Apportioning aerosol natural and anthropogenic sources thorough simultaneous aerosol size distributions and chemical composition in the European high Arctic

Abstract. Understanding aerosol size distributions is crucial to our ability to predict aerosol number concentrations. When of favourable size and composition, both long range transported particles as well as locally formed ones may serve as Cloud Condensation Nuclei (CCN); small changes may have a large impact on the low CCN concentrations currently characteristic of the Arctic environment. Here, we present a cluster analysis of particle size distributions (PSD, size range 8–500 nm) simultaneously collected from three high Arctic sites across Europe during a three year period (2013–2015). Two sites are located in the Svalbard archipelago: Zeppelin research station (474 m above ground), and the nearby Gruvebadet Observatory (about 2 km distance from Zepplelin, 67 m above ground). The third site (Villum Research Station – Station Nord, 30 m above ground) is 600 km to the west-northwest of Zeppelin, at the tip of north-eastern Greenland. An inter-site comparison exercise is carried out for the first time including the Gruvebadet site. K-means analysis provided eight specific aerosol categories, further combined into broad PSD with similar characteristics, namely: pristine low concentrations (12–14 %), new particle formation (16–32 %), Aitken (21–35 %) and accumulation (20–50 %). Confined for longer time periods by consolidated pack sea ice regions, the Greenland site shows PSD with lower ultrafine mode aerosol concentrations during summer, but higher accumulation mode aerosol concentrations during winter relative to the Svalbard sites. By association with chemical composition and Cloud Condensation Nuclei properties, further conclusions can be derived. Three distinct types of accumulation mode aerosol are observed during winter months, associated with sea spray (largest detectable sizes), Arctic haze (main mode at 150 nm) and aged accumulation mode (main mode at 220 nm) aerosols. In contrast, locally produced and most likely of marine biogenic origin particles exhibit size distributions dominated by the nucleation and Atiken mode aerosol during summer months. The obtained data and analysis set now the stage for future studies; including apportioning the relative contribution of primary and secondary aerosol formation processes to the aerosol size distribution in high Arctic, and elucidating anthropogenic aerosol dynamics, transport and removal processes across the Greenland sea. In a region of enormous importance for future climate on Earth, it is imperative to continue strengthening international scientific cooperation, in order to address important research questions on scales beyond singular station or measurement events.