Title: Impacts of pumping on the distribution of arsenic in Bangladesh groundwater
Description: Chronic exposure to naturally occurring arsenic (As) in groundwater threatens the health of >150 million villagers in S/SE Asia. In Bangladesh, low As aquifers offer the best hope of reducing the exposure of 35-40 million remain exposed to elevated levels of As in drinking water (>10 μg/L). These low As aquifers could be affected, however, by massive pumping from shallow (<30 m) depths for growing rice and overexploitation of deeper aquifer for municipal water supply. The goal of this dissertation is to assess the impacts of groundwater pumping on the distribution in groundwater of dissolved As, reactive carbon, and redox-sensitive elements in anoxic aquifers of Bangladesh based on long-term hydrologic measurements, geochemical analyses, and numerical flow modeling. In the second chapter, changes in the well-water As concentrations within a 25 sq. km area over a 10+ year timespan are assessed on the basis of continuous time series for 18 monitoring wells, a set of 271 wells resampled three times, and a large dataset obtained from blanket surveys of several thousand wells in the region.

The two larger data sets both show a 10% decline in the initial areal mean As of 100 μg/L. This decline can be explained by flushing of As in the shallow aquifer by low-As recharge water, evidently compensated to some extent by the desorption of sediment-bound As. The presence of a large exchangeable pool of As in the sediment therefore seems to buffer changes in the distribution of As in the face of large perturbation in groundwater flow, albeit not enough to prevent some trends indicated by the detailed time series. The third chapter provides a complementary perspective on groundwater-sediment interactions by quantifying the rates of adsorption and desorption of As with column experiments conducted in the field for two different types of sediments: grey reduced Holocene sands and orange oxidized Pleistocene sands. The data show that, contrary to widely held beliefs, retardation of As transport by adsorption is quite similar in Holocene and Pleistocene sediments, even if Holocene sands initially contain a much larger pool of easily mobilizable As.

The field column experiments also showed significant changes in solid phase speciation that affected As retention within a timespan of only a few weeks. Detailed field observations and flow modeling in the fourth chapter examine how perturbed flow paths can draw either As or reactive carbon into a Pleistocene aquifer. A groundwater flow model, constrained by head measurements and isotopic tracer data shows that certain portions of the aquifer are becoming increasingly contaminated with As as a result of municipal pumping, but against a background of redox transformation in the aquifer that probably preceded this perturbation. Overall, the research conducted for this thesis shows that alteration of the hydrological system due to local and regional forcing is affecting the distribution of As in groundwater. These changes do not affect all wells yet and, if they do, the increase in As concentrations observed so far are gradual because of the buffering capacity of the sediment. Lowering exposure by targeting low As aquifer should therefore definitely continue in Bangladesh, with particular attention paid to regular monitoring using vulnerability criteria this research has helped to identify.