Arsenic is enriched up to 28 times the average crustal abundance of 4.8 mg kg(-1) for meta-sedimentary rocks of two adjacent formations in central Maine, USA where groundwater in the bedrock aquifer frequently contains elevated As levels. The Waterville Formation contains higher arsenic concentrations (mean As 32.9 mg kg(-1), median 12.1 mg kg(-1), n=38) than the neighboring Vassalboro Group (mean As 19.1 mg kg(-1), median 6.0 mg kg(-1), n=38). The Waterville Formation is a pelitic meta-sedimentary unit with abundant pyrite either visible or observed by scanning electron microprobe. Concentrations of As and S are strongly correlated (r=0.88, p<0.05) in the low grade phyllite rocks, and arsenic is detected up to 1944 mg kg(-1) in pyrite measured by electron microprobe. In contrast, statistically significant (p<0.05) correlations between concentrations of As and S are absent in the calcareous meta-sediments of the Vassalboro Group, consistent with the absence of arsenic-rich pyrite in the protolith. Metamorphism converts the arsenic-rich pyrite to arsenic-poor pyrrhotite (mean As 1 mg kg(-1), n=15) during de-sulfidation reactions: the resulting metamorphic rocks contain arsenic but little or no sulfur indicating that the arsenic is now in new mineral hosts. Secondary weathering products such as iron oxides may host As, yet the geochemical methods employed (oxidative and reductive leaching) do not conclusively indicate that arsenic is associated only with these. Instead, silicate minerals such as biotite and garnet are present in metamorphic zones where arsenic is enriched (up to 130.8 mg kg(-1) As) where S is 0%. Redistribution of already variable As in the protolith during metamorphism and contemporary water-rock interaction in the aquifers, all combine to contribute to a spatially heterogeneous groundwater arsenic distribution in bedrock aquifers.
Keywords: Arsenic; Bedrock aquifer; Prograde metamorphism; Pyrite; Pyrrhotite; Sulfur.
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