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Raw CO2 and CH4 concentration data from a Picarro Cavity Ring Down Spectroscopy (CRDS) during experiments which tested the utility of methane as a tracer to quantify CO2 leakage into aqueous environments, as described in Myers, M., Roberts, J.J., White, C., and Stalker, L (2019) ‘An experimental investigation into quantifying CO2 leakage in aqueous environments using chemical tracers’ Chemical Geology