Increasing mercury isotope ratios from pre‐industrial (1510–1850) to present‐day (1990–2014) in lake sediment cores have been suggested to be a global phenomenon. To assess factors leading to spatiotemporal changes, we compiled mercury concentration (THg) and mercury isotope ratios in 22 lake sediment cores located at various regions of the world. We find that the positive δ202Hg shifts together with THg increases from pre‐industrial to present‐day are a widespread phenomenon. This is caused by increased contribution of mercury from local to regional anthropogenic mercury emission sources, which lead to higher sediment δ202Hg (−1.07 ± 0.69‰, 1 SD) than pre‐industrial sediments (−1.55 ± 0.96‰, 1 SD). The positive Δ199Hg shifts were observed in 15 lake sediment cores, which have low pre‐industrial Δ199Hg (−0.20 ± 0.32‰) compared to the sediment cores with near‐zero to positive pre‐industrial Δ199Hg (0.08 ± 0.07‰). The magnitudes of δ202Hg (r2 = 0.09) and Δ199Hg (r2 = 0.20, both p > 0.05) changes from pre‐industrial to present‐day did not correlate with the magnitude of THg changes. Instead, the magnitudes of δ202Hg and Δ199Hg changes decreased with increasing pre‐industrial δ202Hg and Δ199Hg values, suggesting that the baseline mercury isotope ratios play a more important role in determining the magnitude of mercury isotope changes compared to the degree of THg input. We suggest that the spatiotemporal assessments of δ202Hg in lake sediment cores can be used as an important proxy for monitoring changes in anthropogenic mercury sources for the Minamata Convention on Mercury.

Atmospheric deposition of mercury (Hg) to terrestrial and aquatic ecosystems has significant implications for human and animal exposure. Measurements of Hg isotopic composition can be utilized to trace sources of Hg, but outside of the Arctic there has been little Hg isotopic characterization of snow. To better understand deposition pathways at mid-latitudes, five time series of snowfall were collected at two sites (Dexter and Pellston, Michigan, USA) to investigate the Hg isotopic composition of snowfall, how it changes after deposition, and how it compares to rain. The Hg isotopic composition of a subset of fresh snow samples revealed the influence of reactive surface uptake of atmospheric Hg(0). The first time series collected at Dexter occurred during a polar vortex, demonstrating Hg isotopic fractionation dynamics similar to those in Arctic snow, with increasingly negative Δ199Hg as snow aged with exposure to sunlight. All other time series revealed an increase in Δ199Hg as snow aged, with values reaching up to 3.5‰. This characterization of Hg isotopes in snow suggests a strong influence of oxidants and binding ligands in snow that may mediate Hg isotope fractionation. Additionally, isotopic characterization of Hg in snow deposited to natural ecosystems at mid-latitudes allows for better understanding of atmospheric mercury sources that are deposited to lakes and forests and that may become available for methylation and transfer to food webs.

The atmosphere is a significant global reservoir for mercury (Hg) and its isotopic characterization is important to understand sources, distribution, and deposition of Hg to the Earth's surface. To better understand Hg isotope variability in the remote background atmosphere, we collected continuous 12-h Hg0 samples for 1 week from two high elevation sites, Camp Davis, Wyoming (valley), and Mount Bachelor, Oregon (mountaintop). The samples collected at Camp Davis displayed strong diel variation in δ202Hg values of Hg0, but not in Δ199Hg or Δ200Hg values. We attribute this pattern to nightly atmospheric inversions trapping Hg in the valley and the subsequent nighttime uptake of Hg by vegetation, which depletes Hg from the atmosphere. At Mount Bachelor, the samples displayed diel variation in both δ202Hg and Δ199Hg, but not Δ200Hg. We attribute this pattern to differences in the vertical distribution of Hg in the atmosphere as Mount Bachelor received free tropospheric air masses on certain nights during the sampling period. Near the end of the sampling period at Mount Bachelor, the observed diel pattern dissipated due to the influence of a nearby forest fire. The processes governing the Hg isotopic fractionation differ across sites depending on mixing, topography, and vegetation cover.

The climate and environmental significance of the Deccan Traps large igneous province of west-central India has been the subject of debate in paleontological communities. Nearly one million years of semi-continuous Deccan eruptive activity spanned the Cretaceous-Paleogene boundary, which is renowned for the extinction of most dinosaur groups. Whereas the Chicxulub impactor is acknowledged as the principal cause of these extinctions, the Deccan Traps eruptions are believed to have contributed to extinction patterns and/or enhanced ecological pressures on biota during this interval of geologic time. We present the first coupled records of biogenic carbonate clumped isotope paleothermometry and mercury concentrations as measured from a broad geographic distribution of marine mollusk fossils. These fossils preserve evidence of simultaneous increases in coastal marine temperatures and mercury concentrations at a global scale, which appear attributable to volcanic CO2 and mercury emissions. These early findings warrant further investigation with additional records of combined Late Cretaceous temperatures and mercury concentrations of biogenic carbonate.

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 210Pb and 137Cs 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 δ202Hg and Δ199Hg becoming progressively more positive through time, with shifts of +0.37‰ and +0.23‰ respectively. To explain temporal changes in δ202Hg, Δ199Hg, 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.

Historic point source mercury (Hg) inputs from industrial processes on the South River (Waynesboro, Virginia) ended many decades ago, but sediment and surface water Hg concentrations remain elevated relative to the regional background. To understand Hg sources, mobility, and fate in the South River, we analyzed total Hg concentrations and Hg stable isotope compositions of streambed sediments, bank soils, suspended particles, filtered surface waters, and channel margin hyporheic zone pore waters. Hg isotopes allow for the identification of three distinct Hg end-member inputs to the South River, consisting of a regional background source and two isotopically distinct contaminant sources. Hydrologic conditions are demonstrated to have an influence on within-channel Hg isotope fractionation and Hg partitioning, with no observed isotopic discrimination between suspended particulate Hg and filtered surface water Hg during elevated flow conditions. Channel margin hyporheic zone porewaters had significantly higher delta Hg-202 values than surface waters (delta Hg-202 = - 0.52 +/- 0.44 parts per thousand and delta Hg-202 = -0.89 +/- 0.20 parts per thousand respectively [mean +/- 1SD]). A subset of porewaters exhibited mass independent fractionation signatures (Delta Hg-199 = 0.33 +/- 0.06%0; Delta Hg-200 = 0.19 +/- 0.03 parts per thousand [mean +/- 1SD]) that are suggestive of a precipitation-derived origin for the dissolved Hg pool. Sediments from a floodplain profile were analyzed to explore the temporal variation in Hg isotopic composition within the South River, indicating brief excursions (up to delta Hg-202 = +0.61 parts per thousand) from the average composition observed in modern samples (delta Hg-202 = -0.52 +/- 0.09 parts per thousand). By improving understanding of the spatial, temporal, and hydrologic conditions that contribute to variations in Hg isotopic composition, this study provides insights into the processes that control Hg isotopic end-member sources, Hg-loading to the channel during elevated flows, and Hg fate in the South River.

Historic point source mercury (Hg) contamination from industrial processes on the South River (Waynesboro, Virginia) ended decades ago, but elevated Hg concentrations persist in the river system. In an effort to better understand Hg sources, mobility, and transport in the South River, we analyzed total Hg (THg) concentrations and Hg stable isotope compositions of streambed sediments, stream bank soils, suspended particles, and filtered surface waters. Samples were collected along a longitudinal transect of the South River, starting upstream of the historic Hg contamination point-source and extending downstream to the confluence with the South Fork Shenandoah River. Analysis of the THg concentration and Hg isotopic composition of these environmental samples indicates that the regional background Hg source is isotopically distinct in both Δ199Hg and δ202Hg from Hg derived from the original source of contamination, allowing the tracing of contamination-sourced Hg throughout the study reach. Three distinct end-members are required to explain the Hg isotopic and concentration variation observed in the South River. A consistent negative offset in δ202Hg values (∼0.28‰) was observed between Hg in the suspended particulate and dissolved phases, and this fractionation provides insight into the processes governing partitioning and transport of Hg in this contaminated river system.