Soot, or black carbon (BC), aerosol is a major climate forcer with severe health effects. The impacts depend strongly on particle number concentration, size and mixing state. This work reports on two field campaigns at nearby urban and rural sites, 65 km apart, in southern Sweden during late summer 2018. BC was measured using a single-particle soot photometer (SP2) and Aethalometers (AE33). Differences in BC concentrations between the sites are driven primarily by local traffic emissions. Equivalent and refractory BC mass concentrations at the urban site were on average a factor 2.2 and 2.5, with peaks during rush hour up to a factor similar to 4, higher than the rural background levels. The number fraction of particles containing a soot core was significantly higher in the city. BC particles at the urban site were on average smaller by mass and had less coating owing to fresh traffic emissions. The organic components of the fresh traffic plumes were similar in mass spectral signature to hydrocarbon-like organic aerosol (HOA), commonly associated with traffic. Despite the intense local traffic (similar to 30000 vehicles passing per day), PM1, including organic aerosol, was dominated by aged continental air masses even at the curbside site. The fraction of thickly coated particles at the urban site was highly correlated with the mass concentrations of all measured chemical species of PM1, consistent with aged, internally mixed aerosol. Trajectory analysis for the whole year showed that air masses arriving at the rural site from eastern Europe contained approximately double the amount of BC compared to air masses from western Europe. Furthermore, the largest regional emissions of BC transported to the rural site, from the Malmo-Copenhagen urban area, are discernible above background levels only when precipitation events are excluded. We show that continental Europe and not the Malmo-Copenhagen region is the major contributor to the background BC mass concentrations in southern Sweden.

The chemical composition of non-refractory submicron aerosol (NR-PM1) was characterized at the Villum Research Station (Villum) at Station Nord in North Greenland during spring-summer 2016 using a Time of Flight Aerosol Chemical Speciation Monitor (ToF-ACSM). The composition is dominated by sulfate (48%) and organic species (40%). Positive Matrix Factorization (PMF) identified three key factors corresponding to a primary hydrocarbon-like organic aerosol (HOA), and two types of secondary organic aerosol: oxygenated organic aerosol (OOA) and a marine organic aerosol (MOA). The HOA factor accounts for 5% of the organic aerosol mass, which is consistent with previous findings at Villum. The OOA factor accounts for 77% of the organic aerosol mass and correlates with accumulation mode particles, which supports previous findings indicating that oxidized organic aerosols are predominantly from long-range transport during winter and spring at Villum. The MOA factor was characterized by mass spectral fragments of methane sulfonic acid (MSA) from atmospheric oxidation of dimethyl sulfide, for which reason the MOA factor is considered to be of biogenic origin. MOA accounts for 18% of the organic aerosol mass and correlates with locally produced Aitken mode particles. This indicates that biogenic processes are not only a significant source of aerosols at Villum, but MOA also appears to be formed in the vicinity of the measurement site. This local geographical origin was confirmed through air mass back trajectory modelling and source-receptor analysis. During May, air masses frequently arrived from the east, with source regions for the MOA factor and therewith MSA located in the Barents Sea and Lincoln Sea with lesser contributions from the Greenland Sea. During June, air mass origin shifted to the west, with source regions for the MOA factor and MSA shifting correspondingly to Baffin Bay and the Canadian Arctic Archipelago. While shifting transport patterns between May and June lead to shifting source regions, sea ice likely played a role as well. During May, marginal ice zones were present in the Barents Sea between Svalbard and Franz Josef Land, while during June, sea ice in the northern part of Baffin Bay retreated and sea ice in the Canadian Arctic Archipelago decreased. Although May and June experienced different transport patterns and sea ice conditions, levels of the MOA factor and MSA were similar between the months. This is likely due to similarities between marine biological activities in the Barents Sea and Baffin Bay. This research highlights the complex relationship between transport patterns, sea ice conditions, and atmospheric particle concentrations. Multiyear aerosol chemical composition from several High Arctic sites is encouraged to determine the full effects of ocean-atmosphere interactions and transport patterns on atmospheric aerosol concentrations.

Abstract. Soot, or black carbon (BC), aerosol is a major climate forcer with severe health effects. The impacts depend strongly on particle number concentration, size and mixing state. This work reports on two field campaigns at nearby urban and rural sites, 65 km apart, in southern Sweden during late summer 2018. BC was measured using a single particle soot photometer (SP2) and Aethalometers (AE33). Differences in BC concentrations between the sites are driven primarily by local traffic emissions. Equivalent and refractory BC mass concentrations at the urban site were on average a factor 2.2 and 2.5 higher than at the rural site. Peaks in rush hour BC mass concentrations at the urban site were up to a factor ~4 higher than the background levels. The number fraction of particles containing a soot core was significantly higher in the city. BC particles at the urban site were on average smaller by mass and had less coating owing to fresh traffic emissions. The organic components of the fresh plumes were similar in mass spectral signature to “hydrocarbon-like organic aerosol” (HOA), commonly associated with traffic. Despite the intense local traffic (~30 000 vehicles passing per day), PM1, including organic aerosol, was dominated by aged continental air masses even at the curbside site. The fraction of thickly coated particles at the urban site was highly correlated with the mass concentrations of all measured chemical species of PM1, consistent with aged, internally mixed aerosol. Trajectory analysis for the whole year showed that air masses arriving at the rural site from eastern Europe contained approximately double the amount of BC compared to air masses from western Europe. Furthermore, BC from the largest region emissions in the Malmö/Copenhagen urban area transported to the rural site is discernable above background levels only when precipitation events are excluded.

On the use of "dual vaporizer" in the SP-AMS measurementsWhen engaging the laser there is a small increase in the "Organic" signal due to vaporization of non-refractory components.Additionally, all species signals increase ~10% due to increased sensitivity with dual vaporizers.

Although new particle formation (NPF) events have been studied extensively for some decades, the mechanisms that drive their occurrence and development are yet to be fully elucidated. Laboratory studies have done much to elucidate the molecular processes involved in nucleation, but this knowledge has yet to be conclusively linked to NPF events in the atmosphere. There is great difficulty in successful application of the results from laboratory studies to real atmospheric conditions due to the diversity of atmospheric conditions and observations found, as NPF events occur almost everywhere in the world without always following a clearly defined trend of frequency, seasonality, atmospheric conditions, or event development. The present study seeks common features in nucleation events by applying a binned linear regression over an extensive dataset from 16 sites of various types (combined dataset of 85 years from rural and urban backgrounds as well as roadside sites) in Europe. At most sites, a clear positive relation with the frequency of NPF events is found between the solar radiation intensity (up to R2=0.98), temperature (up to R2=0.98), and atmospheric pressure (up to R2=0.97), while relative humidity (RH) presents a negative relation (up to R2=0.95) with NPF event frequency, though exceptions were found among the sites for all the variables studied. Wind speed presents a less consistent relationship, which appears to be heavily affected by local conditions. While some meteorological variables (such as the solar radiation intensity and RH) appear to have a crucial effect on the occurrence and characteristics of NPF events, especially at rural sites, it appears that their role becomes less marked at higher average values. The analysis of chemical composition data presents interesting results. Concentrations of almost all chemical compounds studied (apart from O3) and the condensation sink (CS) have a negative relationship with NPF event frequency, though areas with higher average concentrations of SO2 had higher NPF event frequency. Particulate organic carbon (OC), volatile organic compounds (VOCs), and particulate-phase sulfate consistently had a positive relation with the growth rate of the newly formed particles. As with some meteorological variables, it appears that at increased concentrations of pollutants or the CS, their influence upon NPF frequency is reduced.

There are few long-term datasets of volatile organic compounds (VOCs) in the High Arctic. Furthermore, knowledge about their source regions remains lacking. To address this matter, we report a multiseason dataset of highly time-resolved VOC measurements in the High Arctic from April to October 2018. We have utilized a combination of measurement and modeling techniques to characterize the mixing ratios, temporal patterns, and sources of VOCs at the Villum Research Station at Station Nord in northeastern Greenland. Atmospheric VOCs were measured using proton-transfer-reaction time-of-flight mass spectrometry. Ten ions were selected for source apportionment with the positive matrix factorization (PMF) receptor model. A four-factor solution to the PMF model was deemed optimal. The factors identified were biomass burning, marine cryosphere, background, and Arctic haze. The biomass burning factor described the variation of acetonitrile and benzene and peaked during August and September. The marine cryosphere factor was comprised of carboxylic acids (formic, acetic, and C3H6O2) as well as dimethyl sulfide (DMS). This factor displayed peak contributions during periods of snow and sea ice melt. A potential source contribution function (PSCF) showed that the source regions for this factor were the coasts around southeastern and northeastern Greenland. The background factor was temporally ubiquitous, with a slight decrease in the summer. This factor was not driven by any individual chemical species. The Arctic haze factor was dominated by benzene with contributions from oxygenated VOCs. This factor exhibited a maximum in the spring and minima during the summer and autumn. This temporal pattern and species profile are indicative of anthropogenic sources in the midlatitudes. This study provides seasonal characteristics and sources of VOCs and can help elucidate the processes affecting the atmospheric chemistry and biogeochemical feedback mechanisms in the High Arctic.

Mixing Ratio and Uncertainty CalculationMixing ratios were calculated, in the absence of suitable reference materials, according to Equation S1.

In recent years, residential wood combustion (RWC) has become a major source of ambient particulate matter (PM) in many developed countries, and in some of these countries even the largest source of primary particle emissions. While other sources of PM have been regulated intensively during the past decades, RWC has been subject to only minor regulation despite of its impact on climate and health. This review covers recent research publications on RWC contributions to ambient PM in different regions of Europe, North America and Australasia, and on key species associated with RWC. Furthermore, factors governing emissions from wood stoves (as the typical appliance used in residential heating) are evaluated. State-of-the-art methods for estimating RWC as a source of ambient PM are discussed. We conclude by highlighting important areas for future research and policies.

Thirteen European Sites 2 3 Dimitrios Bousiotis, Francis D. Pope, David C. Beddows, 4 Manuel Dall’Osto, Andreas Massling, Jacob Klenø Nøjgaard, 5 Claus Nørdstrom, Jarkko V. Niemi, Harri Portin, Tuukka Petäjä, 6 Noemi Perez, Andrés Alastuey, Xavier Querol, Giorgos Kouvarakis, 7 Stergios Vratolis, Konstantinos Eleftheriadis, Alfred Wiedensohler, Kay Weinhold, 8 Maik Merkel, Thomas Tuch and Roy M. Harrison 9 10

Residential wood combustion (RWC) is an important contributor to air quality in numerous regions worldwide. This study is the first extensive evaluation of the influence of RWC on ambient air quality in several Nordic cities. We have analysed the emissions and concentrations of PM2.5 in cities within four Nordic countries: in the metropolitan areas of Copenhagen, Oslo, and Helsinki and in the city of Umeå. We have evaluated the emissions for the relevant urban source categories and modelled atmospheric dispersion on regional and urban scales. The emission inventories for RWC were based on local surveys, the amount of wood combusted, combustion technologies and other relevant factors. The accuracy of the predicted concentrations was evaluated based on urban concentration measurements. The predicted annual average concentrations ranged spatially from 4 to 7 µg m−3 (2011), from 6 to 10 µg m−3 (2013), from 4 to more than 13 µg m−3 (2013) and from 9 to more than 13 µg m−3 (2014), in Umeå, Helsinki, Oslo and Copenhagen, respectively. The higher concentrations in Copenhagen were mainly caused by the relatively high regionally and continentally transported background contributions. The annual average fractions of PM2.5 concentrations attributed to RWC within the considered urban regions ranged spatially from 0 % to 15 %, from 0 % to 20 %, from 8 % to 22 % and from 0 % to 60 % in Helsinki, Copenhagen, Umeå and Oslo, respectively. In particular, the contributions of RWC in central Oslo were larger than 40 % as annual averages. In Oslo, wood combustion was used mainly for the heating of larger blocks of flats. In contrast, in Helsinki, RWC was solely used in smaller detached houses. In Copenhagen and Helsinki, the highest fractions occurred outside the city centre in the suburban areas. In Umeå, the highest fractions occurred both in the city centre and its surroundings.

Abstract. New particle formation (NPF) events occur almost everywhere in the world and can play an important role as a particle source. The frequency and characteristics of NPF events vary spatially and this variability is yet to be fully understood. In the present study, long term particle size distribution datasets (minimum of three years) from thirteen sites of various land uses and climates from across Europe were studied and NPF events, deriving from secondary formation and not traffic related nucleation, were extracted and analysed. The frequency of NPF events was consistently found to be higher at rural background sites, while the growth and formation rates of newly formed particles were higher at roadsides, underlining the importance of the abundance of condensable compounds of anthropogenic origin found there. The growth rate was higher in summer at all rural background sites studied. The urban background sites presented the highest uncertainty due to greater variability compared to the other two types of site. The origin of incoming air masses and the specific conditions associated with them greatly affect the characteristics of NPF events. In general, cleaner air masses present higher probability for NPF events, while the more polluted ones show higher growth rates. However, different patterns of NPF events were found even at sites in close proximity (

There are limited measurements of the chemical composition, abundance and sources of atmospheric particles in the High Arctic To address this, we report 93 d of soot particle aerosol mass spectrometer (SP-AMS) data collected from 20 February to 23 May 2015 at Villum Research Station (VRS) in northern Greenland (81∘36′ N). During this period, we observed the Arctic haze phenomenon with elevated PM1 concentrations ranging from an average of 2.3, 2.3 and 3.3 µg m−3 in February, March and April, respectively, to 1.2 µg m−3 in May. Particulate sulfate (SO42-) accounted for 66 % of the non-refractory PM1 with the highest concentration until the end of April and decreasing in May. The second most abundant species was organic aerosol (OA) (24 %). Both OA and PM1, estimated from the sum of all collected species, showed a marked decrease throughout May in accordance with the polar front moving north, together with changes in aerosol removal processes. The highest refractory black carbon (rBC) concentrations were found in the first month of the campaign, averaging 0.2 µg m−3. In March and April, rBC averaged 0.1 µg m−3 while decreasing to 0.02 µg m−3 in May. Positive matrix factorization (PMF) of the OA mass spectra yielded three factors: (1) a hydrocarbon-like organic aerosol (HOA) factor, which was dominated by primary aerosols and accounted for 12 % of OA mass, (2) an Arctic haze organic aerosol (AOA) factor and (3) a more oxygenated marine organic aerosol (MOA) factor. AOA dominated until mid-April (64 %–81 % of OA), while being nearly absent from the end of May and correlated significantly with SO42-, suggesting the main part of that factor is secondary OA. The MOA emerged late at the end of March, where it increased with solar radiation and reduced sea ice extent and dominated OA for the rest of the campaign until the end of May (24 %–74 % of OA), while AOA was nearly absent. The highest O∕C ratio (0.95) and S∕C ratio (0.011) was found for MOA. Our data support the current understanding that Arctic aerosols are highly influenced by secondary aerosol formation and receives an important contribution from marine emissions during Arctic spring in remote High Arctic areas. In view of a changing Arctic climate with changing sea-ice extent, biogenic processes and corresponding source strengths, highly time-resolved data are needed in order to elucidate the components dominating aerosol concentrations and enhance the understanding of the processes taking place.

The study reports on SP-HR-AMS measurements conducted at Villum Research Station in the north of Greenland from February to May 2015. The authors investigate the concentrations and evolution of refractory black carbon (rBC), particulate sulfate (SO4) and organic aerosol (OA). The first half of the manuscript focuses on rBC, the second on OA that was further investigated by conducting positive matrix factorization (PMF). Three factors were identified: hydrocarbon-like OA (HOA) with the smallest contribution, Arctic haze OA (AOA) with the largest contribution and marine OA (MOA).

We sampled ammonium sulfate particles and indoor particles of outdoor origin through a small chamber covered with polyvinyl chloride flooring. We measured the uptake of semivolatile organic compounds (SVOCs) by the airborne particles in real time. The particles acquired SVOC mass fractions up to 10%. The phthalate ester (di(2-ethylhexyl)phthalate) (DEHP), a known endocrine disruptor, contributed by approximately half of the sorbed SVOC mass. The indoor particles acquired a higher DEHP fraction than laboratory-generated ammonium sulfate aerosol. We attribute this increased uptake to absorption by organic matter present in the indoor particles. Using a thermodenuder to remove volatile components, predominantly organics, reduced the SVOC uptake. Positive matrix factorization applied to the organic mass spectra suggests that hydrocarbon-like organic aerosol (typically fresh traffic exhaust) sorbs DEHP more efficiently than aged organic aerosol. The SVOC uptake is one of the processes that modify outdoor pollution particles after they penetrate buildings, where the majority of exposure occurs. Particles from indoor sources, typically dominated by organic matter, will undergo such processes as well. Aerosol mass spectrometry improves the time resolution of experimental investigations into these processes and enables experiments with lower, relevant particle concentrations. Additionally, particle size-resolved results are readily obtained.

In order to improve our ability to predict cloud properties, radiative balance and climate, it is crucial to understand the mechanisms that trigger the formation of new particles and their growth to activation sizes. Using an array of real time aerosol measurements, we report a categorization of the aerosol population taken at Villum Research Station, Station Nord (VRS) in North Greenland during a period of 88 days (February–May 2015). A number of New Particle Formation (NPF) events were detected and are herein discussed. Air mass back trajectories analysis plotted over snow-sea ice satellite maps allowed us to correlate early spring (April) NPF events with air masses travelling mainly over snow on land and sea ice, whereas late spring (May) NPF events were associated with air masses that have passed mainly over sea ice regions. Concomitant aerosol mass spectrometry analysis suggests methanesulfonic acid (MSA) and molecular iodine (I2) may be involved in the NPF mechanisms. The source of MSA was attributed to open leads within the sea ice. By contrast, iodine was associated with air masses over snow on land and over sea ice, suggesting both abiotic and biotic sources. Measurements of nucleating particle composition as well as gas-phase species are needed to improve our understanding of the links between emissions, aerosols, cloud and climate in the Arctic; therefore our ability to model such processes.

Source apportionment (SA) of carbonaceous aerosol was performed as part of the EMEP Intensive Measurement Periods (EIMPs), conducted in fall 2008 and winter/spring 2009. Levels of elemental carbon (EC), particulate organic carbon (OCp), particulate total carbon (TCp), levoglucosan and 14C in PM10, observed at nine European rural background sites, were used as input for the SA, whereas Latin Hypercube Sampling (LHS) was used to statistically treat the multitude of possible combinations resulting when ambient concentrations were combined with appropriate emission ratios. Five predefined sources/subcategories of carbonaceous aerosol were apportioned: Elemental and organic carbon from combustion of biomass (ECbb and OCbb) and from fossil fuel (ECff and OCff) sources, as well as remaining non-fossil organic carbon (OCrnf), typically dominated by natural sources. The carbonaceous aerosol concentration decreased from South to North, as did the concentration of the apportioned carbonaceous aerosol. OCrnf was more abundant in fall compared to winter/spring, reflecting the vegetative season, and made a larger contribution to TCp than anthropogenic sources (here: ECbb, OCbb, ECff and OCff) at four of the sites, whereas anthropogenic sources dominated at all but one sites in winter/spring. Levels of OCbb and ECbb were typically higher in winter/spring than in fall, due to larger residential wood burning emissions in the heating season, whereas there was no consistent seasonal pattern for fossil fuel emissions. Biomass burning (OCbb + ECbb) was the major anthropogenic source at the Central European sites in fall, whereas fossil fuel sources dominated at the southernmost and the two northernmost sites. In winter/spring, biomass burning was the major anthropogenic source at all but two sites. Addressing EC in particular, fossil fuel sources dominated at all sites in fall, whereas there was as shift towards biomass burning in winter/spring for the southernmost sites. Influence of residential wood burning emissions was substantial already in the first week of sampling in fall, constituting 30–50 % of TCp at most sites, showing that this source can be dominating even at a time of the year when the ambient temperature in Europe is still rather high. Model calculations were made, attempting to reproduce LHS-derived OCbb and ECbb, using two different residential wood burning emission inventories. Both simulations strongly under-predicted the LHS-derived values at most sites outside Scandinavia. Emissions based on a consistent bottom-up inventory for residential combustion (and including intermediate volatility compounds, IVOC) improved model results at most sites compared to the base-case emissions (based mainly on officially reported national emissions), but at the three southernmost sites the modelled OCbb and ECbb concentrations were still much lower than the LHS source apportioned results. The current study shows that natural sources is a major contributor to the carbonaceous aerosol in Europe even in fall and in winter/spring, and that residential wood burning emissions can be equally large or larger than that of fossil fuel sources, depending on season and region. Our results suggest that residential wood burning emissions are still poorly constrained for large parts of Europe. The need to improve emission inventories is obvious, with harmonization of emission factors between countries likely being the most important step to improve model calculations, not only for biomass burning emissions, but for European PM2.5 concentrations in general.

Atmospheric new particle formation (NPF) and growth significantly influences the indirect aerosol-cloud effect within the polar climate system. In this work, the aerosol population is categorised via cluster analysis of aerosol number size distributions (9–915 nm, 65 bins) taken at Villum Research Station, Station Nord (VRS) in North Greenland during a 7 year record (2010–2016). Data are clustered at daily averaged resolution; in total, we classified six categories, five of which clearly describe the ultrafine aerosol population, one of which is linked to nucleation events (up to 39% during summer). Air mass trajectory analyses tie these frequent nucleation events to biogenic precursors released by open water and melting sea ice regions. NPF events in the studied regions seem not to be related to bird colonies from coastal zones. Our results show a negative correlation (r = −0.89) between NPF events and sea ice extent, suggesting the impact of ultrafine Arctic aerosols is likely to increase in the future, given the likely increased sea ice melting. Understanding the composition and the sources of Arctic aerosols requires further integrated studies with joint multi-component ocean-atmosphere observation and modelling.