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Krypton‐81 dating provides new insights into the timing, mechanisms, and extent of meteoric flushing versus retention of saline fluids in the subsurface in response to changes in geologic and/or climatic forcings over 50 ka to 1.2 Ma year timescales. Remnant Paleozoic seawater‐derived brines associated with evaporites in the Paradox Basin, Colorado Plateau, are beyond the 81Kr dating range (>1.2 Ma) and have likely been preserved due to negative fluid buoyancy and low permeability. 81Kr dating of formation waters above the evaporites indicates topographically‐driven meteoric recharge and salt dissolution since the Late Pleistocene (0.03–0.8 Ma). Formation waters below the evaporites (up to 3 km depth), in basal aquifers, contain relatively young meteoric water components (0.4–1.1 Ma based on 81Kr) that partially flushed remnant brines and dissolved evaporites. We demonstrate that recent, rapid denudation of the Colorado Plateau (<4–10 Ma) activated deep, basinal‐scale flow systems as recorded in 81Kr groundwater age distributions. Plain Language Summary: Landscape changes over geological time alter hydraulic gradients and the presence or absence of near‐surface confining units, which drive the evolution of subsurface flow systems. However, our understanding of the time required for groundwater flow systems to respond to geological processes, such as shifts in topography, stratigraphy, and permeability structures, is still limited. This study uses krypton‐81 dating to constrain the age of meteoric waters in the Paradox Basin in the Colorado Plateau and constrain the timing of groundwater recharge into basinal aquifers. We discovered that rapid, widespread erosion and incision in the Colorado Plateau in the last 10 Ma activated deep meteoric circulation, partially flushing residual ancient seawater‐derived brines from aquifers above and below thick, evaporite confining units and dissolving salt. Krypton‐81 dating may provide insights into timescales and drivers of subsurface fluid flow and connectivity with the near‐surface in other environments. Key Points: Meteoric waters up to 3 km in basinal aquifers are <1.1 MaRecent, rapid denudation of the Colorado Plateau enabled deep circulation of meteoric water and flushing of connate brinesKrypton‐81 dating can illuminate the timescales and extent of meteoric circulation in response to geologic and/or climatic forcings [ABSTRACT FROM AUTHOR]

Abstract: Identification of the source of CO2 in natural reservoirs and development of physical models to account for the migration and interaction of this CO2 with the groundwater is essential for developing a quantitative understanding of the long term storage potential of CO2 in the subsurface. We present the results of 57 noble gas determinations in CO2 rich fields (>82%) from three natural reservoirs to the east of the Colorado Plateau uplift province, USA (Bravo Dome, NM., Sheep Mountain, CO. and McCallum Dome, CO.), and from two reservoirs from within the uplift area (St. John’s Dome, AZ., and McElmo Dome, CO.). We demonstrate that all fields have CO2/3He ratios consistent with a dominantly magmatic source. The most recent volcanics in the province date from 8 to 10ka and are associated with the Bravo Dome field. The oldest magmatic activity dates from 42 to 70Ma and is associated with the McElmo Dome field, located in the tectonically stable centre of the Colorado Plateau: CO2 can be stored within the subsurface on a millennia timescale. The manner and extent of contact of the CO2 phase with the groundwater system is a critical parameter in using these systems as natural analogues for geological storage of anthropogenic CO2. We show that coherent fractionation of groundwater 20Ne/36Ar with crustal radiogenic noble gases (4He, 21Ne, 40Ar) is explained by a two stage re-dissolution model: Stage 1: Magmatic CO2 injection into the groundwater system strips dissolved air-derived noble gases (ASW) and accumulated crustal/radiogenic noble gas by CO2/water phase partitioning. The CO2 containing the groundwater stripped gases provides the first reservoir fluid charge. Subsequent charges of CO2 provide no more ASW or crustal noble gases, and serve only to dilute the original ASW and crustal noble gas rich CO2. Reservoir scale preservation of concentration gradients in ASW-derived noble gases thus provide CO2 filling direction. This is seen in the Bravo Dome and St. John’s Dome fields. Stage 2: The noble gases re-dissolve into any available gas stripped groundwater. This is modeled as a Rayleigh distillation process and enables us to quantify for each sample: (1) the volume of groundwater originally ‘stripped’ on reservoir filling; and (2) the volume of groundwater involved in subsequent interaction. The original water volume that is gas stripped varies from as low as 0.0005cm3 groundwater/cm3 gas (STP) in one Bravo Dome sample, to 2.56cm3 groundwater/cm3 gas (STP) in a St. John’s Dome sample. Subsequent gas/groundwater equilibration varies within all fields, each showing a similar range, from zero to ∼100cm3 water/cm3 gas (at reservoir pressure and temperature). [Copyright &y& Elsevier]

The Paradox Basin in the Colorado Plateau (USA) has some of the most iconic records of paleofluid flow, including sandstone bleaching and ore mineralization, and hydrocarbon, CO2, and He reservoirs, yet the sources of fluids responsible for these extensive fluid-rock reactions are highly debated. This study, for the first time, characterizes fluids within the basin to constrain the sources and emergent behavior of paleofluid flow resulting in the iconic rock records. Major ion and isotopic (d18Owater; dDwater; d18OSO4; d34SSO4; d34SH2S; 87Sr/86Sr) signatures of formation waters were used to evaluate the distribution and sources of fluids and water-rock interactions by comparison with the rock record. There are two sources of salinity in basinal fluids: (1) diagenetically altered highly evaporated paleo-seawater-derived brines associated with the Pennsylvanian Paradox Formation evaporites; and (2) dissolution of evaporites by topographically driven meteoric circulation. Fresh to brackish groundwater in the shallow Cretaceous Burro Canyon Formation contains low Cu and high SO4 concentrations and shows oxidation of sulfides by meteoric water, while U concentrations are higher than within other formation waters. Deeper brines in the Pennsylvanian Honaker Trail Formation were derived from evaporated paleo-seawater mixed with meteoric water that oxidized sulfides and dissolved gypsum and have high 87Sr/86Sr indicating interaction with radiogenic siliciclastic minerals. Upward migration of reduced (hydrocarbon- and H2S-bearing) saline fluids from the Pennsylvanian Paradox Formation along faults likely bleached sandstones in shallower sediments and provided a reduced trap for later Cu and U deposition. The distribution of existing fluids in the Paradox Basin provides important constraints to understand the rock record over geological time. [ABSTRACT FROM AUTHOR]