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At least 865 records · Page 48

δ 2 H isotopic offsets in xylem water measurements under cryogenic vacuum distillation: Quantifying and correcting wood‐water hydrogen exchange influences

Stable isotopes δ 18 O and δ 2 H are used to infer vegetation water sources. In some studies, significant xylem water δ 2 H offsets from potential source waters have been observed. The offsets appear to be more prevalent with cryogenic vacuum distillation (CVD) of plant water. Hypothesized mechanisms for these offsets include changes during plant water uptake and transport, and methodological problems. We propose that a large portion of the offsets are due to hydrogen isotope exchange between xylem water and non-crystalline hydroxyl groups of wood cellulose and hemicellulose during CVD. We present a method for estimating the hypothesized isotopic exchange between wood tissues and water, which is the result of Rayleigh and equilibrium fractionation. To estimate the exchange, we use published wood properties for North American tree species and isotope chemical relationships as a function of moisture content, CVD temperature and water extraction efficiency. A simple model of exchange between xylem water and hydroxyl groups captures the range of observations in studies in which CVD and non-CVD methods were compared. To evaluate the model, we compared observed δ 2 H offsets (sw-excess) values from two field datasets (90°C, n = 364, and 170°C, n = 43) to δ 2 H offsets estimated with our chemical model. We found good agreement between observed and estimated δ 2 H offsets for samples extracted at 90°C (r 2 = 0.69) but not for samples extracted at 170°C (r 2 = 0.20). The offset may be eliminated by increasing the extraction temperature to 229°C or by adding a standard sufficient to raise the moisture content to >150%. A correction can also be approximated by applying a theoretical calculation based on the extraction temperature, moisture content and water extraction efficiency.

54 ENVIRONMENTAL SCIENCES↗

Amino acid δ 15 N indicates lack of N isotope fractionation during soil organic nitrogen decomposition

The interpretation of natural abundance δ 15 N in soil profiles and across ecosystems is confounded by a lack of understanding of possible N isotope fractionation associated with soil organic nitrogen (SON) decomposition. We analyzed the δ 15 N of hydrolysable amino acids to test the extent of fractionation associated with the depolymerization of peptides to amino acids and the mineralization of amino acids to NH 4 + (ammonification). Most amino acids are both synthesized and degraded by microbes, complicating interpretation of their δ 15 N. However, the “source” amino acids phenylalanine and hydroxyproline are degraded and recycled but not resynthesized. We therefore used their δ 15 N to isolate the effects of N isotope fractionation during SON depolymerization and ammonification. We used complementary field and laboratory approaches to evaluate the change in amino acid δ 15 N during decomposition. First, we measured amino acid δ 15 N changes with depth in the organic horizons of podzolic soils collected from the Newfoundland and Labrador Boreal Ecosystem Latitudinal Transect (NL-BELT), Canada. The δ 15 N of most amino acids increased with depth by 3–7‰, similar to the increase in bulk δ 15 N. However, the δ 15 N of the “source” amino acids did not change with depth, indicating lack of N isotope fractionation during their depolymerization and ammonification. Second, we assessed the change in amino acid δ 15 N following 400 days of laboratory incubation. This approach isolated the effect of decomposition on δ 15 N by eliminating plant N uptake and reducing leaching of N from the soil. Amino acid δ 15 N did not change during incubation despite extensive turnover of the amino acid pool, supporting our conclusion of a lack of N isotope fractionation during SON decomposition. Finally, our results indicate the often-observed trend of increasing δ 15 N with soil depth likely results from the mycorrhizally-mediated transfer of 14 N from depth to the surface and accumulation of 15 N-enriched necromass of diverse soil microbes at depth, rather than as a direct result of SON decomposition.

59 BASIC BIOLOGICAL SCIENCES↗

Experimental calibration of silicon and oxygen isotope fractionations between quartz and water at 250°C by in situ microanalysis of experimental products and application to zoned low δ 30 Si quartz overgrowths

The interpretation of silicon isotope data for quartz is hampered by the lack of experimentally determined fractionation factors between quartz and fluid. Further, there is a large spread in published oxygen isotope fractionation factors at low temperatures, primarily due to extrapolation from experimental calibrations at high temperature. We report the first measurements of silicon isotope ratios from experimentally precipitated quartz and estimate the equilibrium fractionation vs. dissolved silica using a novel in situ analysis technique applying secondary ion mass spectrometry to directly analyze experimental products. These experiments also yield a new value for oxygen isotope fractionation. Quartz overgrowths up to 235 μm thick were precipitated in silica–H 2 O–NaOH–NaCl fluids, at pH 12–13 and 250 °C. At this temperature, 1000lnα 30 Si(Qtz–fluid) = 0.55 ± 0.10‰ and 1000lnα 18 O(Qtz–fluid) = 10.62 ± 0.13‰, yielding the relations 1000lnα 30 Si(Qtz–fluid) = (0.15 ± 0.03) * 10 6 /T 2 and 1000lnα 18 O(Qtz–fluid) = (2.91 ± 0.04) * 10 6 /T 2 when extended to zero fractionation at infinite temperature. Values of δ 30 Si(Qtz) from diagenetic cement in sandstones from the basal Cambrian Mt. Simon Formation in central North America range from 0 to ₋5.4‰. Paired δ 18 O and δ 30 Si values from individual overgrowths preserve a record of Precambrian weathering and fluid transport. In conclusion, the application of the experimental quartz growth results to observations from natural sandstone samples suggests that precipitation of quartz at low temperatures in nature is dominated by kinetic, rather than equilibrium, processes.

58 GEOSCIENCES↗

Intramolecular 13 C isotope distributions of butane from natural gases

A single-step method allowing the measurement of 13 C intramolecular distribution of butane isomers (n- and i-butane) from natural gas samples was developed. The method builds up on the one that has been developed for propane, using on-line pyrolysis followed by isotope analysis of the pyrolytic fragments. The isotopic filiation between n-butane and its pyrolytic fragments was elucidated using samples spiked with 13 C on terminal positions. The isotopic filiation for i-butane could not be shown experimentally due to the lack of commercially available enriched i-butane. We thus used a recent model named Reaction Mechanism Generator (RMG) to assess the origin of the fragments arising from i-butane pyrolysis. Butanes from natural gas samples from the Carnarvon Basin (Australia) and the Arkoma Basin (USA) were analyzed. The results are consistent with a model for thermogenic natural gas generation and suggest that combined intramolecular isotope composition of propane and n-butane can be related to the gas maturity. In addition, the method allows the detection and shed light on the mechanism of n-butane and i-butane biodegradation in natural gas reservoirs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Assessment of mercury exposure among small-scale gold miners using mercury stable isotopes

Total mercury (Hg) concentrations in hair and urine are often used as biomarkers of exposure to fish-derived methylmercury (MeHg) and gaseous elemental Hg, respectively. We used Hg stable isotopes to assess the validity of these biomarkers among small-scale gold mining populations in Ghana and Indonesia. Urine from Ghanaian miners displayed similar Δ{sup 199}Hg values to Hg derived from ore deposits (mean urine Δ{sup 199}Hg=0.01‰, n=6). This suggests that urine total Hg concentrations accurately reflect exposure to inorganic Hg among this population. Hair samples from Ghanaian miners displayed low positive Δ{sup 199}Hg values (0.23–0.55‰, n=6) and low percentages of total Hg as MeHg (7.6–29%, n=7). These data suggest that the majority of the Hg in these miners' hair samples is exogenously adsorbed inorganic Hg and not fish-derived MeHg. Hair samples from Indonesian gold miners who eat fish daily displayed a wider range of positive Δ{sup 199}Hg values (0.21–1.32‰, n=5) and percentages of total Hg as MeHg (32–72%, n=4). This suggests that total Hg in the hair samples from Indonesian gold miners is likely a mixture of ingested fish MeHg and exogenously adsorbed inorganic Hg. Based on data from both populations, we suggest that total Hg concentrations in hair samples from small-scale gold miners likely overestimate exposure to MeHg from fish consumption. - Highlights: • Mercury isotopes were measured in hair and urine from small-scale gold miners. • Mercury isotopes indicate that Hg in urine comes from mining activity. • Mercury isotopes suggest Hg in hair is a mixture of fish MeHg and inorganic Hg. • A large percentage of Hg in miner’s hair is released during amalgam burning and adsorbed.

54 ENVIRONMENTAL SCIENCES↗

Experimental determination of hydrogen isotopic equilibrium in the system H 2 O (l) -H 2(g) from 3 to 90 °C

Molecular hydrogen (H 2 ) is found in a variety of settings on and in the Earth from low-temperature sediments to hydrothermal vents, and is actively being considered as an energy resource for the transition to a green energy future. The hydrogen isotopic composition of H 2 , given as D/H ratios or δD, varies in nature by hundreds of per mil from ∼−800 ‰ in hydrothermal and sedimentary systems to ∼+450 ‰ in the stratosphere. This range reflects a variety of processes, including kinetic isotope effects associated with formation and destruction and equilibration with water, the latter proceeding at fast (order year) timescales at low temperatures (<100 °C). At isotopic equilibrium, the D/H fractionation factor between liquid water and hydrogen ( D α H2O(l)-H2(g) ) is a function of temperature and can thus be used as a geothermometer for H 2 formation or re-equilibration temperatures. Multiple studies have produced theoretical calculations for hydrogen isotopic equilibrium between H 2 and water vapor. However, only three published experimental calibrations used in geochemistry exist for the H 2 O-H 2 system: two between 51 and 742 °C for H 2 O (g) -H 2(g) (Suess, 1949, Cerrai et al., 1954), and one in the H 2 O (l) -H 2(g) system for temperatures <100 °C (Rolston et al., 1976). Despite these calibrations existing, there is uncertainty on their accuracy at low temperatures (<100 °C; e.g., Horibe and Craig, 1995).

08 HYDROGEN↗

Isotopic fractionation studies of uranium and plutonium using porous ion emitters as thermal ionization mass spectrometry sources

Investigations of the isotope fractionation behaviors of plutonium and uranium reference standards were conducted employing platinum and rhenium (Pt/Re) porous ion emitter (PIE) sources, a relatively new thermal ionization mass spectrometry (TIMS) ion source strategy. The suitability of commonly employed, empirically developed mass bias correction laws (i.e., the Linear, Power, and Russell's laws) for correcting such isotope ratio data was also determined. Corrected plutonium isotope ratio data, regardless of mass bias correction strategy, were statistically identical to that of the certificate, however, the process of isotope fractionation behavior of plutonium using the adopted experimental conditions was determined to be best described by the Power law. Finally, the fractionation behavior of uranium, using the analytical conditions described herein, is also most suitably modeled using the Power law, though Russell's and the Linear law for mass bias correction rendered results that were identical, within uncertainty, to the certificate value.

07 ISOTOPE AND RADIATION SOURCES↗

Maximum Reasonable Radioxenon Releases from Medical Isotope Production Facilities and Their Effect on Monitoring Nuclear Explosions

Fission gases such as 133Xe are used extensively for monitoring the world for signs of nuclear testing in systems such as the International Monitoring System (IMS). These gases are also produced by nuclear reactors and by fission production of 99Mo for medical use. Recently, medical isotope production facilities have been identified as the major contributor to the background of radioactive xenon isotopes (radioxenon) in the atmosphere (Saey, et al., 2009). These releases pose a potential future problem for monitoring nuclear explosions if not addressed. As a starting point, a maximum acceptable daily xenon emission rate was calculated, that is both scientifically defendable as not adversely affecting the IMS, but also consistent with what is possible to achieve in an operational environment. This study concludes that an emission of 5×109 Bq/day from a medical isotope production facility would be both an acceptable upper limit from the perspective of minimal impact to monitoring stations, but also appears to be an achievable limit for large isotope producers.

07 ISOTOPE AND RADIATION SOURCES↗

An isotope identification injection study with GammaTracker

GammaTracker is a portable handheld radioisotope identifier using position sensitive CdZnTe detectors. High confidence isotope identification is possible on GammaTracker owing to the system's relatively high energy resolution and count rate sensitivity. A study was undertaken to evaluate the isotope identification performance of a prototype unit. Background and source spectra for various nuclides were measured and then randomly sampled to simulate various integration times and source intensities. The resulting spectral data sets were then run through the isotope identification algorithm to determine the probability of detection and the false alarm rate for each nuclide. The process was repeated for various isotope identification input parameters until an optimized set was achieved. This paper presents results from the injection study.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

The new Batch Mode Ion Source for stand-alone operation at the Facility for Rare Isotope Beams (FRIB)

Gas stoppers have been used for a long-standing successful science program at Michigan State University with stopped and rare-isotope beams produced by projectile fragmentation. The National Superconducting Cyclotron Laboratory’s Coupled Cyclotron Facility has recently transitioned into the Facility for Rare Isotope Beams (FRIB) laboratory to provide rare isotopes using a high-power superconducting linear accelerator and new production facilities. To allow the science program with stopped and reaccelerated beams to continue during the transition period, a stand-alone capability was added. The Batch Mode Ion Source (BMIS) was built and has been providing beams of long-lived and stable isotopes of a variety of elements for successful user experiments. Finally, the BMIS system is described and results from the production of various beams are presented.

47 OTHER INSTRUMENTATION↗

A new highly enriched 233 U reference material for improved simultaneous determination of uranium amount and isotope amount ratios in trace level samples

A highly-enriched 233 U reference material (>0.99987 n( 233 U)/n(U)) has been prepared and characterized for use as an isotope dilution mass spectrometry spike. An ion exchange separation was performed on 1 g of high purity 233 U to further reduce trace amounts of contaminant Pu in the material. The purified 233 U was then prepared as a master solution which was analyzed for molality of uranium by modified Davies and Gray titration. A portion of the master solution was quantitatively diluted and dispensed for reference material units. Selected units were analyzed for verification of uranium amount and to characterize uranium isotope amount ratios by multi-collector inductively couple plasma mass spectrometry. Furthermore, modelling of spike-corrected isotopic data show that the new spike will enable simultaneous measurements of uranium amount and isotope amount ratios with resulting uncertainties that are substantially less sensitive to over spiking than widely used 233 U certified reference materials.

233U↗

Isotope fractionation in surface ionization ion source of alkaline-earth iodides

The relationship between the isotope fractionation of alkaline-earth elements in the surface ionization ion source and the evaporation filament current, i.e., filament temperature, was studied. It was confirmed that the isotope fractionation depends on the evaporation filament temperature; the isotope fractionation in the case of higher temperature of filament becomes larger. The ionization and evaporation process in the surface ionization ion source was discussed, and it was concluded that the isotope fractionation is suppressed by setting at the lower temperature of evaporation filament because the dissociations are inhibited on the evaporation filament.

07 ISOTOPE AND RADIATION SOURCES↗

An instrumental and numerical method to determine the hydrogenic ratio in isotopic experiments in the TJ-II stellarator

The isotope effect is an important topic that is relevant for future D-T fusion reactors, where the use of deuterium, rather than hydrogen, may lean to improved plasma confinement. An evaluation of the ratio of hydrogen/deuterium is needed for isotope effect studies in current isotopic experiments. Here, the spectral range around H{sub α} and D{sub α} lines, obtained with an intensified multi-channel detector mounted to a 1-m focal length spectrometer, is analyzed using a fit function that includes several Gaussian components. The isotopic ratio evolution for a single operational day of the TJ-II stellarator is presented. The role of injected hydrogen by Neutral Beam Injection heating is also studied.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

MIXING AND TRANSPORT OF SHORT-LIVED AND STABLE ISOTOPES AND REFRACTORY GRAINS IN PROTOPLANETARY DISKS

Analyses of primitive meteorites and cometary samples have shown that the solar nebula must have experienced a phase of large-scale outward transport of small refractory grains as well as homogenization of initially spatially heterogeneous short-lived isotopes. The stable oxygen isotopes, however, were able to remain spatially heterogeneous at the {approx}6% level. One promising mechanism for achieving these disparate goals is the mixing and transport associated with a marginally gravitationally unstable (MGU) disk, a likely cause of FU Orionis events in young low-mass stars. Several new sets of MGU models are presented that explore mixing and transport in disks with varied masses (0.016 to 0.13 M{sub Sun }) around stars with varied masses (0.1 to 1 M{sub Sun }) and varied initial Q stability minima (1.8 to 3.1). The results show that MGU disks are able to rapidly (within {approx}10{sup 4} yr) achieve large-scale transport and homogenization of initially spatially heterogeneous distributions of disk grains or gas. In addition, the models show that while single-shot injection heterogeneity is reduced to a relatively low level ({approx}1%), as required for early solar system chronometry, continuous injection of the sort associated with the generation of stable oxygen isotope fractionations by UV photolysis leads to a sustained, relatively high level ({approx}10%) of heterogeneity, in agreement with the oxygen isotope data. These models support the suggestion that the protosun may have experienced at least one FU Orionis-like outburst, which produced several of the signatures left behind in primitive chondrites and comets.

79 ASTRONOMY AND ASTROPHYSICS↗

Quantifying uncertainty in physics-based predictions of rare-isotope production cross sections via Bayesian-inspired model averaging across nuclear mass tables

Accurate prediction of fragmentation cross sections is essential for rare-isotope beam production, planning new-isotope searches, and designing experiments to study the most exotic regions of the nuclear chart. However, existing reaction models and phenomenological cross-section parametrizations often exhibit significant deviations over broad regions of mass and charge. In this work, a Bayesian-inspired model-averaging framework is developed to combine abrasion-ablation (AA) calculations based on multiple nuclear mass tables into a single statistically weighted estimate. For the calibrated systems, the model weights are assigned empirically according to the relative quality of fit to measured cross sections, thereby reducing systematic model bias while preserving the underlying physics content of the AA description. The weights are constrained using proton-rich fragmentation data for the 78 Kr and 124 Xe projectiles. The resulting parameter trends are then propagated to the 92 Mo and 144 Sm systems through a controlled scaling procedure. In the present implementation, the excitation-energy prescription is fixed, while the averaging is performed across nuclear-mass inputs; the framework provides both weighted cross sections and associated uncertainty estimates. Applied to proton-rich fragmentation, the present approach provides a practical basis for interpolation and limited extrapolation in regions relevant to rare-isotope production. The resulting predictions are used to assess the production of very proton-rich nuclei, and candidate new isotopes are discussed.

Bayesian methods↗

Evolution of isotopic composition of reprocessed uranium during the multiple recycling in light water reactors with natural uranium feed

A complex approach based on the consistent modeling of neutron-physics processes and processes of cascade separation of isotopes is applied for analyzing physical problems of the multiple usage of reprocessed uranium in the fuel cycle of light water reactors. A number of scenarios of multiple recycling of reprocessed uranium in light water reactors are considered. In the process, an excess absorption of neutrons by the {sup 236}U isotope is compensated by re-enrichment in the {sup 235}U isotope. Specific consumptions of natural uranium for re-enrichment of the reprocessed uranium depending on the content of the {sup 232}U isotope are obtained.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Sapflow and xylem water isotopes from Snodgrass Mountain, East River Watershed, Colorado USA

This dataset includes sapflux and stable water isotopes of soil water and xylem water for aspen, fir and spruce trees along the Snodgrass Mountain transect in the East River Watershed, Colorado USA. The purpose of generating this dataset was to understand: (1) the total flux of water being used by trees in the watershed, (2) separate the component of transpiration that was derived from recent precipitation vs. older water such as winter precipitation of groundwater and (3) understand how total water use and water sources for the trees varies between species and position on a hillslope. The data were collected from May 2019 until October 2022. The sap flux data were collected using ICT SFM1 sensors and are presented in both units of cm h^-1 and as kg h^-1 by multiplying the sap flux by the sapwood area of the tree. All sap flow data has been been corrected using estimates of wounding diameter, water content of wood and sap wood depth. The xylem water isotope data were collected approximately weekly from each of the trees instrumented with sap flux. The stems were collected and the water extracted using classic cryogenic methods. Isotope measurements were done using a Picarro 2140i analyzer. We provide an estimate of the Seasonal Origin Index for each measurements following Allen et al., 2019 (10.5194/hess-23-1199-2019) where values of -1 equate to trees relying on winter precipitation and +1 tree relying on summer precipitation. We also provide the simultaneous sap flux for each isotope measurement when this data was available. This is an update to an earlier data repository with the same name that only included 2019 data. The new dataset was posted in January 2023 and is inclusive of the original 2019 data but now includes 2021 and 2022 data. Please note there was an error in the units of transpiration in the original dataset. It was incorrectly listed as mm h-1 when it should have been kg h-1. This change was made in May 2024.

54 ENVIRONMENTAL SCIENCES↗

Electric Dipole Moment Measurements with Rare Isotopes

The origin of matter is one of the deepest questions addressed by science and remains a mystery because our understanding of the Big Bang suggests that equal amounts of matter as antimatter would be created and annihilate leaving nothing from which stars, galaxies, planets and ultimately life as we know it was created. We know this is not the case in the universe, and so the explanation that the laws of physics can distinguish the difference of moving forward and backward in time and provide mechanisms that produce more matter that antimatter so that a little bit was left over. These same laws of physics affect our world today and would very slightly change the shape of an atom, stretching is along the direction of the spin of its nucleus. This subtle shape change has been searched in many systems - the neutron, atoms and molecules, but has not yet been detected, even as the motivation is strengthened by our understanding of their structure. We therefore look to new systems that have special features that make these effects stand out. Rare isotopes provide one possibility and specific radon atoms are our choice. We have developed techniques to make these measurements with short-lived radioactive atoms, studied the nuclei to provide deeper understanding of how these affect arise in such atoms (including radium) and developed new laser-based techniques to measure and control the magnetic fields necessary to perform these exquisitely sensitive measurements. In this work we have shown that radioactive radon atoms can be produced and transported to an apparatus that lines up the spins of the atoms. We have also shown that the nuclei of nearby radium are pear shaped and that the radon nuclei likely oscillate from one pear shape to its mirror reflection. We have also used the techniques which control nuclear spin to study the magnetic environment in a magnetically shielded room, which has the smallest magnetic field in a large volume in the universe. Measuring magnetic fields and detecting noble atoms' shapes using lasers will provide new techniques for these measurements and impact a broad range of applications including measurements of the neutron EDM. Harvesting rare isotopes at the future FRIB facility at Michigan State University will provide much stronger sources of the isotopes of radon and radium for future-generation experiments and also provide new isotopes for applications including medicine.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗