Hg Isotopes Reveal Importance of In-Stream Processing and Legacy Inputs in East Fork Poplar Creek, Oak Ridge, Tennessee, USA.

Understanding how mercury (Hg) contaminated ecosystems will recover as atmospheric emissions and industrial point source discharges are controlled has become a driving motivation of mercury research. Key to predicting recovery of mercury contaminated ecosystems is an understanding of the mobilization of legacy Hg sources, and the subsequent bioavailability and biogeochemical cycling of mobilized Hg within aquatic ecosystems. Herein, we utilize natural abundance stable Hg isotope techniques to place new constraints on mercury sources, transport, and transformations along the flow path of East Fork Poplar Creek (EFPC), Oak Ridge, Tennessee. The isotopic composition of mercury in stream water and suspended sediment along the flow path suggest that: (1) physical processes such as dilution and sedimentation cannot fully explain decreases in total mercury concentrations along the flow path and that in-stream processes may be more important than previously realized; (2) in-stream processes include photochemical transformations (~20%), but microbial reduction is likely more dominant (~80%); and (3) additional sources of mercury inputs to EFPC at base-flow may predominantly arise from the hyporheic zone during the growing season, with adjacent riparian wetlands and non-point-source impacted tributaries increasing in importance during the dormant season when the stream channel is more hydrologically connected to the watershed.