Modelling wintertime Arctic Haze and sea-spray aerosols
Authors: Ioannidis Eleftherios , Law Kathy S. , Raut Jean-Christophe , Marelle Louis , Onishi Tatsuo , Kirpes Rachel M. , Upchurch Lucia , Massling Andreas , Skov Henrik , Quinn Patricia K. , Pratt Kerri A. 
Published: May 2022

Abstract. Anthropogenic and natural emissions contribute to enhanced concentrations of aerosols, so-called Arctic Haze in the Arctic winter and early spring. Models still have difficulties reproducing available observations. Whilst most attention has focused on the contribution of anthropogenic aerosols, there has been less focus on natural components such as sea-spray aerosols (SSA), including sea-salt sulphate and marine organics, which can make an important contribution to fine and coarse mode aerosols, particularly in coastal areas. Models tend to underestimate sub-micron and overestimate super-micron SSA in polar regions, including in the Arctic region. Quasi-hemispheric runs of the Weather Research Forecast model, coupled with chemistry model (WRF-Chem) are compared to aerosol composition data at remote Arctic sites to evaluate the model performance simulating wintertime Arctic Haze. Results show that the model overestimates sea-salt (sodium and chloride) and nitrate and underestimates sulphate aerosols. Inclusion of more recent wind-speed and sea-surface temperature dependencies for sea-salt emissions, as well as inclusion of marine organic and sea-salt sulphate aerosol emissions leads to better agreement with the observations during wintertime. The model captures better the contribution of SSA to total mass for different aerosol modes, ranging from 20–93 % in the observations. The sensitivity of modelled SSA to processes influencing SSA production are examined in regional runs over northern Alaska (United States) where the model underestimates episodes of high SSA, particularly in the sub-micron, that were observed in winter 2014 during field campaigns at the Barrow Observatory, Utqiaġvik. A local source of marine organics is also included following previous studies showing evidence for an important contribution from marine emissions. Model results show relatively small sensitivity to aerosol dry removal with more sensitivity (improved biases) to using a higher wind speed dependence based on sub-micron data reported from an Arctic cruise. Sea-ice fraction, including sources from open leads, is shown to be a more important factor controlling modelled super-micron SSA than sub-micron SSA. The findings of this study support analysis of the field campaign data pointing out that open leads are the primary source of SSA, including marine organic aerosols during wintertime at the Barrow Observatory, Utqiaġvik. Nevertheless, episodes of high observed SSA are still underestimated by the model at this site, possibly due to missing sources such as SSA production from breaking waves. An analysis of the observations and model results does not suggest an influence from blowing snow and frost flowers to SSA during the period of interest. Reasons for the high concentrations of sub-micron SSA observed at this site, higher than other Arctic sites, require further investigation.