Table DR-2- Sampling Details Water samples were collected over a 3 year period from private rural ground water wells. Wells are ~15 cm in diameter and steel-cased through surficial deposits to bedrock (depths of which are provided in Table 1, data appendix/ repository), and then open to the bedrock aquifer below the base of casing. Locations of wells sampled are shown in Figure 1. Water was sampled using residential production pumps and if water treatment systems were present, they were bypassed. Samples were collected in acid-washed, High Density Polyethylene (HDPE) bottles and stored on ice for delivery to analytical laboratories. A calibrated YSI multiprobe was used to measure water temperature, conductivity, pH, oxidationreduction potential (ORP), and % dissolved oxygen (DO) in the field – samples were collected once all parameters had attained steady values. Table DR-3- Analytical Methods and Precision for Groundwater Geochemistry Groundwater samples were analyzed for gross alpha (GA) radiation, 226radium, 228radium, and uranium at the Vermont Department of Health Laboratory in Burlington, Vermont. GA was analyzed via the EERF 00-02 method, 226Ra by the SM 7500 Ra-B method, 228Ra by the EERF Ra-05 method, and U by the EPA 200.8 method. Concentrations of metals and anions were analyzed at the Vermont Department of Environmental Conservation Laboratory in Waterbury. Samples were acidified and digested before analysis. The methods by which all metals and anions were determined are shown below. Representative precision, accuracy, and detection limit data are shown in Table 2. 1) Al, Sb, As, Ba, Be, Cd, Ca, Cr, Co, Cu, Fe, PB, Mg, Mn, Mo, Ni, K, Se, Ag, Na, Sr, Tl, Total Calculated Hardness, U, V, and Zn – EPA 6020 method (Inductively Coupled Plasma Mass Spectrometry (ICP-MS)). 2) Hg – EPA 245.1 method. 3) Cl- – either the EPA 300.0 or SM 4500CL-G. 4) SO4-2 and NO3-1 – EPA 300.0. 5) P – SM 4500-PH. 6) SiO2 – SM 4500 SiO2 F. 7) Alkalinity – SM 2320B. Representative Quality Control Run on Water Analyses by Vt DEC Lab QC % RPD Test Type Recovery % Recovery Limits RPD Limits 103 80-120 U MS 103 80-120 MSD 0 8 80-120 MS 106 Na 101 80-120 MS Mg 97 80-120 MS K 124 80-120 MS Ca 97 80-120 MS Ba 95 80-120 1 8 MSD 86 80-120 MS Cu 87 80-120 1 8 MSD 92 80-120 MS Fe 92 80-120 0 8 MSD 91 80-120 MS Mn 92 80-120 1 8 MSD 100 80-120 MS Mo 100 80-120 1 8 MSD 101 80-120 MS Pb 101 80-120 0 8 MSD 101 80-120 MS Sr 101 80-120 0 8 MSD MS= Matrix Spike; MSD=Matrix Spike Duplicate; RPD= Relative % Deviation Table DR-4- Analytical Methods and Precision for Whole-Rock Geochemistry Rock samples were cleaned of weathering rinds with a water-cooled rock saw, passed through a ceramic Spex Jaw Crusher and milled into powder using a Shatterbox. Powders were ignited at 1000 oC to determine loss-on-ignition (LOI), fused at 1050 oC in graphite crucibles with lithium metaborate flux, and dissolved in 10% HNO3. Concentrations of the 10 major elements (SiO2, Al2O3, TiO2, MgO, Fe2O3, CaO, Na2O, K2O, MnO, and P2O5) and the trace elements Ba, Co, Cr, Cu, Ni, Sc, Sr, V, Y, Zn and Zr were determined on a Thermo Elemental IRIS 1000 DUO inductively coupled plasma–atomic emission spectrometer (ICP-AES) at Middlebury College. Concentrations of the 14 rare earth elements and of numerous other trace elements including Rb, Th, and U were determined by inductively coupled plasma–mass spectrometry (ICP-MS) at Acme Analytical Laboratories, Vancouver, Canada. Major element compositions of 3 samples were determined by X-ray fluorescence (XRF) at XRAL laboratories in Ontario, Canada. Analytical precision of ICP-AES analyses was evaluated by running standard solutions that encompassed compositional ranges as quality checks before and after each 5-sample run, while accuracy was measured by comparison to U.S. Geological Survey certified standards G2 and MRG-1 (Table 4). Uncertainties determined by replicate analyses and comparison to USGS standards for SiO2, Al2O3, Fe2O3 and CaO are + 3%, whereas for TiO2, MnO, MgO, K2O and Na2O, uncertainties are + 10%. Uncertainties for trace elements are + 10%. Whole rock geochemical analyses were normalized to 100% on an anhydrous basis, and statistical calculations involving concentrations of elements lower than detection limits were performed using the value of the limit (Cloutier et al., 2006). Mineralogical and textural characteristics of selected samples were analyzed by transmitted light microscopy and by scanning electron microscopy (SEM) paired with energy dispersive X-ray (EDX) elemental analysis in a Zeiss DSM 940A at Middlebury College. In some cases analyses were performed in back-scatter electron (BSE) mode to enhance identification of U- and Th-bearing minerals (e.g. zircon, apatite, sphene and monazite).