Temporal evolution of 36Cl abundances in the Great Lakes

•36Cl/Cl ratios are the highest in Lake Superior and the lowest in Lake Erie.•36Cl concentrations in the Great Lakes are much higher than expected natural values.•Conservative 36Cl model underestimates observed values in Lakes Erie and Ontario.•Large fraction of 36Cl atoms deposited on the watersheds are retained for decades.

The observed 36Cl isotopic abundance in Great Lakes water decreases from west to east, with the highest 36Cl/Cl ratio of 1332 × 10−15 in Lake Superior and the lowest 36Cl/Cl ratio of 151 × 10−15 in Lake Erie, whereas the 36Cl concentration (36Cl atoms/L) is lowest in Lake Superior and higher in the other Great Lakes. The 36Cl concentration in Lake Superior is much higher than expected from normal atmospheric deposition over the basin, consistent with deposition of nuclear bomb-produced 36Cl during 1952–1964. A conservative mass-balance model constrained by hydrological parameters and available 36Cl fluence measurements predicts the 36Cl abundances in the Great Lakes from 1945 to 2015, in excellent agreement with available data for Lakes Superior, Michigan, and Huron, but the model underestimates 36Cl abundances for Lakes Erie and Ontario. However, assuming that 36Cl demonstrates non-conservative behavior and is significantly retained in the drainage basins, a model incorporating a delayed input parameter successfully predicts observed 36Cl concentrations in all of the Great Lakes.