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  1. Abstract

    The noble gas temperature climate proxy is an established tool that has previously been applied to determine the source of groundwater recharge, however, unanswered questions remain. In fractured media (e.g., volcanic islands) recharge can be so rapid that groundwater is significantly depleted in heavy noble gases, indicating that the water has retained noble gas concentrations from higher elevations. Previous studies of rain samples have confirmed a match to patterns seen in fractured‐rock groundwater for heavy noble gases along with a significant helium excess. Snow has been shown to be a credible source for both the helium excess and the observed heavy noble gas pattern. Here, liquid cloud water samples were collected at two mountainous sites and analyzed for noble gas concentrations. A pattern like that of rainwater was found. However, an analysis of diffusive uptake of noble gases into cloud water demonstrates that droplets of 1 mm diameter and smaller should be in constant solubility equilibrium with the atmosphere. To explain this, we present a novel hypothesis that relies on the assumption that liquid water consists of two types of water molecule clusters bounded by hydrogen bonds: a low‐density ice‐like structure and a high‐density condensed structure. In this model, the pressure gradient near the surface of a droplet resulting from surface tension could allow for the formation of a surface layer that is rich in ice‐like low density clusters. This can explain both the helium excess and the heavy noble gas depletion seen in the samples.

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  2. Extensive development of shale gas has generated some concerns about environmental impacts such as the migration of natural gas into water resources. We studied high gas concentrations in waters at a site near Marcellus Shale gas wells to determine the geological explanations and geochemical implications. The local geology may explain why methane has discharged for 7 years into groundwater, a stream, and the atmosphere. Gas may migrate easily near the gas wells in this location where the Marcellus Shale dips significantly, is shallow (∼1 km), and is more fractured. Methane and ethane concentrations in local water wells increased after gas development compared with predrilling concentrations reported in the region. Noble gas and isotopic evidence are consistent with the upward migration of gas from the Marcellus Formation in a free-gas phase. This upflow results in microbially mediated oxidation near the surface. Iron concentrations also increased following the increase of natural gas concentrations in domestic water wells. After several months, both iron and SO42−concentrations dropped. These observations are attributed to iron and SO42−reduction associated with newly elevated concentrations of methane. These temporal trends, as well as data from other areas with reported leaks, document a way to distinguish newly migrated methane from preexisting sources of gas. This study thus documents both geologically risky areas and geochemical signatures of iron and SO42−that could distinguish newly leaked methane from older methane sources in aquifers.

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