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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.

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 (∼3.1×106 km2) 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.

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.

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.

In this work, we analysed aerosol measurements from lidar and PM10 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 (ββ), colour ratio (CR), linear particle depolarisation ratio (δδ) 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-SO42−) 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 ββ) above 700 m changed by less than a factor of 3.5. On the contrary, the daily nss-SO42− 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-SO42− 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-SO42− 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.

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.

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.

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.

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.

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.

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.