (anions and cations pre-concentration columns) using a flow analysis system, thus avoiding uptake of contaminants from the laboratory atmosphere. Sensitivity, linear range, reproducibility and detection limit were evaluated for each chemical species. Anion or cation detection limits ranged from 0.01 to 0.15μgL−1 by using a relatively small sample volume (1.5mL). Such values are significantly lower than those reported in literature for almost all the components. These methods were successfully applied to the analysis of cations and anions at trace levels in the Dome C ice core. The composition of the atmospheric aerosol for the last 850kyr was reconstructed by high-resolution continuous chemical stratigraphies. Concentration trends in the last nine glacial-interglacial climatic cycles were shown and briefly discussed. [Copyright &y& Elsevier]

The chemical analysis of shallow firn cores sampled in coastal and plateau areas in Northern Victoria Land and along a transect from Talos Dome to Dome C (East Antarctica, Pacific Ocean sector) allowed a global view of spatial and temporal changes in chemical composition of snow depositions over the last 100 years. Variations in concentration of primary (sea spray) and secondary (biogenic emission, atmospheric inputs) source markers were observed and discussed as a function of distance from the sea and altitude. In the stations characterized by relatively high snow accumulation rates, the sub-sampling resolution was sufficient to obtain a stratigraphic dating by using the periodical variations of seasonal markers. In these stations, a subdivision in "summer" and "winter" samples was carried out in order to study the seasonal changes of the contributions of the measured compounds to the snow composition as elevation and distance from the sea increase. Some evidence of post-depositional effects which are able to change the original deposition of chloride and nitrate, was observed at stations with low accumulation rates. The reliability of the depth/concentration profile of these substances for reconstructing past deposition was also discussed. [ABSTRACT FROM AUTHOR]

High-resolution chemical records of main and trace ionic components of snow precipitation over the last 250 years were obtained by analysing the first 36 m of a firn core drilled at Talos Dome, a dome located in the ice divide between northern Victoria Land and Oates Land (East Antarctica Pacific Ocean/Ross Sea sector). The concentration/depth profiles of some relevant chemical parameters are discussed on the basis of a previous stratigraphic dating, set up following the seasonal signatures of non-sea-salt (nss) sulphate deposition and synchronised by using tritium and volcanic temporally known horizons. Particular attention is paid to the study of the temporal trends of the sea spray components (Na + , Cl - , Mg 2+ ) and S and N cycle compounds ( ) to understand the main sources, transport mechanisms and depositional processes of these compounds at the deposition site. Good correlations between the sea spray markers show that the primary marine contribution is relevant, though Talos Dome is located at a relatively high altitude (2316 m a.s.l.) and far from the coast line (about 250 km). The study of the snow chemical composition and of the recent (for the last few centuries) atmosphere/snow relationship at Talos Dome is important as a preliminary survey at this station, which will probably be chosen for a deep ice coring project. [ABSTRACT FROM AUTHOR]

In this work, we present chemical stratigraphies of two sampling lines collected within a 4 m depth snow pit dug in Dome C during the Antarctic summer Campaign 2017/2018, 12 years after the last reported snow pit. The first sampling line was analyzed for nine anionic and cationic species using Ion Chromatography (IC); the second sampling line was analyzed for seven major elements in an innovative way with Inductively Coupled Plasma Optical Emission Spectroscopy (ICP-OES) after sample pre-concentration, allowing the study of deposition processes of new markers especially related to crustal source. This coupled analysis, besides confirming previous studies, allowed us to investigate the depositions of the last decades at Dome C, enriching the number of the detected chemical markers, and yielding these two techniques complementary for the study of different markers in this kind of matrix. As a result of the dating, the snow layers analyzed covered the last 50 years of snow depositions. The assessment of the accumulation rate, estimated about 9 cm yr−1, was accomplished only for the period 1992–2016, as the eruption of 1992 constituted the only tie-point found in nssSO42− depth profile. Na, the reliable sea salt marker, together with Mg and Sr, mainly arose from marine sources, whereas Ca, Al and Fe originated from crustal inputs. Post-depositional processes occurred on Cl− as well as on NO3− and methanesulfonic acid (MSA); compared to the latter, Cl− had a more gradual decrease, reporting a threshold at 2.5 m for the post-depositional process completion. For NO3− and MSA, instead, the threshold was shallower, at about 1 m depth, with a loss of 87% for NO3− and of 50% for MSA. [ABSTRACT FROM AUTHOR]

The harmonization of sampling, sample preparation and laboratory analysis methods to detect carbon compounds in snow requires detailed documentation of those methods and their uncertainties. Moreover, intercomparison experiments are needed to reveal differences and quantify the uncertainties further. Here, we document our sampling, filtering, and analysis protocols used in the intercomparison experiment from three laboratories to detect water-insoluble carbon in seasonal surface snow in the high-mountain environment at Kolm Saigurn (47.067842° N, 12.98394° E, alt 1598 m a.s.l.), Austria. The participating laboratories were TU Wien (Austria), the University of Florence (Italy), and the Finnish Meteorological Institute (Finland). For the carbon analysis, the NIOSH5040 and EUSAAR2 protocols of the OCEC thermal-optical method were used. The median of the measured concentrations of total carbon (TC) was 323 ppb, organic carbon (OC) 308 ppb, and elemental carbon (EC) 16 ppb. The methods and protocols used in this experiment did not reveal large differences between the laboratories, and the TC, OC, and EC values of four inter-comparison locations, five meters apart, did not show meter-scale horizontal variability in surface snow. The results suggest that the presented methods are applicable for future research and monitoring of carbonaceous particles in snow. Moreover, a recommendation on the key parameters that an intercomparison experiment participant should be asked for is presented to help future investigations on carbonaceous particles in snow. The work contributes to the harmonization of the methods for measuring the snow chemistry of seasonal snow deposited on the ground. [ABSTRACT FROM AUTHOR]

Ship traffic, population, infrastructure development, and mining activities are expected to increase in the Arctic due to its rising temperatures. This is expected to produce a major impact on aerosol composition. Metals contained in atmospheric particles are powerful markers and can be extremely helpful to gain insights on the different aerosol sources. This work aims at studying the sources of metals in the Arctic aerosol sampled at the Thule High Arctic Atmospheric Observatory (THAAO; Greenland, 76.5°N 68.8°W). Due to the particular composition of Greenlandic soils and to properties of other sources, it was possible to find several signatures of natural and anthropogenic aerosols transported from local and long-range regions. Arctic haze (AH) at Thule builds up on long-range transported aerosol mainly from Canada and Nord America. From a chemical standpoint, this aerosol is characterized by a high concentration of sulfate, Pb, As and Cd and by a La/Ce ratio larger than 1. The Ti/Al and Fe/Al ratios in the AH aerosol are lower (Ti/Al = 0.04 w/w; Fe/Al = 0.79 w/w) than for local aerosol (Ti/Al = 0.07 w/w; Fe/Al = 0.89 w/w). Conversely, aerosol arising from coastal areas of South-West Greenland is characterized by a high concentration of V, Ni, and Cr. These metals, generally considered anthropogenic, arise here mainly from natural crustal sources. In some summer samples, however, the V/Ni ratio becomes larger than 3. In particular, cases displaying this characteristic ratio, as also shown by backward trajectories, are associated with sporadic transport to Thule of ship aerosol from ships passing through Baffin Bay and arriving to Thule during summer. Although further measurements are necessary to confirm the discussed results, the analysis carried out in this work on a large number of metals sampled in coastal Greenland aerosol is unprecedented. Unlabelled Image • Metals in aerosol samples from THAAO (Thule) are determined by ICP – AES. • Arctic Haze is characterized by high concentration of Pb, As and Cd and La/Ce > 1. • V, Ni and Cr are not from anthropic sources, but generally arise from Greenland soils. • Sporadic evidence of ship aerosol having V/Ni > 3 are evident in some summer samples. • Ti/Al and Fe/Al can be used as local and long range crustal aerosol fingerprints. [ABSTRACT FROM AUTHOR]

Different analytical techniques were used in this work to investigate the relationships between oxidative potential (OP) and metal, Br, P, S, and Se concentration in PM10 samples. Dithiothreitol and ascorbic acid acellular assays were used to determine the oxidative potential (OP) in PM10 samples. The particle-induced X-ray emission technique was used to estimate the mass concentration of specific chemical elements. PM10 samples were collected in Lecce, a coastal site of the Central Mediterranean away from large sources of local pollution. Both winter and spring samples were analyzed to study the seasonal dependence of the relationships between OP values and chemical element concentrations. The Redundancy Discriminant Analysis (RDA) was applied to (volume- and mass-normalized) OP values as response variables and metal, Br, P, S, and Se concentrations as explanatory variables. RDA triplots allowed to visualize the main relationships between PM10 OP values and corresponding chemical element concentrations. Spearman correlation coefficients were also used to investigate the relationships between OP values and metal, Br, P, S, and Se concentrations, besides comparing RDA outcomes. The integrated approach based on two different techniques allowed to better highlight the potentially harmful effects associated with specific metals and other chemical elements in PM10 samples. [ABSTRACT FROM AUTHOR]

In remote marine areas, biogenic productivity and atmospheric particulate are coupled through dimethylsulfide (DMS) emission by phytoplankton. Once in the atmosphere, the gaseous DMS is oxidized to produce H2SO4 and methanesulfonic acid (MSA); both species can affect the formation of cloud condensation nuclei. This study analyses eight years of biogenic aerosol evolution and variability at two Arctic sites: Thule (76.5° N, 68.8° W) and Ny Ålesund (78.9° N, 11.9° E). Sea ice plays a key role in determining the MSA concentration in polar regions. At the beginning of the melting season, in April, up to June, the biogenic aerosol concentration appears inversely correlated with sea ice extent and area, and positively correlated with the extent of the ice-free area in the marginal ice zone (IF-MIZ). The upper ocean stratification induced by sea ice melting might have a role in these correlations, since the springtime formation of this surface layer regulates the accumulation of phytoplankton and nutrients, allowing the DMS to escape from the sea to the atmosphere. The multiyear analysis reveals a progressive decrease in MSA concentration in May at Thule and an increase in July August at Ny Ålesund. Therefore, while the MSA seasonal evolution is mainly related with the sea ice retreat in April, May, and June, the IF-MIZ extent appears as the main factor affecting the longer-term behavior of MSA. [ABSTRACT FROM AUTHOR]

An inductively coupled plasma sector field mass spectrometer (ICP-SFMS) was used to develop an analytical method for the fast determination of Na, Al, Sc, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Y, Mo, Cd, Ba, La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, and Pb in Arctic size-segregated aerosol samples (PM 10 ), after microwave acidic digestion. The ICP-SFMS was coupled with a microflow nebulizer and a desolvation system for the sample introduction, which reduced the isobaric interferences due to oxides and the required volume of sample solutions, compared to the usual nebulization chamber methods. With its very low limit of detection, and taking into account the level of blanks, this method allowed the quantification of many metals in very low concentration. Particular attention was given to Rare Earth Elements (REEs - La to Lu). The efficiency in the extraction of REEs was proved to be acceptable, with recoveries over 83% obtained with a Certified Reference Material (AMiS 0356). The analytical method was then applied to particulate matter samples, collected at ground level in Ny Ålesund (Svalbard Islands, Norway), during spring and summer, from 2010 to 2015, with daily resolution and using a low-volume device. Thus, for the first time, a large atmospheric concentrations dataset of metals in Arctic particulate matter at high temporal resolution is presented. On the basis of differences in LREE/HREE ratio and Ce and Eu anomalies in spring and summer samples, basic information to distinguish local and long-range transported dust were achieved. [ABSTRACT FROM AUTHOR]

An airborne microwave wide-band radiometer (500–2000 MHz) was operated for the first time in Antarctica to better understand the emission properties of sea ice, outlet glaciers and the interior ice sheet from Terra Nova Bay to Dome C. The different glaciological regimes were revealed to exhibit unique spectral signatures in this portion of the microwave spectrum. Generally, the brightness temperatures over a vertically homogeneous ice sheet are warmest at the lowest frequencies, consistent with models that predict that those channels sensed the deeper, warmer parts of the ice sheet. Vertical heterogeneities in the ice property profiles can alter this basic interpretation of the signal. Spectra along the lengths of outlet glaciers were modulated by the deposition and erosion of snow, driven by strong katabatic winds. Similar to previous experiments in Greenland, the brightness temperatures across the frequency band were low in crevasse areas. Variations in brightness temperature were consistent with spatial changes in sea ice type identified in satellite imagery and in situ ground-penetrating radar data. The results contribute to a better understanding of the utility of microwave wide-band radiometry for cryospheric studies and also advance knowledge of the important physics underlying existing L-band radiometers operating in space. [ABSTRACT FROM AUTHOR]

An integrated system, based on Inductively Coupled Plasma-Sector Field Mass Spectrometry (ICP-SFMS) and Inductively Coupled Plasma-Atomic Emission Spectrophotometry (ICP-AES) techniques, was optimised for the geochemical characterisation of soils and marine sediments. Sample mineralization was carried out with HF, HNO 3 and HClO 4 . Operative blanks were at least two orders of magnitude lower than the lowest concentration measured in real samples. For ICP-SFMS, the detection power of the method in high resolution mode was sufficient for an accurate quantification of metals, yet avoiding REEs' (Rare Earth Elements) isobaric interferences. Once tested the accuracy on six certified materials, the methods were applied to the analysis of 39 major and trace metals on the top 90 m of sediments from the ANDRILL AND-1B core, covering the last million years. Stratigraphies of REEs and of normalised markers from this core clearly highlight a discontinuity at about 660,000 years before present. This pattern is well shown by the results of a PMF (Positive Matrix Factorization) statistical analysis, revealing two different sources for the sedimentary material, whose relative contribution changed around that time. Such a result is consistent with previous studies and confirms the net change in the provenance of glacial fluxes in the McMurdo region (Ross Ice Shelf, Antarctica) in the last million years. [ABSTRACT FROM AUTHOR]

Size-segregated (PM 10 ) aerosol samples were collected at Ny-Ålesund (Svalbard Islands, Norwegian Arctic) from April to September 2012 and analysed for lead content and isotopic composition ( 207 Pb/ 206 Pb and 208 Pb/ 206 Pb), along with other chemical tracers, such as aluminium (crustal marker) and non-sea-salt sulphates (anthropogenic and marine biogenic marker). It was found that most of lead reaching Ny-Ålesund is anthropogenic, with a marked seasonality of both the concentration and isotopic signature. Particularly, average lead concentration in summer was significantly lower than in spring ( p = 0.003), whereas 208 Pb/ 206 Pb decreased from 2.107 ± 0.002 to 2.090 ± 0.005 (mean ± 95%-confidence level, p = 6.0 10 −6 ). A comparison of the measured isotopic ratios to literature data suggests that the atmospheric lead reaching the Arctic during spring can be mainly related to inputs from eastern Eurasia, whereas North America appeared to be the major source during the summer. Experimental results and sampling strategy also indicate that local inputs of crustal and anthropogenic lead play a minor role. The source-receptor relationship was confirmed by a back-trajectory cluster analysis of air-masses reaching the sampling site. [ABSTRACT FROM AUTHOR]

Organic (OC) and elemental carbon (EC), inorganic ions (Cl−, NO3−, SO42−, Na+, NH4+, K+, Ca2+), methanesulfonate (MSA−) and metals (Al, Fe, Pb, Mn, Ba, V) were monitored in PM1 and PM2.5 samples collected at a suburban site in south-eastern Italy, to contribute to the characterisation of fine particles in the Central Mediterranean. Mean mass concentrations are 13 µg/m3and 22 µg/m3in PM1 and PM2.5, respectively. OC, EC, SO42−, NH4+, NO3−, K+and Ca2+are predominant components and account for 54% and 56% of the PM1 and PM2.5 mass, respectively. OC, EC, SO42−, NH4+, K+and Ca2+concentrations lie in the range of the corresponding ones measured in PM1 and PM2.5 samples collected at suburban/urban Mediterranean sites. NO3−and trace element concentrations lie in the range of the corresponding ones measured in PM1 and PM2.5 samples collected at remote/background Mediterranean sites. The biogenic nss-SO42−accounts for ~5% and 4% of nss-SO42−in PM1 and PM2.5, respectively. The seasonal trend of the components partitioning and the interspecies correlation analysis in PM1 and PM2.5-1 indicated that the PM1 and PM2.5-1 components depend on season and are likely not controlled by similar sources, and/or similar generation processes, and/or similar transport patterns. The sulfur and nitrogen oxidation ratios were calculated to contribute to the understanding of the seasonal dependence of nitrate and sulfate concentrations in PM1 and PM2.5-1. The mass closure analysis showed that organic matter (OM), EC, and nitrate mass percentages are larger in autumn–winter. NH4+, nss-SO42−, and crustal matter mass percentages are larger in spring–summer. Finally, the ratio of the crustal matter in PM1 to that in PM2.5-1, which is 0.2 and 0.3 in spring–summer and autumn–winter, respectively, and the higher (OM+EC) contribution in PM1 than in PM2.5-1 led to the conclusion that PM1 would be a better indicator for fine-anthropogenic particles than PM2.5. [ABSTRACT FROM AUTHOR]

While more and more studies are being conducted on carbonaceous fractions—organic carbon (OC) and elemental carbon (EC)—in urban areas, there are still too few studies about these species and their effects in polar areas due to their very low concentrations; further, studies in the literature report only data from intensive campaigns, limited in time. We present here for the first time EC–OC concentration long-time data records from the sea-level sampling site of Ny-Ålesund, in the High Arctic (5 years), and from Dome C, in the East Antarctic Plateau (1 year). Regarding the Arctic, the median (and the interquartile range (IQR)) mass concentrations for the years 2011–2015 are 352 (IQR: 283–475) ng/m3 for OC and 4.8 (IQR: 4.6–17.4) ng/m3 for EC, which is responsible for only 3% of total carbon (TC). From both the concentration data sets and the variation of the average monthly concentrations, the influence of the Arctic haze on EC and OC concentrations is evident. Summer may be interested by high concentration episodes mainly due to long-range transport (e.g., from wide wildfires in the Northern Hemisphere, as happened in 2015). The average ratio of EC/OC for the summer period is 0.05, ranging from 0.02 to 0.10, and indicates a clean environment with prevailing biogenic (or biomass burning) sources, as well as aged, highly oxidized aerosol from long-range transport. Contribution from ship emission is not evident, but this result may be due to the sampling time resolution. In Antarctica, a 1 year-around data set from December 2016 to February 2018 is shown, which does not present a clear seasonal trend. The OC median (and IQR) value is 78 (64–106) ng/m3; for EC, it is 0.9 (0.6–2.4) ng/m3, weighing for 3% on TC values. The EC/OC ratio mean value is 0.20, with a range of 0.06–0.35. Due to the low EC and OC concentrations in polar areas, correction for the blank is far more important than in campaigns carried out in other regions, largely affecting uncertainties in measured concentrations. Through the years, we have thus developed a new sampling strategy that is presented here for the first time: samplers were modified in order to collect a larger amount of particulates on a small surface, enhancing the capability of the analytical method since the thermo-optical analyzer is sensitive to carbonaceous aerosol areal density. Further, we have recently coupled such modified samplers with a sampling strategy that makes a more reliable blank correction of every single sample possible. [ABSTRACT FROM AUTHOR]

Seasonal variations of ionic species concentrations in PM 10 and PM 2.5 aerosols were investigated at King Sejong Station (King George Island, Antarctic Peninsula) in 2013. Seasonal variations of PM 2.5 mass were also determined, and found to be in the range: 2482.2 ± 944.4 ng m−3 (austral winter) to 3493.3 ± 1223.8 ng m−3 (austral fall). On a weight basis, the PM 2.5 ionic species consisted mainly of primary ions from sea spray (~30% in summer, ~50% in winter) and partly from secondary ions (~20% in summer), with the ratios of sea spray and secondary ion components to PM 2.5 mass showing clear seasonal variation. The seasonal cycle of sea spray components was not well defined, but was weakly correlated with wind speed (r2 = 0.38). This correlation was likely attributable to a combination of the seasonal properties of wind and the measurement site's location at the western tip of Barton Peninsula. The concentrations of sulphur species (CH 3 SO 3 − and non sea salt SO 4 2−) were clearly higher during austral summer. Notably, these concentrations were ~2–3 times higher during in January 2013 than in other summer months of the field observation period. This was attributed to an increased biomass of algae in the ocean area surrounding King George Island and more frequent air mass passage over ocean areas with algae blooms. The NH 4 + concentration was also clearly higher in austral summer 2013, mainly due to secondary formation from the NH 3 released from local emission sources such as penguin colonies and ocean areas near the measurement site with acidic aerosol, but also affected by local meteorology specific to the summer of 2014. [ABSTRACT FROM AUTHOR]

Major explosive volcanic eruptions may significantly alter the global atmosphere for about 2–3 years. During that period, volcanic products (mainly H2SO4) with high residence time, stored in the stratosphere or, for shorter times, in the troposphere are gradually deposited onto polar ice caps. Antarctic snow may thus record acidic signals providing a history of past volcanic events. The high resolution sulphate concentration profile along a 197 m long ice core drilled at GV7 (Northern Victoria land) was obtained by Ion Chromatography on around 3500 discrete samples. The relatively high accumulation rate (241 ± 13 mm we yr −1) and the 5-cm sampling resolution allowed a preliminary counted age scale. The obtained stratigraphy covers roughly the last millennium and 24 major volcanic eruptions were identified, dated, and tentatively ascribed to a source volcano. The deposition flux of volcanic sulphate was calculated for each signature and the results were compared with data from other Antarctic ice cores at regional and continental scale. Our results show that the regional variability is of the same order of magnitude as the continental one. [ABSTRACT FROM AUTHOR]

Abstract A methodology to detect the weekly cycle impact of the particulate matter (PM), and PM sources on the near surface temperature and wind speed is discussed in the paper. Chemically-speciated PM10 and PM2.5 samples are analyzed to detect the weekly cycle of both the PM mass concentrations and the PM sources identified by the Positive Matrix Factorization technique. The average percent departure (APD) of the PM mass concentration from the mean value calculated for each day of the week shows that a positive (higher values during midweek) and a negative (higher values during weekend) weekly cycle characterizes the PM10 and PM2.5 mass concentrations in Autumn-Winter (AW, September–February) and Spring-Summer (SS, March–August), respectively. The westerly transport of pollution seems to have a role on the negative PM weekly cycle found in SS. The analysis of the six identified aerosol sources indicates that in SS the mixed anthropogenic and the reacted dust sources likely impact the PM10 negative weekly cycle and that the mixed anthropogenic source likely impacts the PM2.5 negative weekly cycle. The mixed anthropogenic and soil dust sources likely affect in AW the positive weekly cycle of the PM10 mass concentration. Both sources in addition to the reacted dust source seem to affect the PM2.5 mass concentration in AW. The APD analysis of the temperature (T) and wind speed (WS) at the surface from measurements co-located in space and time with the PM ones reveals that the WS and T values are characterized by a negative weekly cycle in AW. Conversely, in SS, the WS-APD value decreases on Sunday and the T-APD values increase in the second half of the week. These last results likely give evidence of the PM impact on the near-surface temperature and wind speed at the study site. Graphical abstract Unlabelled Image Highlights • Weekly cycles of PM10 and PM2.5 mass concentrations and seasonal dependence • Weekly cycles of temperature and wind speed at the surface and seasonal dependence • Chemical speciation of PM10 and PM2.5 samples • Aerosol source identification by Positive Matrix Factorization • Aerosol source impact on the weekly cycles of PM10 and PM2.5 mass concentrations [ABSTRACT FROM AUTHOR]

An extended study on the oxidative potential (OP) of PM 10 particles collected from December 2014 to October 2015 at a peninsular site of the Central Mediterranean basin has been performed. PM 10 particles have been selected to better account for all different aged/fresh particle types. Two acellular assays, i.e., the dithiothreitol (DTT) and ascorbic acid (AA) methods, were used to measure the OP of PM 10 particles chemically speciated by more than 40 species. DTT and AA assays provide close mean values of volume normalized OP V responses, with similar variability range, i.e., mean OP DTT V  = 0.24 ± 0.12 nmol DTT min −1 m −3 and mean OP AA V  = 0.29 ± 0.18 nmol AA min −1 m −3 . Also mass normalized OP m responses are similar for both assays, with mean value close to 0.008 nmol min −1 μg −1 . The measured OP DTT V and OP AA V are correlated with several inorganic species, namely ions and metals, and with organic/elemental carbon. The discrimination of the data according seasonality, i.e., Autumn-Winter (AW, October–March) and Spring-Summer (SS, April–September) days, shows a clear seasonal trend of correlation coefficients. In AW, OP DTT V is strongly correlated with nss-K + and nss-Ca 2+ , in addition to Ba, Cd, Ce, Cr, Cu, Fe, and Mn (traffic-related metals) and with EC, OC, and POC associated with the traffic exhaust source and/or with the combustion including biomass-burning source. Otherwise, OP DTT V of SS samples is correlated only with NH 4 + , Cu, EC, OC, and POC. The OP AA V of AW samples is well correlated with Ba, Ce, Cr, Cu, Fe, Mn, nss-K + , EC, OC, and POC, which are related with traffic and/or combustion emissions. Conversely, in SS, OP AA V is mainly correlated with NH 4 + , nss-K + , nss-Mg 2+ , nss-Ca 2+ , nss-SO 4 2− , Cu, Mn, P, Pb, and oxalate, that are species related to secondary aerosols and resuspended soil from vehicular traffic and/or transported Saharan dust. These findings point the importance of both organic components and transition metals to PM oxidative properties, and also suggest that synergistic/antagonistic interactions and cross-correlations between the PM redox-active components are likely responsible for the seasonal variation of the AA and DTT assay response. The inter-correlation among all analysed species has been investigated to explain contrasting results and the negative correlations between OP values and some chemical species. [ABSTRACT FROM AUTHOR]

This work is part of the TOBICUP (TOxicity of BIomass Combustion generated Ultrafine Particles) project which aimed at providing the composition of ultrafine particles (UFPs, i.e. particles with aerodynamic diameter, d ae , lower than 100 nm) emitted by wood combustion and elucidating the related toxicity. Results here reported are from two ambient monitoring campaigns carried out at an alpine town in Northern Italy, where wood burning is largely diffused for domestic heating in winter. Wintertime and summertime UFP samples were analyzed to assess their chemical composition (i.e. elements, ions, total carbon, anhydrosugars, and polycyclic aromatic hydrocarbons) and biological activity. The induction of the pro-inflammatory cytokine interleukin-8 (IL-8) by UFPs was investigated in two human cells lines (A549 and THP-1) and in human peripheral blood leukocytes. In addition, UFP-induced oxidative stress and genotoxicity were investigated in A549 cells. Ambient UFP-related effects were compared to those induced by traffic-emitted particles (DEP) taken from the NIES reference material “vehicle exhaust particulates”. Ambient air UFPs induced a dose-related IL-8 release in both A549 and THP-1 cells; the effect was more relevant on summer samples and in general THP-1 cells were more sensitive than A549 cells. On a weight basis our data did not support a higher biological activity of ambient UFPs compared to DEP. The production of IL-8 in the whole blood assay indicated that UFPs reached systemic circulation and activated blood leukocytes. Comet assay and γ-H2AX evaluation showed a significant DNA damage especially in winter UFPs samples compared to control samples. Our study showed that ambient UFPs can evoke a pulmonary inflammatory response by inducing a dose-related IL-8 production and DNA damage, with different responses to UFP samples collected in the summer and winter periods. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

This study aimed to collect, characterize ultrafine particles (UFP) generated from the combustion of wood pellets and logs (softwood and hardwood) and to evaluate their pro-inflammatory effects in THP-1 and A549 cells. Both cell lines responded to UFP producing interleukin-8 (IL-8), with wood log UFP being more active compared to pellet UFP. With the exception of higher effect observed with beech wood log UFP in THP-1, the ability of soft or hard woods to induce IL-8 release was similar. In addition, on weight mass, IL-8 release was similar or lower compared to diesel exhaust particles (DEP), arguing against higher biological activity of smaller size particles. UFP-induced IL-8 could be reduced by SB203580, indicating a role of p38MAPK activation in IL-8 production. The higher activity of beech wood log UFP in THP-1 was not due to higher uptake or endotoxin contamination. Qualitatively different protein adsorption profiles were observed, with less proteins bound to beech UFP compared to conifer UFP or DEP, which may provide higher intracellular availability of bioactive components, i.e. levoglucosan and galactosan, toward which THP-1 were more responsive compared to A549 cells. These results contribute to our understanding of particles emitted by domestic appliances and their biological effects. [ABSTRACT FROM AUTHOR]

Amongst Ion Beam Analysis (IBA) techniques applied to the study of atmospheric aerosol samples, Elastic Backscattering Spectrometry (EBS) and Particle Elastic Scattering Analysis (PESA) with MeV energy proton beams allows obtaining quantitative information about the concentration of C and other low-Z atoms like H, N and O in the sample. With these nuclear techniques a direct measurement of elemental carbon (EC) and organic carbon (EC) is not possible. Nevertheless, the detection of all the aforemetioned light elements may help to infer some information on the aerosol chemical composition. The H concentration obtained by PESA may be used as a proxy of OC; then, EC can be obtained as the difference between total carbon measured simultaneously by EBS and OC as estimated by PESA. The feasibility of the quantification of EC and OC following this approach in particulate matter samples collected on Teflon filters, where this information cannot be obtained by standard thermo-optical analyses, will be discussed. Moreover, thanks to the simultaneous measurements of H, C, N and O in the aerosol samples, the organic component of the aerosols (particulate organic matter, POM) can be directly calculated and thus the validity of the POM/OC conversion factors found in the literature can be tested. [ABSTRACT FROM AUTHOR]

From January to December 2010, surface snow samples were collected with monthly resolution at the Concordia station (75°06’S, 123°20’E), on the Antarctic plateau, and analysed for major and trace elements in both dissolved and particulate (i.e. insoluble particles, >0.45 μm) phase. Additional surface snow samples were collected with daily resolution, for the determination of sea-salt sodium and not-sea-salt calcium, in order to support the discussion on the seasonal variations of trace elements. Concentrations of alkaline and alkaline-earth elements were higher in winter (April–October) than in summer (November–March) by a factor of 1.2–3.3, in agreement with the higher concentration of sea-salt atmospheric particles reaching the Antarctic plateau during the winter. Similarly, trace elements were generally higher in winter by a factor of 1.2–1.5, whereas Al and Fe did not show any significant seasonal trend. Partitioning between dissolved and particulate phases did not change with the sampling period, but it depended only on the element: alkaline and alkaline-earth elements, as well as Co, Cu, Mn, Pb and Zn were for the most part (>80%) in the dissolved phase, whereas Al and Fe were mainly associated with the particulate phase (>80%) and Cd, Cr, V were nearly equally distributed between the phases. Finally, the estimated marine and crustal enrichment factors indicated that Cd, Cr, Cu, Pb and Zn have a dominant anthropogenic origin, with a possible contribution from the Concordia station activities. [ABSTRACT FROM AUTHOR]

Abstract: We report on the existence and nature of Holocene solar and climatic variations on centennial to millennial timescales. We introduce a new solar activity proxy, based on nitrate (NO3 −) concentration from the Talos Dome ice core, East Antarctica. We also use a new algorithm for computing multiple-cross wavelet spectra in time–frequency space that is generalized for multiple time series (beyond two). Our results provide a new interpretive framework for relating Holocene solar activity variations on centennial to millennial timescales to co-varying climate proxies drawn from a widespread area around the globe. Climatic proxies used represent variation in the North Atlantic Ocean, Western Pacific Warm Pool, Southern Ocean and the East Asian monsoon regions. Our wavelet analysis identifies fundamental solar modes at 2300-yr (Hallstattzeit), 1000-yr (Eddy), and 500-yr (unnamed) periodicities, leaves open the possibility that the 1500–1800-yrcycle may either be fundamental or derived, and identifies intermediary derived cycles at 700-yr and 300-yr that may mark rectified responses of the Atlantic thermohaline circulation to external solar modulation and pacing. Dating uncertainties suggest that the 1500-yr and 1800-yrcycles described in the literature may represent either the same or two separate cycles, but in either case, and irrespective too of whether it is a fundamental or derived mode in the sense of Dima and Lohmann (2009), the 1500–1800-yr periodicity is widely represented in a large number of paleoclimate proxy records. It is obviously premature to reject possible links between changing solar activity at these multiple scales and the variations that are commonly observed in paleoclimatic records. [Copyright &y& Elsevier]

Here we present the first multi-year record of nitrate in the atmospheric aerosol (2005-2008) and surface snow (2006-08) from central Antarctica. PM10 and size-segregated aerosol, together with superficial snow, have been collected all year-round at high resolution (daily for all the snow samples and for most of aerosol samples) at Dome C since the 2004/05 field season and analysed for main and trace ionic markers. The suitability of the sampling location in terms of possible contamination from the base is shown in detail. In spite of the relevance of nitrate in Antarctic atmosphere, both for better understanding the chemistry of N cycle in the plateau boundary layer and for improving the interpretation of long-term nitrate records from deep ice core records, nitrate sources in Antarctica are not well constrained yet, neither in extent nor in timing. A recurring seasonal pattern was pointed out in both aerosol and snow records, showing summer maxima and winter minima, although aerosol maxima lead the snow ones of 1-2 months, possibly due to a higher acidity in the atmosphere in mid-summer, favouring the repartition of nitrate as nitric acid and thus its uptake by the surface snow layers. On the basis of a meteorological analysis of one major nitrate event, of data related to PSC I extent and of irradiance values, we propose that the high nitrate summer levels in aerosol and snow are likely due to a synergy of enhanced source of nitrate and/or its precursors (such as the stratospheric inputs), higher solar irradiance and higher oxidation rates in this season. Moreover, we show here a further evidence of the substantial contribution of HNO3/NOx re-emission from the snowpack, already shown in previous works, and which can explain a significant fraction of atmospheric nitrate, maintaining the same seasonal pattern in the snow. As concerning snow specifically, the presented data suggest that nitrate is likely to be controlled mainly by atmospheric processes, not on the daily timescale but rather on the seasonal one. [ABSTRACT FROM AUTHOR]

Simple Summary: This study aims to quantify the effects of smoke originating from boreal biomass-burning fires on solar radiation propagating through the atmosphere. The wildfires that took place in summer 2017 along Greenland's west coast and northern Canada produced a considerable amount of particles that were transported north and northeast, respectively, and were detected at the Thule High Arctic Atmospheric Observatory (THAAO; 76.53 ∘ N, 68.74 ∘ W). Solar radiation measurements carried out at THAAO, satellite data, and modeled radiations allowed the estimation of surface cooling and the warming aloft at two atmospheric layers (at altitudes of approximately 5 and 11 km asl) due to the presence of the biomass-burning aerosol particles. Boreal fires have increased during the last years and are projected to become more intense and frequent as a consequence of climate change. Wildfires produce a wide range of effects on the Arctic climate and ecosystem, and understanding these effects is crucial for predicting the future evolution of the Arctic region. This study focuses on the impact of the long-range transport of biomass-burning aerosol into the atmosphere and the corresponding radiative perturbation in the shortwave frequency range. As a case study, we investigate an intense biomass-burning (BB) event which took place in summer 2017 in Canada and subsequent northeastward transport of gases and particles in the plume leading to exceptionally high values (0.86) of Aerosol Optical Depth (AOD) at 500 nm measured in northwestern Greenland on 21 August 2017. This work characterizes the BB plume measured at the Thule High Arctic Atmospheric Observatory (THAAO; 76.53 ∘ N, 68.74 ∘ W) in August 2017 by assessing the associated shortwave aerosol direct radiative impact over the THAAO and extending this evaluation over the broader region ( 60 ∘ N– 80 ∘ N, 110 ∘ W– 0 ∘ E). The radiative transfer simulations with MODTRAN6.0 estimated an aerosol heating rate of up to 0.5 K/day in the upper aerosol layer (8–12 km). The direct aerosol radiative effect (ARE) vertical profile shows a maximum negative value of −45.4 Wm − 2 for a 78 ∘ solar zenith angle above THAAO at 3 km altitude. A cumulative surface ARE of −127.5 TW is estimated to have occurred on 21 August 2017 over a portion (∼ 3.1 × 10 6 km 2 ) of the considered domain ( 60 ∘ N– 80 ∘ N, 110 ∘ W– 0 ∘ E). ARE regional mean daily values over the same portion of the domain vary between −65 and −25 Wm − 2 . Although this is a limited temporal event, this effect can have significant influence on the Arctic radiative budget, especially in the anticipated scenario of increasing wildfires. [ABSTRACT FROM AUTHOR]

Abstract: Continuous sea salt and mineral dust aerosol records have been studied on the two EPICA (European Project for Ice Coring in Antarctica) deep ice cores. The joint use of these records from opposite sides of the East Antarctic plateau allows for an estimate of changes in dust transport and emission intensity as well as for the identification of regional differences in the sea salt aerosol source. The mineral dust flux records at both sites show a strong coherency over the last 150 kyr related to dust emission changes in the glacial Patagonian dust source with three times higher dust fluxes in the Atlantic compared to the Indian Ocean sector of the Southern Ocean (SO). Using a simple conceptual transport model this indicates that transport can explain only 40% of the atmospheric dust concentration changes in Antarctica, while factor 5–10 changes occurred. Accordingly, the main cause for the strong glacial dust flux changes in Antarctica must lie in environmental changes in Patagonia. Dust emissions, hence environmental conditions in Patagonia, were very similar during the last two glacials and interglacials, respectively, despite 2–4 °C warmer temperatures recorded in Antarctica during the penultimate interglacial than today. 2–3 times higher sea salt fluxes found in both ice cores in the glacial compared to the Holocene are difficult to reconcile with a largely unchanged transport intensity and the distant open ocean source. The substantial glacial enhancements in sea salt aerosol fluxes can be readily explained assuming sea ice formation as the main sea salt aerosol source with a significantly larger expansion of (summer) sea ice in the Weddell Sea than in the Indian Ocean sector. During the penultimate interglacial, our sea salt records point to a 50% reduction of winter sea ice coverage compared to the Holocene both in the Indian and Atlantic Ocean sector of the SO. However, from 20 to 80 ka before present sea salt fluxes show only very subdued millennial changes despite pronounced temperature fluctuations, likely due to the large distance of the sea ice salt source to our drill sites. [Copyright &y& Elsevier]

Surface mass balance (SMB) distribution and its temporal and spatial variability is an essential input parameter in mass balance studies. Different methods were used, compared and integrated (stake farms, ice cores, snow radar, surface morphology, remote sensing) at eight sites along a transect from Terra Nova Bay (TNB) to Dome C (DC) (East Antarctica), to provide detailed information on the SMB. Spatial variability measurements show that the measured maximum snow accumulation (SA) in a 15 km area is well correlated to firn temperature. Wind-driven sublimation processes, controlled by the surface slope in the wind direction, have a huge impact (up to 85% of snow precipitation) on SMB and are significant in terms of past, present and future SMB evaluations. The snow redistribution process is local and has a strong impact on the annual variability of accumulation. The spatial variability of SMB at the kilometre scale is one order of magnitude higher than its temporal variability (20-30%) at the centennial time scale. This high spatial variability is due to wind-driven sublimation. Compared with our SMB calculations, previous compilations generally over-estimate SMB, up to 65% in some areas. [ABSTRACT FROM AUTHOR]

The results of a preliminary investigation of the dust sources in the Arctic based on their geochemical properties by potential source contribution function (PSCF) analysis are presented in this paper. For this purpose, we considered one year of aerosol geochemical data from Ny-Ålesund, Svalbard, and a short list of chemical elements (i.e., Al, Fe, Mn, Ti, Cr, V, Ni, Cu, and Zn) variably related to the dust fraction. Based on PSCF analysis: (i) four different dust source areas (i.e., Eurasia, Greenland, Arctic-Alaska, and Iceland) were characterized by distinguishing geochemical ranges and seasonal occurrence; and (ii) a series of typical dust days from the distinct source areas were identified based on the corresponding back trajectory patterns. Icelandic dust samples revealed peculiar but very variable characteristics in relation to their geographical source regions marked by air mass back trajectories. The comparison between pure and mixed Icelandic dust samples (i.e., aerosols containing Icelandic dust along with natural and/or anthropogenic components) revealed the occurrence of different mixing situations. Comparison with Icelandic soils proved the existence of dilution effects related to the emission and the transport processes. [ABSTRACT FROM AUTHOR]

In this work, we analysed aerosol measurements from lidar and PM 10 samples around the European Arctic site of Ny-Ålesund during late winter–early spring 2019. Lidar observations above 700 m revealed time-independent values for the aerosol backscatter coefficient (β), colour ratio (CR), linear particle depolarisation ratio (δ) and lidar ratio (LR) from January to April. In contrast to previous years, in 2019 the early springtime backscatter increase in the troposphere, linked to Arctic haze, was not observed. In situ nss-sulphate (nss-SO 4 2 − ) concentration was measured both at a coastal (Gruvebadet) and a mountain (Zeppelin) station, a few kilometres apart. As we employed different measurement techniques at sites embedded in complex orography, we investigated their agreement. From the lidar perspective, the aerosol load (indicated by β) above 700 m changed by less than a factor of 3.5. On the contrary, the daily nss-SO 4 2 − concentration erratically changed by a factor of 25 (from 0.1 to 2.5 ng m − 3 ) both at Gruvebadet and Zeppelin station, with the latter mostly lying above the boundary layer. Moreover, daily nss-SO 4 2 − concentration was remarkably variable (correlation about 0.7 between the sites), despite its long-range origin. However, on a seasonal average basis the in situ sites agreed very well. Therefore, it can be argued that nss-SO 4 2 − advection mainly takes place in the lowest free troposphere, while under complex orography it is mixed downwards by local boundary layer processes. Our study suggests that at Arctic sites with complex orography ground-based aerosol properties show higher temporal variability compared to the free troposphere. This implies that the comparison between remote sensing and in situ observations might be more reasonable on longer time scales, i.e., monthly and seasonal basis even for nearby sites. [ABSTRACT FROM AUTHOR]

An extensive field campaign was carried out in Florence (Tuscany) to investigate the PM2.5 composition and to identify its sources. The scientific objective of this study is providing a reliable source apportionment, which is mandatory for the application of effective mitigation actions. Particulate matter (PM) was collected for one year, simultaneously in a traffic site, in an urban background, and in a regional background site. While the use of two filter types (quartz and Teflon) allowed obtaining a comprehensive chemical characterization (elemental and organic carbon, ions, elements) by the application of different analytical techniques, the location of the three sampling sites allowed getting a better separation among local, urban, regional and transboundary sources. During shorter periods, the aerosol was also collected by means of a streaker sampler and PIXE (Particle Induced X-ray Emission) analysis of these samples allowed the assessment of hourly resolution elemental time trends. Positive matrix factorisation (PMF) identified seven main sources: traffic, biomass burning, secondary sulphate, secondary nitrates, urban dust, Saharan dust and marine aerosol. Traffic mass concentration contributions were found to be strong only at the traffic site (~8 μg·m−3, 33% of PM2.5). Biomass burning turned out to be an important PM2.5 source in Florence (~4 μg·m−3), with very similar weights in both city sites while at the regional background site its weight was negligible. Secondary sulphate is an important PM2.5 source on a regional scale, with comparable values in all three sites (~3.5 μg·m−3). On average, the contribution of the "natural" components (e.g., mineral dust and marine aerosols) to PM2.5 is moderate (~1 μg·m−3) except during Saharan dust intrusions where this contribution is higher (detected simultaneously in all three sites). High-time resolution data confirmed and reinforced these results. [ABSTRACT FROM AUTHOR]

During the summers of 2011 and 2012, two scientific cruises were carried out over the Arctic Ocean aiming at the determination of the aerosol chemical composition in this pristine environment. First, mass spectrometry was applied to study the concentration and gas/particle partitioning of polycyclic aromatic hydrocarbons (PAHs) and n-alkanes. Experimental and modelled data of phase partitioning were compared: results demonstrated an equilibrium between gas and particle phase for PAHs, while n-alkanes showed a particle-oriented partitioning, due to the local marine origin of them, confirmed by the extremely low value of their carbon preference index. Moreover, the inorganic and organic ions (carboxylic acids and amines) concentrations, together with those of elemental carbon (EC) and organic matter (OM), were analyzed: 63% of aerosol was composed of ionic compounds (>90% from sea-salt) and the OM content was very high (30.5%; close to 29.0% of Cl−) in agreement with n-alkanes' marine signature. Furthermore, the amines' (dimethylamine, trimethylamine, diethylamine) concentrations were 3.98 ± 1.21, 1.70 ± 0.82, and 1.06 ± 0.56 p.p.t.v., respectively, fully in keeping with concentration values used in the CLOUD (Cosmics Leaving OUtdoor Droplet)-chamber experiments to simulate the ambient nucleation rate in a H2SO4-DMA-H2O system, showing the amines' importance in polar regions to promote new particle formation. Finally, high resolution mass spectrometry was applied to determine trace elements, including Rare Earth Elements (REEs), highlighting the dominant natural versus anthropic inputs for trace metals (e.g., Fe, Mn, Ti vs. As, Cd, Ni) and possible signatures of such anthropic activity. [ABSTRACT FROM AUTHOR]