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Measurements of the natural radiocarbon content of methane (14C-CH4) dissolved in seawater and freshwater have been used to investigate sources and dynamics of methane. However, during investigations along the Atlantic, Pacific, and Arctic Ocean Margins of the United States, as well as in the North American Great Lakes, some samples revealed highly elevated 14C-CH4 values, as much as 4-5 times above contemporary atmospheric 14C-CH4 levels. Natural production of the 14CH4 isotopologue is too low to cause these observations nor can it explain the variations i