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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. 

Abstract. The number concentration and properties of aerosol particles serving ascloud condensation nuclei (CCN) are important for understanding cloudproperties, including in the tropical Atlantic marine boundary layer (MBL), where marine cumulus clouds reflect incoming solar radiation and obscure thelow-albedo ocean surface. Studies linking aerosol source, composition, andwater uptake properties in this region have been conducted primarily duringthe summertime dust transport season, despite the region receiving a varietyof aerosol particle types throughout the year. In this study, we comparesize-resolved aerosol chemical composition data to the hygroscopicityparameter κ derived from size-resolved CCN measurements made duringthe Elucidating the Role of Clouds–Circulation Coupling in Climate (EUREC4A) and Atlantic Tradewind Ocean-Atmosphere Mesoscale Interaction Campaign (ATOMIC) campaigns from January to February 2020. Weobserved unexpected periods of wintertime long-range transport of Africansmoke and dust to Barbados. During these periods, the accumulation-mode aerosol particle and CCN number concentrations as well as the proportions ofdust and smoke particles increased, whereas the average κ slightlydecreased (κ=0.46±0.10) from marine backgroundconditions (κ=0.52±0.09) when the submicron particles were mostly composed of marine organics and sulfate. Size-resolved chemicalanalysis shows that smoke particles were the major contributor to theaccumulation mode during long-range transport events, indicating that smokeis mainly responsible for the observed increase in CCN numberconcentrations. Earlier studies conducted at Barbados have mostly focused onthe role of dust on CCN, but our results show that aerosol hygroscopicity and CCN number concentrations during wintertime long-range transport events over the tropical North Atlantic are also affected by African smoke. Ourfindings highlight the importance of African smoke for atmospheric processesand cloud formation over the Caribbean. 

Abstract. In early 2020, an international team set out to investigatetrade-wind cumulus clouds and their coupling to the large-scale circulationthrough the field campaign EUREC4A: ElUcidating the RolE ofClouds-Circulation Coupling in ClimAte. Focused on the western tropicalAtlantic near Barbados, EUREC4A deployed a number of innovativeobservational strategies, including a large network of water isotopicmeasurements collectively known as EUREC4A-iso, to study the tropicalshallow convective environment. The goal of the isotopic measurements was toelucidate processes that regulate the hydroclimate state – for example, byidentifying moisture sources, quantifying mixing between atmospheric layers,characterizing the microphysics that influence the formation and persistenceof clouds and precipitation, and providing an extra constraint in theevaluation of numerical simulations. During the field experiment,researchers deployed seven water vapor isotopic analyzers on two aircraft,on three ships, and at the Barbados Cloud Observatory (BCO). Precipitationwas collected for isotopic analysis at the BCO and from aboard four ships.In addition, three ships collected seawater for isotopic analysis. All told,the in situ data span the period 5 January–22 February 2020 andcover the approximate area 6 to 16∘ N and 50 to 60∘ W,with water vapor isotope ratios measured from a few meters above sea levelto the mid-free troposphere and seawater samples spanning the ocean surfaceto several kilometers depth. This paper describes the full EUREC4A isotopic in situ data collection– providing extensive information about sampling strategies and datauncertainties – and also guides readers to complementary remotely sensedwater vapor isotope ratios. All field data have been made publicly availableeven if they are affected by known biases, as is the case for high-altitudeaircraft measurements, one of the two BCO ground-based water vapor timeseries, and select rain and seawater samples from the ships. Publication ofthese data reflects a desire to promote dialogue around improving waterisotope measurement strategies for the future. The remaining, high-qualitydata create unprecedented opportunities to close water isotopic budgets andevaluate water fluxes and their influence on cloudiness in the trade-windenvironment. The full list of dataset DOIs and notes on data quality flagsare provided in Table 3 of Sect. 5 (“Data availability”).

 

The ability of atmospheric aerosols to impact climate through water uptake and cloud formation is fundamentally determined by the size, composition, and phase (liquid, semisolid, or solid) of individual particles. Particle phase is dependent on atmospheric conditions (relative humidity and temperature) and chemical composition and, importantly, solid particles can inhibit the uptake of water and other trace gases, even under humid conditions. Particles composed primarily of ammonium sulfate are presumed to be liquid at the relative humidities (67 to 98%) and temperatures (−2 to 4 °C) of the summertime Arctic. Under these atmospheric conditions, we report the observation of solid organic-coated ammonium sulfate particles representing 30% of particles, by number, in a key size range (<0.2 µm) for cloud activation within marine air masses from the Arctic Ocean at Utqiaġvik, AK. The composition and size of the observed particles are consistent with recent Arctic modeling and observational results showing new particle formation and growth from dimethylsulfide oxidation to form sulfuric acid, reaction with ammonia, and condensation of marine biogenic sulfate and highly oxygenated organic molecules. Aqueous sulfate particles typically undergo efflorescence and solidify at relative humidities of less than 34%. Therefore, the observed solid phase is hypothesized to occur from contact efflorescence during collision of a newly formed Aitken mode sulfate particle with an organic-coated ammonium sulfate particle. With declining sea ice in the warming Arctic, this particle source is expected to increase with increasing open water and marine biogenic emissions. 

Abstract. Even though the Arctic is remote, aerosol properties observed there arestrongly influenced by anthropogenic emissions from outside the Arctic. Thisis particularly true for the so-called Arctic haze season (January throughApril). In summer (June through September), when atmospheric transportpatterns change, and precipitation is more frequent, local Arctic sources,i.e., natural sources of aerosols and precursors, play an important role.Over the last few decades, significant reductions in anthropogenic emissionshave taken place. At the same time a large body of literature shows evidencethat the Arctic is undergoing fundamental environmental changes due toclimate forcing, leading to enhanced emissions by natural processes that mayimpact aerosol properties. In this study, we analyze 9 aerosol chemical species and 4 particleoptical properties from 10 Arctic observatories (Alert, Kevo, Pallas,Summit, Thule, Tiksi, Barrow/Utqiaġvik, Villum, and Gruvebadet and ZeppelinObservatory – both at Ny-Ålesund Research Station) to understand changesin anthropogenic and natural aerosol contributions. Variables includeequivalent black carbon, particulate sulfate, nitrate, ammonium,methanesulfonic acid, sodium, iron, calcium and potassium, as well asscattering and absorption coefficients, single scattering albedo andscattering Ångström exponent. First, annual cycles are investigated, which despite anthropogenic emissionreductions still show the Arctic haze phenomenon. Second, long-term trendsare studied using the Mann–Kendall Theil–Sen slope method. We find in total41 significant trends over full station records, i.e., spanning more than adecade, compared to 26 significant decadal trends. The majority ofsignificantly declining trends is from anthropogenic tracers and occurredduring the haze period, driven by emission changes between 1990 and 2000.For the summer period, no uniform picture of trends has emerged. Twenty-sixpercent of trends, i.e., 19 out of 73, are significant, and of those 5 arepositive and 14 are negative. Negative trends include not only anthropogenictracers such as equivalent black carbon at Kevo, but also natural indicatorssuch as methanesulfonic acid and non-sea-salt calcium at Alert. Positivetrends are observed for sulfate at Gruvebadet. No clear evidence of a significant change in the natural aerosolcontribution can be observed yet. However, testing the sensitivity of theMann–Kendall Theil–Sen method, we find that monotonic changes of around 5 % yr−1 in an aerosol property are needed to detect a significanttrend within one decade. This highlights that long-term efforts well beyonda decade are needed to capture smaller changes. It is particularly importantto understand the ongoing natural changes in the Arctic, where interannualvariability can be high, such as with forest fire emissions and theirinfluence on the aerosol population. To investigate the climate-change-induced influence on the aerosolpopulation and the resulting climate feedback, long-term observations oftracers more specific to natural sources are needed, as well as of particlemicrophysical properties such as size distributions, which can be used toidentify changes in particle populations which are not well captured bymass-oriented methods such as bulk chemical composition. 

Abstract. Sea salt aerosols play an important role in the radiationbudget and atmospheric composition over the Arctic, where the climate israpidly changing. Previous observational studies have shown that Arctic sea ice leads are an important source of sea salt aerosols, and modeling efforts have also proposed blowing snow sublimation as a source. In this study,size-resolved atmospheric particle number concentrations and chemicalcomposition were measured at the Arctic coastal tundra site ofUtqiaġvik, Alaska, during spring (3 April–7 May 2016). Blowing snow conditions were observed during 25 % of the 5-week study period andwere overpredicted by a commonly used blowing snow parameterization based solely on wind speed and temperature. Throughout the study, open leads werepresent locally. During periods when blowing snow was observed, significantincreases in the number concentrations of 0.01–0.06 µm particles(factor of 6, on average) and 0.06–0.3 µm particles (67 %, on average) and a significant decrease (82 %, on average) in 1–4 µmparticles were observed compared to low wind speed periods. These size distribution changes were likely caused by the generation of ultrafineparticles from leads and/or blowing snow, with scavenging of supermicronparticles by blowing snow. At elevated wind speeds, both submicron andsupermicron sodium and chloride mass concentrations were enhanced,consistent with wind-dependent local sea salt aerosol production. Atmoderate wind speeds below the threshold for blowing snow as well as during observed blowing snow, individual sea spray aerosol particles were measured.These individual salt particles were enriched in calcium relative to sodiumin seawater due to the binding of this divalent cation with organic matter in the sea surface microlayer and subsequent enrichment during seawaterbubble bursting. The chemical composition of the surface snowpack alsoshowed contributions from sea spray aerosol deposition. Overall, theseresults show the contribution of sea spray aerosol production from leads onboth aerosols and the surface snowpack. Therefore, if blowing snowsublimation contributed to the observed sea salt aerosol, the snow beingsublimated would have been impacted by sea spray aerosol deposition rather than upward brine migration through the snowpack. Sea spray aerosol production from leads is expected to increase, with thinning and fracturingof sea ice in the rapidly warming Arctic. 

The Atlantic Tradewind Ocean-Atmosphere Mesoscale Interaction Campaign (ATOMIC) took place from 7 January to 11 July 2020 in the tropical North Atlantic between the eastern edge of Barbados and 51∘ W, the longitude of the Northwest Tropical Atlantic Station (NTAS) mooring. Measurements were made to gather information on shallow atmospheric convection, the effects of aerosols and clouds on the ocean surface energy budget, and mesoscale oceanic processes. Multiple platforms were deployed during ATOMIC including the NOAA RV Ronald H. Brown (RHB) (7 January to 13 February) and WP-3D Orion (P-3) aircraft (17 January to 10 February), the University of Colorado's Robust Autonomous Aerial Vehicle-Endurant Nimble (RAAVEN) uncrewed aerial system (UAS) (24 January to 15 February), NOAA- and NASA-sponsored Saildrones (12 January to 11 July), and Surface Velocity Program Salinity (SVPS) surface ocean drifters (23 January to 29 April). The RV Ronald H. Brown conducted in situ and remote sensing measurements of oceanic and atmospheric properties with an emphasis on mesoscale oceanic–atmospheric coupling and aerosol–cloud interactions. In addition, the ship served as a launching pad for Wave Gliders, Surface Wave Instrument Floats with Tracking (SWIFTs), and radiosondes. Details of measurements made from the RV Ronald H. Brown, ship-deployed assets, and other platforms closely coordinated with the ship during ATOMIC are provided here. These platforms include Saildrone 1064 and the RAAVEN UAS as well as the Barbados Cloud Observatory (BCO) and Barbados Atmospheric Chemistry Observatory (BACO). Inter-platform comparisons are presented to assess consistency in the data sets. Data sets from the RV Ronald H. Brown and deployed assets have been quality controlled and are publicly available at NOAA's National Centers for Environmental Information (NCEI) data archive (https://www.ncei.noaa.gov/archive/accession/ATOMIC-2020, last access: 2 April 2021). Point-of-contact information and links to individual data sets with digital object identifiers (DOIs) are provided herein.