A comprehensive characterisation of natural aerosol sources in the high Arctic during the onset of sea ice melt.

The interactions between aerosols and clouds are still one of the largest sources of uncertainty in quantifying anthropogenic radiative forcing. To reduce this uncertainty, we must first determine the baseline natural aerosol loading for different environments. In the pristine and hardly accessible polar regions, the exact nature of local aerosol sources remains poorly understood. It is unclear how oceans, including sea ice, control the aerosol budget, influence cloud formation, and determine the cloud phase. One critical question relates to the abundance and characteristics of biological aerosol particles that are important for the formation and microphysical properties of Arctic mixed-phase clouds. Within this work, we conducted a comprehensive analysis of various potential local sources of natural aerosols in the high Arctic over the pack ice during the ARTofMELT expedition in May-June 2023. Samples of snow, sea ice, seawater, and the sea surface microlayer (SML) were analysed for their microphysical, chemical, and fluorescent properties immediately after collection. Accompanied analyses of ice nucleating properties and biological cell quantification were performed at a later stage. We found that increased biological activity in seawater and the SML during the late Arctic spring led to higher emissions of fluorescent primary biological aerosol particles (fPBAPs) and other highly fluorescent particles (OHFPs, here organic-coated sea salt particles). Surprisingly, the concentrations of ice nucleating particles (INPs) in the corresponding liquid samples did not follow this trend. Gradients in OHFPs, fPBAPs, and black carbon indicated an anthropogenic pollution signal in surface samples especially in snow but also in the top layer of the sea ice core and SML samples. Salinity did not affect the aerosolisation of fPBAPs or sample ice nucleating activity. Compared to seawater, INP and fPBAP concentrations were enriched in sea ice samples. All samples showed distinct differences in their biological, chemical, and physical properties, which can be used in future work for an improved source apportionment of natural Arctic aerosol to reduce uncertainties associated with their representation in models and impacts on Arctic mixed-phase clouds.