Relationship between chemistry of air, fresh snow and firn cores for aerosol species in coastal Antarctica

Aerosol and fresh snow concentrations have been determined at three coastal Antarctic stations, Dumont d'Urville, Halley, and Neumayer. Model estimates suggest that dry deposition, including that caused by wind pumping, is only a minor contributor (of order 1%) to chemical fluxes at these sites with relatively high snow accumulation. Larger dry deposition fluxes are possible for very large aerosol particles, including sea‐salt aerosol. Measurements of surface snow on successive days provide experimental data that constrain the contribution of dry deposition to probably less than 10% of annual fluxes for all ions, although very high episodic fluxes of giant sea‐salt aerosol cannot be ruled out. Spatial variability, and frequent snow, fog and drift events, make it difficult to improve this quantification. Both theory and measurement suggest that fog deposition is also a minor contributor to the annual flux (probably <1%). Sublimation of surface snow and of blowing snow may increase snow concentrations by a few percent, with a larger role in summer, but should not affect fluxes. Wet deposition in falling snow appears to be by far the major contributor. However, the relationship between concentrations in snow and in simultaneously sampled aerosol at ground level was poor for most species. Scavenging ratios derived from these data are higher than those from the limited data previously available, but have huge uncertainties associated with them. Particularly at sites with frequent drifting snow, groundlevel aerosol measurements may be inappropriate for deriving scavenging ratios. Despite this, there is a general seasonal coincidence of high aerosol concentrations and high snow concentrations. We are also able to trace the chemistry of fresh snowfall to an ice core collected up to 2 years later. Although some major snowfall events may be missing, it seems that, as expected, there is no significant postdepositional modification of chemistry for aerosol species in the top meter of firn.