Seasonal variation in the input of atmospheric selenium to northwestern Greenland snow

Oxygen isotope ratio (δ(18)O) and concentrations of Al, Na(+), methanesulfonic acid (MSA), SO4(2-), and selenium (Se) in a continuous series of 70 snow samples from a 3.2-m snow pit at a site in northwestern Greenland were determined using ultraclean procedures. Well-defined depth profiles of δ(18)O, Al, and sea-salt-Na(+) allowed the determination of chronology of the snow pit that spanned approximately 6 years from spring 2003 to summer 2009. Se concentrations were at a low pg/g level, ranging from 7.2 to 45 pg/g, and exhibited high variability with generally higher values during winter and spring and lower values during summer and fall. Very high crustal enrichment factors (EFc) of Se averaging approximately 26,600 for the entire time period indicate a small contribution from crust dust. High Se/MSA ratios are generally observed in the winter and spring snow layers, in which the Se concentrations were relatively high (>20 pg/g). This suggests that a significant component of the Se present in the snow layers is of anthropogenic origin. During the summer season, however, high EFc values are accompanied with low Se/MSA, indicating an increased contribution of marine biogenic sources. Significant correlations between Se, Al, and non-sea-salt SO4(2-) highlight that significant inputs of Se to the snow are likely controlled by the seasonality in the transport efficiency of anthropogenic Se from the source regions to the site. Based on the seasonal changes in Se concentrations, Se/MSA, and Se/S ratios observed in the samples, the input of anthropogenic Se to the site appears to be governed by the long-range transportation of Se emitted from coal combustion in East Asian countries, especially in China.