Search

Few studies have investigated the impact of new particle formation (NPF) on cloud condensation nuclei (CCN) in remote Antarctica, and none has elucidated the relationship between NPF and CCN production. To address that knowledge gap, we continuously measured the number size distribution of 2.5–300 nm particles and CCN number concentrations at King Sejong Station on the Antarctic Peninsula from 1 January to 31 December 2018. Ninety-seven NPF events were detected throughout the year. Clear annual and seasonal patterns of NPF were observed: high concentration and frequency of nucleation-mode particles in summer (December–February: 53 NPF cases) and undetected nucleation-mode particles in winter (June–August: no NPF cases). We estimated the spatial scale of NPF by multiplying the time during which a distinct nucleation mode can be observed at the sampling site by the locally measured wind speed. The estimated median spatial scale of NPF around the Antarctic Peninsula was found to be approximately 155 km, indicating the large scale of NPF events. Air back-trajectory analysis revealed that 80 cases of NPF events were associated with air masses originating over the ocean, followed by sea-ice (12 cases), multiple (3 cases), and land (2 cases) regions. We present and discuss three major NPF categories: (1) marine NPF, (2) sea-ice NPF, and (3) multiple NPF. Satellite estimates for sea-surface dimethylsulfoniopropionate (DMSP; a precursor of gaseous dimethyl sulfide) data showed that the production of oceanic biogenic precursors could be a key component in marine NPF events, whereas halogen compounds released from ice-covered areas could contribute to sea-ice NPF events. Terrestrial sources (wildlife colonies, vegetation, and meltwater ponds) from Antarctica could affect aerosol production in multiple air masses. Out of 97 observed NPF events, 83 cases were characterized by the simultaneous increase in the CCN concentration by 2 %–270 % (median 44 %) in the following 1 to 36 h (median 8 h) after NPF events. Overall, Antarctic NPF events were found to be a significant source of particles with different physical characteristics and related to biogenic sources in and around the Antarctic Peninsula, which subsequently grew to cloud condensation nuclei.

This paper presents the results of 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). 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 dimethylsufoniopropionate (DMSP) concentration in seawater, atmospheric DMS remains low, probably due to its fast biological turnover in seawater in this period. The intensity and timing of the DMS evolution during the two years suggest 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 us 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 air masses with low DMS content, an enrichment of nssSO42- with respect to MSA, is observed. We estimate that the mean contribution of freshly formed biogenic aerosol 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 for long-term measurements of seawater and atmospheric DMS and biogenic aerosol along the Antarctic coast and in the Southern Ocean.

The Zeppelin Observatory (78.90∘ N, 11.88∘ E) is located on Zeppelin Mountain at 472 m a.s.l. on Spitsbergen, the largest island of the Svalbard archipelago. Established in 1989, the observatory is part of Ny-Ålesund Research Station and an important atmospheric measurement site, one of only a few in the high Arctic, and a part of several European and global monitoring programmes and research infrastructures, notably the European Monitoring and Evaluation Programme (EMEP); the Arctic Monitoring and Assessment Programme (AMAP); the Global Atmosphere Watch (GAW); the Aerosol, Clouds and Trace Gases Research Infrastructure (ACTRIS); the Advanced Global Atmospheric Gases Experiment (AGAGE) network; and the Integrated Carbon Observation System (ICOS). The observatory is jointly operated by the Norwegian Polar Institute (NPI), Stockholm University, and the Norwegian Institute for Air Research (NILU). Here we detail the establishment of the Zeppelin Observatory including historical measurements of atmospheric composition in the European Arctic leading to its construction. We present a history of the measurements at the observatory and review the current state of the European Arctic atmosphere, including results from trends in greenhouse gases, chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs), other traces gases, persistent organic pollutants (POPs) and heavy metals, aerosols and Arctic haze, and atmospheric transport phenomena, and provide an outline of future research directions.

Seasonal to interannual variations in the concentrations of sulfur aerosols (< 2.5 µm in diameter; non sea-salt sulfate: NSS-SO42-; anthropogenic sulfate: Anth-SO42-; biogenic sulfate: Bio-SO42-; methanesulfonic acid: MSA) in the Arctic atmosphere were investigated using measurements of the chemical composition of aerosols collected at Ny-Ålesund, Svalbard (78.9∘ N, 11.9∘ E) from 2015 to 2019. In all measurement years the concentration of NSS-SO42- was highest during the pre-bloom period and rapidly decreased towards summer. During the pre-bloom period we found a strong correlation between NSS-SO42- (sum of Anth-SO42- and Bio-SO42-) and Anth-SO42-. This was because more than 50 % of the NSS-SO42- measured during this period was Anth-SO42-, which originated in northern Europe and was subsequently transported to the Arctic in Arctic haze. Unexpected increases in the concentration of Bio-SO42- aerosols (an oxidation product of dimethylsulfide: DMS) were occasionally found during the pre-bloom period. These probably originated in regions to the south (the North Atlantic Ocean and the Norwegian Sea) rather than in ocean areas in the proximity of Ny-Ålesund. Another oxidation product of DMS is MSA, and the ratio of MSA to Bio-SO42- is extensively used to estimate the total amount of DMS-derived aerosol particles in remote marine environments. The concentration of MSA during the pre-bloom period remained low, primarily because of the greater loss of MSA relative to Bio-SO42- and the suppression of condensation of gaseous MSA onto particles already present in air masses being transported northwards from distant ocean source regions (existing particles). In addition, the low light intensity during the pre-bloom period resulted in a low concentration of photochemically activated oxidant species including OH radicals and BrO; these conditions favored the oxidation pathway of DMS to Bio-SO42- rather than to MSA, which acted to lower the MSA concentration at Ny-Ålesund. The concentration of MSA peaked in May or June and was positively correlated with phytoplankton biomass in the Greenland and Barents seas around Svalbard. As a result, the mean ratio of MSA to the DMS-derived aerosols was low (0.09 ± 0.07) in the pre-bloom period but high (0.32 ± 0.15) in the bloom and post-bloom periods. There was large interannual variability in the ratio of MSA to Bio-SO42- (i.e., 0.24 ± 0.11 in 2017, 0.40 ± 0.14 in 2018, and 0.36 ± 0.14 in 2019) during the bloom and post-bloom periods. This was probably associated with changes in the chemical properties of existing particles, biological activities surrounding the observation site, and air mass transport patterns. Our results indicate that MSA is not a conservative tracer for predicting DMS-derived particles, and the contribution of MSA to the growth of newly formed particles may be much larger during the bloom and post-bloom periods than during the pre-bloom period.

We conducted continuous measurements of nanoparticles down to 3 nm size in the Arctic at Mount Zeppelin, Ny Ålesund, Svalbard, from October 2016 to December 2018, providing a size distribution of nanoparticles (3–60 nm). A significant number of nanoparticles as small as 3 nm were often observed during new particle formation (NPF), particularly in summer, suggesting that these were likely produced near the site rather than being transported from other regions after growth. The average NPF frequency per year was 23 %, having the highest percentage in August (63 %). The average formation rate (J) and growth rate (GR) for 3–7 nm particles were 0.04 cm−3 s−1 and 2.07 nm h−1, respectively. Although NPF frequency in the Arctic was comparable to that in continental areas, the J and GR were much lower. The number of nanoparticles increased more frequently when air mass originated over the south and southwest ocean regions; this pattern overlapped with regions having strong chlorophyll a concentration and dimethyl sulfide (DMS) production capacity (southwest ocean) and was also associated with increased NH3 and H2SO4 concentration, suggesting that marine biogenic sources were responsible for gaseous precursors to NPF. Our results show that previously developed NPF occurrence criteria (low loss rate and high cluster growth rate favor NPF) are also applicable to NPF in the Arctic.

There are few shipborne observations addressing the factors influencing the relationships of the formation and growth of aerosol particles with cloud condensation nuclei (CCN) in remote marine environments. In this study, the physical properties of aerosol particles throughout the Arctic Ocean and Pacific Ocean were measured aboard the Korean icebreaker R/V Araon during the summer of 2017 for 25 d. A number of new particle formation (NPF) events and growth were frequently observed in both Arctic terrestrial and Arctic marine air masses. By striking contrast, NPF events were not detected in Pacific marine air masses. Three major aerosol categories are therefore discussed: (1) Arctic marine (aerosol number concentration CN2.5: 413±442 cm−3), (2) Arctic terrestrial (CN2.5: 1622±1450 cm−3) and (3) Pacific marine (CN2.5: 397±185 cm−3), following air mass back-trajectory analysis. A major conclusion of this study is not only that the Arctic Ocean is a major source of secondary aerosol formation relative to the Pacific Ocean but also that open-ocean sympagic and terrestrially influenced coastal ecosystems both contribute to shaping aerosol size distributions. We suggest that terrestrial ecosystems – including river outflows and tundra – strongly affect aerosol emissions in the Arctic coastal areas, possibly more than anthropogenic Arctic emissions. The increased river discharge, tundra emissions and melting sea ice should be considered in future Arctic atmospheric composition and climate simulations. The average CCN concentrations at a supersaturation ratios of 0.4 % were 35±40 cm−3, 71±47 cm−3 and 204±87 cm−3 for Arctic marine, Arctic terrestrial and Pacific marine aerosol categories, respectively. Our results aim to help evaluate how anthropogenic and natural atmospheric sources and processes affect the aerosol composition and cloud properties.

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-range-transported – 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 north-eastern 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 processes 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.

Marine biota is an important source of atmospheric aerosol particles in the remote marine atmosphere. However, the relationship between new particle formation and marine biota is poorly quantified. Long-term observations (from 2009 to 2016) of the physical properties of atmospheric aerosol particles measured at the Antarctic Peninsula (King Sejong Station; 62.2∘ S, 58.8∘ W) and satellite-derived estimates of the biological characteristics were analyzed to identify the link between new particle formation and marine biota. New particle formation events in the Antarctic atmosphere showed distinct seasonal variations, with the highest values occurring when the air mass originated from the ocean domain during the productive austral summer (December, January and February). Interestingly, new particle formation events were more frequent in the air masses that originated from the Bellingshausen Sea than in those that originated from the Weddell Sea. The monthly mean number concentration of nanoparticles (2.5–10 nm in diameter) was >2-fold higher when the air masses passed over the Bellingshausen Sea than the Weddell Sea, whereas the biomass of phytoplankton in the Weddell Sea was more than ∼70 % higher than that of the Bellingshausen Sea during the austral summer period. Dimethyl sulfide (DMS) is of marine origin and its oxidative products are known to be one of the major components in the formation of new particles. Both satellite-derived estimates of the biological characteristics (dimethylsulfoniopropionate, DMSP; precursor of DMS) and phytoplankton taxonomic composition and in situ methanesulfonic acid (84 daily measurements during the summer period in 2013 and 2014) analysis revealed that DMS(P)-rich phytoplankton were more dominant in the Bellingshausen Sea than in the Weddell Sea. Furthermore, the number concentration of nanoparticles was positively correlated with the biomass of phytoplankton during the period when DMS(P)-rich phytoplankton predominate. These results indicate that oceanic DMS emissions could play a key role in the formation of new particles; moreover, the taxonomic composition of phytoplankton could affect the formation of new particles in the Antarctic Ocean.

The physical characteristics of aerosol particles during particle bursts observed at King Sejong Station in the Antarctic Peninsula from March 2009 to December 2016 were analyzed. This study focuses on the seasonal variation in parameters related to particle formation such as the occurrence, formation rate (FR) and growth rate (GR), condensation sink (CS) and source rate of condensable vapor. The number concentrations during new particle formation (NPF) events varied from 1707 to 83 120 cm−3, with an average of 20 649 ± 9290 cm−3, and the duration of the NPF events ranged from 0.6 to 14.4 h, with a mean of 4.6±1.5 h. The NPF event dominantly occurred during austral summer period (∼72 %). The measured mean values of FR and GR of the aerosol particles were 2.79±1.05 cm−3 s−1 and 0.68±0.27 nm h−1, respectively, showing enhanced rates in the summer season. The mean value of FR at King Sejong Station was higher than that at other sites in Antarctica, at 0.002–0.3 cm−3 s−1, while those of growth rates were relatively similar to the results observed by previous studies, at 0.4–4.3 nm h−1. The derived average values of CS and source rate of condensable vapor were (6.04±2.74)×10-3 s−1 and (5.19±3.51)×104 cm−3 s−1, respectively. The contribution of particle formation to cloud condensation nuclei (CCN) concentration was also investigated. The CCN concentration during the NPF period increased by approximately 11 % compared with the background concentration. In addition, the effects of the origin and pathway of air masses on the characteristics of aerosol particles during a NPF event were determined. The FRs were similar regardless of the origin and pathway, whereas the GRs of particles originating from the Antarctic Peninsula and the Bellingshausen Sea, at 0.77±0.25 and 0.76±0.30 nm h−1, respectively, were higher than those of particles originating from the Weddell Sea (0.41±0.15 nm h−1).

Seasonal variability in the physical characteristics of aerosol particles sampled from the King Sejong Station in the Antarctic Peninsula was investigated over the period between March 2009 and February 2015. Clear seasonal cycles for the total particle concentration (CN) were observed. The mean monthly concentration of particles larger than 2.5 nm (CN2.5) was highest during the austral summer, with an average value of 1080.39 ± 595.05 cm−3, and lowest during the austral winter, with a mean value of 197.26 ± 71.71 cm−3. The seasonal patterns in the concentrations of cloud condensation nuclei (CCN) and CN coincide, with both concentrations being at a minimum in winter and maximum in summer. The measured CCN spectra were approximated by fitting a power-law function relating the number of CCN for a given supersaturation (SS) to each SS value, with fitting coefficients C and kT. The values for C varied from 6.35 to 837.24 cm−3, with a mean of 171.48 ± 62.00 cm−3. The values for kT ranged from 0.07 to 2.19, with a mean of 0.41 ± 0.10. In particular, the kT values during the austral summer were higher than those during the winter, indicating that aerosol particles are more sensitive to SS changes during summer. Furthermore, the annual mean hygroscopicity parameter, κ, was estimated as 0.15 ± 0.05, for a SS of 0.4 %. The effects of the origin and pathway travelled by the air mass on the physical characteristics of the aerosol particles were also determined. The modal diameter of aerosol particles originating in the South Pacific Ocean showed a seasonal variation varying from 0.023 µm in winter to 0.034 µm in summer for the Aitken mode, and from 0.086 µm in winter to 0.109 µm in summer for the accumulation mode.

The connection between marine biogenic dimethyl sulfide (DMS) and the formation of aerosol particles in the Arctic atmosphere was evaluated by analyzing atmospheric DMS mixing ratio, aerosol particle size distribution and aerosol chemical composition data that were concurrently collected at Ny-Ålesund, Svalbard (78.5° N, 11.8° E), during April and May 2015. Measurements of aerosol sulfur (S) compounds showed distinct patterns during periods of Arctic haze (April) and phytoplankton blooms (May). Specifically, during the phytoplankton bloom period the contribution of DMS-derived SO42− to the total aerosol SO42− increased by 7-fold compared with that during the proceeding Arctic haze period, and accounted for up to 70 % of fine SO42− particles (42− aerosols was significantly associated with an increase in the atmospheric DMS mixing ratio. More importantly, two independent estimates of the formation of DMS-derived SO42− aerosols, calculated using the stable S-isotope ratio and the non-sea-salt SO42− ∕ methanesulfonic acid ratio, respectively, were in close agreement, providing compelling evidence that the contribution of biogenic DMS to the formation of aerosol particles was substantial during the Arctic phytoplankton bloom period.