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USGS2024

Characterizing sulfur redox state and geochemical implications in deep-time using mineral chemistry network analysis

Sulfur (S) is a central element in global biogeochemical cycling and Earth’s redox evolution. Minerals that contain S are an important record of local environmental conditions at the time of their formation based on chemical speciation and redox. However, the oxidation state of S for hundreds of different S-containing minerals and thousands of S-containing mineral localities is unknown, largely sulfides and sulfosalts, and the redox state alone does not fully capture mineral chemistry diversity, thus limiting understanding of S redox evolution. Here, we use mineral chemistry network analysis and the weighted Mineral Element Electronegativity Coefficient of Variation (wMEE CV ) metric to investigate the element interactions and localities of S-containing minerals from the Mineral Evolution Database (MED) to infer the redox state of S in minerals where the redox state is unknown (S U ). Louvain community detection of the S mineral chemistry redox network reveals that there are three main network communities that are separated by redox state. The S 6+ community includes minerals that contain the S 6+ redox state and a small number of S 4+ and S 2+ minerals, the S 2− community includes S 2− -containing minerals, and the S U community includes minerals in which the redox state of S is unknown. The wMEE CV values of the S U community closely overlap with the wMEE CV values of the S 2− community, and do not overlap with the wMEE CV values of the S 6+ community, indicating the S U community minerals contain predominately reduced S. Assuming that S U community minerals contain reduced S, as supported by their network chemical associations and wMEE CV values, then reduced S-containing minerals make up approximately 81 % of S-containing mineral localities in the S mineral chemistry network, even though the majority of all mineral localities (S-containing and non-S-containing) are oxygen (O)-containing minerals. Additionally, reduced S-containing minerals make up the majority (∼75 %) of all non-O containing mineral localities in the MED, representing the importance of reduced S as an electron source and substrate in the evolution of microbial metabolic networks. The range wMEE CV values of S 6+ community minerals expands through time due primarily to formation of chemically diverse sulfate minerals, coinciding with crustal oxidation from the late Proterozoic to Phanerozoic and the expansion of the marine sulfate reservoir. The intersection of shared constituent elements among reduced and oxidized S in the mineral chemistry network represents redox convergence of weathered S in the geosphere that was crucial in the formation of natural resource deposits and the evolution of biogeochemical cycles.

Geochimica et Cosmochimica Acta↗

USGS2007

Methane-derived authigenic carbonates from the northern Gulf of Mexico - MD02 Cruise

Authigenic carbonates were sampled in piston cores collected from both the Tunica Mound and the Mississippi Canyon area on the continental slope of the northern Gulf of Mexico during a Marion Dufresne cruise in July 2002. The carbonates are present as hardgrounds, porous crusts, concretions or nodules and shell fragments with or without carbonate cements. Carbonates occurred at gas venting sites which are likely to overlie gas hydrates bearing sediments. Electron microprobe, X-ray diffraction (XRD) and thinsection investigations show that these carbonates are high-Mg calcite (6–21 mol% MgCO 3 ), with significant presence of framboidal pyrite. All carbonates are depleted in 13 C ( δ 13 C = − 61.9 to − 31.5‰ PDB) indicating that the carbon is derived mainly from anaerobic methane oxidation (AMO). Age estimates based on 14 C dating of shell fragments and on regional sedimentation rates indicate that these authigenic carbonates formed within the last 1000 yr in the Mississippi Canyon and within 5500 yr at the Tunica Mound. The oxygen isotopic composition of carbonates ranges from + 3.4 to + 5.9‰ PDB. Oxygen isotopic compositions and Mg 2+ contents of carbonates, and present in-situ temperatures of bottom seawater/sediments, show that some of these carbonates, especially from a core associated with underlying massive gas hydrates precipitated in or near equilibrium with bottom-water. On the other hand, those carbonates more enriched in 18 O are interpreted to have precipitated from 18 O-rich fluids which are thought to have been derived from the dissociation of gas hydrates. The dissociation of gas hydrates in the northern Gulf of Mexico within the last 5500 yr may be caused by nearby salt movement and related brines.

Journal of Geochemical Exploration↗

USGS2023

Precipitation, submarine groundwater discharge of nitrogen, and red tides along the southwest Florida Gulf coast

Blooms of the dinoflagellate Karenia brevis occur almost every year along the southwest Florida Gulf coast. Long-duration blooms with especially high concentrations of K. brevis , known as red tides, destroy marine life through production of neurotoxins. Current hypotheses are that red tides originate in oligotrophic waters far offshore using nitrogen (N) from upwelling bottom water or, alternatively, from blooms of Trichodesmium , followed by advection to nearshore waters. But the amount of N available from terrestrial sources does not appear to be adequate to maintain a nearshore red tide. To explain this discrepancy, we hypothesize that contemporary red tides are associated with release of N from offshore submarine groundwater discharge (SGD) that has accumulated in benthic sediment biomass by dissimilatory nitrate reduction to ammonium (DNRA). The release occurs when sediment labile organic carbon (LOC), used as the electron donor in DNRA, is exhausted. Detritus from the resulting destruction of marine life restores the sediment LOC to continue the cycle of red tides. The severity of individual red tides increases with increased bloom-year precipitation in the geographic region where the SGD originates, while the severity of ordinary blooms is relatively unaffected.

Florida↗

USGS2004

Ancient wet aeolian environments on Earth: Clues to presence of fossil/live microorganisms on Mars

Ancient wet aeolian (wet-sabkha) environments on Earth, represented in the Entrada and Navajo sandstones of Utah, contain pipe structures considered to be the product of gas/water release under pressure. The sediments originally had considerable porosity allowing the ingress of living plant structures, microorganisms, clay minerals, and fine-grained primary minerals of silt and sand size from the surface downward in the sedimentary column. Host rock material is of a similar size and porosity and presumably the downward migration of fine-grained material would have been possible prior to lithogenesis and final cementation. Recent field emission scanning electron microscopy (FESEM) and EDS (energy-dispersive spectrometry) examination of sands from fluidized pipes in the Early Jurassic Navajo Sandstone reveal the presence of fossil forms resembling fungal filaments, some bearing hyphopodium-like structures similar to those produced by modern tropical leaf parasites. The tropical origin of the fungi is consistent with the paleogeography of the sandstone, which was deposited in a tropical arid environment. These fossil fungi are silicized, with minor amounts of CaCO3 and Fe, and in some cases a Si/Al ratio similar to smectite. They exist as pseudomorphs, totally depleted in nitrogen, adhering to the surfaces of fine-grained sands, principally quartz and orthoclase. Similar wet aeolian paleoenvironments are suspected for Mars, especially following catastrophic sediment-charged floods of enormous magnitudes that are believed to have contributed to rapid formation of large water bodies in the northern plains, ranging from lakes to oceans. These events are suspected to have contributed to a high frequency of constructional landforms (also known as pseudocraters) related to trapped volatiles and water-enriched sediment underneath a thick blanket of materials that were subsequently released to the martian surface, forming piping structures at the near surface and constructional landforms at the surface. This constructional process on Mars may help unravel the complex history of some of the piping structures observed on Earth; on Earth, evidence for the constructional landforms has been all but erased and the near-surface piping structures exposed through millions of years of differential erosion and topographic inversion now occur as high-standing promontories. If the features on both Earth and Mars formed by similar processes, especially involving water and other volatiles, and since the piping structures of Earth provided suitable environments for life to thrive in, the martian features in the northern plains should be considered as prime targets for physico/mineral/chemical/microbiological analyses once the astrobiological exploration of the red planet begins in earnest. ?? 2004 Elsevier Inc. All rights reserved.

Icarus↗

USGS2010

The High Resolution Imaging Science Experiment (HiRISE) during MRO's Primary Science Phase (PSP)

The High Resolution Imaging Science Experiment (HiRISE) on the Mars Reconnaissance Orbiter (MRO) acquired 8 terapixels of data in 9137 images of Mars between October 2006 and December 2008, covering ∼0.55% of the surface. Images are typically 5–6 km wide with 3-color coverage over the central 20% of the swath, and their scales usually range from 25 to 60 cm/pixel. Nine hundred and sixty stereo pairs were acquired and more than 50 digital terrain models (DTMs) completed; these data have led to some of the most significant science results. New methods to measure and correct distortions due to pointing jitter facilitate topographic and change-detection studies at sub-meter scales. Recent results address Noachian bedrock stratigraphy, fluvially deposited fans in craters and in or near Valles Marineris, groundwater flow in fractures and porous media, quasi-periodic layering in polar and non-polar deposits, tectonic history of west Candor Chasma, geometry of clay-rich deposits near and within Mawrth Vallis, dynamics of flood lavas in the Cerberus Palus region, evidence for pyroclastic deposits, columnar jointing in lava flows, recent collapse pits, evidence for water in well-preserved impact craters, newly discovered large rayed craters, and glacial and periglacial processes. Of particular interest are ongoing processes such as those driven by the wind, impact cratering, avalanches of dust and/or frost, relatively bright deposits on steep gullied slopes, and the dynamic seasonal processes over polar regions. HiRISE has acquired hundreds of large images of past, present and potential future landing sites and has contributed to scientific and engineering studies of those sites. Warming the focal-plane electronics prior to imaging has mitigated an instrument anomaly that produces bad data under cold operating conditions.

Icarus↗

USGS2013

Weakening of ice by magnesium perchlorate hydrate

We show that perchlorate hydrates, which have been detected at high circumpolar martian latitudes, have a dramatic effect upon the rheological behavior of polycrystalline water ice under conditions applicable to the North Polar Layered Deposits (NPLD). We conducted subsolidus creep tests on mixtures of ice and magnesium perchlorate hydrate, Mg(ClO4)2·6H2O (MP6), of 0.02, 0.05, 0.10, and 0.47 volume fraction MP6. We found these mixtures to be increasingly weak with increasing MP6 content. For mixtures with ⩽0.10 volume fraction MP6, we resolved a stress exponent of n ≈ 2 at low stresses transitioning to n ≈ 4 above 10 MPa. Scanning electron microscopy of deformed specimens revealed MP6 to be distributed as an interconnected film between ice grains. These results suggest that grain boundary sliding (GBS) may be enhanced with respect to pure ice. As the enhancement of GBS is expected in polycrystalline aggregates containing a few percent melt or otherwise weak material distributed along grain boundaries, the observed n ≈ 2 is consistent with the mutual accommodation of basal slip and GBS. If ice containing trace concentrations of MP6 is also much weaker than pure ice at low stresses, flow in the NPLD could be significantly enhanced, particularly at the warmer basal temperatures associated with higher martian obliquities.

Icarus↗

USGS2025

Reaction kinetics and accelerant effects of sulfides in early mature hydrocarbon generation using hydrous pyrolysis

Hydrocarbon generation in organic-rich sediments is influenced by the molecular organic composition and relative abundance of associated minerals. Certain mineral-derived elements act as catalysts and reaction intermediaries, facilitating early-stage hydrocarbon formation in potential source rocks. This study investigated the role of sulfur contributed from pyrite as an accelerant in thermal reaction, focusing on its effects on early maturation and consequent hydrocarbon generation from gilsonite (low-sulfur solid petroleum). Hydrous pyrolysis (HP) experiments were conducted on mixtures of gilsonite and pyrite in varying ratios (1:0.1, 1:0.5, 1:1, 1:2, and 1:10 w/w gilsonite:pyrite) at 320, 350, and 370 °C for 72 h. Untreated and thermally altered residues were analyzed using solid bitumen reflectance (BR o , %), total organic carbon (TOC) content, programmed temperature pyrolysis, scanning electron microscopy with energy-dispersive spectroscopy (SEM-EDS), and X-ray diffraction (XRD) to evaluate the potential accelerant role of pyritic sulfur in hydrocarbon formation. The results show HP residues at 320 and 350 °C with greater pyrite concentrations had higher BR o , while reflectance values were similar in the 370 °C residues, regardless of pyrite concentration, suggesting enhanced reaction at lower thermal conditions. Increasing pyrite content systematically decreased hydrogen index (HI) values while increasing the transformation ratio (TR) and production index (PI), indicating enhanced conversion of organic matter to hydrocarbons with increasing pyrite concentrations. Gas yields increased with pyrite addition, particularly at 350 °C, confirming secondary cracking effects. However, gas production stabilized or declined at higher pyrite loadings (1:10), suggesting alternative reaction pathways such as coke formation. Our data indicate the presence of pyrite lowers the activation energy for thermal cracking, shifting peak experimental hydrocarbon generation temperatures downward by 20–30 °C, with the most pronounced accelerant effects observed at moderate pyrite concentrations (1:0.5 and 1:1). The thermodynamic framework reveals that pyrite stability is influenced by experimental conditions, with pyrrhotite formation favored in the presence of gilsonite due to reduced oxygen fugacity. Pyrite transformation to pyrrhotite, as observed through XRD, SEM-EDS, and predicted by thermodynamic data, further supports the accelerant role of S, as pyrrhotite exhibits a higher hydrogen transfer potential, promoting early oil generation. These findings highlight the importance of pyrite in modulating hydrocarbon generation pathways in organic-rich systems.

Journal of Analytical and Applied Pyrolysis↗

USGS2009

Biogeochemistry at a wetland sediment-alluvial aquifer interface in a landfill leachate plume

The biogeochemistry at the interface between sediments in a seasonally ponded wetland (slough) and an alluvial aquifer contaminated with landfill leachate was investigated to evaluate factors that can effect natural attenuation of landfill leachate contaminants in areas of groundwater/surface-water interaction. The biogeochemistry at the wetland-alluvial aquifer interface differed greatly between dry and wet conditions. During dry conditions (low water table), vertically upward discharge was focused at the center of the slough from the fringe of a landfill-derived ammonium plume in the underlying aquifer, resulting in transport of relatively low concentrations of ammonium to the slough sediments with dilution and dispersion as the primary attenuation mechanism. In contrast, during wet conditions (high water table), leachate-contaminated groundwater discharged upward near the upgradient slough bank, where ammonium concentrations in the aquifer where high. Relatively high concentrations of ammonium and other leachate constituents also were transported laterally through the slough porewater to the downgradient bank in wet conditions. Concentrations of the leachate-associated constituents chloride, ammonium, non-volatile dissolved organic carbon, alkalinity, and ferrous iron more than doubled in the slough porewater on the upgradient bank during wet conditions. Chloride, non-volatile dissolved organic carbon (DOC), and bicarbonate acted conservatively during lateral transport in the aquifer and slough porewater, whereas ammonium and potassium were strongly attenuated. Nitrogen isotope variations in ammonium and the distribution of ammonium compared to other cations indicated that sorption was the primary attenuation mechanism for ammonium during lateral transport in the aquifer and the slough porewater. Ammonium attenuation was less efficient, however, in the slough porewater than in the aquifer and possibly occurred by a different sorption mechanism. A stoichiometrically balanced increase in magnesium concentration with decreasing ammonium and potassium concentrations indicated that cation exchange was the sorption mechanism in the slough porewater. Only a partial mass balance could be determined for cations exchanged for ammonium and potassium in the aquifer, indicating that some irreversible sorption may be occurring. Although wetlands commonly are expected to decrease fluxes of contaminants in riparian environments, enhanced attenuation of the leachate contaminants in the slough sediment porewater compared to the aquifer was not observed in this study. The lack of enhanced attenuation can be attributed to the fact that the anoxic plume, comprised largely of recalcitrant DOC and reduced inorganic constituents, interacted with anoxic slough sediments and porewaters, rather than encountering a change in redox conditions that could cause transformation reactions. Nevertheless, the attenuation processes in the narrow zone of groundwater/surface-water interaction were effective in reducing ammonium concentrations by a factor of about 3 during lateral transport across the slough and by a factor of 2 to 10 before release to the surface water. Slough porewater geochemistry also indicated that the slough could be a source of sulfate in dry conditions, potentially providing a terminal electron acceptor for natural attenuation of organic compounds in the leachate plume.

Journal of Contaminant Hydrology↗

USGS2012

Cyclic biogeochemical processes and nitrogen fate beneath a subtropical stormwater infiltration basin

A stormwater infiltration basin in north–central Florida, USA, was monitored from 2007 through 2008 to identify subsurface biogeochemical processes, with emphasis on N cycling, under the highly variable hydrologic conditions common in humid, subtropical climates. Cyclic variations in biogeochemical processes generally coincided with wet and dry hydrologic conditions. Oxidizing conditions in the subsurface persisted for about one month or less at the beginning of wet periods with dissolved O 2 and NO 3 - showing similar temporal patterns. Reducing conditions in the subsurface evolved during prolonged flooding of the basin. At about the same time O 2 and NO 3 - reduction concluded, Mn, Fe and SO 4 2 - reduction began, with the onset of methanogenesis one month later. Reducing conditions persisted up to six months, continuing into subsequent dry periods until the next major oxidizing infiltration event. Evidence of denitrification in shallow groundwater at the site is supported by median NO 3 -–N less than 0.016 mg L -1 , excess N 2 up to 3 mg L -1 progressively enriched in δ 15 N during prolonged basin flooding, and isotopically heavy δ 15 N and δ 18 O of NO 3 - (up to 25&permil; and 15&permil;, respectively). Isotopic enrichment of newly infiltrated stormwater suggests denitrification was partially completed within two days. Soil and water chemistry data suggest that a biogeochemically active zone exists in the upper 1.4 m of soil, where organic carbon was the likely electron donor supplied by organic matter in soil solids or dissolved in infiltrating stormwater. The cyclic nature of reducing conditions effectively controlled the N cycle, switching N fate beneath the basin from NO 3 - leaching to reduction in the shallow saturated zone. Results can inform design of functionalized soil amendments that could replace the native soil in a stormwater infiltration basin and mitigate potential NO 3 - leaching to groundwater by replicating the biogeochemical conditions under the observed basin.

Florida↗

USGS2013

Complex resistivity signatures of ethanol biodegradation in porous media

Numerous adverse effects are associated with the accidental release of ethanol (EtOH) and its persistence in the subsurface. Geophysical techniques may permit non-invasive, real time monitoring of microbial degradation of hydrocarbon. We performed complex resistivity (CR) measurements in conjunction with geochemical data analysis on three microbial-stimulated and two control columns to investigate changes in electrical properties during EtOH biodegradation processes in porous media. A Debye Decomposition approach was applied to determine the chargeability ( m ), normalized chargeability ( m n ) and time constant ( τ ) of the polarization magnitude and relaxation length scale as a function of time. The CR responses showed a clear distinction between the bioaugmented and control columns in terms of real ( σ′ ) and imaginary ( σ″ ) conductivity, phase ( ϕ ) and apparent formation factor ( F app ). Unlike the control columns, a substantial decrease in σ′ and increase in F app occurred at an early time (within 4 days) of the experiment for all three bioaugmented columns. The observed decrease in σ′ is opposite to previous studies on hydrocarbon biodegradation. These columns also exhibited increases in ϕ (up to ~ 9 mrad) and σ″ (up to two order of magnitude higher) 5 weeks after microbial inoculation. Variations in m and m n were consistent with temporal changes in ϕ and σ″ responses, respectively. Temporal geochemical changes and high resolution scanning electron microscopy imaging corroborated the CR findings, thus indicating the sensitivity of CR measurements to EtOH biodegradation processes. Our results offer insight into the potential application of CR measurements for long-term monitoring of biogeochemical and mineralogical changes during intrinsic and induced EtOH biodegradation in the subsurface.

Journal of Contaminant Hydrology↗

USGS2018

Uptake and distribution of organo-iodine in deep-sea corals

Understanding iodine concentration, transport, and bioavailability is essential in evaluating iodine's impact to the environment and its effectiveness as an environmental biogeotracer. While iodine and its radionuclides have proven to be important tracers in geologic and biologic studies, little is known about transport of this element to the deep sea and subsequent uptake in deep-sea coral habitats. Results presented here on deep-sea black coral iodine speciation and iodine isotope variability provides key information on iodine behavior in natural and anthropogenic environments, and its geochemical pathway in the Gulf of Mexico. Organo-iodine is the dominant iodine species in the black corals, demonstrating that binding of iodine to organic matter plays an important role in the transport and transfer of iodine to the deep-sea corals. The identification of growth bands captured in high-resolution scanning electron images (SEM) with synchronous peaks in iodine variability suggest that riverine delivery of terrestrial-derived organo-iodine is the most plausible explanation to account for annual periodicity in the deep-sea coral geochemistry. Whereas previous studies have suggested the presence of annual growth rings in deep-sea corals, this present study provides a mechanism to explain the formation of annual growth bands. Furthermore, deep-sea coral ages based on iodine peak counts agree well with those ages derived from radiocarbon ( 14 C) measurements. These results hold promise for developing chronologies independent of 14 C dating, which is an essential component in constraining reservoir ages and using radiocarbon as a tracer of ocean circulation. Furthermore, the presence of enriched 129 I/ 127 I ratios during the most recent period of skeleton growth is linked to nuclear weapons testing during the 1960s. The sensitivity of the coral skeleton to record changes in surface water 129 I composition provides further evidence that iodine composition and isotope variability captured in proteinaceous deep-sea corals is a promising geochronometer as well as an emerging tracer for continental material flux.

Journal of Environmental Radioactivity↗

USGS2013

Combined ESR/U-series chronology of Acheulian hominid-bearing layers at Trinchera Galería site, Atapuerca, Spain

The Sierra de Atapuerca, northern Spain, is known from many prehistoric and palaeontological sites documenting human prehistory in Europe. Three major sites, Gran Dolina, Galería and Sima del Elefante, range in age from the oldest hominin of Western Europe dated to 1.1 to 1.3 Ma (millions of years ago) at Sima del Elefante to c.a. 0.2 Ma on the top of the Galería archaeological sequence. Recently, a chronology based on luminescence methods (Thermoluminescence [TL] and Infrared Stimulated Luminescence [IRSL]) applied to cave sediments was published for the Gran Dolina and Galería sites. The authors proposed for Galería an age of 450 ka (thousands of years ago) for the units lower GIII and GII, suggesting that the human occupation there is younger than the hominid remains of Sima de los Huesos (>530 ka) around 1 km away. In this paper, we present new results obtained by combined Electron Spin Resonance/Uranium-series (ESR/U-series) dating on 20 herbivorous teeth from different levels at the Galería site. They are in agreement with the TL results for the upper part of the stratigraphic sequence (GIV and GIIIb), in the range of between 200 and 250 ka. But for the GIIIa to GIIb levels, the TL ages become abruptly older by 200 ka while ESR ages remain relatively constant. Finally, the TL and ESR data agree in the lowest part of the section (GIIa); both fall in the range of around 350–450 ka. Our results suggest a different interpretation for the GII, GIII and GIV units of Galería and the upper part of Gran Dolina (TD10 and TD11) than obtained by TL. The ESR/U-series results are supported by a Bayesian analysis, which allows a better integration between stratigraphic information and radiometric data.

Atapuerca Mountains↗

USGS2007

Aquifer-scale controls on the distribution of nitrate and ammonium in ground water near La Pine, Oregon, USA

Geochemical and isotopic tools were applied at aquifer, transect, and subtransect scales to provide a framework for understanding sources, transport, and fate of dissolved inorganic N in a sandy aquifer near La Pine, Oregon. NO3 is a common contaminant in shallow ground water in this area, whereas high concentrations of NH4-N (up to 39 mg/L) are present in deep ground water. N concentrations, N/Cl ratios, tracer-based apparent ground-water ages, N isotope data, and hydraulic gradients indicate that septic tank effluent is the primary source of NO3. N isotope data, N/Cl and N/C relations, 3H data, and hydraulic considerations point to a natural, sedimentary organic matter source for the high concentrations of NH4, and are inconsistent with an origin as septic tank N. Low recharge rates and flow velocities have largely restricted anthropogenic NO3 to isolated plumes within several meters of the water table. A variety of geochemical and isotopic data indicate that denitrification also affects NO3 gradients in the aquifer. Ground water in the La Pine aquifer evolves from oxic to increasingly reduced conditions. Suboxic conditions are achieved after about 15-30 y of transport below the water table. NO3 is denitrified near the oxic/suboxic boundary. Denitrification in the La Pine aquifer is characterized well at the aquifer scale with a redox boundary approach that inherently captures spatial variability in the distribution of electron donors.

Oregon↗

USGS2007

Evidence of CFC degradation in groundwater under pyrite-oxidizing conditions

A detailed local-scale monitoring network was used to assess CFC distribution in an unconfined sand aquifer in southwestern Ontario where the zone of 1–5-year-old groundwater was known with certainty because of prior use of a bromide tracer. Groundwater ⩽5 years old was confined to an aerobic zone at ⩽5 m depth and had CFC concentrations consistent with modern atmospheric mixing ratios at recharge temperatures of 7–11 °C, as was observed in the 3-m thick vadose zone at the site. At depths below 6 m, the groundwater became progressively more reducing, however, with a denitrifying horizon at 6–7 m depth, and a Mn and Fe reducing zone below 7 m depth. In the anaerobic zone, 3 H/ 3 He ratios indicated that groundwater-age continued to increase uniformly with depth, to a maximum value of 27 years at 13 m depth. CFC concentrations, however, decreased abruptly within the denitrifying zone, leading to substantial age overestimation compared to the 3 H/ 3 He ages. Noble gas data indicated that the apparent CFC mass loss was not likely the result of gas stripping from possible bubble formation; thus, CFC degradation was indicated in the anoxic zone. The field data are consistent with first-order degradation rates of 0.3 yr −1 for CFC-12, 0.7 yr −1 for CFC-11, and 1.6 yr −1 for CFC-113. CFC attenuation at this site coincides with a zone where reduced S (pyrite) is actively oxidized by NO 3 and dissolved oxygen (DO). Similar behavior has been observed at other sites [Tesoriero, A.J., Liebscher, H., Cox, S.E., 2000. Mechanism and rate of denitrification in an agricultural watershed: electron and mass balance along groundwater flow path. Water Resour. Res. 36 (6), 1545–1559; Hinsby, K., Hojberg, A.L., Engesgaard, P., Jensen, K.H., Larsen, F., Plummer, L.N., Busenberg, E., Accepted for publication. Transport and degradation of chlorofluorocarbons (CFCs) in a pyritic aquifer, Rabis Creek, Denmark. Water Resour. Res.], further demonstrating that the use of CFCs for age-dating anaerobic groundwater should be approached with caution, particularly if the sediment contains pyrite.

Journal of Hydrology↗

USGS2008

Inverse geochemical modeling of groundwater evolution with emphasis on arsenic in the Mississippi River Valley alluvial aquifer, Arkansas (USA)

Inverse geochemical modeling (PHREEQC) was used to identify the evolution of groundwater with emphasis on arsenic (As) release under reducing conditions in the shallow (25-30 m) Mississippi River Valley Alluvial aquifer, Arkansas, USA. The modeling was based on flow paths defined by high-precision (??2 cm) water level contour map; X-ray diffraction (XRD), scanning electron microscopic (SEM), and chemical analysis of boring-sediments for minerals; and detailed chemical analysis of groundwater along the flow paths. Potential phases were constrained using general trends in chemical analyses data of groundwater and sediments, and saturation indices data (MINTEQA2) of minerals in groundwater. Modeling results show that calcite, halite, fluorite, Fe oxyhydroxide, organic matter, H2S (gas) were dissolving with mole transfers of 1.40E - 03, 2.13E - 04, 4.15E - 06, 1.25E + 01, 3.11, and 9.34, respectively along the dominant flow line. Along the same flow line, FeS, siderite, and vivianite were precipitating with mole transfers of 9.34, 3.11, and 2.64E - 07, respectively. Cation exchange reactions of Ca2+ (4.93E - 04 mol) for Na+ (2.51E - 04 mol) on exchange sites occurred along the dominant flow line. Gypsum dissolution reactions were dominant over calcite dissolution in some of the flow lines due to the common ion effect. The concentration of As in groundwater ranged from <0.5 to 77 ??g/L. Twenty percent total As was complexed with Fe and Mn oxyhydroxides. The redox environment, chemical data of sediments and groundwater, and the results of inverse geochemical modeling indicate that reductive dissolution of Fe oxyhydroxide is the dominant process of As release in the groundwater. The relative rate of reduction of Fe oxyhydroxide over SO42 - with co-precipitation of As into sulfide is the limiting factor controlling dissolved As in groundwater. ?? 2007 Elsevier B.V. All rights reserved.

Journal of Hydrology↗

USGS2016

Regional oxygen reduction and denitrification rates in groundwater from multi-model residence time distributions, San Joaquin Valley, USA

Rates of oxygen and nitrate reduction are key factors in determining the chemical evolution of groundwater. Little is known about how these rates vary and covary in regional groundwater settings, as few studies have focused on regional datasets with multiple tracers and methods of analysis that account for effects of mixed residence times on apparent reaction rates. This study provides insight into the characteristics of residence times and rates of O 2 reduction and denitrification (NO 3 − reduction) by comparing reaction rates using multi-model analytical residence time distributions (RTDs) applied to a data set of atmospheric tracers of groundwater age and geochemical data from 141 well samples in the Central Eastern San Joaquin Valley, CA. The RTD approach accounts for mixtures of residence times in a single sample to provide estimates of in-situ rates. Tracers included SF 6 , CFCs, 3 H, He from 3 H (tritiogenic He), 14 C, and terrigenic He. Parameter estimation and multi-model averaging were used to establish RTDs with lower error variances than those produced by individual RTD models. The set of multi-model RTDs was used in combination with NO 3 − and dissolved gas data to estimate zero order and first order rates of O 2 reduction and denitrification. Results indicated that O 2 reduction and denitrification rates followed approximately log-normal distributions. Rates of O 2 and NO 3 − reduction were correlated and, on an electron milliequivalent basis, denitrification rates tended to exceed O 2 reduction rates. Estimated historical NO 3 − trends were similar to historical measurements. Results show that the multi-model approach can improve estimation of age distributions, and that relatively easily measured O 2 rates can provide information about trends in denitrification rates, which are more difficult to estimate.

California↗

USGS2025

Advancing broadscale spatial evapotranspiration modelling by incorporating sun-induced chlorophyll fluorescence measurements

Evapotranspiration (ET) describes the sum of water transfer from the ground surface through soil evaporation and water loss from leaf stomata into the atmosphere − critical factors linking the global water and carbon cycles. Myriad ET models based on remote sensing data provide spatially continuous estimates of ET; however, leaf photosynthetic information is critical to ensure accurate ET estimates, which are difficult to measure from space. Remotely sensed sun-induced chlorophyll fluorescence (SIF) provides a proxy of stomatal conductance activity with high performance in predicting plant transpiration, which can account for a large proportion of terrestrial and riverine ET. This study aims to improve estimates of tree water use in semi-arid to arid environments. In this study, a fixed stomatal conductance model and three SIF-driven canopy conductance (g sc ) models were applied to model potential ET (PET). The models estimated PET using the Penman-Monteith equation with: (1) a constant leaf stomatal conductance; (2) a transpiration-driven g sc model; (3) a g sc model based on electron-transfer rate and vapor pressure deficit, and a (4) Ball-Berry stomatal conductance model. A machine learning model was then applied to scale PET to actual ET (AET) using remote sensing and climate data. Accordingly, four AET models were cross-validated with in-situ measured AET at 52 sites, including 21 eddy covariance flux tower sites, and 31 sap-flow measurement sites (semi-arid and plantation area), for various plant functional types in Australia. This study demonstrated that SIF effectively captured seasonal variations of g sc , finding that AET models with SIF-driven g sc models correlated well with in-situ measured AET (R 2 = 0.64). Modelled AET with dynamic variations of g sc generated lower prediction error (0.85 mm day −1 ), while the AET model with fixed stomatal conductance tended to overestimate AET in floodplains and underestimate it in evergreen broadleaf forests, indicating using fixed stomatal conductance results in unstable performance when modelling AET. This study demonstrated that SIF-driven AET models improved broadscale estimation of ET. Our findings provide vital broadscale hydrological data to assist catchment and regional water management, particularly over unmonitored areas at risk of future climate-driven reductions in rainfall.

Journal of Hydrology↗

USGS2005

Anatahan, Northern Mariana Islands: Reconnaissance geological observations during and after the volcanic crisis of spring 1990, and monitoring prior to the May 2003 eruption

Anatahan island is 9.5 km east–west by 3.5 km north–south and truncated by an elongate caldera 5 km east–west by 2.5 km north–south. A steep-walled pit crater ∼1 km across and ∼200 m deep occupies the eastern part of the caldera. The island is the summit region of a mostly submarine stratovolcano. The oldest subaerial rocks (stage 1) are exposed low on the outer flanks and in the caldera walls. These include thick (∼10 m) and thin (2–3 m) lava flows, well-indurated tuffs, and scoria units that make up the bulk of the island. Rock compositions range from basaltic andesite to dacite, and most are plagioclase-phyric. On the steep north and south flanks of the volcano, these rocks are cut by numerous east–west-oriented, few-hundred-m-long lineaments of undetermined origin. Indurated breccias unconformably overlie scarps cut into stage 1 units low on the south flank. Intermediate-age eruptive units (stage 2) include caldera-filling lava flows and pyroclastic deposits and, on the outer flanks, vents and valley-filling lava flows. The youngest pre-2003 volcanic unit on Anatahan (stage 3) is a hydromagmatic surge and fall deposit rich in accretionary lapilli. Prior to 2003, this unit was found over almost the entire island, and in many places original depositional surfaces and outcrops could be found in high-energy environments along the coast, indicating a young (but undetermined) age. During reconnaissance visits in 1990, 1992, 1994, and 2001, geothermal activity (fumaroles as well as pits with boiling, sediment-laden pools) was observed in the southern part of the pit crater. In March and April 1990, increased local seismicity, a large regional earthquake, and reported increased fumarolic activity in the pit crater prompted evacuation of Anatahan village, at the west end of the island. Our first field investigation took place in late April 1990 to assess the level of volcanic unrest, conduct reconnaissance geological observations, collect rock and geothermal water samples, and set up a geophysical monitoring network. Results at this time were inconclusive with respect to determining whether the activity was anomalous. Water in some of the geothermal pits within the pit crater was boiling, and pH values as low as 0.7 were recorded in the field. An electronic distance measurement (EDM) network was installed, and over a ∼1-week period, up to 9 cm of extension occurred across some lines but not others. Seismicity was characterized by intermittent local earthquakes but no sustained swarms or tremor. A brief visit in June 1990 revealed that the shallow lake near the boiling pits was gone, but activity in the pits themselves was similar to that of April 1990. Only minor extension had occurred along a single EDM line since the previous visit, and no earthquakes >M2.5 occurred during the visit. Subsequent 1- to 2-day visits occurred in October 1990, May 1992, May 1994, and June 2001. Activity within the geothermal pits was relatively constant during every visit, although during this 11-year period the level of the water in each pit decreased. In June 2001, a ∼50-m-wide region of mud pots and steaming ground in the central part of the geothermal area had developed. No geologic evidence, however, suggested that an eruption would occur < 2 years afterward. Most of the EDM lines showed slight extension between late 1990 and 1992, followed by very gradual contraction from 1992 to 2001. A more extensive seismic-monitoring system was installed on the Northern Mariana Islands during these visits, and it recorded a small seismic swarm at Anatahan from May to July 1993. The telemetry component of the seismic equipment broke prior to 2001 and had not been repaired by the time of the May 2003 eruption, so no precursory seismic data were recorded to indicate pre-eruption unrest.

Northern Mariana Islands↗