The Arctic is sensitive to cloud radiative forcing. Due to the limited number of aerosols present throughout much of the year, cloud formation is susceptible to the presence of cloud condensation nuclei and ice nucleating particles (INPs). Primary biological aerosol particles (PBAP) contribute to INPs and can impact cloud phase, lifetime, and radiative properties. We present yearlong observations of hyperfluorescent aerosols (HFA), tracers for PBAP, conducted with a Wideband Integrated Bioaerosol Sensor, New Electronics Option during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition (October 2019–September 2020) in the central Arctic. We investigate the influence of potential anthropogenic and natural sources on the characteristics of the HFA and relate our measurements to INP observations during MOSAiC. Anthropogenic sources influenced HFA during the Arctic haze period. But surprisingly, we also found sporadic “bursts” of HFA with the characteristics of PBAP during this time, albeit with unclear origin. The characteristics of HFA between May and August 2020 and in October 2019 indicate a strong contribution of PBAP to HFA. Notably from May to August, PBAP coincided with the presence of INPs nucleating at elevated temperatures, that is, >−9°C, suggesting that HFA contributed to the “warm INP” concentration. The air mass residence time and area between May and August and in October were dominated by the open ocean and sea ice, pointing toward PBAP sources from within the Arctic Ocean. As the central Arctic changes drastically due to climate warming with expected implications on aerosol–cloud interactions, we recommend targeted observations of PBAP that reveal their nature (e.g., bacteria, diatoms, fungal spores) in the atmosphere and in relevant surface sources, such as the sea ice, snow on sea ice, melt ponds, leads, and open water, to gain further insights into the relevant source processes and how they might change in the future.

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.

Sea spray aerosol (SSA) is one of the major natural aerosol sources and is produced when wave breaking entrains air into ocean surface water, which subsequently breaks up into bubbles. These bubbles rise to the surface and can scavenge biogenic material. Once they reach the surface, they burst and produce both a large number of relatively small film drops that result from the disintegration of the bubble film cap and a smaller number of jet drops that result from the collapse of the bubble cavity and are typically larger in size than the film drops. The production of SSA is influenced by several factors, including wind speed, sea state, seawater temperature, salinity, and the physicochemical and biological condition of the ocean. SSA can significantly impact Earth's radiation budget by scattering incoming solar radiation directly and by acting as cloud condensation nuclei. To improve our understanding of the impact of sea spray aerosols on the Earth’s climate, it is critical to understand the physical mechanisms which determine the size-resolved SSA production flux. Furthermore, SSA can be a vector for the emission of primary biological airborne particles (PBAP) from the oceans to the atmosphere. PBAP encompass bacteria, viruses, pollen and spores and can be present in the atmosphere in form of agglomerates, single particles or cell fractions.  Although, the abundance of PBAP typically only make up < 0.1% of the number of aerosols, this does not imply their insignificance. On the contrary, PBAP are known to be very efficient cloud- and ice condensation nuclei and thus can influence cloud properties such as cloud phase, albedo and lifetime, thereby affecting the Earth’s climate as well as biogeochemical cycles. As the Earth is 70% covered by oceans, of which most could be characterized as remote, quantifying the PBAP emissions over these waters are important for the enhancement of climate models.

The goal of this thesis was to study the factors impacting SSA emissions and the emission of primary biological particles with SSA with particular focus on bacteria emissions. This was done both through laboratory and field experiments in the Baltic Sea and in the Azores archipelago using a plunging jet sea spray simulation chamber and various techniques to characterize aerosol emissions. More specifically, a parameterization for the SSA production flux as a function of salinity and temperature was derived from laboratory experiments and a wind speed and sea state dependent parameterization were derived from ambient eddy covariance (EC) flux measurements in the Baltic Sea. The combination of EC flux measurements and laboratory generated SSA allowed to derive a chamber specific scaling factor that could be applied to derive bacteria emission fluxes ranging between 16-63 cells m⁻² s⁻¹ from the Baltic Sea. Bacteria were found to be 13-488 and 9-148 times enriched in SSA compared to the underlying seawater from mesocosm experiments in the Baltic Sea and Azores, respectively. A comparison of single cell abundance estimates from fluorescence microscopy and real-time measurements of PBAP with diameters > 0.8 µm using a bioaerosol sensor revealed that the latter yielded consistently lower concentrations. The discrepancy was explained by differences in the sampling approach and size cut-offs (i.e. single cells versus agglomerates or particle-attached cells). As such, both methods are applicable to different research questions and should be considered complementary.

An analysis of the microbial community composition in the aerosols and underlying seawater showed selective aerosolization of certain bacteria taxa. Furthermore, selective growth and a decrease in alpha diversity in the seawater was observed when the mesocosm experiments were operated in a closed mode (meaning that the seawater was not exchanged over the duration of each experiment), which can however be circumvented by continuously replacing the water in the mesocosm.

Ambient measurements of PBAP revealed diurnal variations with a peak during the early morning hours that was correlated to changes wind speed, wave height, air temperature, relative humidity, latent and sensitive heat flux.

The amount of ice versus supercooled water in clouds is important for their radiative properties and role in climate feedbacks. Hence, knowledge of the concentration of ice-nucleating particles (INPs) is needed. Generally, the concentrations of INPs are found to be very low in remote marine locations allowing cloud water to persist in a supercooled state. We had expected the concentrations of INPs at the North Pole to be very low given the distance from open ocean and terrestrial sources coupled with effective wet scavenging processes. Here we show that during summer 2018 (August and September) high concentrations of biological INPs (active at >−20°C) were sporadically present at the North Pole. In fact, INP concentrations were sometimes as high as those recorded at mid-latitude locations strongly impacted by highly active biological INPs, in strong contrast to the Southern Ocean. Furthermore, using a balloon borne sampler we demonstrated that INP concentrations were often different at the surface versus higher in the boundary layer where clouds form. Back trajectory analysis suggests strong sources of INPs near the Russian coast, possibly associated with wind-driven sea spray production, whereas the pack ice, open leads, and the marginal ice zone were not sources of highly active INPs. These findings suggest that primary ice production, and therefore Arctic climate, is sensitive to transport from locations such as the Russian coast that are already experiencing marked climate change.

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.

The chemical composition of cloud water can be used to infer the sources of particles upon which cloud droplets and ice crystals have formed. In order to obtain cloud water for analysis of chemical composition for elevated clouds in the pristine high Arctic, balloon-borne active cloud water sampling systems are the optimal approach. However, such systems have not been feasible to deploy previously due to their weight and the challenging environmental conditions. We have taken advantage of recent developments in battery technology to develop a miniaturised cloud water sampler for balloon-borne collection of cloud water. Our sampler is a bulk sampler with a cloud drop cutoff diameter of approximately 8 mu m and an estimated collection efficiency of 70%. The sampler was heated to prevent excessive ice accumulation and was able to operate for several hours under the extreme conditions encountered in the high Arctic. We have tested and deployed the new sampler on a tethered balloon during the Microbiology-Ocean-Cloud-Coupling in the High Arctic (MOCCHA) campaign in August and September 2018 close to the North pole. The sampler was able to successfully retrieve cloud water samples that were analysed to determine their chemical composition as well as their ice-nucleating activity. Given the pristine conditions found in the high Arctic we have placed significant emphasis on the development of a suitable cleaning procedure to minimise background contamination by the sampler itself.