Arctic Aerosol Research Articles

From Polar Day to Polar Night: A Comprehensive Sun and Star Photometer Study of Trends in Arctic Aerosol Properties in Ny-Ålesund, Svalbard

The climate impact of Arctic aerosols, like the Arctic Haze, and their origin are not fully understood. Therefore, long-term aerosol observations in the Arctic are performed. In this study, we present a homogenised data set from a sun and star photometer operated in the European Arctic, in Ny-Ålesund, Svalbard, of the 20 years from 2004–2023. Due to polar day and polar night, it is crucial to use observations of both instruments. Their data is evaluated in the same way and follows the cloud-screening procedure of AERONET. Additionally, an improved method for the calibration of the star photometer is presented. We found out, that autumn and winter are generally more polluted and have larger particles than summer. While the monthly median Aerosol Optical Depth (AOD) decreases in spring, the AOD increases significantly in autumn. A clear signal of large particles during the Arctic Haze can not be distinguished from large aerosols in winter. With autocorrelation analysis, we found that AOD events usually occur with a duration of several hours. We also compared AOD events with large-scale processes, like large-scale oscillation patterns, sea ice, weather conditions, or wildfires in the Northern Hemisphere but did not find one single cause that clearly determines the Arctic AOD. Therefore the observed optical depth is a superposition of different aerosol sources.

Surface warming in Svalbard may have led to increases in highly active ice-nucleating particles

The roles of Arctic aerosols as ice-nucleating particles remain poorly understood, even though their effects on cloud microphysics are crucial for assessing the climate sensitivity of Arctic mixed-phase clouds and predicting their response to Arctic warming. Here we present a full-year record of ice-nucleating particle concentrations over Svalbard, where surface warming has been anomalously faster than the Arctic average. While the variation of ice-nucleating particles active at around −30 °C was relatively small, those active at higher temperatures (i.e., highly active ice-nucleating particles) tended to increase exponentially with rising surface air temperatures when the surface air temperatures rose above 0 °C and snow/ice-free barren and vegetated areas appeared in Svalbard. The aerosol population relevant to their increase was largely characterized by dust and biological organic materials that likely originated from local/regional terrestrial sources. Our results suggest that highly active ice-nucleating particles could be actively released from Arctic natural sources in response to surface warming.

γ-Lactones in Canadian high arctic aerosols: Tracers for the oxidation of unsaturated fatty acids and intramolecular esterification of γ-hydroxyacids during polar sunrise

In this study, we detected for the first time a series of γ-lactones (C7-C16) isolated from Canadian high arctic aerosols collected from late February to June as the sun rises from below the horizon to the maximum. γ-Lactones were identified and quantified by GC-MS utilizing the fragment ion (m/z 85) of [C4H5O2]+. Their molecular distributions showed the predominance of C9 species (on average, 25 pg/m3) followed by C10, C8, C11, C12, C16, C15, and C7. The odd-carbon numbered γ-lactones such as C9 and C11 are produced by the oxidation of oleic (Δ9C18:1) and eicosanoic (Δ9C20:1) acids, respectively, to monocarboxylic acids in the atmosphere, followed by the subsequent oxidation to positional isomers of hydroxy acids and intramolecular esterification of γ-hydroxy acids. Unsaturated fatty acids, plausible sources of the γ-lactones, can originate from marine phytoplankton and terrestrial vegetation via long-range atmospheric transport to the Arctic. Series of ω-oxoacids were also detected with the predominance of C9 species, supporting the photochemical oxidation of biogenic unsaturated fatty acids in the Arctic atmosphere after polar sunrise and/or during the long-range transport to the Arctic.

Assessment of Hygroscopic Behavior of Arctic Aerosol by Contemporary Lidar and Radiosonde Observations

Assessment of Hygroscopic Behavior of Arctic Aerosol by Contemporary Lidar and Radiosonde Observations

Seasonal dynamics of airborne biomolecules influence the size distribution of Arctic aerosols

Organic matter is crucial in aerosol–climate interactions, yet the physicochemical properties and origins of organic aerosols remain poorly understood. Here we show the seasonal characteristics of submicron organic aerosols in Arctic Svalbard during spring and summer, emphasizing their connection to transport patterns and particle size distribution. Microbial-derived organic matter (MOM) and terrestrial-derived organic matter (TOM) accounted for over 90% of the total organic mass in Arctic aerosols during these seasons, comprising carbohydrate/protein-like and lignin/tannin-like compounds, respectively. In spring, aerosols showed high TOM and low MOM intensities due to biomass-burning influx in the central Arctic. In contrast, summer exhibited elevated MOM intensity, attributed to the shift in predominant atmospheric transport from the central Arctic to the biologically active Greenland Sea. MOM and TOM were associated with Aitken mode particles (<100 nm diameter) and accumulation mode particles (>100 nm diameter), respectively. This association is linked to the molecular size of biomolecules, impacting the number concentrations of corresponding aerosol classes. These findings highlight the importance of considering seasonal atmospheric transport patterns and organic source-dependent particle size distributions in assessing aerosol properties in the changing Arctic.

Chemical composition, source characteristics, and hygroscopic properties of organic-enriched aerosols in the high Arctic during summer

Arctic regions are extremely sensitive to global warming. Aerosols are one of the most important short-lived climate-forcing agents affecting the Arctic climate. The present study examines the summertime chemical characteristics and potential sources of various organic and inorganic aerosols at a Norwegian Arctic site, Ny-Ålesund (79°N). The results show that organic matter (OM) accounts for 60 % of the total PM10 mass, followed by sulfate (SO42−). Water-soluble organic carbon (WSOC) contributes 62 % of OC. Photochemical processes involving diverse anthropogenic and biogenic precursor compounds are identified as the major sources of WSOC, while water-insoluble organic carbon (WIOC) aerosols are predominantly linked to primary marine emissions. Despite being a remote pristine site, the aerosols show a sign of chemical aging, evidenced by a significant chloride depletion, which was about 82 % on average during the study period. Nitrogen-containing aerosols are likely stemming from migratory seabird colonies and local dust sources around the sampling site. While biogenic, crustal, and sea salt-derived SO42- account for 37%, 8%, and 5% respectively, the remaining 50% is attributed to anthropogenic SO42-. Through chemical tracers, Pearson correlation coefficient matrix, and Hierarchical Cluster Analysis (HCA), the present study identifies soil biota (terrestrial biogenic) and marine emissions, along with their photochemical oxidation processes, as potential sources of Arctic aerosols during summer, while biomass burning and combustion-related sources have a minor contribution. The chemical closure of hygroscopicity highlights that while organics predominantly control aerosol hygroscopicity in the Arctic summer, specific inorganic components like (NH4)2SO4 can significantly increase it on certain days, affecting aerosol-cloud interactions and climate processes over the Arctic during summer. The present study highlights the high abundance of organics and their vital role in the Arctic climate during summer when natural aerosols are conquered.

Air Composition over the Russian Arctic–4: Atmospheric Aerosols

This work presents the analysis of the spatial distribution of number concentration, size distribution, and chemical composition of aerosol particles measured for the first time over the seas of the Russian Arctic. Various types of vertical distribution of the number concentration were recorded, characteristic of both coastal marine and continental areas. Most of them turned out to be of the continental type. Attention is also drawn to the almost complete absence of coarse particles above 2–3 km over all seas. The chemical composition of the Arctic aerosol at altitudes of both 200 m and 5000 m contains ions that can be referred to as both marine and continental. The identifiable carbon- and salt-free elemental part of the aerosol over the Arctic is 3–4 times larger than that of ions. Over all seas and at both altitudes, the Arctic aerosols mainly contain elements of terrigenous origin – Al, Cu, Fe, and Si. Over almost all seas, except the Barents Sea, Si is dominant in the elemental composition of the aerosol, its contribution over the Chukchi Sea reaching 85%. The analysis of backward trajectories showed that in all cases considered, whether the aerosol was formed over the continent or sea, air trajectories passed both over sea and over land. In this case, the formed particles could be enriched with additional ions and elements along their pathway. This work completes a cycle of the papers, devoted to studying air composition, which was carried out over the seas of the Russian Arctic in September 2020. Our results can be used to model the atmospheric processes occurring in the Arctic under the conditions of changing climate.

Improvement of Aerosol Coarse-Mode Detection through Additional Use of Infrared Wavelengths in the Inversion of Arctic Lidar Data

An Nd:YAG-based Raman lidar provides a mature technology to derive profiles of the optical properties of aerosols over a wide altitude range. However, the derivation of micro-physical parameters is an ill-posed problem. Hence, increasing the information content of lidar data is desirable. Recently, ceilometers and wind lidar systems, both operating in the near-infrared region, have been successfully employed in aerosol research. In this study, we demonstrate that the inclusion of additional backscatter coefficients from these two latter instruments clearly improves the inversion of micro-physical parameters such as volume distribution function, effective radius, or single-scattering albedo. We focus on the Arctic aerosol and start with the typical volume distribution functions of Arctic haze and boreal biomass burning. We forward calculate the optical coefficients that the lidar systems should have seen and include or exclude the backscatter coefficients of the ceilometer (910 nm) and wind lidar data (1500 nm) to analyze the value of these wavelengths in their ability to reproduce the volume distribution function, which may be mono- or bimodal. We found that not only the coarse mode but also the properties of the accumulation mode improved when the additional wavelengths were considered. Generally, the 1500 nm wavelength has greater value in correctly reproducing the aerosol properties.

Impact of Biomass Burning on Arctic Aerosol Composition.

Emissions from biomass burning (BB) occurring at midlatitudes can reach the Arctic, where they influence the remote aerosol population. By using measurements of levoglucosan and black carbon, we identify seven BB events reaching Svalbard in 2020. We find that most of the BB events are significantly different to the rest of the year (nonevents) for most of the chemical and physical properties. Aerosol mass and number concentrations are enhanced by up to 1 order of magnitude during the BB events. During BB events, the submicrometer aerosol bulk composition changes from an organic- and sulfate-dominated regime to a clearly organic-dominated regime. This results in a significantly lower hygroscopicity parameter κ for BB aerosol (0.4 ± 0.2) compared to nonevents (0.5 ± 0.2), calculated from the nonrefractory aerosol composition. The organic fraction in the BB aerosol showed no significant difference for the O:C ratios (0.9 ± 0.3) compared to the year (0.9 ± 0.6). Accumulation mode particles were present during all BB events, while in the summer an additional Aitken mode was observed, indicating a mixture of the advected air mass with locally produced particles. BB tracers (vanillic, homovanillic, and hydroxybenzoic acid, nitrophenol, methylnitrophenol, and nitrocatechol) were significantly higher when air mass back trajectories passed over active fire regions in Eastern Europe, indicating agricultural and wildfires as sources. Our results suggest that the impact of BB on the Arctic aerosol depends on the season in which they occur, and agricultural and wildfires from Eastern Europe have the potential to disturb the background conditions the most.

Investigation of Icelandic Dust Presence in the Aerosols Collected at Hornsund (Svalbard, Norwegian Arctic) in Spring 2019

Investigation of Icelandic Dust Presence in the Aerosols Collected at Hornsund (Svalbard, Norwegian Arctic) in Spring 2019

Marine carbohydrates in Arctic aerosol particles and fog – diversity of oceanic sources and atmospheric transformations

Abstract. Carbohydrates, originating from marine microorganisms, enter the atmosphere as part of sea spray aerosol (SSA) and can influence fog and cloud microphysics as cloud condensation nuclei (CCN) or ice-nucleating particles (INP). Particularly in the remote Arctic region, significant knowledge gaps persist about the sources, the sea-to-air transfer mechanisms, atmospheric concentrations, and processing of this substantial organic group. In this ship-based field study conducted from May to July 2017 in the Fram Strait, Barents Sea, and central Arctic Ocean, we investigated the sea-to-air transfer of marine combined carbohydrates (CCHO) from concerted measurements of the bulk seawater, the sea surface microlayer (SML), aerosol particles and fog. Our results reveal a wide range of CCHO concentrations in seawater (22–1070 µg L−1), with notable variations among different sea-ice-related sea surface compartments. Enrichment factors in the sea surface microlayer (SML) relative to bulk water exhibited variability in both dissolved (0.4–16) and particulate (0.4–49) phases, with the highest values in the marginal ice zone (MIZ) and aged melt ponds. In the atmosphere, CCHO was detected in super- and submicron aerosol particles (CCHOaer,super: 0.07–2.1 ng m−3; CCHOaer,sub: 0.26–4.4 ng m−3) and fog water (CCHOfog,liquid: 18–22 000 µg L−1; CCHOfog,atmos: 3–4300 ng m−3). Enrichment factors for sea–air transfer varied based on assumed oceanic emission sources. Furthermore, we observed rapid atmospheric aging of CCHO, indicating both biological/enzymatic processes and abiotic degradation. This study highlights the diverse marine emission sources in the Arctic Ocean and the atmospheric processes shaping the chemical composition of aerosol particles and fog.

Sources, variability, long-term trends, and radiative forcing of aerosols in the Arctic: implications for Arctic amplification.

Atmospheric pollution in the Arctic has been an important driver for the ongoing climate change there. Increase in the Arctic aerosols causes the phenomena of Arctic haze and Arctic amplification. Our analysis of aerosol optical depth (AOD), black carbon (BC), and dust using ground-based, satellite, and reanalysis data in the Arctic for the period 2003-2019 shows that the lowest amount of all these is found in Greenland and Central Arctic. There is high AOD, BC, and dust in the northern Eurasia and parts of North America. All aerosols show their highest values in spring. Significant positive trends in AOD (> 0.003year-1) and BC (0.0002-0.0003year-1) are found in the northwestern America and northern Asia. Significant negative trends are observed for dust (- 0.0001year-1) around Central Arctic. Seasonal analysis of AOD, BC, and dust reveals an increasing trend in summer and decreasing trend in spring in the Arctic. The major sources of aerosols are the nearby Europe, Russia, and North America regions, as assessed using the potential source contribution function (PSCF). Anthropogenic emissions from the transport, energy, and household sectors along with natural sources such as wildfires contribute to the positive trends of aerosols in the Arctic. These increasing aerosols in the Arctic influence Arctic amplification through radiative effects. Here, we find that the net aerosol radiative forcing is high in Central Arctic, Greenland, Siberia, and Canadian Arctic, about 2-4 W/m2, which can influence the regional temperature. Therefore, our study can assist policy decisions for the mitigation of Arctic haze and Arctic amplification in this environmental fragile region of the Earth.

Annual cycle of aerosol properties over the central Arctic during MOSAiC 2019–2020 – light-extinction, CCN, and INP levels from the boundary layer to the tropopause

Abstract. The MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition was the largest Arctic field campaign ever conducted. MOSAiC offered the unique opportunity to monitor and characterize aerosols and clouds with high vertical resolution up to 30 km height at latitudes from 80 to 90∘ N over an entire year (October 2019 to September 2020). Without a clear knowledge of the complex aerosol layering, vertical structures, and dominant aerosol types and their impact on cloud formation, a full understanding of the meteorological processes in the Arctic, and thus advanced climate change research, is impossible. Widespread ground-based in situ observations in the Arctic are insufficient to provide these required aerosol and cloud data. In this article, a summary of our MOSAiC observations of tropospheric aerosol profiles with a state-of-the-art multiwavelength polarization Raman lidar aboard the icebreaker Polarstern is presented. Particle optical properties, i.e., light-extinction profiles and aerosol optical thickness (AOT), and estimates of cloud-relevant aerosol properties such as the number concentration of cloud condensation nuclei (CCN) and ice-nucleating particles (INPs) are discussed, separately for the lowest part of the troposphere (atmospheric boundary layer, ABL), within the lower free troposphere (around 2000 m height), and at the cirrus level close to the tropopause. In situ observations of the particle number concentration and INPs aboard Polarstern are included in the study. A strong decrease in the aerosol amount with height in winter and moderate vertical variations in summer were observed in terms of the particle extinction coefficient. The 532 nm light-extinction values dropped from &gt;50 Mm−1 close to the surface to &lt;5 Mm−1 at 4–6 km height in the winter months. Lofted, aged wildfire smoke layers caused a re-increase in the aerosol concentration towards the tropopause. In summer (June to August 2020), much lower particle extinction coefficients, frequently as low as 1–5 Mm−1, were observed in the ABL. Aerosol removal, controlled by in-cloud and below-cloud scavenging processes (widely suppressed in winter and very efficient in summer) in the lowermost 1–2 km of the atmosphere, seems to be the main reason for the strong differences between winter and summer aerosol conditions. A complete annual cycle of the AOT in the central Arctic could be measured. This is a valuable addition to the summertime observations with the sun photometers of the Arctic Aerosol Robotic Network (AERONET). In line with the pronounced annual cycle in the aerosol optical properties, typical CCN number concentrations (0.2 % supersaturation level) ranged from 50–500 cm−3 in winter to 10–100 cm−3 in summer in the ABL. In the lower free troposphere (at 2000 m), however, the CCN level was roughly constant throughout the year, with values mostly from 30 to 100 cm−3. A strong contrast between winter and summer was also given in terms of ABL INPs which control ice production in low-level clouds. While soil dust (from surrounding continents) is probably the main INP type during the autumn, winter, and spring months, local sea spray aerosol (with a biogenic aerosol component) seems to dominate the ice nucleation in the ABL during the summer months (June–August). The strong winter vs. summer contrast in the INP number concentration by roughly 2–3 orders of magnitude in the lower troposphere is, however, mainly caused by the strong cloud temperature contrast. A unique event of the MOSAiC expedition was the occurrence of a long-lasting wildfire smoke layer in the upper troposphere and lower stratosphere. Our observations suggest that the smoke particles frequently triggered cirrus formation close to the tropopause from October 2019 to May 2020.

Measurements of aerosol microphysical and chemical properties in the central Arctic atmosphere during MOSAiC

The Arctic environment is transforming rapidly due to climate change. Aerosols’ abundance and physicochemical characteristics play a crucial, yet uncertain, role in these changes due to their influence on the surface energy budget through direct interaction with solar radiation and indirectly via cloud formation. Importantly, Arctic aerosol properties are also changing in response to climate change. Despite their importance, year-round measurements of their characteristics are sparse in the Arctic and often confined to lower latitudes at Arctic land-based stations and/or short high-latitude summertime campaigns. Here, we present unique aerosol microphysics and chemical composition datasets collected during the year-long Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition, in the central Arctic. These datasets, which include aerosol particle number concentrations, size distributions, cloud condensation nuclei concentrations, fluorescent aerosol concentrations and properties, and aerosol bulk chemical composition (black carbon, sulfate, nitrate, ammonium, chloride, and organics) will serve to improve our understanding of high-Arctic aerosol processes, with relevance towards improved modelling of the future Arctic (and global) climate.

Composition and mixing state of individual aerosol particles from northeast Greenland and Svalbard in the Arctic during spring 2018

The Arctic region is warming about four times faster than the rest of the globe, and thus it is important to understand the processes driving climate change in this region. Aerosols are a significant component of the Arctic climate system as they form ice crystals and liquid droplets that control the dynamics of clouds and also directly interact with solar radiation, depending on the compositions and mixing states of individual particles. Here, we report on the characteristics of submicron-sized aerosol particles using transmission electron microscopy obtained at two high Arctic sites, northeast Greenland (Villum Research Station) and Svalbard (Zeppelin Observatory), during spring 2018. The results showed that a dominant compound in the submicron-sized spring aerosols was sulfate, followed by sea salt particles. Both model simulations and observations at the Zeppelin Observatory showed that sea salt particles became more prevalent when low-pressure systems passed by the station. Model simulations indicate that both sampling sites were affected by diffused and diluted long-range transport of anthropogenic aerosols from lower latitudes with negligible influences of biomass burning emissions during the observation period. Overall, the composition of measured aerosol particles from the two Arctic sites was generally similar and showed no apparent variation except for the sea salt fractions. This study shows a general picture of high Arctic aerosol particles influenced by marine sources and diffused long-range transport of anthropogenic sources during the Arctic spring period. These results will contribute to a better knowledge of the aerosol composition and mixing state during the Arctic spring, which helps to understand the contributions of aerosols to the Arctic climate.

A signature of aged biogenic compounds detected from airborne VOC measurements in the high arctic atmosphere in March/April 2018

During the PAMARCMiP 2018 campaign (March and April 2018) a proton-transfer-reaction mass spectrometer (PTR-MS) was deployed onboard the POLAR 5 research aircraft and sampled the high Arctic atmosphere under Arctic haze conditions. More than 100 compounds exhibited levels above 1 pmol/mol in at least 25% of the measurements. We used acetone mixing ratios, ozone concentrations, and back trajectories to identify periods with and without long-range transport from continental sources. During two flights, surface ozone depletion events (ODE) were observed that coincided with enhanced levels of acetone, and methylethylketone, and ice nucleating particles (INP).Air masses with continental influence contained elevated levels of compounds associated with aged biogenic emissions and anthropogenic pollution (e.g., methanol, peroxyacetylnitrate (PAN), acetone, acetic acid, methylethylketone (MEK), proprionic acid, and pentanone). Almost half of all positively detected compounds (>100) in the high Arctic atmosphere can be associated with terpene oxidation products, likely produced from monoterpenes and sesquiterpenes emitted from boreal forests. We speculate that the transport of biogenic terpene emissions may constitute an important control of the High Arctic aerosol burden. The sum concentration of the detected aerosol forming vapours is ∼12 pmol/mol, which is of the same order than measured dimethylsulfide (DMS) mixing ratios and their mass density corresponds to approximately one fifth of the measured non-black-carbon particles.

Long‐Term Observations of Levoglucosan in Arctic Aerosols Reveal Its Biomass Burning Source and Implication on Radiative Forcing

AbstractBiomass burning (BB) has a significant influence on the Arctic environment. Here, we determined the atmospheric levels of BB‐specific tracer compounds such as levoglucosan (Lev), galactosan (Gan), and mannosan (Man) in Arctic aerosols during 2010–2018. The average concentrations of Lev during the study period ranged between 0.43 and 4.15 ng m−3. Both Lev/Man (0–30) and Man/Gan (0–3) ratios further suggested their origin from softwood/hardwood burning. The North Atlantic Oscillation (NAO) was the main driver of the Lev variability during the study period and Lev could be advected to Arctic air during the NAO was in a positive phase. Based upon the levels of Lev, black carbon (BC) generated from BB was estimated, and the corresponding radiative forcing was then calculated by Santa Barbara DISORT Atmospheric Radiative Transfer. BC has a potential warming effect in the atmosphere (+4.28 W/m2) while shows a cooling effect on the surface, which is equivalent to a large volcanic eruption (−3 W/m2). Since climate change is expected to intensify BB around the Arctic, such BC aerosols should be considered in future climate model projections.

Modelling wintertime sea-spray aerosols under Arctic haze conditions

Abstract. Anthropogenic and natural emissions contribute to enhanced concentrations of aerosols in the Arctic winter and early spring, with most attention being paid to anthropogenic aerosols that contribute to so-called Arctic haze. Less-well-studied wintertime sea-spray aerosols (SSAs) under Arctic haze conditions are the focus of this study, since they can make an important contribution to wintertime Arctic aerosol abundances. Analysis of field campaign data shows evidence for enhanced local sources of SSAs, including marine organics at Utqiaġvik (formerly known as Barrow) in northern Alaska, United States, during winter 2014. Models tend to underestimate sub-micron SSAs and overestimate super-micron SSAs in the Arctic during winter, including the base version of the Weather Research Forecast coupled with Chemistry (WRF-Chem) model used here, which includes a widely used SSA source function based on Gong et al. (1997). Quasi-hemispheric simulations for winter 2014 including updated wind speed and sea-surface temperature (SST) SSA emission dependencies and sources of marine sea-salt organics and sea-salt sulfate lead to significantly improved model performance compared to observations at remote Arctic sites, notably for coarse-mode sodium and chloride, which are reduced. The improved model also simulates more realistic contributions of SSAs to inorganic aerosols at different sites, ranging from 20 %–93 % in the observations. Two-thirds of the improved model performance is from the inclusion of the dependence on SSTs. The simulation of nitrate aerosols is also improved due to less heterogeneous uptake of nitric acid on SSAs in the coarse mode and related increases in fine-mode nitrate. This highlights the importance of interactions between natural SSAs and inorganic anthropogenic aerosols that contribute to Arctic haze. Simulation of organic aerosols and the fraction of sea-salt sulfate are also improved compared to observations. However, the model underestimates episodes with elevated observed concentrations of SSA components and sub-micron non-sea-salt sulfate at some Arctic sites, notably at Utqiaġvik. Possible reasons are explored in higher-resolution runs over northern Alaska for periods corresponding to the Utqiaġvik field campaign in January and February 2014. The addition of a local source of sea-salt marine organics, based on the campaign data, increases modelled organic aerosols over northern Alaska. However, comparison with previous available data suggests that local natural sources from open leads, as well as local anthropogenic sources, are underestimated in the model. Missing local anthropogenic sources may also explain the low modelled (sub-micron) non-sea-salt sulfate at Utqiaġvik. The introduction of a higher wind speed dependence for sub-micron SSA emissions, also based on Arctic data, reduces biases in modelled sub-micron SSAs, while sea-ice fractions, including open leads, are shown to be an important factor controlling modelled super-micron, rather than sub-micron, SSAs over the north coast of Alaska. The regional results presented here show that modelled SSAs are more sensitive to wind speed dependence but that realistic modelling of sea-ice distributions is needed for the simulation of local SSAs, including marine organics. This study supports findings from the Utqiaġvik field campaign that open leads are the primary source of fresh and aged SSAs, including marine organic aerosols, during wintertime at Utqiaġvik; these findings do not suggest an influence from blowing snow and frost flowers. To improve model simulations of Arctic wintertime aerosols, new field data on processes that influence wintertime SSA production, in particular for fine-mode aerosols, are needed as is improved understanding about possible local anthropogenic sources.

Measurement report: High Arctic aerosol hygroscopicity at sub- and supersaturated conditions during spring and summer

Abstract. Aerosol hygroscopic growth and cloud droplet formation influence the radiation transfer budget of the atmosphere and thereby the climate. In the Arctic, these aerosol properties may have a more pronounced effect on the climate compared to the midlatitudes. Hygroscopic growth and cloud condensation nuclei (CCN) concentrations of high Arctic aerosols were measured during two field studies in the spring and summer of 2016. The study site was the Villum Research Station (Villum) at Station Nord in the northeastern region of Greenland. Aerosol hygroscopic growth was measured with a hygroscopic tandem differential mobility analyzer (HTDMA) over a total of 23 d, and CCN concentrations were measured over a period of 95 d. Continuous particle number size distributions were recorded, facilitating calculations of aerosol CCN activation diameters and aerosol κ values. In spring, average CCN concentrations, at supersaturations (SSs) of 0.1 % to 0.3 %, ranged from 53.7 to 85.3 cm−3, with critical activation diameters ranging from 130.2 to 80.2 nm and κCCN ranging from 0.28–0.35. In summer, average CCN concentrations were 20.8 to 47.6 cm−3, while critical activation diameters and κCCN were from 137.1 to 76.7 nm and 0.23–0.35, respectively. Mean particle hygroscopic growth factors ranged from 1.60 to 1.75 at 90 % relative humidity in spring, while values between 1.47 and 1.67 were observed in summer depending on the initial dry size. Although the summer aerosol number size distributions were characterized by frequent new particle formation events, the CCN population at cloud-relevant supersaturations was determined by accumulation-mode aerosols.

Vertical Gradient of Size-Resolved Aerosol Compositions over the Arctic Reveals Cloud Processed Aerosol in-Cloud and above Cloud

Arctic aerosols play a significant role in aerosol-radiation and aerosol-cloud interactions, but ground-based measurements are insufficient to explain the interaction of aerosols and clouds in a vertically stratified Arctic atmosphere. This study shows the vertical variability of a size resolved aerosol composition via a tethered balloon system at Oliktok Point, Alaska, at different cloud layers for two representative case studies (background aerosol and polluted conditions). Multimodal microspectroscopy analysis during the background case reveals a broadening of chemically specific size distribution above the cloud top with a high abundance of sulfate particles and core-shell morphology, suggesting possible cloud processing of aerosols. The polluted case also indicates broadening of aerosol size distribution at the upper layer within the clouds with the dominance of carbonaceous particles, which suggests that the carbonaceous particles play a potential role in modulating Arctic cloud properties.