Geology topics

David A. Stonestrom

Publications and source records attributed to David A. Stonestrom.

At least 19 recordsLinked to original sources

USGS2018

Solute profiles in soils, weathering gradients and exchange equilibrium/disequilibrium

The spatial and temporal changes in hydrology and pore water elemental and 87/86 Sr compositions were used to determine contemporary weathering rates in a 65 to 226 ky old soil chronosequence formed from granitic sediments deposited on marine terraces along coastal California. Cl-corrected Na, K and Si increased with depth denoting inputs from the weathering of plagioclase and K-feldspar. Solute 87/86 Sr exhibited progressive mixing of sea water-dominated precipitation with inputs from less radiogenic plagioclase. Linear approximations to these weathering gradients were used to determine plagioclase weathering rates of between 0.38 and 8.9×10 −15 moles m −2 s −1 . The lack of corresponding weathering gradients for Ca and Sr indicated short-term equilibrium with the clay ion exchange pool which requires periodic resetting by natural perturbations to maintain continuity, in spite of soil composition changes reflecting the effects of long-term weathering.

Mineralogical Magazine↗

USGS2018

Unsaturated zone CO2, CH4, and δ13C-CO2 at an arid region low-level radioactive waste disposal site

Elevated tritium, radiocarbon, Hg, and volatile organic compounds associated with low-level radioactive waste (LLRW) at the USGS Amargosa Desert Research Site (ADRS) have stimulated research on factors and processes that affect contaminant gas distribution and transport. Consequently, we examined the sources, mixing, and biogeochemistry of CO 2 and CH 4 , two additional important species in the unsaturated zone at ADRS. In spring 2015 and 2016, shallow unsaturated zone gas samples were collected from the 1.5-m depth both inside and outside the LLRW disposal area. Samples also were collected from two 110-m-deep multilevel gas-sampling boreholes and a distant background site. These samples were analyzed for CO 2 mole fraction ( x CO 2 ) and C isotopic composition (δ 13 C-CO 2 ) and CH 4 mole fraction ( x CH 4 ). Graphical analysis of the results indicates mixing of CO 2 characteristic of the root zone (δ 13 C −18 to −19‰), deep soil gas of the capillary fringe (−13 to −15‰), and CO 2 produced by microbial respiration of organic matter disposed in the LLRW trenches (−22 to −25‰). Distribution of CH 4 overall reflects atmospheric sources and production in anaerobic microzones in the LLRW area and methanotrophy in the undisturbed shallow subsurface outside the LLRW area. Although x CH 4 reflecting lateral transport from the LLRW area is decreasing with time in the deep profiles, deep unsaturated zone x CO 2 has changed little in recent decades. The results imply that CH 4 and δ 13 C-CO 2 may serve as good tracers of anthropogenic effects in the unsaturated zone even when CO 2 primarily reflects natural processes.

Nevada↗

USGS2017

Steady state fractionation of heavy noble gas isotopes in a deep unsaturated zone

To explore steady state fractionation processes in the unsaturated zone (UZ), we measured argon, krypton, and xenon isotope ratios throughout a ∼110 m deep UZ at the United States Geological Survey (USGS) Amargosa Desert Research Site (ADRS) in Nevada, USA. Prior work has suggested that gravitational settling should create a nearly linear increase in heavy-to-light isotope ratios toward the bottom of stagnant air columns in porous media. Our high-precision measurements revealed a binary mixture between (1) expected steady state isotopic compositions and (2) unfractionated atmospheric air. We hypothesize that the presence of an unsealed pipe connecting the surface to the water table allowed for direct inflow of surface air in response to extensive UZ gas sampling prior to our first (2015) measurements. Observed isotopic resettling in deep UZ samples collected a year later, after sealing the pipe, supports this interpretation. Data and modeling each suggest that the strong influence of gravitational settling and weaker influences of thermal diffusion and fluxes of CO 2 and water vapor accurately describe steady state isotopic fractionation of argon, krypton, and xenon within the UZ. The data confirm that heavy noble gas isotopes are sensitive indicators of UZ depth. Based on this finding, we outline a potential inverse approach to quantify past water table depths from noble gas isotope measurements in paleogroundwater, after accounting for fractionation during dissolution of UZ air and bubbles.

Nevada↗

USGS2017

Nutrient processes at the stream-lake interface for a channelized versus unmodified stream mouth

Inorganic forms of nitrogen and phosphorous impact freshwater lakes by stimulating primary production and affecting water quality and ecosystem health. Communities around the world are motivated to sustain and restore freshwater resources and are interested in processes controlling nutrient inputs. We studied the environment where streams flow into lakes, referred to as the stream-lake interface (SLI), for a channelized and unmodified stream outlet. Channelization is done to protect infrastructure or recreational beach areas. We collected hydraulic and nutrient data for surface water and shallow groundwater in two SLIs to develop conceptual models that describe characteristics that are representative of these hydrologic features. Water, heat, and solute transport models were used to evaluate hydrologic conceptualizations and estimate mean residence times of water in the sediment. A nutrient mass balance model is developed to estimate net rates of adsorption and desorption, mineralization, and nitrification along subsurface flow paths. Results indicate that SLIs are dynamic sources of nutrients to lakes and that the common practice of channelizing the stream at the SLI decreases nutrient concentrations in pore water discharging along the lakeshore. This is in contrast to the unmodified SLI that forms a barrier beach that disconnects the stream from the lake and results in higher nutrient concentrations in pore water discharging to the lake. These results are significant because nutrient delivery through pore water seepage at the lakebed from the natural SLI contributes to nearshore algal communities and produces elevated concentrations of inorganic nutrients in the benthic zone where attached algae grow.

Water Resources Research↗

USGS2017

Long-term flow-through column experiments and their relevance to natural granitoid weathering rates

Four pairs of fresh and partly-weathered granitoids, obtained from well-characterized watersheds—Merced River, CA, USA; Panola, GA, USA; Loch Vale, CO, USA, and Rio Icacos, Puerto Rico—were reacted in columns under ambient laboratory conditions for 13.8 yrs, the longest running experimental weathering study to date. Low total column mass losses (<1 wt. %), correlated with the absence of pitting or surface roughening of primary silicate grains. BET surface area (S BET ) increased, primarily due to Fe-oxyhydroxide precipitation. Surface areas returned to within factors of 2 to 3 of their original values after dithionite extraction. Miscible displacement experiments indicated homogeneous plug flow with negligible immobile water, commonly cited for column experiments. Fresh granitoid effluent solute concentrations initially declined rapidly, followed by much slower decreases over the next decade. Weathered granitoid effluent concentrations increased modestly over the same time period, indicating losses of natural Fe-oxide and/or clay coatings and the increased exposure of primary mineral surfaces. Corresponding (fresh and weathered) elemental effluent concentrations trended toward convergence during the last decade of reaction. NETPATH/PHREEQC code simulations indicated non-stoichiometric dissolution involving Ca release from disseminated calcite and excess K release from interlayer biotite. Effluent 87 Sr/ 85 Sr ratios reflected a progressive weathering sequence beginning and ending with 87 Sr/ 85 Sr values of plagioclase with an additional calcite input and a radiogenic biotite excursion proportional to the granitoid ages. Effluents became thermodynamically saturated with goethite and gibbsite, slightly under-saturated with kaolinite and strongly under-saturated with plagioclase, consistent with kinetically-limited weathering in which solutes such as Na varied with column flow rates. Effluent Na concentrations showed no clear trend with time during the last decade of reaction (fresh granitoids) or increased slowly with time (weathered granitoids). Analysis of cumulative Na release indicated that plagioclase dissolution achieved steady state in 3 of the 4 fresh granitoids during the last decade of reaction. Surface-area normalized plagioclase dissolution rates exhibited a narrow range (0.95 to 1.26 10 -13 moles m -2 s -1 ), in spite of significant stoichiometric differences (An 0.21 to An 0.50 ). Rates were an order of magnitude slower than previously reported in shorter duration experiments but generally 2 to 3 orders of magnitude faster than corresponding natural analogs. CrunchFlow simulations indicated that more than a hundredfold decrease in column flow rates would be required to produce near-saturation reaction affinities that would start to slow plagioclase weathering to real-world levels. Extending simulations to approximate long term weathering in naturally weathered profiles required additional decreases in the intrinsic plagioclase dissolution and kaolinite precipitation rates and relatively large decreases in the fluid flow rate, implying that exposure to reactive mineral surfaces is significantly limited in the natural environment compared to column experiments.

Geochimica et Cosmochimica Acta↗

USGS2016

Groundwater exchanges near a channelized versus unmodified stream mouth discharging to a subalpine lake

The terminus of a stream flowing into a larger river, pond, lake, or reservoir is referred to as the stream-mouth reach or simply the stream mouth . The terminus is often characterized by rapidly changing thermal and hydraulic conditions that result in abrupt shifts in surface water/groundwater (sw/gw) exchange patterns, creating the potential for unique biogeochemical processes and ecosystems. Worldwide shoreline development is changing stream-lake interfaces through channelization of stream mouths, i.e., channel straightening and bank stabilization to prevent natural meandering at the shoreline. In the central Sierra Nevada (USA), Lake Tahoe's shoreline has an abundance of both “unmodified” (i.e., not engineered though potentially impacted by broader watershed engineering) and channelized stream mouths. Two representative stream mouths along the lake's north shore, one channelized and one unmodified, were selected to compare and contrast water and heat exchanges. Hydraulic and thermal properties were monitored during separate campaigns in September 2012 and 2013 and sw/gw exchanges were estimated within the stream mouth-shoreline continuum. Heat-flow and water-flow patterns indicated clear differences in the channelized versus the unmodified stream mouth. For the channelized stream mouth, relatively modulated, cool-temperature, low-velocity longitudinal streambed flows discharged offshore beneath warmer buoyant lakeshore water. In contrast, a seasonal barrier bar formed across the unmodified stream mouth, creating higher-velocity subsurface flow paths and higher diurnal temperature variations relative to shoreline water. As a consequence, channelization altered sw/gw exchanges potentially altering biogeochemical processing and ecological systems in and near the stream mouth.

California, Nevada↗

USGS2016

Experimental studies and model analysis of noble gas fractionation in porous media

The noble gases, which are chemically inert under normal terrestrial conditions but vary systematically across a wide range of atomic mass and diffusivity, offer a multicomponent approach to investigating gas dynamics in unsaturated soil horizons, including transfer of gas between saturated zones, unsaturated zones, and the atmosphere. To evaluate the degree to which fractionation of noble gases in the presence of an advective–diffusive flux agrees with existing theory, a simple laboratory sand column experiment was conducted. Pure CO2 was injected at the base of the column, providing a series of constant CO2 fluxes through the column. At five fixed sampling depths within the system, samples were collected for CO2 and noble gas analyses, and ambient pressures were measured. Both the advection–diffusion and dusty gas models were used to simulate the behavior of CO2 and noble gases under the experimental conditions, and the simulations were compared with the measured depth-dependent concentration profiles of the gases. Given the relatively high permeability of the sand column (5 ´ 10−11 m2), Knudsen diffusion terms were small, and both the dusty gas model and the advection–diffusion model accurately predicted the concentration profiles of the CO2 and atmospheric noble gases across a range of CO2 flux from ?700 to 10,000 g m−2 d−1. The agreement between predicted and measured gas concentrations demonstrated that, when applied to natural systems, the multi-component capability provided by the noble gases can be exploited to constrain component and total gas fluxes of non-conserved (CO2) and conserved (noble gas) species or attributes of the soil column relevant to gas transport, such as porosity, tortuosity, and gas saturation.

Vadose Zone Journal↗

USGS2016

Structured heterogeneity in a marine terrace chronosequence: Upland mottling

Soil mottles generally are interpreted as a product of reducing conditions during periods of water saturation. The upland soils of the Santa Cruz, CA, marine terrace chronosequence display an evolving sequence of reticulate mottling from the youngest soil (65 ka) without mottles to the oldest soil (225 ka) with well-developed mottles. The mottles consist of an interconnected network of clay and C-enriched regions (gray, 2.5Y 6/1) bordered by leached parent material (white, 2.5Y 8/1) within a diminishing matrix of oxidized parent material (orange, 7.5YR 5/8). The mottles develop in soils that formed from relatively uniform nearshore sediments and occur below the depth of soil bioturbation. To explore how a presumably wetland feature occurs in an unsaturated upland soil, physical and chemical characteristics of mottle separates (orange, gray, and white) were compared through the deep time represented by the soil chronosequence. Mineralogical, isotopic, and surface-area differences among mottle separates indicate that rhizogenic centimeter-scale mass transfer acting across millennia is an integral part of weathering, pedogenesis, and C and nutrient transfer. Elemental analysis, electron microscopy, and Fe-isotope systematics indicate that mottle development is driven by deep roots together with their fungal and microbial symbionts. Taken together, these data suggest that deep soil horizons on old stable landforms can develop reticulate mottling as the long-term imprint of rhizospheric processes. The processes of rhizogenic mottle formation appear to regulate pedogenesis, nutrients, and C sequestration at depth in unsaturated zones.

California↗

USGS2016

Implications of projected climate change for groundwater recharge in the western United States

Existing studies on the impacts of climate change on groundwater recharge are either global or basin/location-specific. The global studies lack the specificity to inform decision making, while the local studies do little to clarify potential changes over large regions (major river basins, states, or groups of states), a scale often important in the development of water policy. An analysis of the potential impact of climate change on groundwater recharge across the western United States (west of 100° longitude) is presented synthesizing existing studies and applying current knowledge of recharge processes and amounts. Eight representative aquifers located across the region were evaluated. For each aquifer published recharge budget components were converted into four standard recharge mechanisms: diffuse, focused, irrigation, and mountain-systems recharge. Future changes in individual recharge mechanisms and total recharge were then estimated for each aquifer. Model-based studies of projected climate-change effects on recharge were available and utilized for half of the aquifers. For the remainder, forecasted changes in temperature and precipitation were logically propagated through each recharge mechanism producing qualitative estimates of direction of changes in recharge only (not magnitude). Several key patterns emerge from the analysis. First, the available estimates indicate average declines of 10–20% in total recharge across the southern aquifers, but with a wide range of uncertainty that includes no change. Second, the northern set of aquifers will likely incur little change to slight increases in total recharge. Third, mountain system recharge is expected to decline across much of the region due to decreased snowpack, with that impact lessening with higher elevation and latitude. Factors contributing the greatest uncertainty in the estimates include: (1) limited studies quantitatively coupling climate projections to recharge estimation methods using detailed, process-based numerical models; (2) a generally poor understanding of hydrologic flowpaths and processes in mountain systems; (3) difficulty predicting the response of focused recharge to potential changes in the frequency and intensity of extreme precipitation events; and (4) unconstrained feedbacks between climate, irrigation practices, and recharge in highly developed aquifer systems.

Journal of Hydrology↗

USGS2016

Groundwater

Introduction Groundwater represents the terrestrial subsurface component of the hydrologic cycle. As such, groundwater is generally in motion, moving from elevated areas of recharge to lower areas of discharge. Groundwater usually moves in accordance with Darcy’s law (Dalmont, Paris: Les Fontaines Publiques de la Ville de Dijon, 1856). Groundwater residence times can be under a day in small upland catchments to over a million years in subcontinental-sized desert basins. The broadest definition of groundwater includes water in the unsaturated zone, considered briefly here. Water chemically bound to minerals, as in gypsum (CaSO 4 • 2H 2 O) or hydrated clays, cannot flow in response to gradients in total hydraulic head (pressure head plus elevation head); such water is thus usually excluded from consideration as groundwater. In 1940, M. King Hubbert showed Darcy’s law to be a special case of thermodynamically based potential field equations governing fluid motion, thereby establishing groundwater hydraulics as a rigorous engineering science ( Journal of Geology 48, pp. 785–944). The development of computer-enabled numerical methods for solving the field equations with real-world approximating geometries and boundary conditions in the mid-1960s ushered in the era of digital groundwater modeling. An estimated 30 percent of global fresh water is groundwater, compared to 0.3 percent that is surface water, 0.04 percent atmospheric water, and 70 percent that exists as ice, including permafrost ( Shiklomanov and Rodda 2004 , cited under Groundwater Occurrence ). Groundwater thus constitutes the vast majority—over 98 percent—of the unfrozen fresh-water resources of the planet, excluding surface-water reservoirs. Environmental dimensions of groundwater are equally large, receiving attention on multiple disciplinary fronts. Riparian, streambed, and spring-pool habitats can be sensitively dependent on the amount and quality of groundwater inputs that modulate temperature and solutes, including nutrients and dissolved oxygen. Groundwater withdrawals can negatively impact riparian habitats by depriving ecosystems of adequate fresh water and fragmenting communities when streams go dry. Biochemical reactions in shallow groundwater can remove anthropogenically elevated nitrogen compounds and reduce—but only to a point—the greening of waterways and shorelines with periphyton and harmful algal blooms. Groundwater extraction for beneficial use is increasingly limited by water-quality constraints imposed by naturally occurring and introduced substances. Overdrafting can cause land-surface subsidence, damaging buildings and roads and disrupting canals, sewers, and other gravity-flow conveyances. Increases in groundwater levels can cause soil salinization in dry regions and erosive sapping and flooding in wet regions. Coastal saltwater intrusion, groundwater flooding, salinization associated with groundwater-irrigated agriculture, induced seismicity from injected wastes, and the detrimental impacts of groundwater depletion are among the major environmental challenges of our time.

Book chapter↗

USGS2015

Multimodel analysis of anisotropic diffusive tracer-gas transport in a deep arid unsaturated zone

Gas transport in the unsaturated zone affects contaminant flux and remediation, interpretation of groundwater travel times from atmospheric tracers, and mass budgets of environmentally important gases. Although unsaturated zone transport of gases is commonly treated as dominated by diffusion, the characteristics of transport in deep layered sediments remain uncertain. In this study, we use a multimodel approach to analyze results of a gas-tracer (SF 6 ) test to clarify characteristics of gas transport in deep unsaturated alluvium. Thirty-five separate models with distinct diffusivity structures were calibrated to the tracer-test data and were compared on the basis of Akaike Information Criteria estimates of posterior model probability. Models included analytical and numerical solutions. Analytical models provided estimates of bulk-scale apparent diffusivities at the scale of tens of meters. Numerical models provided information on local-scale diffusivities and feasible lithological features producing the observed tracer breakthrough curves. The combined approaches indicate significant anisotropy of bulk-scale diffusivity, likely associated with high-diffusivity layers. Both approaches indicated that diffusivities in some intervals were greater than expected from standard models relating porosity to diffusivity. High apparent diffusivities and anisotropic diffusivity structures were consistent with previous observations at the study site of rapid lateral transport and limited vertical spreading of gas-phase contaminants. Additional processes such as advective oscillations may be involved. These results indicate that gases in deep, layered unsaturated zone sediments can spread laterally more quickly, and produce higher peak concentrations, than predicted by homogeneous, isotropic diffusion models.

California, Nevada↗

USGS2015

Global patterns and environmental controls of perchlorate and nitrate co-occurrence in arid and semi-arid environments

Natural perchlorate (ClO 4 − ) is of increasing interest due to its wide-spread occurrence on Earth and Mars, yet little information exists on the relative abundance of ClO 4 − compared to other major anions, its stability, or long-term variations in production that may impact the observed distributions. Our objectives were to evaluate the occurrence and fate of ClO 4 − in groundwater and soils/caliche in arid and semi-arid environments (southwestern United States, southern Africa, United Arab Emirates, China, Antarctica, and Chile) and the relationship of ClO 4 − to the more well-studied atmospherically deposited anions NO 3 − and Cl − as a means to understand the prevalent processes that affect the accumulation of these species over various time scales. ClO 4 − is globally distributed in soil and groundwater in arid and semi-arid regions on Earth at concentrations ranging from 10 −1 to 10 6 μg/kg. Generally, the ClO 4 − concentration in these regions increases with aridity index, but also depends on the duration of arid conditions. In many arid and semi-arid areas, NO 3 − and ClO 4 − co-occur at molar ratios (NO 3 − /ClO 4 − ) that vary between ∼10 4 and 10 5 . We hypothesize that atmospheric deposition ratios are largely preserved in hyper-arid areas that support little or no biological activity (e.g. plants or bacteria), but can be altered in areas with more active biological processes including N 2 fixation, N mineralization, nitrification, denitrification, and microbial ClO 4 − reduction, as indicated in part by NO 3 − isotope data. In contrast, much larger ranges of Cl − /ClO 4 − and Cl − /NO 3 − ratios indicate Cl − varies independently from both ClO 4 − and NO 3 − . The general lack of correlation between Cl − and ClO 4 − or NO 3 − implies that Cl − is not a good indicator of co-deposition and should be used with care when interpreting oxyanion cycling in arid systems. The Atacama Desert appears to be unique compared to all other terrestrial locations having a NO 3 − /ClO 4 − molar ratio ∼10 3 . The relative enrichment in ClO 4 − compared to Cl − or NO 3 − and unique isotopic composition of Atacama ClO 4 − may reflect either additional in-situ production mechanism(s) or higher relative atmospheric production rates in that specific region or in the geological past. Elevated concentrations of ClO 4 − reported on the surface of Mars, and its enrichment with respect to Cl − and NO 3 − , could reveal important clues regarding the climatic, hydrologic, and potentially biologic evolution of that planet. Given the highly conserved ratio of NO 3 − /ClO 4 − in non-biologically active areas on Earth, it may be possible to use alterations of this ratio as a biomarker on Mars and for interpreting major anion cycles and processes on both Mars and Earth, particularly with respect to the less-conserved NO 3 − pool terrestrially.

Geochimica et Cosmochimica Acta↗

USGS2014

Book review: Terrestrial biosphere-atmosphere fluxes and transport in the atmosphere-vegetation-soil continuum

No abstract available.

Groundwater↗

USGS2014

Field-scale sulfur hexafluoride tracer experiment to understand long distance gas transport in the deep unsaturated zone

A gas-tracer test in a deep arid unsaturated zone demonstrates that standard estimates of effective diffusivity from sediment properties allow a reasonable first-cut assessment of gas contaminant transport. Apparent anomalies in historic transport behavior at this and other waste disposal sites may result from factors other than nonreactive gas transport properties. A natural gradient SF 6 tracer experiment provided an unprecedented evaluation of long distance gas transport in the deep unsaturated zone (UZ) under controlled (known) conditions. The field-scale gas tracer test in the 110-m-thick UZ was conducted at the U.S. Geological Survey’s Amargosa Desert Research Site (ADRS) in southwestern Nevada. A history of anomalous (theoretically unexpected) contaminant gas transport observed at the ADRS, next to the first commercial low-level radioactive waste disposal facility in the United States, provided motivation for the SF 6 tracer study. Tracer was injected into a deep UZ borehole at depths of 15 and 48 m, and plume migration was observed in a monitoring borehole 9 m away at various depths (0.5–109 m) over the course of 1 yr. Tracer results yielded useful information about gas transport as applicable to the spatial scales of interest for off-site contaminant transport in arid unsaturated zones. Modeling gas diffusion with standard empirical expressions reasonably explained SF 6 plume migration, but tended to underpredict peak concentrations for the field-scale experiment given previously determined porosity information. Despite some discrepancies between observations and model results, rapid SF 6 gas transport commensurate with previous contaminant migration was not observed. The results provide ancillary support for the concept that apparent anomalies in historic transport behavior at the ADRS are the result of factors other than nonreactive gas transport properties or processes currently in effect in the undisturbed UZ.

California, Nevada↗

USGS2014

Soil, plant, and terrain effects on natural perchlorate distribution in a desert landscape

Perchlorate (ClO 4 − ) is a contaminant that occurs naturally throughout the world, but little is known about its distribution and interactions in terrestrial ecosystems. The objectives of this Amargosa Desert, Nevada study were to determine (i) the local-scale distribution of shallow-soil (0–30 cm) ClO 4 − with respect to shrub proximity (far and near) in three geomorphic settings (shoulder slope, footslope, and valley floor); (ii) the importance of soil, plant, and terrain variables on the hillslope-distribution of shallow-soil and creosote bush [ Larrea tridentata (Sessé & Moc. ex DC.) Coville] ClO 4 − ; and (iii) atmospheric (wet plus dry, including dust) deposition of ClO 4 − in relation to soil and plant reservoirs and cycling. Soil ClO 4 − ranged from 0.3 to 5.0 μg kg −1 . Within settings, valley floor ClO 4 − was 17× less near shrubs due in part to enhanced leaching, whereas shoulder and footslope values were ∼2× greater near shrubs. Hillslope regression models (soil, R 2 = 0.42; leaf, R 2 = 0.74) identified topographic and soil effects on ClO 4 − deposition, transport, and cycling. Selective plant uptake, bioaccumulation, and soil enrichment were evidenced by leaf ClO 4 − concentrations and Cl − /ClO 4 − molar ratios that were ∼8000× greater and 40× less, respectively, than soil values. Atmospheric deposition ClO 4 − flux was 343 mg ha −1 yr −1 , ∼10× that for published southwestern wet-deposition fluxes. Creosote bush canopy ClO 4 − (1310 mg ha−1) was identified as a previously unrecognized but important and active reservoir. Nitrate δ 18 O analyses of atmospheric deposition and soil supported the leaf-cycled–ClO 4 − input hypothesis. This study provides basic data on ClO 4 − distribution and cycling that are pertinent to the assessment of environmental impacts in desert ecosystems and broadly transferable to anthropogenically contaminated systems.

Nevada↗

USGS2013

Tritium plume dynamics in the shallow unsaturated zone in an arid environment

The spatiotemporal variability of a tritium plume in the shallow unsaturated zone and the mechanisms controlling its transport were evaluated during a 10-yr study. Plume movement was minimal and its mass declined by 68%. Upward-directed diffusive-vapor tritium fluxes and radioactive decay accounted for most of the observed plume-mass declines. Effective isolation of tritium ( 3 H) and other contaminants at waste-burial facilities requires improved understanding of transport processes and pathways. Previous studies documented an anomalously widespread (i.e., theoretically unexpected) distribution of 3 H (>400 m from burial trenches) in a dry, sub-root-zone gravelly layer (1–2-m depth) adjacent to a low-level radioactive waste (LLRW) burial facility in the Amargosa Desert, Nevada, that closed in 1992. The objectives of this study were to: (i) characterize long-term, spatiotemporal variability of 3 H plumes; and (ii) quantify the processes controlling 3 H behavior in the sub-root-zone gravelly layer beneath native vegetation adjacent to the facility. Geostatistical methods, spatial moment analyses, and mass flux calculations were applied to a spatiotemporally comprehensive, 10-yr data set (2001–2011). Results showed minimal bulk-plume advancement during the study period and limited Fickian spreading of mass. Observed spreading rates were generally consistent with theoretical vapor-phase dispersion. The plume mass diminished more rapidly than would be expected from radioactive decay alone, indicating net efflux from the plume. Estimates of upward 3 H efflux via diffusive-vapor movement were >10× greater than by dispersive-vapor or total-liquid movement. Total vertical fluxes were >20× greater than lateral diffusive-vapor fluxes, highlighting the importance of upward migration toward the land surface. Mass-balance calculations showed that radioactive decay and upward diffusive-vapor fluxes contributed the majority of plume loss. Results indicate that plume losses substantially exceeded any continuing 3 H contribution to the plume from the LLRW facility during 2001 to 2011 and suggest that the widespread 3 H distribution resulted from transport before 2001.

Nevada↗

USGS2013

On the conversion of tritium units to mass fractions for hydrologic applications

We develop a general equation for converting laboratory-reported tritium levels, expressed either as concentrations (tritium isotope number fractions) or mass-based specific activities, to mass fractions in aqueous systems. Assuming that all tritium is in the form of monotritiated water simplifies the derivation and is shown to be reasonable for most environmental settings encountered in practice. The general equation is nonlinear. For tritium concentrations c less than 4.5×10 12 tritium units (TU) - i.e. specific tritium activities<5.3×10 11 Bq kg -1 - the mass fraction w of tritiated water is approximated to within 1 part per million by w ≈ c×2.22293×10 -18 , i.e. the conversion is linear for all practical purposes. Terrestrial abundances serve as a proxy for non-tritium isotopes in the absence of sample-specific data. Variation in the relative abundances of non-tritium isotopes in the terrestrial hydrosphere produces a minimum range for the mantissa of the conversion factor of [2.22287; 2.22300].

Isotopes in Environmental and Health Studies↗

USGS2012

Volatile organic compounds in the unsaturated zone from radioactive wastes

Volatile organic compounds (VOCs) are often comingled with low-level radioactive wastes (LLRW), but little is known about subsurface VOC emanations from LLRW landfills. The current study systematically quantified VOCs associated with LLRW over an 11-yr period at the USGS Amargosa Desert Research Site (ADRS) in southwestern Nevada. Unsaturated-zone gas samples of VOCs were collected by adsorption on resin cartridges and analyzed by thermal desorption and GC/MS. Sixty of 87 VOC method analytes were detected in the 110-m-thick unsaturated zone surrounding a LLRW disposal facility. Chlorofluorocarbons (CFCs) were detected in 100% of samples collected. Chlorofluorocarbons are powerful greenhouse gases, deplete stratospheric ozone, and are likely released from LLRW facilities worldwide. Soil-gas samples collected from a depth of 24 m and a horizontal distance 100 m south of the nearest waste-disposal trench contained >60,000 ppbv total VOCs, including >37,000 ppbv CFCs. Extensive sampling in the shallow unsaturated zone (0–2 m deep) identified areas where total VOC concentrations exceeded 5000 ppbv at the 1.5-m depth. Volatile organic compound concentrations exceeded background levels up to 300 m from the facility. Maximum vertical diffusive fluxes of total VOCs were estimated to be 1 g m -2 yr -1 . Volatile organic compound distributions were similar but not identical to those previously determined for tritium and elemental mercury. To our knowledge, this study is the first to characterize the unsaturated zone distribution of VOCs emanating from a LLRW landfill. Our results may help explain anomalous transport of radionuclides at the ADRS and elsewhere.

Nevada↗