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  • 1
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 14 ( 2022-07-29), p. 9721-9745
    Abstract: Abstract. Aerosol particles acting as cloud condensation nuclei (CCN) or ice-nucleating particles (INPs) play a major role in the formation and glaciation of clouds. Thereby they exert a strong impact on the radiation budget of the Earth. Data on abundance and properties of both types of particles are sparse, especially for remote areas of the world, such as the Southern Ocean (SO). In this work, we present unique results from ship-borne aerosol-particle-related in situ measurements and filter sampling in the SO region, carried out during the Antarctic Circumnavigation Expedition (ACE) in the austral summer of 2016–2017. An overview of CCN and INP concentrations over the Southern Ocean is provided and, using additional quantities, insights regarding possible CCN and INP sources and origins are presented. CCN number concentrations spanned 2 orders of magnitude, e.g. for a supersaturation of 0.3 % values ranged roughly from 3 to 590 cm−3. CCN showed variable contributions of organic and inorganic material (inter-quartile range of hygroscopicity parameter κ from 0.2 to 0.9). No distinct size dependence of κ was apparent, indicating homogeneous composition across sizes (critical dry diameter on average between 30 and 110 nm). The contribution of sea spray aerosol (SSA) to the CCN number concentration was on average small. Ambient INP number concentrations were measured in the temperature range from −5 to −27 ∘C using an immersion freezing method. Concentrations spanned up to 3 orders of magnitude, e.g. at −16 ∘C from 0.2 to 100 m−3. Elevated values (above 10 m−3 at −16 ∘C) were measured when the research vessel was in the vicinity of land (excluding Antarctica), with lower and more constant concentrations when at sea. This, along with results of backward-trajectory analyses, hints towards terrestrial and/or coastal INP sources being dominant close to ice-free (non-Antarctic) land. In pristine marine areas INPs may originate from both oceanic sources and/or long-range transport. Sampled aerosol particles (PM10) were analysed for sodium and methanesulfonic acid (MSA). Resulting mass concentrations were used as tracers for primary marine and secondary aerosol particles, respectively. Sodium, with an average mass concentration around 2.8 µg m−3, was found to dominate the sampled, identified particle mass. MSA was highly variable over the SO, with mass concentrations up to 0.5 µg m−3 near the sea ice edge. A correlation analysis yielded strong correlations between sodium mass concentration and particle number concentration in the coarse mode, unsurprisingly indicating a significant contribution of SSA to that mode. CCN number concentration was highly correlated with the number concentration of Aitken and accumulation mode particles. This, together with a lack of correlation between sodium mass and Aitken and accumulation mode number concentrations, underlines the important contribution of non-SSA, probably secondarily formed particles, to the CCN population. INP number concentrations did not significantly correlate with any other measured aerosol physico-chemical parameter.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2069847-1
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  • 2
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 22 ( 2019-11-27), p. 14339-14364
    Abstract: Abstract. In a warming Arctic the increased occurrence of new particle formation (NPF) is believed to originate from the declining ice coverage during summertime. Understanding the physico-chemical properties of newly formed particles, as well as mechanisms that control both particle formation and growth in this pristine environment, is important for interpreting aerosol–cloud interactions, to which the Arctic climate can be highly sensitive. In this investigation, we present the analysis of NPF and growth in the high summer Arctic. The measurements were made on-board research vessel Polarstern during the PS106 Arctic expedition. Four distinctive NPF and subsequent particle growth events were observed, during which particle (diameter in a range 10–50 nm) number concentrations increased from background values of approx. 40 up to 4000 cm−3. Based on particle formation and growth rates, as well as hygroscopicity of nucleation and the Aitken mode particles, we distinguished two different types of NPF events. First, some NPF events were favored by negative ions, resulting in more-hygroscopic nucleation mode particles and suggesting sulfuric acid as a precursor gas. Second, other NPF events resulted in less-hygroscopic particles, indicating the influence of organic vapors on particle formation and growth. To test the climatic relevance of NPF and its influence on the cloud condensation nuclei (CCN) budget in the Arctic, we applied a zero-dimensional, adiabatic cloud parcel model. At an updraft velocity of 0.1 m s−1, the particle number size distribution (PNSD) generated during nucleation processes resulted in an increase in the CCN number concentration by a factor of 2 to 5 compared to the background CCN concentrations. This result was confirmed by the directly measured CCN number concentrations. Although particles did not grow beyond 50 nm in diameter and the activated fraction of 15–50 nm particles was on average below 10 %, it could be shown that the sheer number of particles produced by the nucleation process is enough to significantly influence the background CCN number concentration. This implies that NPF can be an important source of CCN in the Arctic. However, more studies should be conducted in the future to understand mechanisms of NPF, sources of precursor gases and condensable vapors, as well as the role of the aged nucleation mode particles in Arctic cloud formation.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 23 ( 2020-12-08), p. 15191-15206
    Abstract: Abstract. Ambient concentrations of ice-forming particles measured during ship expeditions are collected and summarised with the aim of determining the spatial distribution and variability in ice nuclei in oceanic regions. The presented data from literature and previously unpublished data from over 23 months of ship-based measurements stretch from the Arctic to the Southern Ocean and include a circumnavigation of Antarctica. In comparison to continental observations, ship-based measurements of ambient ice nuclei show 1 to 2 orders of magnitude lower mean concentrations. To quantify the geographical variability in oceanic areas, the concentration range of potential ice nuclei in different climate zones is analysed by meridionally dividing the expedition tracks into tropical, temperate and polar climate zones. We find that concentrations of ice nuclei in these meridional zones follow temperature spectra with similar slopes but vary in absolute concentration. Typically, the frequency with which specific concentrations of ice nuclei are observed at a certain temperature follows a log-normal distribution. A consequence of the log-normal distribution is that the mean concentration is higher than the most frequently measured concentration. Finally, the potential contribution of ship exhaust to the measured ice nuclei concentration on board research vessels is analysed as function of temperature. We find a sharp onset of the influence at approximately −36 ∘C but none at warmer temperatures that could bias ship-based measurements.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
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  • 4
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 3 ( 2020-02-06), p. 1431-1449
    Abstract: Abstract. In the framework of the MarParCloud (Marine biological production, organic aerosol particles and marine clouds: a Process Chain) project, measurements were carried out on the islands of Cabo Verde (a.k.a. Cape Verde) to investigate the abundance, properties and sources of aerosol particles in general, and cloud condensation nuclei (CCN) in particular, both close to sea level and at the cloud level. A thorough comparison of particle number concentration (PNC), particle number size distribution (PNSD) and CCN number concentration (NCCN) at the Cape Verde Atmospheric Observatory (CVAO, sea-level station) and Monte Verde (MV, cloud-level station) reveals that during times without clouds the aerosols at CVAO and MV are similar and the boundary layer is generally well mixed. Therefore, data obtained at CVAO can be used to describe the aerosol particles at cloud level. Cloud events were observed at MV during roughly 58 % of the time, and during these events a large fraction of particles was activated to cloud droplets. A trimodal parameterization method was deployed to characterize PNC at CVAO. Based on number concentrations in different aerosol modes, four well-separable types of PNSDs were found, which were named the marine type, mixture type, dust type1 and dust type2. Aerosol particles differ depending on their origins. When the air masses came from the Atlantic Ocean, sea spray can be assumed to be one source for particles besides new particle formation. For these air masses, PNSDs featured the lowest number concentration in Aitken, accumulation and coarse modes. Particle number concentrations for sea spray aerosol (SSA, i.e., the coarse mode for these air masses) accounted for about 3.7 % of NCCN,0.30 % (CCN number concentration at 0.30 % supersaturation) and about 1.1 % to 4.4 % of Ntotal (total particle number concentration). When the air masses came from the Sahara, we observed enhanced Aitken, accumulation and coarse mode particle number concentrations and overall increased NCCN; NCCN,0.30 % during the strongest observed dust periods is about 2.5 times higher than that during marine periods. However, the particle hygroscopicity parameter κ for these two most different periods shows no significant difference and is generally similar, independent of air mass. Overall, κ averaged 0.28, suggesting the presence of organic material in particles. This is consistent with previous model work and field measurements. There is a slight increase in κ with increasing particle size, indicating the addition of soluble, likely inorganic, material during cloud processing.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2069847-1
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