The Effect of Seawater Salinity and Seawater Temperature on Sea Salt Aerosol Production

2022 | J. Geophys. Res.-Atmos. | 127

To improve our understanding of the impact of sea salt aerosols (SSA) on the Earth's climate, it is critical to understand the physical mechanisms which determine the size-resolved SSA production flux. Of the factors affecting SSA emissions, seawater salinity has perhaps received the least attention in the literature and previous studies have produced conflicting results. Here, we present a series of laboratory experiments designed to investigate the role of salinity on aerosol production from artificial seawater using a continuous plunging jet. During these experiments, the aerosol and surface bubble size distributions were monitored while the salinity was decreased from 35 to 0 g kg−1. Three distinct salinity regimes were identified: (a) A high salinity regime, 10–35 g kg−1, where lower salinity resulted in only minor reductions in particle number flux but notable reductions in particle volume flux; (b) an intermediate salinity regime, 5–10 g kg−1, with a local maximum in particle number flux; (c) a low salinity regime, <5 g kg−1, characterized by a rapid decrease in particle number flux at lower salinities and dominated by small particles and larger bubbles. We discuss the implications of our results through comparison of the size-resolved aerosol flux and the surface bubble population at different salinities. Finally, by varying the seawater temperature at three specific salinities we have also developed a simple parameterization of the particle production flux as a function of seawater temperature and salinity. The range of seawater salinity and temperature studied is representative of the global oceans and lower salinity water bodies such as the Baltic Sea.

Airborne and marine microplastics from an oceanographic survey at the Baltic Sea: an emerging role of air-sea interaction?

Luca Ferrero; Lorenzo Scibetta; Piotr Markuszewski; Mikolaj Mazurkiewic; Violetta Drozdowska; Przemyslaw Makuch; Patrycja Jutzenka-Trzbiatowska; Adriana Zaleska-Medynska; Sergio Ando; Franscesco Seliu; ; E. Douglas Nilsson; Ezio Bolzacchini
2022 | Sci. Total Environ. | 824 (153709) (1-16)
air-sea interaction , atmosphere , baltic salmon , Microplastic , sea

Microplastics (MPs) pollution is one of the most important problems of the Earth. They have been found in all the natural
environments, including oceans and the atmosphere. In this study, the concentrations of both atmospheric and
marine MPs were measured over the Baltic along a research cruise that started in the Gdansk harbour, till the Gotland
island, and the way back. A deposition box (based on a combination of active/passive sampling) was used to collect
airborne MPs while, marine MPs concentrations were investigated during the cruise using a dedicated net. Ancillary
data were obtained using a combination of particle counters (OPC, LAS and CPC), Aethalometer (AE33 Magee Scientific),
spectrofluorometer (sea surface samples, Varian Cary Eclipse), and meteorological sensors. Results showed airborne
microplastics average concentrations higher in the Gdansk harbour (161 ± 75 m−3) compared to the open
Baltic Sea and to the Gotland island (24± 9 and 45 ±20 m−3). These latter values are closer to the ones measured
in the sea (79±18m−3). The MPs composition was investigated using μ-Raman (for the airborne ones) and FTIR (for marine ones); similar results (e.g. polyethylene, polyethylene terephthalates, polyurethane) were found in the two environmental

<compartments. The concentrations and sd<dimilar composition in air and sea suggested a linkag e between
the two compartments. For this purpose, the atmospheric MPs' equivalent aerodynamic diameter was calculated (28
±3μm) first showing the capability of atmospheric MPs to remain suspended in the air. At the same time, the computed
turnover times (0.3–90 h; depending on MPs size) limited the transport distance range. The estimated M-^Ps sea emission fluxes (4–18 ∗ 10^-6 μm^3 m−2 s−1 range) finally showed the contemporary presence of atmospheric transport
together with a continuous emission fromthe sea surface enabling a grasshopper long-range transport ofmicroplastics
across the sea.

Atmospheric ageing of inorganic sea spray aerosol: implications for hygroscopicity and cloud activation potential

Bernadette Rosati; Sigurd Christiansen; Anders Dinesen; Pontus Roldin; Andreas Massling; E. Douglas Nilsson; Merete Bilde
2021 | Sci Rep | 11 (10008) (1-13)

Sea spray aerosol (SSA) contributes significantly to natural aerosol particle concentrations globally, in marine areas even
dominantly. The potential changes of the omnipresent inorganic fraction of SSA due to atmospheric ageing is largely unexplored.
We demonstrate that ageing of liquid NaCl and artificial sea salt aerosol by exposure to ozone and UV light leads to a substantial
decrease in hygroscopicity and cloud activation potential. The results point towards surface reactions that are more crucial
for small particles and the formation of salt structures with water bound within the aerosols, termed hydrates. Our findings
suggest an increased formation of hydrate forming salts during ageing and the presence of hydrates in dried SSA. Field
observations indicate a reduced hygroscopic growth of sub-micrometre SSA in the marine atmosphere compared to pure NaCl gfgddwhich is typically attributed to organic matter or sulphates. Aged inorganic sea salt offers an additional explanation for reduced
hygroscopicity and cloud activation potential.

Baltic Sea Spray Emissions: In Situ Eddy Covariance Fluxes vs. Simulated Tank Sea Spray

Nilsson, E. Douglas ; Hultin, Kim A.H.; Mårtensson, E. Monica; Markuszewski, Piotr; Rosman, Kai; Krejci, Radovan
2021 | ATMOSPHERE | 12(2) (274) (1-33)
sea spray; eddy covariance; Baltic Sea; sea spray flux; organic sea spray; brackish water; organic surfactants

We present the first ever evaluation of sea spray aerosol eddy covariance (EC) fluxes at near coastal conditions and with limited fetch, and the first over water with brackish water (on aver-age 7 ppt). The measurements were made on the island of Garpen in the Baltic Sea (56°23’ N, 16°06’ E) in September 2005. We found that wind speed is a major factor that is driving an expo-nential increase in sea spray sea salt emissions, comparable to previous studies over waters with higher salinity. We were able to show that the inclusion of a thermodenuder in the EC system al-lowed for the parallel measurements of the dry unheated aerosol flux (representing both organic and sea salt sea spray emissions) and the heated (300 ˚C) non-volatile sea salt emissions. This study’s experimental approach also included measurements of the artificial sea spray formed in a tank in locally sampled water at the same location as the EC fluxes. We attempted to use the EC aerosol flux measurements to scale the tank measurements to aerosol emissions in order to derive a complete size distribution for the sea spray emission fluxes below the size range (0.3–2 µm dry diameter) of the optical particle counters (OPCs) in the EC system, covering in total 0.01 µm to 2 µm diameter. In the wind directions with long fetches (corresponding to conditions similar to open sea), we were able to distinguish between the aerosol emission fluxes of dry aerosol and heated non-volatile (sea salt only) in the smallest size bins of the OPC, and could therefore indi-rectly estimate the organic sea spray fraction. In agreement with several previous ambient and tank experiments deriving the size resolved chemical mass concentration of sea salt and wa-ter-insoluble organic sea spray, our EC fluxes showed that sea sprays were dominated by sea salt at sizes ≥1 µm diameter, and by organics at the smallest OPC sizes. Since we used direct measures of the sea spray emission fluxes, we confirmed previous suggestions that this size distribution of sea salt and organics is a signature of sea spray aerosols. We were able to show that two sea salt source parameterizations (Mårtensson et al. (2003) and Salter et al. (2015)) agreed fairly well with our observed heated EC aerosol emission fluxes, as long as their predicted emissions were modi-fied for the actual salinity by shifting the particle diameters proportionally to the cubic rote of the salinity. If, in addition, we added organics to the parameterized sea spray following the mono-layer model by Ellison et al. (1999), the combined sea spray parameterizations for sea salt and organics fell reasonably close to the observed fluxes for diameters > 0.15 µm, while one of them overpredicted the sea spray emissions below this size. The organic mono-layer model by El-lison et al. appeared to be able to explain most of the differences we observed between the aerosol emission fluxes with and without the thermodenuder.

The impact of atmospheric oxidation on hygroscopicity and cloud droplet activation of inorganic sea spray aerosol

Rosati, B; Christiansen, S; Dinesen, A; Roldin, P; Massling, A; Nilsson, ED; Bilde, M
2021 | Sci Rep | 11 (1)
condensation nuclei , knudsen cell , optical-properties , ozone oxidation , particles , perchlorate production , primary marine aerosol , salt , secondary organic aerosol , water-uptake
Sea spray aerosol (SSA) contributes significantly to natural aerosol particle concentrations globally, in marine areas even dominantly. The potential changes of the omnipresent inorganic fraction of SSA due to atmospheric ageing is largely unexplored. In the atmosphere, SSA may exist as aqueous phase solution droplets or as dried solid or amorphous particles. We demonstrate that ageing of liquid NaCl and artificial sea salt aerosol by exposure to ozone and UV light leads to a substantial decrease in hygroscopicity and cloud activation potential of the dried particles of the same size. The results point towards surface reactions on the liquid aerosols that are more crucial for small particles and the formation of salt structures with water bound within the dried aerosols, termed hydrates. Our findings suggest an increased formation of hydrate forming salts during ageing and the presence of hydrates in dried SSA. Field observations indicate a reduced hygroscopic growth factor of sub-micrometre SSA in the marine atmosphere compared to fresh laboratory generated NaCl or sea salt of the same dry size, which is typically attributed to organic matter or sulphates. Aged inorganic sea salt offers an additional explanation for such a measured reduced hygroscopic growth factor and cloud activation potential.

Using land-based stations for air–sea interaction studies

Rutgersson, A.; Pettersson, H.; Nilsson, E.; Bergström, H.; Wallin, M. B.; Nilsson, E. D.; Sahlée, E.; Wu., L.; Mårtensson, E. M.
2019 | Tellus | A (72: 1) (1-23)

In situ measurements representing the marine atmosphere and air–sea interaction
are taken at ships, buoys, stationary moorings and land-based towers, where
each observation platform has structural restrictions. Air–sea fluxes are often
small, and due to the limitations of the sensors, several corrections are applied.
Land-based towers are convenient for long-term observations, but one critical
aspect is the representativeness of marine conditions. Hence, a careful analysis
of the sites and the data is necessary. Based on the concept of flux footprint, we
suggest defining flux data from land-based marine micrometeorological sites in
categories depending on the type of land influence:
1) CAT1: Marine data representing open sea,
2) CAT2: Disturbed wave field resulting in physical properties different
from open sea conditions and heterogeneity of water properties in the footprint
region, and
3) CAT3: Mixed land–sea footprint, very heterogeneous conditions and
possible active carbon production/consumption.
Characterization of data would be beneficial for combined analyses using
several sites in coastal and marginal seas and evaluation/comparison of
properties and dynamics. Aerosol fluxes are a useful contribution to
characterizing a marine micrometeorological field station; for most conditions,
they change sign between land and sea sectors.
Measured fluxes from the land-based marine station Östergarnsholm are used as
an example of a land-based marine site to evaluate the categories and to present
an example of differences between open sea and coastal conditions.
At the Östergarnsholm site the surface drag is larger for CAT2 and CAT3 than
for CAT1 when wind speed is below 10 m/s. The heat and humidity fluxes show
a distinctive distinguished seasonal cycle; latent heat flux is larger for CAT2 and
CAT3 compared to CAT1. The flux of carbon dioxide is large from the coastal
and land–sea sectors, showing a large seasonal cycle and significant variability (compared to the open sea sector). Aerosol fluxes are partly dominated by sea
spray emissions comparable to those observed at other open sea conditions.

Concerns of young protesters are justified

Gregor Hagedorn; Peter Kalmus; Michael Mann; Sara Vicca; Joke Van den Berge; Jean-Pascal van Ypersele; Dominique Bourg; Jan Rotmans; Roope Kaaronen; Stefan Rahmstorf; Helga Kromp-Kolb; Gottfried Kirchengast; Reto Knutti; Sonia I. Seneviratne; Philippe Thalmann; Raven Cretney; Alison Green; Kevin Anderson; Martin Hedberg; Douglas Nilsson; Amita Kuttner; Katharine Hayhoe
2019 | Science | 364 (6436) (139-140)

Global transport of perfluoralkyl acids via sea spray aerosol

2019 | Environ. Sci.-Process Impacts | 21 (4) (635-649)

Perfluoroalkyl acids (PFAAs) are persistent organic pollutants found throughout the world's oceans. Previous
research suggests that long-range atmospheric transport of these substances may be substantial. However,
it remains unclear what the main sources of PFAAs to the atmosphere are. We have used a laboratory sea
spray chamber to study water-to-air transfer of 11 PFAAs via sea spray aerosol (SSA). We observed significant
enrichment of all PFAAs relative to sodium in the SSA generated. The highest enrichment was observed in
aerosols with aerodynamic diameter < 1.6 mm, which had aerosol PFAA concentrations up to 62 000 times
higher than the PFAA water concentrations in the chamber. In surface microlayer samples collected from
the sea spray chamber, the enrichment of the substances investigated was orders of magnitude smaller
than the enrichment observed in the aerosols. In experiments with mixtures of structural isomers,
a lower contribution of branched PFAA isomers was observed in the surface microlayer compared to the
bulk water. However, no clear trend was observed in the comparison of structural isomers in SSA and
bulk water. Using the measured enrichment factors of perfluorooctanoic acid and perfluorooctane
sulfonic acid versus sodium we have estimated global annual emissions of these substances to the
atmosphere via SSA as well as their global annual deposition to land areas. Our experiments suggest that
SSA may currently be an important source of these substances to the atmosphere and, over certain
areas, to terrestrial environments.

Interactions between the atmosphere, cryosphere, and ecosystems at northern high latitudes

Boy, M; Thomson, ES; Navarro, JCA; Arnalds, O; Batchvarova, E; Back, J; Berninger, F; Bilde, M; Brasseur, Z; Dagsson-Waldhauserova, P; Castarede, D; Dalirian, M; de Leeuw, G; Dragosics, M; Duplissy, EM; Duplissy, J; Ekman, AML; Fang, KY; Gallet, JC; Glasius, M; Gryning, SE; Grythe, H; Hansson, HC; Hansson, M; Isaksson, E; Iversen, T; Jonsdottir, I; Kasurinen, V; Kirkevag, A; Korhola, A; Krejci, R; Kristjansson, JE; Lappalainen, HK; Lauri, A; Lepparanta, M; Lihavainen, H; Makkonen, R; Massling, A; Meinander, O; Nilsson, ED; Olafsson, H; Pettersson, JBC; Prisle, NL; Riipinen, I; Roldin, P; Ruppel, M; Salter, M; Sand, M; Seland, O; Seppa, H; Skov, H; Soares, J; Stohl, A; Strom, J; Svensson, J; Swietlicki, E; Tabakova, K; Thorsteinsson, T; Virkkula, A; Weyhenmeyer, GA; Wu, YS; Zieger, P; Kulmala, M
2019 | Atmos. Chem. Phys. | 19 (3) (2015-2061)
aerosol-climate interactions , biogenic volatile emissions , black carbon deposition , boreal forest , cloud droplet activation , earth system model , elemental carbon , eurasian experiment peex , organic compounds , sea-ice conditions

The Nordic Centre of Excellence CRAICC (Cryosphere-Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011-2016, is the largest joint Nordic research and innovation initiative to date, aiming to strengthen research and innovation regarding climate change issues in the Nordic region. CRAICC gathered more than 100 scientists from all Nordic countries in a virtual centre with the objectives of identifying and quantifying the major processes controlling Arctic warming and related feedback mechanisms, outlining strategies to mitigate Arctic warming, and developing Nordic Earth system modelling with a focus on short-lived climate forcers (SLCFs), including natural and anthropogenic aerosols. The outcome of CRAICC is reflected in more than 150 peer-reviewed scientific publications, most of which are in the CRAICC special issue of the journal Atmospheric Chemistry and Physics. This paper presents an overview of the main scientific topics investigated in the centre and provides the reader with a state-of-the-art comprehensive summary of what has been achieved in CRAICC with links to the particular publications for further detail. Faced with a vast amount of scientific discovery, we do not claim to completely summarize the results from CRAICC within this paper, but rather concentrate here on the main results which are related to feedback loops in climate change-cryosphere interactions that affect Arctic amplification.

Calcium enrichment in sea spray aerosol particles

Salter, M.; Hamacher-Barth, E.; Leck, C.; Werner, J.; Johnson, C.; Riipinen, I.; Nilsson, D.; Zieger, P.
2016 | Geophys Res Lett

Sea spray aerosol particles are an integral part of the Earth's radiation budget. To date, the inorganic composition of nascent sea spray aerosol particles have widely been assumed to be equivalent to the inorganic composition of seawater. Here we challenge this assumption using a laboratory sea spray chamber containing both natural and artificial seawater, as well as with ambient aerosol samples collected over the central Arctic Ocean during summer. We observe significant enrichment of calcium in submicrometer (<1μm in diameter) sea spray aerosol particles when particles are generated from both seawater sources in the laboratory as well as in the ambient aerosols samples. We also observe a tendency for increasing calcium enrichment with decreasing particle size. Our results suggest that calcium enrichment in sea spray aerosol particles may be environmentally significant with implications for our understanding of sea spray aerosol, its impact on Earth's climate, as well as the chemistry of the marine atmosphere.

An empirically derived inorganic sea spray source function incorporating sea surface temperature

Salter, M. E.; Zieger, P.; Acosta Navarro, J. C.; Grythe, H.; Kirkevag, A.; Rosati, B.; Riipinen, I.; Nilsson, E. D.
2015 | Atmos. Chem. Phys. | 15 (11047-11066)

We have developed an inorganic sea spray source function that is based upon state-of-the-art measurements of sea spray aerosol production using a temperature-controlled plunging jet sea spray aerosol chamber. The size-resolved particle production was measured between 0.01 and 10 μm dry diameter. Particle production decreased non-linearly with increasing seawater temperature (between −1 and 30 °C) similar to previous findings. In addition, we observed that the particle effective radius, as well as the particle surface, particle volume and particle mass, increased with increasing seawater temperature due to increased production of particles with dry diameters greater than 1 μm. By combining these measurements with the volume of air entrained by the plunging jet we have determined the size-resolved particle flux as a function of air entrainment. Through the use of existing parameterisations of air entrainment as a function of wind speed, we were subsequently able to scale our laboratory measurements of particle production to wind speed. By scaling in this way we avoid some of the difficulties associated with defining the "white area" of the laboratory whitecap – a contentious issue when relating laboratory measurements of particle production to oceanic whitecaps using the more frequently applied whitecap method.

The here-derived inorganic sea spray source function was implemented in a Lagrangian particle dispersion model (FLEXPART – FLEXible PARTicle dispersion model). An estimated annual global flux of inorganic sea spray aerosol of 5.9 ± 0.2 Pg yr−1 was derived that is close to the median of estimates from the same model using a wide range of existing sea spray source functions. When using the source function derived here, the model also showed good skill in predicting measurements of Na+ concentration at a number of field sites further underlining the validity of our source function.

In a final step, the sensitivity of a large-scale model (NorESM – the Norwegian Earth System Model) to our new source function was tested. Compared to the previously implemented parameterisation, a clear decrease of sea spray aerosol number flux and increase in aerosol residence time was observed, especially over the Southern Ocean. At the same time an increase in aerosol optical depth due to an increase in the number of particles with optically relevant sizes was found. That there were noticeable regional differences may have important implications for aerosol optical properties and number concentrations, subsequently also affecting the indirect radiative forcing by non-sea spray anthropogenic aerosols.

Contact information

Visiting addresses:

Geovetenskapens Hus,
Svante Arrhenius väg 8, Stockholm

Arrheniuslaboratoriet, Svante Arrhenius väg 16, Stockholm (Unit for Toxicological Chemistry)

Mailing address:
Department of Environmental Science
Stockholm University
106 91 Stockholm

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