Insights into methane dynamics from analysis of authigenic carbonates and chemosynthetic mussels at newly-discovered Atlantic Margin seeps

The recent discovery of active methane venting along the US northern and mid-Atlantic margin represents a new source of global methane not previously accounted for in carbon budgets from this region. However, uncertainty remains as to the origin and history of methane seepage along this tectonically inactive passive margin. Here we present the first isotopic analyses of authigenic carbonates and methanotrophic deep-sea mussels, Bathymodiolus sp., and the first direct constraints on the timing of past methane emission, based on samples collected at the upper slope Baltimore Canyon (similar to 385 m water depth) and deepwater Norfolk (similar to 1600 m) seep fields within the area of newly-discovered venting. The authigenic carbonates at both sites were dominated by aragonite, with an average delta C-13 signature of -47 parts per thousand, a value consistent with microbially driven anaerobic oxidation of methane-rich fluids occurring at or near the sediment-water interface. Authigenic carbonate U and Sr isotope data further support the inference of carbonate precipitation from seawater-derived fluids rather than from formation fluids from deep aquifers. Carbonate stable and radiocarbon (delta C-13 and Delta C-13) isotope values from living Bathymodiolus sp. specimens are lighter than those of seawater dissolved inorganic carbon, highlighting the influence of fossil carbon from methane on carbonate precipitation. U-Th dates on authigenic carbonates suggest seepage at Baltimore Canyon between 14.7 +/- 0.6 ka to 15.7 +/- 1.6 ka, and at the Norfolk seep field between 1.0 +/- 0.7 ka to 3.3 +/- 1.3 ka, providing constraint on the longevity of methane efflux at these sites. The age of the brecciated authigenic carbonates and the occurrence of pockmarks at the Baltimore Canyon upper slope could suggest a link between sediment delivery during Pleistocene sea-level lowstand, accumulation of pore fluid overpressure from sediment compaction, and release of overpressure through subsequent venting. Calculations show that the Baltimore Canyon site probably has not been within the gas hydrate stability zone (GHSZ) in the past 20 ka, meaning that in-situ release of methane from dissociating gas hydrate cannot be sustaining the seep. We cannot rule out updip migration of methane from dissociation of gas hydrate that occurs farther down the slope as a source of the venting at Baltimore Canyon, but consider that the history of rapid sediment accumulation and overpressure may play a more important role in methane emissions at this site. Published by Elsevier B.V.