Influence of forest canopies on the deposition of methylmercury to boreal ecosystem watersheds.

Although it has been previously shown that forest canopies significantly increase the total deposition of Hg to watersheds, sources and fates of atmospherically deposited MeHg in particular remain poorly understood. In this study, net loadings of MeHg to a watershed were quantified, and the retention and (photo)reduction of MeHg on foliage were measured using unique stable Hg isotope experiments. Annual loadings of MeHg in throughfall (0.34 ± 0.01 to 0.60 ± 0.16 mg ha⁻¹ yr⁻¹) and litterfall (0.77 ± 0.07 to 0.97 ± 0.34 mg ha⁻¹ yr⁻¹) were collectively 3-4 times higher under different forest canopies than loadings of MeHg in the open (0.41 mg ha⁻¹ yr⁻¹), suggesting dry deposition of MeHg to forest canopies. Using Me¹⁹⁹Hg, we found that a portion of MeHg wet deposited to forest canopies is retained on foliage over time, eventually contributing to MeHg in litterfall. Average half-lives (t½) of Me¹⁹⁹Hg on spruce, jack pine, and birch foliage were 204 ± 66, 187 ± 101, and 8 ± 3 days, respectively. We also found using Me¹⁹⁹Hg that following wet deposition, MeHg is rapidly (photo)reduced to ¹⁹⁹Hg(0) on canopy foliage, which then evades to the atmosphere. We were unable to quantify concentrations of particulate-bound MeHg (p-MeHg) in the air using vacuum pumps and quartz microfiber air sampling filters, despite the possibility that p-MeHg does exist in small quantities. As a result, the source of dry deposited MeHg remains partially elusive.