Predicting Behavior and Fate of Atmospheric Mercury in Soils: Age-Dating METAALICUS Hg Isotope Spikes with Fallout Radionuclide Chronometry.

Soils accumulate anthropogenic mercury (Hg) from atmospheric deposition to terrestrial ecosystems. However, possible reemission of gaseous elemental mercury (GEM) back to the atmosphere as well as downward migration of Hg with soil leachate influence soil sequestration of Hg in ways not sufficiently understood in global biogeochemical models. Here, we apply fallout radionuclide (FRN) chronometry to understand soil Hg dynamics by revisiting the METAALICUS experiments 20 years after enriched isotope tracers (Hg, Hg, Hg, and Hg) were applied to two boreal watersheds in northwestern Ontario, Canada. Hg spikes formed well-defined peaks in organic horizons of both watersheds at depths of 3-6 cm and were accurately dated to the year of spike application in 6 of 7 cases (error = -0.8 ± 1.2 years). A seventh site was depleted by ca. 90% of both the Hg spike and background Hg, and the spike was dated 16 years older than its application. Robust FRN age models and mass balances demonstrate that loss of Hg is attributable to its specific physicochemical behavior at this site, but more work is required to attribute this to reemission or leaching. This study demonstrates the potential of FRN chronometry to provide insights into Hg accumulation, mobilization, and fate in forest soils.