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Methane is a powerful greenhouse gas and a key player in atmospheric chemistry. Important uncertainties remain in the global atmospheric methane budget, with natural geologic emissions being one of the particularly uncertain terms. In recent bottom-up studies, geologic emissions have been estimated to comprise up to 10% of the global budget (40–60 Teragrams of methane per year, Tg CH4 yr–1). In contrast, top-down constraints from 14C of methane in preindustrial air extracted from ice cores indicate that the geologic methane source is approximately an order of magnitude lower. Recent bottom-up inventories propose microseepage (diffuse low-level flux of methane through soils over large areas) as the largest single component of the geologic methane flux. In this study, we present new measurements of methane microseepage from the Appalachian Basin (Western New York State) and compare these with prior microseepage measurements from other regions and with predicted values from the most recent bottom-up inventory. Our results show lower microseepage values than most prior data sets and indicate that positive microseepage fluxes in this region are not as widespread as previously assumed. A statistical analysis of our results indicates that mean microseepage flux in this region has very likely been overestimated by the bottom-up inventory, even though our measurements more likely than not underestimate the true mean flux. However, this is a small data set from a single region and as such cannot be used to evaluate the validity of the microseepage emissions inventory as a whole. Instead, the results demonstrate the need for a more extensive network of direct geologic emission measurements in support of improved bottom-up inventories. 

Abstract. Important uncertainties remain in our understanding of the spatial andtemporal variability of atmospheric hydroxyl radical concentration ([OH]).Carbon-14-containing carbon monoxide (14CO) is a useful tracer that canhelp in the characterization of [OH] variability. Prior measurements ofatmospheric 14CO concentration ([14CO] are limited in both theirspatial and temporal extent, partly due to the very large air sample volumes that have been required for measurements (500–1000 L at standardtemperature and pressure, L STP) and the difficulty and expense associatedwith the collection, shipment, and processing of such samples. Here wepresent a new method that reduces the air sample volume requirement to≈90 L STP while allowing for [14CO] measurement uncertainties that are on par with or better than prior work (≈3 % or better, 1σ). The method also for the first time includes accurate characterization of the overall procedural [14CO] blank associated with individual samples, which is a key improvement over prior atmospheric 14CO work. The method was used to make measurements of [14CO] at the NOAA Mauna Loa Observatory, Hawaii, USA, between November 2017 and November 2018. The measurements show the expected [14CO] seasonal cycle (lowest in summer)and are in good agreement with prior [14CO] results from anotherlow-latitude site in the Northern Hemisphere. The lowest overall [14CO]uncertainties (2.1 %, 1σ) are achieved for samples that aredirectly accompanied by procedural blanks and whose mass is increased to≈50 µgC (micrograms of carbon) prior to the 14Cmeasurement via dilution with a high-CO 14C-depleted gas.