Changes in the mercury isotopic composition of sediments from a remote alpine lake in Wyoming, USA

Abstract Mercury (Hg) deposition from the atmosphere has increased dramatically since 1850 and Hg isotope records in lake sediments can be used to identify changes in the sources and cycling of Hg. We collected a sediment core from a remote lake (Lost Lake, Wyoming, USA) and measured vertical variation of Hg concentration and isotopic composition as well as 210 Pb and 137 Cs activities to establish a chronology. We also analyzed vegetation and soil samples from the watershed which has a small ratio of watershed area to lake surface area (2.06). The Hg flux remains constant from ~1350 to 1850 before increasing steadily to modern values that are approximately four times pre-1850 values. The modern Hg isotopic composition preserved in the sediments is distinct from the Hg isotopic composition of pre-1850 samples with both δ 202 Hg and Δ 199 Hg becoming progressively more positive through time, with shifts of +0.37‰ and +0.23‰ respectively. To explain temporal changes in δ 202 Hg, Δ 199 Hg, and Hg concentration in the core segments, we estimated a present-day atmospheric endmember based on precipitation and snow samples collected near Lost Lake. The observed change in Hg isotopic values through time cannot be explained solely by addition of anthropogenic Hg with the isotopic composition that has been estimated by others for global anthropogenic emissions. Instead, the isotope variation suggests that the relative importance of redox transformations, whether in the atmosphere, within the lake, or both, have changed since 1850.