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Total arsenic, dissolved organic carbon (DOC), iron, major cations and anions were measured in tube-well waters used for drinking by people to investigate the geochemical condition of subsurface aquifer, source of arsenic and mechanism of arsenic release to groundwater of Bangladesh. Solid phases of total arsenic, iron, manganese and aluminum oxide and organic carbon (TOC) content in sediments were determined to find out their interrelationships. Arsenic concentrations in groundwaters vary from 0.03 to 0.75 mg/l with the mean value of 0.41 mg/l that exceed the maximum permissible limit of WHO (0.01 mg/l) and Bangladesh (0.05 mg/l) for drinking water. Arsenic concentrations demonstrate negative covariation with the concentrations of sulfate and nitrate but correlate weakly with iron concentrations and positively with those of ammonium ions. Dissolved iron exhibits a negative covariance with the …