“…The forward models start with evaporated rainwater reacted with the smallest amount of minerals (Table SI.8) to produce dilute groundwater that is simulated to have a high concentration of 226 Ra (on the order of 1 pCi/L), derived from surficial aquifer sources, because of inefficient adsorption of Ra at low pH as detailed elsewhere. − Model 1 (black curves) reacts the dilute groundwater with a high concentration of NaCl to simulate the influence of road-deicing salt leachate (Figures , SI.2, and SI.3F). The Na:Cl of about 1.0 for slightly acidic or near-neutral samples (Figure A) indicates mixing of dilute rainwater with saltwater aerosols, road salt, and wastewater. − Models 2, 3, and 4 (red, blue, and green curves, respectively) react the “dilute” groundwater with approximately 10-fold of additional minerals. Model 2 (red curves), without cation exchange, generally explains the compositions of samples having high 226 Ra in “hard” water with considerable Ca and near-neutral pH (samples B–D; 226 Ra 0.97–1.08 pCi/L; Figures , SI.3A–D,G, SI.4, and Table SI.4B; PC2 in Table SI.6).…”