Ship-based measurements of sea spray aerosol (SSA) gradient fluxes in the size range of 0.5–47 µm in diameter were conducted between 2009–2017 in both the Baltic Sea and the North Atlantic Ocean. Measured total SSA fluxes varied between 8.9 × 103 ± 6.8 × 105 m−2 s−1 for the Baltic Sea and 1.0 × 104 ± 105 m−2 s−1 for the Atlantic Ocean. The analysis uncovered a significant decrease (by a factor of 2.2 in the wind speed range of 10.5–14.5 m s−1) in SSA fluxes, with chlorophyll a (chl a) concentration higher than 3.5 mg m−3 in the Baltic Sea area. We found statistically significant correlations for both regions of interest between SSA fluxes and various environmental factors, including wind speed, wind acceleration, wave age, significant wave height, and wave Reynolds number. Our findings indicate that higher chl a concentrations are associated with reduced SSA fluxes at higher wind speeds in the Baltic Sea, while the influence of wave age showed higher aerosol emissions in the Baltic Sea for younger waves compared to the Atlantic Ocean. These insights underscore the complex interplay between biological activity and physical dynamics in regulating SSA emissions. Additionally, in both measurement regions, we observed weak correlations between SSA fluxes and air and water temperature and between SSA fluxes and atmospheric stability. Comparing the Baltic Sea and the North Atlantic, we noted distinct emission behaviors, with higher emissions in the Baltic Sea at low wave age values compared to the Atlantic Ocean. This study represents the first comparative analysis of SSA flux measurements using the same methodology in these contrasting marine environments.

Primary biological aerosol particles (PBAPs) can influence the climate and affect human health. To investigate the aerosolization of PBAPs by sea spray aerosol (SSA), we conducted ship-based campaigns in the central Baltic Sea near Östergarnsholm in May and August 2021. Using a plunging-jet sea spray simulation chamber filled with local seawater, we performed controlled chamber experiments to collect filters and measure aerosols. We determined the abundance of microbial cells in the chamber air and seawater using staining and fluorescence microscopy, normalizing these values to sodium concentrations to calculate enrichment factors. Our results showed that microbes were enriched in the aerosol by 13 to 488 times compared to the underlying seawater, with no significant enrichment observed in the sea surface microlayer. Microbial abundances obtained through microscopy were compared with estimates of fluorescent PBAPs (fPBAPs) using a single-particle fluorescence spectrometer. We estimated microbial emission fluxes using two independent approaches: (1) applying the enrichment factors derived from this study with mass flux estimates from previous SSA parameterizations and (2) using a scaling approach from a companion study. Both methods produced microbial emission flux estimates that were in good agreement and of the same order of magnitude as previous studies, while fPBAP emission flux estimates were significantly lower. Furthermore, 16S rRNA sequencing identified the diversity of bacteria enriched in the nascent SSA compared to the underlying seawater.

To compare in situ and laboratory estimates of sea spray aerosol (SSA) production fluxes, we conducted two research campaigns in the vicinity of an eddy covariance (EC) flux tower on the island of Östergarnsholm in the Baltic Sea during May and August 2021. To accomplish this, we performed EC flux measurements for particles with diameters between 0.25 and 2.5 µm simultaneously with laboratory measurements using a plunging jet sea spray simulation chamber containing local seawater sampled close to the footprint of the flux tower. We observed a log-linear relationship between wind speed and EC-derived SSA emission fluxes, a power-law relationship between significant wave height and EC-derived SSA emission fluxes, and a linear relationship between wave Reynolds number and EC-derived SSA emission fluxes, all of which are consistent with earlier studies. Although we observed a weak negative relationship between particle production in the sea spray simulation chamber and seawater chlorophyll-α concentration and a weak positive relationship with the concentration of fluorescent dissolved organic matter in seawater, we did not observe any significant impact of dissolved oxygen on particle production in the chamber.

To obtain an estimate of the size-resolved emission spectrum for particles with dry diameters between 0.015 and 10 µm, we combined the estimates of SSA particle production fluxes obtained using the EC measurements and the chamber measurements in three different ways: (1) using the traditional continuous whitecap method, (2) using air entrainment measurements, and (3) simply scaling the chamber data to the EC fluxes. In doing so, we observed that the magnitude of the EC-derived emission fluxes compared relatively well to the magnitude of the fluxes obtained using the chamber air entrainment method as well as the previous flux measurements of Nilsson et al. (2021) and the parameterizations of Mårtensson et al. (2003) and Salter et al. (2015). As a result of these measurements, we have derived a wind-speed-dependent and wave-state-dependent SSA parameterization for particles with dry diameters between 0.015 and 10 µm for low-salinity waters such as the Baltic Sea, thus providing a more accurate estimation of SSA production fluxes.

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 ± 18 m⁻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 similar composition in air and sea suggested a linkage between the two compartments. For this purpose, the atmospheric MPs' equivalent aerodynamic diameter was calculated (28 ± 3 μm) 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 MPs sea emission fluxes (4–18 ∗ 10⁶ μm³ m⁻² s⁻¹ range) finally showed the contemporary presence of atmospheric transport together with a continuous emission from the sea surface enabling a grasshopper long-range transport of microplastics across the sea.

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.

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 average 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 exponential 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 allowed 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 indirectly 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 water-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 modified 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 Ellison et al. appeared to be able to explain most of the differences we observed between the aerosol emission fluxes with and without the thermodenuder. 

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.

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 similar 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.

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.

The surface-wind speed influences on aerosol optical depth (AOD), derived from the Moderate Resolution Imaging Spectroradiometer (MODIS) Aqua daily observations over the central North Pacific during the period 2003-2016, have been investigated in this study. The cloud coverage is relatively low over the present investigation area compared to other marine areas, which favors AOD derived from passive remote sensing from space. In this study, we have combined MODIS AOD with 2 m wind speed (U-2m) on a satellite-pixel basis, which has been interpolated from National Centers for Environmental Prediction (NCEP) reanalysis. In addition, daily averaged AOD derived from Aerosol Robotic Network (AERONET) measurements in the free-troposphere at the Mauna Loa Observatory (3397 m above sea level), Hawaii, was subtracted from the MODIS column AOD values. The latter was to reduce the contribution of aerosols above the planetary boundary layer. This study shows relatively strong power-law relationships between MODIS mean AOD and surface-wind speed for marine background conditions in summer, fall and winter of the current period. However, previous established relationships between AOD and surface-wind speed deviate substantially. Even so, for similar marine conditions the present relationship agrees reasonable well with a power-law relationship derived for north-east Atlantic conditions. The present MODIS retrievals of AOD in the marine atmosphere agree reasonably well with ground-based remote sensing of AOD.