Regional-scale hydrogeochemical evolution across the arsenic-enriched transboundary aquifers of the Ganges River Delta system, India and Bangladesh

Arsenic (As) dynamics within the extensively contaminated aquifers of the Ganges River delta have been widely studied over the past few decades, but the hydrogeochemical signatures across the delta aquifers remain to be characterized. Here, we characterize the varied geochemical and isotopic (δ18O, δ2H) signatures of groundwater across the delta and interpret the hydrogeochemical evolution pathways and the driving processes on a regional-scale as a function of the delta hydrostratigraphy. Our hydrostratigraphic model identifies three major aquifer sub-systems across the delta from north-west to south-east: a single continuous unconfined aquifer (Type I); a semiconfined vertically-segregated aquifer sub-system (Type II); and a nearly confined multilayered aquifer sub-system (Type III). The Type I aquifer is dominated by Ca-Mg-HCO3-rich waters, while the aquifers to the south (Type II and Type III) exhibits increasing dominance of Na-Cl hydrogeochemical facies at shallow and intermediate depths and Na-HCO3 hydrogeochemical facies in the deep aquifers. The spatial distribution of As is also found to be heavily dictated by hydrostratigraphy, wherein the Type I aquifer sub-system yields similar concentrations across depths, while the Type II and Type III aquifer sub-systems exhibit a sharp increase in As-safe aquifers with depth. Although dominant reducing conditions occur within the delta groundwater, co-occurrence of redox-sensitive solutes from varying redox stability fields indicates to the development of overlapping redox zones. Stable isotopic signatures of groundwater exhibit a progressive depletion away from the Bay of Bengal. The Type I aquifer exhibits relatively homogenous hydrogeochemical signatures, possibly suggesting deeper infiltration of recharge under higher vertical hydraulic gradients, while the Type II and Type III aquifers exhibit variability across depth, which is possibly a reflection of horizontally stratified groundwater flows, dictated by the spatial geometry of the intervening aquitard layers.