Temporal evolution of (36)Cl abundances in the Great Lakes.

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