Title: The vulnerability of low-arsenic aquifers in Bangladesh
Description: The worldwide natural occurrence of high levels of arsenic (As) in groundwater and its deleterious effects on human health have inspired a great amount of related research in public health and geosciences internationally. With >100 million people in South and Southeast Asia exposed to >10 µg/L As in shallow groundwater that they use for drinking, the installation of deeper, low-As wells has emerged as a major strategy for lowering the exposure. As the magnitude of deep pumping continues to increase, this work focuses on the geochemical and hydrologic questions surrounding the vulnerability and sustainability of low-As aquifers in Bangladesh, the country most affected by As crisis. In an effort to better understand the residence time of groundwater in low-As aquifers at depth, radiocarbon (14C) and 13C in dissolved inorganic carbon, tritium (3H), stable isotopes of hydrogen (2H) and oxygen (18O), and noble gas concentrations were measured across a ~25 km2 area of Araihazar, ~30 km east of Dhaka.

Groundwater from >120 m depth is shown to be ~10,000 years old and its isotopic signatures indicate that recharge occurred at the time of changing climate from the late Pleistocene to early Holocene, with little recharge occurring since. In contrast, the intermediate depth low-As aquifers (<120 m) have a heterogeneous distribution of groundwater chemistry and ages, and contain groundwater recharged <60 years ago in certain locations. In one such area surrounding a small village, the effects that subsurface clay layer distribution has on recharge patterns and redox status of the intermediate aquifer was investigated. The relevant hydrogeologic and geochemical processes that led to documented failures of a community well at the site were assessed using a combination of solid and water phase geochemistry with tritium-helium (3H/3He) dating, hydraulic head monitoring, and pumping tests. Organic matter seeping from a compressible clay layer, which is subject to a pumping-induced, downward hydraulic gradient, reduces iron oxides and helps release As in the grey, upper part of the intermediate aquifer.

No recent recharge was detected by 3H measurements in the upper, grey sand layer, however a layer of orange sand beneath it contains groundwater that was recharged 10-60 years ago. This groundwater laterally bypasses the confining clay layer to recharge the middle of the aquifer and contains dissolved As levels of <10 µg/L. In this particular case, the pore water that leaches from clay layers contributes to As contamination, whereas the lateral recharge with shallow groundwater coincides with the low-As depth. Thus, clay layers may not always protect the low-As aquifers from As contamination, even if they can block direct vertical recharge with shallow groundwater enriched in As and organics. Finally, the adsorption of As to aquifer sediments, as a natural mechanism of the low-As aquifer defense against contamination, was assessed in the field via a column study. The column experiments were conducted by pumping shallow, high-As groundwater through freshly collected sediment cores to quantify the retardation of As transport through the aquifer.

This study demonstrated an elegant method of assessing contaminant transport under nearly in situ conditions that resulted in sorption estimates similar to those made by field studies using more challenging methods or located at hard-to-find sites with convenient flow patterns. My work, therefore, contributed to a better understanding of low-As aquifers in Bangladesh from the perspectives of both the groundwater flow and water-sediment interactions on various scales, and it integrated methods that can be employed elsewhere to characterize aquifers and study contaminant transport.