Search

The study of aerosol chemical composition in the Antarctic plateau can provide basic information on the main natural (and also anthropogenic) inputs, atmospheric reactivity, and long-range transport processes of the aerosol components. Moreover, chemical and physical processes occurring at the atmosphere-snow interface are yet not fully understood and work is needed to assess the impact of atmospheric chemistry on snow composition and to better interpret ice core records retrieved at those sites.At this purpose, simultaneous aerosol and surface snow samplings were set up and run at Dome C station (75° 06’ S; 123° 20’ E, 3233 m a.s.l) all year-round since 2004/05 and are still ongoing through various PNRA Projects, particularly LTCPAA (2016-2020) and STEAR (2020-2023).Aerosol and snow samples were analysed for main and trace ion markers, aiming to better constrain extent and timing of the main natural sources (sea salt, marine biogenic, mineral dust) and to detect the possible contribution of anthropic inputs (biomass burning, wildfires, local contamination). In addition, such a study might help in improving our knowledge of transport processes (free troposphere, stratosphere-troposphere exchange) and atmospheric reaction processes (such as neutralization, chemical fractionation).A comparison with ozone measurements, carried out continuously over the same period, is also attempted, to better address the atmospheric processes involving the atmosphere-snow exchanges of N-cycle species and atmosphere oxidative properties.

The water isotope composition of snow precipitations, archived in the Antarctic ice sheet every year, is an important proxy of climatic conditions. This signal depends on several parameters such as local temperature, altitude, moisture source areas and air mass pathways.However, especially in areas where snow accumulation is very low (as on the East Antarctic Plateau), the isotopic composition is affected by additional spatial variability induced by the interactions between the atmosphere and snow surface, and the pristine signal may be modified through isotopic exchanges, sublimation processes and mechanical mixing originated from wind action.Here, we present the isotopic composition (δD and δ18O) and the second-order parameter d-excess of surface snow and snowpit samples collected during the Italian-French campaign in Antarctica (2019-2020). The sampling sites cover the area from Dumont D'Urville to Concordia Station and from Concordia Station towards the South Pole (EAIIST – East Antarctic International Ice Sheet Traverse). These data, compared with a previous dataset of Antarctic surface snow isotopic composition (Masson-Delmotte et al. 2008), are analyzed to determine the variability of the spatial relationship between precipitation isotopic composition and local temperature in relation to geographical parameters (latitude, distance from the coast and elevation). The interpretation of these factors determining the isotope signature is the base to better define the amount of the effects caused by subsequent interaction between atmosphere and surface snow, and by the wind action.Understanding the spatial variability of this proxy, which strongly decreases the signal-to-noise ratio, could permit to improve the use of the “isotopic thermometer” to quantify past changes in temperature based on the stable isotopic record of deep ice cores.

As part of the “East Antarctic International Ice Sheet Traverse” (EAIIST) project, surface snow and snow pit samples were collected along a traverse from Dome C toward the geographic South Pole during the 2019–2020 Antarctic campaign. Results on spatial distribution of major ions are here reported to understand deposition and post deposition processes in sites with very low snow accumulation rate in the East Antarctic Plateau where megadune and wind crust areas are present. The volcanic signature of Pinatubo eruption (occurred in 1991) was clearly visible in the non-sea salt SO42− stratigraphy from two snow pits (AGO-5 and PALEO) allowing the determination of annual accumulation rates that revealed to be 25.7 and 22.6 mm of water equivalent/year, respectively at the two sites. Moreover, a decreasing trend in accumulation rate as the distance from the Indian Ocean increases was detected. Mineral dust concentration and size show presence of a criptotephra layer in AGO5 and PALEO stratigraphies which is stratigraphically compatible with the deposition of volcanic ash related to the Puyehue-Cordón Caulle explosive eruption occurred in June 2011. The ssNa+ fraction, accounting for the 92.5 % of the total Na+, is preserved stably in the snow layers and was chosen as marker of sea spray deposition. Despite the very low accumulation rate in this area, the main deposition process of sea spray aerosol is the wet deposition. Conversely, both biogenic and crustal nssSO42− are dry deposited, the total flux of nssSO42− resulted to be constant in the Antarctic plateau, but the biogenic to crustal ratio increases as distance from Dome C increases. The presence and quantification (by nssCa2+) of a dry deposited crustal source, as the biogenic one, sheds light on the interpretation of nssSO42− biogenic stratigraphy during glacial and interglacial time in Antarctic ice cores. NssCl− represent the fraction of Cl− deposited as HCl and arises from the exchange reactions between chloride in the sea salt aerosol and acidic species such as H2SO4 and HNO3 that occurs both into the atmosphere (in this case HCl is deposited by wet deposition) and into the snow (at the expenses of NaCl or MgCl2 deposited as sea salt aerosol). The latter process could be particularly efficient in sites affected by wind crust formation, probably because of a longer exposure time of the snow layers to the atmosphere favouring the HCl volatilization . Another important marker in ice core is HNO3, that in the considered sites is found at very high concentration in the most superficial 3 cm of snow due to the uptake by superficial snow and possibly concentration effects from the layers beneath, but it is reversibly deposited. The depth of the active layer for HNO3 reemission was calculated and it spans from 22 cm to 12 cm; in addition, the concentration preserved in the snow decreases as the accumulation rate decreases, but wind scouring increases the efficiency of re-emission processes in the active layer. The knowledge and quantification of all the above reported processes will allow the interpretation of the ice core stratigraphies in low accumulation site likely hopefully recording, at selected sites, the climate history of more than one million years ago.

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.

In this study, we modeled the aerosol particle formation along air mass trajectories arriving at the remote Arctic research stations Gruvebadet (67 m a.s.l.) and Zeppelin (474 m a.s.l.), Ny-Ålesund, during May 2018. The aim of this study was to improve our understanding of processes governing secondary aerosol formation in remote Arctic marine environments. We run the Lagrangian chemistry transport model ADCHEM, along air mass trajectories generated with FLEXPART v10.4. The air masses arriving at Ny-Ålesund spent most of their time over the open ice-free ocean. In order to capture the secondary aerosol formation from the DMS emitted by phytoplankton from the ocean surface, we implemented a recently developed comprehensive DMS and halogen multi-phase oxidation chemistry scheme, coupled with the widely used Master Chemical Mechanism (MCM). The modeled median particle number size distributions are in close agreement with the observations in the marine-influenced boundary layer near-sea-surface Gruvebadet site. However, while the model reproduces the accumulation mode particle number concentrations at Zeppelin, it overestimates the Aitken mode particle number concentrations by a factor of ∼5.5. We attribute this to the deficiency of the model to capture the complex orographic effects on the boundary layer dynamics at Ny-Ålesund. However, the model reproduces the average vertical particle number concentration profiles within the boundary layer (0–600 m a.s.l.) above Gruvebadet, as measured with condensation particle counters (CPCs) on board an unmanned aircraft system (UAS). The model successfully reproduces the observed Hoppel minima, often seen in particle number size distributions at Ny-Ålesund. The model also supports the previous experimental findings that ion-mediated H2SO4–NH3 nucleation can explain the observed new particle formation in the marine Arctic boundary layer in the vicinity of Ny-Ålesund. Precursors resulting from gas- and aqueous-phase DMS chemistry contribute to the subsequent growth of the secondary aerosols. The growth of particles is primarily driven via H2SO4 condensation and formation of methane sulfonic acid (MSA) through the aqueous-phase ozonolysis of methane sulfinic acid (MSIA) in cloud and deliquescent droplets.

To control the spread of COVID-19, exceptional restrictive measures were taken in March 2020 that imposed a radical change on the lifestyle of millions of citizens around the world, albeit for a short period. The national lockdown, which lasted from 10 March to 18 May 2020 in Italy, was a unique opportunity to observe the variation in air quality in urban environments under conditions comprising almost total traffic restriction and a strong reduction in work activities. In this paper, the data from 17 urban monitoring sites in Tuscany are presented, and the PM and NO2 concentrations in the 2 months before the start of the lockdown and the 2 months after lockdown are compared with the corresponding months of the previous 3 years. The results show that the total loads of PM2.5 and PM10 (particulate matter with an aerodynamic diameter smaller than 2.5 and 10 µm, respectively) decreased, but they did not exhibit significant changes compared to previous years, whereas NO2 underwent a drastic reduction. For three of these sites, the chemical composition of the collected samples was measured using thermal–optical techniques, ion chromatography, and particle-induced X-ray emission analysis, and the application of multivariate positive matrix factorization analysis also allowed for PM10 source identification and apportionment. Using these analyses, it was possible to explain the low sensitivity of PM10 to the lockdown effects as being due to different, sometimes inverse, behaviors of the different sources that contribute to PM. The results clearly indicate a decline in pollution levels related to urban traffic and an increase in the concentration of sulfate for all sites during the lockdown period.

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 the inland ice sheet were warmest at the lowest frequencies consistent with models that predict that those channels sensed the deeper, warmer parts of the ice sheet. 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.

Gruvebadet Observatory at Ny-Ålesund (Svalbard Islands) has been recognized as a valuable facility for long-term studies of atmospheric chemistry in the High Arctic, with particular attention to natural and anthropic aerosol sources and transport processes by using chemical tracers.A long-term study of the chemical composition of PM10 aerosol is being accomplished at Gruvebadet Observatory since 2010 by continuous collection at high resolution (1 to 2 days) and chemical analysis of major and trace ions and elements.The contribution of different sources (sea spray, crustal, biogenic and anthropogenic) to the total sulphate budget was estimated by using specific markers (namely sodium, calcium and methanesulphonate) and their characteristic marker-to-sulphate ratios in sea water, mineral dust and marine biogenic source. The obtained data set was also compared with the one derived from the Zeppelin Observatory, also located in Ny-Ålesund.The anthropogenic fraction resulted to be the dominant 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 although some differences in extent were observed, probably due to discrepancies in the timing and resolution of sampling campaigns as well as to different analytical procedures.The temporal profile of the anthropogenic fraction, evaluated in both sites, showed no evident continuous trend from 2010 to 2019, even though higher concentrations were observed in the 2017-19 period, 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, eventually causing a decrease in aerosol acidity, was observed at Gruvebadet, from the 2010 to 2017, to reach fairly constant values later. Instead, a decrease in ammonia concentration was found at Zeppelin since 2015, leading to an increase of the non sea salt sulphate/ammonium ratio in the same period.

In this study, we modeled the aerosol particle formation along air mass trajectories arriving at the remote Arctic research stations Gruvebadet (67 m a.s.l) and Zeppelin (474 m a.s.l), Ny-Ålesund during May 2018. The aim of this study was to improve our understanding of processes governing secondary aerosol formation in remote Arctic marine environments. We run the Lagrangian chemistry transport model ADCHEM, along air mass trajectories generated with FLEXPART v10.4. The air masses arriving at Ny-Ålesund spend most of their time over the open ice-free ocean. In order to capture the secondary aerosol formation from the DMS emitted by phytoplankton on the ocean surface, we implemented a recently developed comprehensive DMS and halogen multi-phase oxidation chemistry scheme, coupled with the widely used Master Chemical Mechanism (MCM). The modeled median particle number size distributions are in close agreement with the observations in the marine influenced boundary layer at near sea surface Gruvebadet site. However, while the model reproduces the accumulation mode particle number concentrations at Zeppelin, it overestimates the Aitken mode particle number concentrations by a factor of ~5.5. We attribute this to the deficiency of the model to capture the complex orographic effects on the boundary layer dynamics at Ny-Ålesund. The model also reproduces the average vertical particle number concentration profiles within the boundary layer (0–600 m a.s.l.) above Gruvebadet, as measured with Condensation Particle Counters (CPCs) on board an Unmanned Aircraft Systems (UAS). The model successfully reproduces the observed Hoppel minima, often seen in particle number size distributions at Ny-Ålesund. The model also supports the previous experimental findings that ion mediated H2SO4-NH3 nucleation can explain the observed new particle formation in the marine Arctic boundary layer in the vicinity of Ny-Ålesund. Precursors resulting from gas and aqueous phase DMS chemistry contribute to the subsequent growth of the secondary aerosols. The growth of particles is primarily driven via H2SO4 condensation and formation of methane sulfonic acid (MSA) through the aqueous-phase ozonolysis of methane sulfinic acid (MSIA) in cloud and deliquescent droplets.

This paper presents the results on simultaneous high time resolution measurements of biogenic aerosol (methane sulfonic acid-MSA, non-sea salt sulfate nssSO42-) with its gaseous precursor dimethylsulfide (DMS) performed at the Italian coastal base Mario Zucchelli Station (MZS) in Terra Nova Bay (MZS) during two summer campaigns (2018–2019 and 2019–2020). The study provides information on marine biological activity in the nearby polynya in the Ross Sea and on the influence of biogenic and atmospheric processes on biogenic aerosol formation. Data on atmospheric DMS concentration are scarce especially in Antarctica. The DMS-maximum at MZS occurs in December, one month earlier than at other Antarctic stations. The maximum of DMS concentration is connected with the phytoplanktonic senescent phase following the bloom of Phaeocystis antarctica that occurs in the polynya when sea ice opens up. The second plankton bloom occurs in January and, despite the high Dimethylsulfopropionate (DMSP) concentration in sea water, atmospheric DMS remains low probably due to its fast biological turnover in sea water in this period. The intensity and timing of the DMS evolution during the two years suggests that only the portion of the polynya close to the sampling site produces a discernible effect on the measured DMS. The closeness to the DMS source area, and the occurrence of air masses containing DMS and freshly formed oxidation products allow to study the kinetic of biogenic aerosol formation and the reliable derivation of the branch ratio between MSA and nssSO42- from DMS oxidation that is estimated to be 0.84 ± 0.06. Conversely, for aged airmasses with low DMS content, an enrichment of nssSO42- with respect to MSA, due to the presence of background concentration of nssSO42- from volcanic origin (Erebus) or from long range transport, takes place. Therefore, the aged air mass presents an MSA / nssSO42- ratio lower than in newly formed biogenic aerosol. By considering the sum of MSA and biogenic nssSO42-, we estimate that the mean contribution of biogenic particulate matter to PM10 is 17 %, with a maximum of 56 %. The high contribution of biogenic aerosol to the total PM10 mass in summer in this area highlights the dominant role of the polynya on biogenic aerosol formation. Finally, due to the regional and year-to year variability of DMS and related biogenic aerosol formation, we stress the need of long-term measurements of atmospheric DMS and biogenic aerosol along the Antarctic coast and in the Southern Ocean.

We examined the relationships linking atmospheric in-situ data of gas phase methane sulfonic acid (CH3SO3H, MSA), sulfuric acid (H2SO4, SA), iodic acid (HIO3), highly oxidized organic molecules (HOM) and aerosol particle concentrations in the size ranges of 10‒50 nm and 100‒450 nm with satellite-derived chlorophyll a (Chl-a) and oceanic primary production (PP) during two time spans – the phytoplankton early bloom period, April‒May 2017 (30 March‒1 June, springtime) and phytoplankton late bloom; June‒July 2017 (2 June‒4 August, summertime) – in two ocean domains; Greenland Sea and Barents Sea. Atmospheric data were collected at Ny-Ålesund site in Svalbard, Norway. In general, Chl-a and PP in the Barents Sea were higher than in the Greenland Sea during the April‒May period, whereas the Greenland Sea had higher Chl-a and PP during June‒July. Phytoplankton bloom started by the loss of sea ice coverage in the Barents Sea at the marginal ice zone (MIZ) during April‒May, and in the Greenland Sea close to Svalbard Island during June‒July. From the April‒May period to the June‒July period, the correlation between the ocean color data (Chl-a and PP) and MSA decreased in the Barents Sea and increased in the Greenland Sea, which establishes a direct relationship between the sea ice melting, phytoplankton bloom and atmospheric vapour composition. Both MSA and SA concentrations increased strongly during the bloom period, suggesting marine phytoplankton metabolism and resulting dimethyl sulphide (DMS) as the primary source of both MSA and SA in the Arctic atmosphere during spring–summer time. The highest correlation among all the atmospheric components and ocean color properties was observed between HIO3 and Chl-a in both ocean domains during the springtime, but this feature may be connected to processes associated with the melting of sea ice. HOMs showed a low correlation with Chl-a and PP in comparison to other atmospheric vapours. The plausible explanation for such low correlation is that the primary source of volatile organic compounds (VOC) – precursors of HOM – is the soil or terrestrial vegetation of Svalbard archipelago rather than the ocean. In springtime, small-particles (10‒50 nm) correlated strongly with Chl-a in the Barents Sea and with PP in both oceanic domains, suggesting that biogenic productivity has a strong impact on new particle formation (NPF) in the springtime. In the summertime, small-particle concentrations showed almost no correlation with biogenic parameters, indicating that compounds not connected with phytoplankton metabolism, such as HOMs, have a critical role in summertime NPF. Larger particles (100‒450 nm) showed an anti-correlation with Chl-a and PP in springtime, probably due to dilution of anthropogenic air pollution (arctic haze) during spring. In the end of the Arctic haze period in April, particle-phase SA (non-sea-salt sulphate, nss-SO4-2) and particle phase MSA (MS-) showed almost no correlation, whereas a connection between the gas phase MSA and SA concentrations was found. The likely reason for this is the same origin for gas phase MSA and SA (DMS oxidation), whereas SA in particle phase mostly originated from a long-distance continental source.

While carbon dioxide is the main cause for global warming, modeling short-lived climate forcers (SLCFs) such as methane, ozone, and particles in the Arctic allows us to simulate near-term climate and health impacts for a sensitive, pristine region that is warming at 3 times the global rate. Atmospheric modeling is critical for understanding the long-range transport of pollutants to the Arctic, as well as the abundance and distribution of SLCFs throughout the Arctic atmosphere. Modeling is also used as a tool to determine SLCF impacts on climate and health in the present and in future emissions scenarios. In this study, we evaluate 18 state-of-the-art atmospheric and Earth system models by assessing their representation of Arctic and Northern Hemisphere atmospheric SLCF distributions, considering a wide range of different chemical species (methane, tropospheric ozone and its precursors, black carbon, sulfate, organic aerosol, and particulate matter) and multiple observational datasets. Model simulations over 4 years (2008–2009 and 2014–2015) conducted for the 2022 Arctic Monitoring and Assessment Programme (AMAP) SLCF assessment report are thoroughly evaluated against satellite, ground, ship, and aircraft-based observations. The annual means, seasonal cycles, and 3-D distributions of SLCFs were evaluated using several metrics, such as absolute and percent model biases and correlation coefficients. The results show a large range in model performance, with no one particular model or model type performing well for all regions and all SLCF species. The multi-model mean (mmm) was able to represent the general features of SLCFs in the Arctic and had the best overall performance. For the SLCFs with the greatest radiative impact (CH4, O3, BC, and SO), the mmm was within ±25 % of the measurements across the Northern Hemisphere. Therefore, we recommend a multi-model ensemble be used for simulating climate and health impacts of SLCFs. Of the SLCFs in our study, model biases were smallest for CH4 and greatest for OA. For most SLCFs, model biases skewed from positive to negative with increasing latitude. Our analysis suggests that vertical mixing, long-range transport, deposition, and wildfires remain highly uncertain processes. These processes need better representation within atmospheric models to improve their simulation of SLCFs in the Arctic environment. As model development proceeds in these areas, we highly recommend that the vertical and 3-D distribution of SLCFs be evaluated, as that information is critical to improving the uncertain processes in models. Assessments from the Russian ship-based campaign were performed with the support of RFBR project no. 20-55-12001 and according to the development program of the Interdisciplinary Scientific and Educational School of M.V. Lomonosov Moscow State University “Future Planet and Global Environmental Change”. Development of the methodology for aethalometric data treatment was supported by RSF project no. 19-77-30004. The BC observations on R/V Mirai were supported by the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan (Arctic Challenge for Sustainability (ArCS) project). Contributions by SMHI were funded by the Swedish Environmental Protection Agency under contract NV-03174-20 and the Swedish Climate and Clean Air Research program (SCAC) as well as partly by the Swedish National Space Board (NORD-SLCP, grant agreement ID: 94/16) and the EU Horizon 2020 project Integrated Arctic Observing System (INTAROS, grant agreement ID: 727890). Work on ACE-FTS analysis was supported by the Natural Sciences and Engineering Research Council of Canada (NSERC). Julia Schmale received funding from the Swiss National Science Foundation (project no. 200021_188478). Duncan Watson-Parris received funding from NERC projects NE/P013406/1 (A-CURE) and NE/S005390/1 (ACRUISE) as well as funding from the European Union's Horizon 2020 research and innovation program iMIRACLI under Marie Skłodowska-Curie grant agreement no. 860100. LATMOS has been supported by the EU iCUPE (Integrating and Comprehensive Understanding on Polar Environments) project (grant agreement no. 689443) under the European Network for Observing our Changing Planet (ERA-Planet), as well as access to IDRIS HPC resources (GENCI allocation A009017141) and the IPSL mesoscale computing center (CICLAD: Calcul Intensif pour le CLimat, l’Atmosphère et la Dynamique) for model simulations. Naga Oshima was supported by the Japan Society for the Promotion of Science KAKENHI (grant nos. JP18H03363, JP18H05292, and JP21H03582), the Environment Research and Technology Development Fund (grant nos. JPMEERF20202003 and JPMEERF20205001) of the Environmental Restoration and Conservation Agency of Japan, the Arctic Challenge for Sustainability II (ArCS II) under program grant no. JPMXD1420318865, and a grant for the Global Environmental Research Coordination System from the Ministry of the Environment, Japan (MLIT1753). The research with GISS-E2.1 has been supported by the Aarhus University Interdisciplinary Centre for Climate Change (iClimate) OH fund (no. 2020-0162731), the FREYA project funded by the Nordic Council of Ministers (grant agreement nos. MST-227-00036 and MFVM-2019-13476), and the EVAM-SLCF funded by the Danish Environmental Agency (grant agreement no. MST-112-00298). Jesper Christensen (for DEHM model) received funding from the Danish Environmental Protection Agency (DANCEA funds for Environmental Support to the Arctic Region project; grant no. 2019-7975). Maria Sand has been supported by the Research Council of Norway (grant 315195, ACCEPT). Peer Reviewed "Article signat per més de 50 autors/es: Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons "

Optical properties of surface aerosols at Dome C, Antarctica, in 2007–2013 and their potential source areas are presented. Scattering coefficients (σsp) were calculated from measured particle number size distributions with a Mie code and from filter samples using mass scattering efficiencies. Absorption coefficients (σap) were determined with a three-wavelength Particle Soot Absorption Photometer (PSAP) and corrected for scattering by using two different algorithms. The scattering coefficients were also compared with σsp measured with a nephelometer at the South Pole Station (SPO). The minimum σap was observed in the austral autumn and the maximum in the austral spring, similar to other Antarctic sites. The darkest aerosol, i.e., the lowest single-scattering albedo ωo≈0.91, was observed in September and October and the highest ωo≈0.99 in February and March. The uncertainty of the absorption Ångström exponent αap is high. The lowest αap monthly medians were observed in March and the highest in August–October. The equivalent black carbon (eBC) mass concentrations were compared with eBC measured at three other Antarctic sites: the SPO and two coastal sites, Neumayer and Syowa. The maximum monthly median eBC concentrations are almost the same (∼3±1 ng m−3) at all these sites in October–November. This suggests that there is no significant difference in eBC concentrations between the coastal and plateau sites. The seasonal cycle of the eBC mass fraction exhibits a minimum f(eBC) ≈0.1 % in February–March and a maximum ∼4 %–5 % in August–October. Source areas were calculated using 50 d FLEXPART footprints. The highest eBC concentrations and the lowest ωo were associated with air masses coming from South America, Australia and Africa. Vertical simulations that take BC particle removal processes into account show that there would be essentially no BC particles arriving at Dome C from north of latitude 10∘ S at altitudes m. The main biomass-burning regions Africa, Australia and Brazil are more to the south, and their smoke plumes have been observed at higher altitudes than that, so they can get transported to Antarctica. The seasonal cycle of BC emissions from wildfires and agricultural burning and other fires in South America, Africa and Australia was calculated from data downloaded from the Global Fire Emissions Database (GFED). The maximum total emissions were in August–September, but the peak of monthly average eBC concentrations is observed 2–3 months later in November, not only at Dome C, but also at the SPO and the coastal stations. The air-mass residence-time-weighted BC emissions from South America are approximately an order of magnitude larger than from Africa and Oceania, suggesting that South American BC emissions are the largest contributors to eBC at Dome C. At Dome C the maximum and minimum scattering coefficients were observed in austral summer and winter, respectively. At the SPO σsp was similar to that observed at Dome C in the austral summer, but there was a large difference in winter, suggesting that in winter the SPO is more influenced by sea-spray emissions than Dome C. The seasonal cycles of σsp at Dome C and at the SPO were compared with the seasonal cycles of secondary and primary marine aerosol emissions. The σsp measured at the SPO correlated much better with the sea-spray aerosol emission fluxes in the Southern Ocean than σsp at Dome C. The seasonal cycles of biogenic secondary aerosols were estimated from monthly average phytoplankton biomass concentrations obtained from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite sensor data. The analysis suggests that a large fraction of the biogenic scattering aerosol observed at Dome C has been formed in the polar zone, but it may take a month for the aerosol to be formed, be grown and get transported from the sea level to Dome C.

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.

10 pages, 3 figures, 1 table, supporting information https://doi.org/10.1021/acs.est.1c07796, Atmospheric aerosols are important drivers of Arctic climate change through aerosol–cloud–climate interactions. However, large uncertainties remain on the sources and processes controlling particle numbers in both fine and coarse modes. Here, we applied a receptor model and an explainable machine learning technique to understand the sources and drivers of particle numbers from 10 nm to 20 μm in Svalbard. Nucleation, biogenic, secondary, anthropogenic, mineral dust, sea salt and blowing snow aerosols and their major environmental drivers were identified. Our results show that the monthly variations in particles are highly size/source dependent and regulated by meteorology. Secondary and nucleation aerosols are the largest contributors to potential cloud condensation nuclei (CCN, particle number with a diameter larger than 40 nm as a proxy) in the Arctic. Nonlinear responses to temperature were found for biogenic, local dust particles and potential CCN, highlighting the importance of melting sea ice and snow. These results indicate that the aerosol factors will respond to rapid Arctic warming differently and in a nonlinear fashion, This research was supported by the Natural Environment Research Council (grant no. NE/S00579X/1) and endorsed by the Surface Ocean-Lower Atmosphere Study (SOLAS), With the institutional support of the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000928-S)

The Arctic atmosphere is warming rapidly and its relatively pristine environment is sensitive to the long-range transport of atmospheric pollutants. While carbon dioxide is the main cause for global warming, short-lived climate forcers (SLCFs) such as methane, ozone, and particles also play a role in Arctic climate on near-term time scales. Atmospheric modelling is critical for understanding the abundance and distribution of SLCFs throughout the Arctic atmosphere, and is used as a tool towards determining SLCF impacts on climate and health in the present and in future emissions scenarios. In this study, we evaluate 18 state-of-the-art atmospheric and Earth system models, assessing their representation of Arctic and Northern Hemisphere atmospheric SLCF distributions, considering a wide range of different chemical species (methane, tropospheric ozone and its precursors, black carbon, sulfate, organic aerosol, and particulate matter) and multiple observational datasets. Model simulations over four years (2008–2009 and 2014–2015) conducted for the 2021 Arctic Monitoring and Assessment Programme (AMAP) SLCF assessment report are thoroughly evaluated against satellite, ground, ship and aircraft-based observations. The results show a large range in model performance, with no one particular model or model type performing well for all regions and all SLCF species. The multi-model mean was able to represent the general features of SLCFs in the Arctic, though vertical mixing, long-range transport, deposition, and wildfire emissions remain highly uncertain processes. These need better representation within atmospheric models to improve their simulation of SLCFs in the Arctic environment.

Organic aerosols in the Arctic are predominantly fuelled by anthropogenic sources in winter and natural sources in summer, according to observations from eight sites across the Arctic Aerosols play an important yet uncertain role in modulating the radiation balance of the sensitive Arctic atmosphere. Organic aerosol is one of the most abundant, yet least understood, fractions of the Arctic aerosol mass. Here we use data from eight observatories that represent the entire Arctic to reveal the annual cycles in anthropogenic and biogenic sources of organic aerosol. We show that during winter, the organic aerosol in the Arctic is dominated by anthropogenic emissions, mainly from Eurasia, which consist of both direct combustion emissions and long-range transported, aged pollution. In summer, the decreasing anthropogenic pollution is replaced by natural emissions. These include marine secondary, biogenic secondary and primary biological emissions, which have the potential to be important to Arctic climate by modifying the cloud condensation nuclei properties and acting as ice-nucleating particles. Their source strength or atmospheric processing is sensitive to nutrient availability, solar radiation, temperature and snow cover. Our results provide a comprehensive understanding of the current pan-Arctic organic aerosol, which can be used to support modelling efforts that aim to quantify the climate impacts of emissions in this sensitive region.

To control the spread of COVID-19, in March 2020 exceptional restrictive measures were taken imposing a radical change in the lifestyle of millions of citizens around the world, albeit for a short period of time. The national lockdown, which in Italy lasted from 10 March to 18 May 2020, was a unique opportunity to observe the variation in air quality in urban environments in a condition of almost total traffic block and a strong reduction in work activities. In this paper, the data from seventeen urban monitoring sites in Tuscany are presented by comparing PM and NO2 of the two months before the start of the lockdown and the two after with the corresponding months of the previous three years. The results show that the total load of PM2.5 and PM10 decreased but it did not exhibit significant changes compared to previous years, while NO2 undergoes a drastic reduction. For three of these sites, the chemical composition of the collected samples was measured by thermo-optical, ion chromatography and PIXE analysis, and the application of multivariate PMF analysis allowed the PM10 source identification and apportionment. Thanks to these analyses it was possible to explain the low sensitiveness of PM10 to the lockdown effects as due to different, sometimes opposite, behaviors of the different sources that contribute to PM. The results clearly indicated a decline in pollution levels related to urban traffic and an increase in the concentration of sulfate for all sites during the lockdown period.

19 pages, 9 figures, 1 table, Aerosols are an integral part of the Arctic climate system due to their direct interaction with radiation and indirect interaction through cloud formation. Understanding aerosol size distributions and their dynamics is crucial for the ability to predict these climate relevant effects. When of favourable size and composition, both long-rangetransported-and locally formed particles-may serve as cloud condensation nuclei (CCN). Small changes of composition or size may have a large impact on the low CCN concentrations currently characteristic of the Arctic environment. We present a cluster analysis of particle size distributions (PSDs; size range 8-500 nm) simultaneously collected from three high Arctic sites during a 3-year period (2013-2015). Two sites are located in the Svalbard archipelago: Zeppelin research station (ZEP; 474 m above ground) and the nearby Gruvebadet Observatory (GRU; about 2 km distance from Zeppelin, 67 m above ground). The third site (Villum Research Station at Station Nord, VRS; 30 m above ground) is 600 km west-northwest of Zeppelin, at the tip of northeastern Greenland. The GRU site is included in an inter-site comparison for the first time. K-means cluster analysis provided eight specific aerosol categories, further combined into broad PSD classes with similar characteristics, namely pristine low concentrations (12 %-14 % occurrence), new particle formation (16 %-32 %), Aitken (21 %-35 %) and accumulation (20 %-50 %). Confined for longer time periods by consolidated pack sea ice regions, the Greenland site GRU shows PSDs with lower ultrafine-mode aerosol concentrations during summer but higher accumulation-mode aerosol concentrations during winter, relative to the Svalbard sites. By association with chemical composition and cloud condensation nuclei properties, further conclusions can be derived. Three distinct types of accumulation-mode aerosol are observed during winter months. These are associated with sea spray (largest detectable sizes, > 400 nm), Arctic haze (main mode at 150 nm) and aged accumulation-mode (main mode at 220 nm) aerosols. In contrast, locally produced particles, most likely of marine biogenic origin, exhibit size distributions dominated by the nucleation and Aitken mode during summer months. The obtained data and analysis point towards future studies, including apportioning the relative contribution of primary and secondary aerosol formation pro cesses and elucidating anthropogenic aerosol dynamics and transport and removal processes across the Greenland Sea. In order to address important research questions in the Arctic on scales beyond a singular station or measurement events, it is imperative to continue strengthening international scientific cooperation, This research has been supported by the Spanish Ministry of Economy through project BIO-NUC (CGL2013-49020-R), PI-ICE (CTM2017-89117-R) and the Ramon y Cajal fellowship (RYC-2012-11922). The research leading to these results has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement no. 654109, the Danish Council for Independent Research (project NUMEN, DFF-FTP-4005-00485B) and previously from the European Union Seventh Framework Programme (FP7/2007-2013) under grant agreement no. 262254. The work at Villum Research Station, Station Nord, was financially supported by the Danish Environmental Protection Agency via the MIKA/DANCEA funds for Environmental Support to the Arctic Region. The Villum Foundation funded the construction of Villum Research Station, Station Nord. CCN measurements are supported by a KOPRI program (PN19081), funded by a National Research Foundation of Korea grant (NRF-2016M1A5A1901769). The authors acknowledge financial support (to David C. S. Beddows) from the Natural Environment Research Council's funding of the National Centre for Atmospheric Science (NCAS) (grant number R8/H12/83/011)

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 particulate matter (PM) source apportionment study was carried out in one of the most polluted districts of Tuscany (Italy), close to an old waste incinerator plant. Due to the high PM10 levels, an extensive field campaign was supported by the Regional Government to identify the main PM sources and quantify their contributions. PM10 daily samples were collected for one year and analysed by different techniques to obtain a complete chemical characterisation (elements, ions and carbon fractions). Hourly fine (2.5 μm) and coarse (2.5-10 μm) aerosol samples were collected by a Streaker sampler for a shorter period and hourly elemental concentrations were obtained by PIXE. Positive Matrix Factorization (PMF) analysis of daily and hourly data allowed the identification of 10 main sources: six anthropogenic (Biomass Burning, Traffic, Secondary Nitrates, Secondary Sulphates, Incinerator, Heavy Oil combustion), two natural (Saharan Dust and Fresh Sea Salt) and two mixed sources (Local Dust and Aged Sea Salt). Biomass burning turned out to be the main source of PM, accounting for 30% of the PM10 mass as annual average, followed by Traffic (18%) and Secondary Nitrates (14%). Emissions from the Incinerator turned out to be only 2% of PM10 mass on average. PM10 composition and source apportionment have been assessed in a polluted area near a waste incinerator, by PMF analysis on daily and hourly compositional data sets.

Optical properties of surface aerosols at Dome C, Antarctica in 2007–2013 and their potential source areas are presented. Scattering coefficients (σsp) were calculated from measured particle number size distributions with a Mie code and from filter samples using mass scattering efficiencies. Absorption coefficients (σap) were determined with a 3-wavelength Particle Soot Absorption Photometer (PSAP) and corrected for scattering by using two different algorithms. The scattering coefficients were also compared with σsp measured with a nephelometer at the South Pole Station (SPO). The minimum σap was observed in the austral autumn and the maximum in the austral spring, similar to other Antarctic sites. The darkest aerosol, i.e., the lowest single scattering albedo ωo ≈ 0.91 was observed in September and October and the highest ωo ≈ 0.99 in February and March. The uncertainty of the absorption Ångström exponent αap is high. The lowest αap monthly medians were observed in March and the highest in August–October. The equivalent black carbon (eBC) mass concentrations were compared with eBC measured at three other Antarctic sites: the SPO and two coastal sites, Neumayer and Syowa. The maximum monthly median eBC concentrations are almost the same (≈ 3 ± 1 ng m−3) at all these sites in October–November. This suggests that there is no significant difference in eBC between the coastal and plateau sites. The seasonal cycle of the eBC mass fraction exhibits a minimum f(eBC) ≈ 0.1 % in February–March and a maximum ≈ 4–5 % in August–October. Source areas were calculated using 50-day FLEXPART footprints. The highest eBC concentrations and the lowest ωo were associated with air masses coming from South America, Australia and Africa. Vertical simulations that take BC particle removal processes into account show that there would be essentially no BC particles arriving at Dome C from north of latitude 10° S at altitudes sp was similar to that observed at Dome C in the austral summer but there was a large difference in winter, suggesting that in winter SPO is more influenced by sea spray emissions than Dome C. The seasonal cycles of σsp at Dome C and at the SPO were compared with the seasonal cycles of secondary and primary marine aerosol emissions. The σsp measured at SPO correlated much better with the sea-spray aerosol emission fluxes in the Southern Ocean than σsp at Dome C. The seasonal cycles of biogenic secondary aerosols were estimated from monthly average phytoplankton biomass concentrations obtained from the CALIOP satellite sensor data. The analysis suggests that a large fraction of the biogenic scattering aerosol observed at Dome C has been formed in the polar zone but it may take a month for the aerosol to be formed, grown and get transported from the sea level to Dome C.

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.

Ten years of data of biogenic aerosol (methane sulfonic acid, MSA, and non-sea salt sulfate, nssSO42−) collected at Concordia Station in the East Antarctic plateau (75° 06′ S, 123° 20′ E) are interpreted as a function of the Southern Annular Mode (SAM), Chlorophyll-a concentration (Chl-a; a proxy for phytoplankton biomass), sea ice extent and area. It is possible to draw three different scenarios that link these parameters in early, middle, and late summer. In early summer, the biogenic aerosol is significantly correlated to sea ice retreats through the phytoplankton biomass increases. Chl-a shows a significant correlation with nssSO42− in the finest fraction (< 1 μm). In contrast, only Chl-a in West Pacific and Indian Ocean sectors correlates with MSA in the coarse fraction. The transport routes towards the inner Antarctic plateau and aerosol formation processes could explain the different correlation patterns of the two compounds both resulting from the DMS oxidation. In mid-summer, Chl-a concentrations are at the maximum and are not related to sea ice melting. Due to the complexity of transport processes of air masses towards the Antarctic plateau, the MSA concentrations are low and not related to Chl-a concentration. In late summer, MSA and nssSO42− present the highest concentrations in their submicrometric aerosol fraction, and both are significantly correlated with Chl-a but not with the sea ice. In early and mid-summer, the enhanced efficiency of transport processes from all the surrounding oceanic sectors with air masses traveling at low elevation can explain the highest concentrations of nssSO42− and especially MSA. Finally, considering the entire time series, MSA shows significant year-to-year variability. This variability is significantly correlated with SAM but with a different time lag in early (0-month lag) and late summer (4-months lag). This correlation likely occurs through the effect of the SAM on phytoplankton blooms.

Ice core dating is the first step for a correct interpretation of climatic and environmental changes. In this work, we release a stratigraphic dating of the uppermost 197 m of the 250 m deep GV7(B) ice core (drilling site, 70°41’S, 158°52’E, 1950 m a.s.l.) with a sub-annual resolution. Chemical stratigraphies of NO3−, MSA (methanesulfonic acid), non-sea salt SO42−, sea-salt ions and the oxygen isotopic composition (δ18O) were used in the annual layer counting upon the identification of a seasonal profile in their records. Different procedures were tested and thanks to the volcanic history of the core, obtained in previous works, an accurate age-depth correlation was obtained for the period 1179–2009 CE. Once the dating of the core was finalized, the annual mean accumulation rate was evaluated throughout the analyzed 197 m of the core, obtaining an annually resolved history of the snow accumulation on site in the last millennium. A small, yet consistent, rise in accumulation rate was found for the last 830 years since the middle of the 18th century.

Extended and intense wildfires occurred in Northern Canada and, unexpectedly, on the Greenlandic West coast during summer 2017. The thick smoke plume emitted into the atmosphere was transported to the high Arctic, producing one of the largest impacts ever observed in the region. Evidence of Canadian and Greenlandic wildfires was recorded at the Thule High Arctic Atmospheric Observatory (THAAO, 76.5°N, 68.8°W, www.thuleatmos-it.it) by a suite of instruments managed by ENEA, INGV, Univ. of Florence, and NCAR. Ground-based observations of the radiation budget have allowed quantification of the surface radiative forcing at THAAO. Excess biomass burning chemical tracers such as CO, HCN, H2CO, C2H6, and NH3 were measured in the air column above Thule starting from August 19 until August 23. The aerosol optical depth (AOD) reached a peak value of about 0.9 on August 21, while an enhancement of wildfire compounds was detected in PM10. The measured shortwave radiative forcing was -36.7 W/m2 at 78° solar zenith angle (SZA) for AOD=0.626.MODTRAN6.0 radiative transfer model (Berk et al., 2014) was used to estimate the aerosol radiative effect and the heating rate profiles at 78° SZA. Measured temperature profiles, integrated water vapour, surface albedo, spectral AOD and aerosol extinction profiles from CALIOP onboard CALIPSO were used as model input. The peak aerosol heating rate (+0.5 K/day) was reached within the aerosol layer between 8 and 12 km, while the maximum radiative effect (-45.4 W/m2) is found at 3 km, below the largest aerosol layer.The regional impact of the event that occurred on August 21 was investigated using a combination of atmospheric radiative transfer modelling with measurements of AOD and ground surface albedo from MODIS. The aerosol properties used in the radiative transfer model were constrained by in situ measurements from THAAO. Albedo data over the ocean have been obtained from Jin et al. (2004). Backward trajectories produced through HYSPLIT simulations (Stein et al., 2015) were also employed to trace biomass burning plumes.The radiative forcing efficiency (RFE) over land and ocean was derived, finding values spanning from -3 W/m2 to -132 W/m2, depending on surface albedo and solar zenith angle. The fire plume covered a vast portion of the Arctic, with large values of the daily shortwave RF (< -50 W/m2) lasting for a few days. This large amount of aerosol is expected to influence cloud properties in the Arctic, producing significant indirect radiative effects.

19 pages, 8 figures,1 table, 1 appendix.-- Data availability: The APS data can be accessed from https://doi.org/10.5281/zenodo.3961473 (Traversi et al., 2020). The absorption coefficient data are available upon request from Gilardoni et al. (2020). Data supporting this publication can be accessed upon request from the corresponding authors, Understanding aerosol–cloud–climate interactions in the Arctic is key to predicting the climate in this rapidly changing region. Whilst many studies have focused on submicrometer aerosol (diameter less than 1 µm), relatively little is known about the supermicrometer aerosol (diameter above 1 µm). Here, we present a cluster analysis of multiyear (2015–2019) aerodynamic volume size distributions, with diameter ranging from 0.5 to 20 µm, measured continuously at the Gruvebadet Observatory in the Svalbard archipelago. Together with aerosol chemical composition data from several online and offline measurements, we apportioned the occurrence of the coarse-mode aerosols during the study period (mainly from March to October) to anthropogenic (two sources, 27 %) and natural (three sources, 73 %) origins. Specifically, two clusters are related to Arctic haze with high levels of black carbon, sulfate and accumulation mode (0.1–1 µm) aerosol. The first cluster (9 %) is attributed to ammonium sulfate-rich Arctic haze particles, whereas the second one (18 %) is attributed to larger-mode aerosol mixed with sea salt. The three natural aerosol clusters were open-ocean sea spray aerosol (34 %), mineral dust (7 %) and an unidentified source of sea spray-related aerosol (32 %). The results suggest that sea-spray-related aerosol in polar regions may be more complex than previously thought due to short- and long-distance origins and mixtures with Arctic haze, biogenic and likely blowing snow aerosols. Studying supermicrometer natural aerosol in the Arctic is imperative for understanding the impacts of changing natural processes on Arctic aeroso, This research has been supported by the Natural Environment Research Council (grant no. NE/S00579X/1). We acknowledge support of the publication fee by the CSIC Open Access Publication Support Initiative through its Unit of Information Resources for Research (URICI), With the institutional support of the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000928-S)

Seasonal to interannual variations in the concentrations of sulfur aerosols (

Seasonal to interannual variations in the concentrations of sulfur aerosols (

Ice core dating is the first step for a correct interpretation of climatic and environmental changes. In this work, we release the dating of the uppermost 197 m of the 250 m deep GV7(B) ice core (drill site, 70∘41′ S, 158∘52′ E; 1950 m a.s.l. in Oates Land, East Antarctica) with a sub-annual resolution. Chemical records of NO3-, MSA (methanesulfonic acid), non-sea-salt SO42- (nssSO42-), sea-salt ions and water stable isotopes (δ18O) were studied as candidates for dating due to their seasonal pattern. Different procedures were tested but the nssSO42- record proved to be the most reliable on the short- and long-term scales, so it was chosen for annual layer counting along the whole ice core. The dating was constrained by using volcanic signatures from historically known events as tie points, thus providing an accurate age–depth relationship for the period 1179–2009 CE. The achievement of the complete age scale allowed us to calculate the annual mean accumulation rate throughout the analyzed 197 m of the core, yielding an annually resolved history of the snow accumulation on site in the last millennium. A small yet consistent rise in accumulation rate (Tr = 1.6, p<0.001) was found for the last 830 years starting around mid-18th century.

Oceanic dimethyl sulfide (DMS) emissions have been recognized as a biological regulator of climate by contributing to cloud formation. Despite decades of research, the climatic role of DMS remains ambiguous largely because of limited observational evidence for DMS-induced cloud condensation nuclei (CCN) enhancement. Here, we report concurrent measurement of DMS, physiochemical properties of aerosol particles, and CCN in the Arctic atmosphere during the phytoplankton bloom period of 2010. We encountered multiple episodes of new particle formation (NPF) and particle growth when DMS mixing ratios were both low and high. The growth of particles to sizes at which they can act as CCN accelerated in response to an increase in atmospheric DMS. Explicitly, the sequential increase in all relevant parameters (including the source rate of condensable vapor, the growth rate of particles, Aitken mode particles, hygroscopicity, and CCN) was pronounced at the DMS-derived NPF and particle growth events. This field study unequivocally demonstrates the previously unconfirmed roles of DMS in the growth of particles into climate-relevant size and eventual CCN activation.

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.

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 interesting owing to 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.

The current inadequate understanding of ice nucleating particle (INP) sources in the Arctic region affects the uncertainty in global radiative budgets and in regional climate predictions. In this study, we present atmospheric INP concentrations by offline analyses on samples collected at ground level in Ny-Ålesund (Svalbard), in spring and summer 2018. The ice nucleation properties of the samples were characterized by means of two offline instruments: the Dynamic Filter Processing Chamber (DFPC), detecting condensation freezing INPs, and the West Texas Cryogenic Refrigerator Applied to Freezing Test system (WT-CRAFT), measuring INPs by immersion freezing. Both measurements agreed within an order of magnitude although with some notable offset. INP concentration measured by DFPC ranged 33–185 (median 88), 5–107 (50) and 3–66 (20) m−3, for T = −22, −18 and −15 °C, respectively, while at the same activation temperatures WT-CRAFT measured 3–199 (26), 1–34 (6) and 1–4 (2) m−3, with an offset apparently dependent on the INP activation temperature. This observation may indicate a different sensitivity of Arctic INPs to different ice nucleation modes, even though a contribution from measurement and/or sampling uncertainties cannot be ruled out. An increase in the coarse INP fraction was observed from spring to summer, particularly at the warmest temperature (up to ~ 70 % at −15 °C). This suggests a non-negligible contribution from local sources of biogenic aerosol particles. This conclusion is also supported by the INP temperature spectra, showing ice-forming activity at temperatures higher than −15 °C. Contrary to recent works (e.g., INP measurements from Ny-Ålesund in 2012), our results do not show a sharp spring-to-summer increase of the INP concentration, with distinct behaviors for particles active in different temperature ranges. This likely indicates that the inter-annual variability of conditions affecting the INP emission by local sources may be wider than previously considered and suggests a complex interplay between INP sources. This demonstrate the necessity of further data coverage. Analysis of INP concentrations, active site density, low-travelling back-trajectories (

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 &mu, g&middot, m&minus, 3, 33% of PM2.5). Biomass burning turned out to be an important PM2.5 source in Florence (~4 &mu, 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 &mu, 3). On average, the contribution of the &ldquo, natural&rdquo, components (e.g., mineral dust and marine aerosols) to PM2.5 is moderate (~1 &mu, 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.

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.