The contributions of snow, fog, and dry deposition to the summer flux of anions and cations at Summit, Greenland

Abstract

Experiments were performed during the period May–July of 1993 at Summit, Greenland. Aerosol mass size distributions as well as daily average concentrations of several anionic and cationic species were measured. Dry deposition velocities for SO42− were estimated using surrogate surfaces (symmetric airfoils) as well as impactor data. Real‐time concentrations of particles greater than 0.5 μm and greater than 0.01 μm were measured. Snow and fog samples from nearly all of the events occurring during the field season were collected. Filter sampler results indicate that SO42− is the dominant aerosol anion species, with Na+, NH4+, and Ca2+ being the dominant cations. Impactor results indicate that MSA and SO42− have similar mass size distributions. Furthermore, MSA and SO42− have mass in both the accumulation and coarse modes. A limited number of samples for NH4+ indicate that it exists in the accumulation mode. Na, K, Mg, and Ca exist primarily in the coarse mode. Dry deposition velocities estimated from impactor samples and a theory for dry deposition to snow range from 0.017 cm/s +/− 0.011 cm/s for NH4+ to 0.110 cm/s +/− 0.021 cm/s for Ca. SO42− dry deposition velocity estimates using airfoils are in the range 0.023 cm/s to 0.062 cm/s, as much as 60% greater than values calculated using the airborne size distribution data. The rough agreement between the airfoil and impactor‐estimated dry deposition velocities suggests that the airfoils may be used to approximate the dry deposition to the snow surface. Laser particle counter (LPC) results show that particles > 0.5 μm in diameter efficiently serve as nuclei to form fog droplets. Condensation nuclei (CN) measurements indicate that particles < 0.5 μm are not as greatly affected by fog. Furthermore, impactor measurements suggest that from 50% to 80% of the aerosol SO42− serves as nuclei for fog droplets. Snow deposition is the dominant mechanism transporting chemicals to the ice sheet. For NO3−, a species that apparently exists primarily in the gas phase as HNO3(g), 93% of the seasonal inventory (mass of a deposited chemical species per unit area during the season) is due to snow deposition, which suggests efficient scavenging of HNO3(g) by snowflakes. The contribution of snow deposition to the seasonal inventories of aerosols ranges from 45% for MSA to 76% for NH4+. The contribution of fog to the seasonal inventories ranges from 13% for Na+ and Ca2+ to 26% and 32% for SO42− and MSA. The dry deposition contribution to the seasonal inventories of the aerosol species is as low as 5% for NH4+ and as high as 23% for MSA. The seasonal inventory estimations do not take into consideration the spatial variability caused by blowing and drifting snow. Overall, results indicate that snow deposition of chemical species is the dominant flux mechanism during the summer at Summit and that all three deposition processes should be considered when estimating atmospheric concentrations based on ice core chemical signals.