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NASA NTRS2023

Pervasive aqueous alteration in the early Solar System revealed by potassium isotopic variations in Ryugu samples and carbonaceous chondrites

C-type asteroids are the presumed home to carbonaceous chondrites, some of which contain abundant life-forming volatiles and organics. For the first time, samples from a C-type asteroid (162173 Ryugu) were successfully returned to Earth by JAXA’s Hayabusa2 mission. These pristine samples, uncontaminated by the terrestrial environment, allow a direct comparison with carbonaceous chondrites. This study reports the stable K isotopic compositions (expressed as δ 41 K) of Ryugu samples and seven carbonaceous chondrites to constrain the origin of K isotopic variations in the early Solar System. Three aliquots of Ryugu particles collected at two touchdown sites have identical δ 41 K values, averaged at -0.194 ± 0.038‰ (2SD). The K isotopic composition of Ryugu falls within the range of δ 41 K values measured on representative CI chondrites, and together, they define an average δ 41 K value of -0.185 ± 0.078‰ (2SE), which provides the current best estimate of the K isotopic composition of the bulk Solar System. Samples of CI chondrites with δ 41 K values that deviate from this range likely reflect terrestrial contaminations or compositional heterogeneities at sampled sizes. In addition to CI chondrites, substantial K isotopic variability is observed in other carbonaceous chondrites and within individual chondritic groups, with δ 41 K values inversely correlated with K abundances in many cases. These observations indicate widespread fluid activity occurred in chondrite parent bodies, which significantly altered the original K abundances and isotopic compositions of chondrules and matrices established at their accretion.

Asteroid Ryugu↗

DOE OSTI2022

Investigating preservation of stable isotope ratios in subfossil deep-sea proteinaceous coral skeletons as paleo-recorders of biogeochemical information over multimillennial timescales

Paleoproxy records in deep-sea proteinaceous coral skeletons can reconstruct past ocean conditions on centennial to millennial time scales. Commonly recovered subfossil specimens could potentially extend these archives through the Holocene. However, protein matrix stability and integrity of stable isotope proxies over multi-millennial timescales in such specimens have never been examined. Here we compare amino acid (AA) composition together with bulk and AA compound-specific carbon (δ 13 C) and nitrogen (δ 15 N) isotopes in live-collected and subfossil (~9.6–11.6 kyrs BP) Kulamanamana haumeaae deep-sea coral specimens from the central Pacific to understand the effects of long-duration benthic oxic exposure on primary coral chemistry. We find large coupled shifts in bulk δ 15 N (~7‰) and δ 13 C (~2‰) in the outermost portion (0–10 mm) of the subfossil coral, coincident with extensive alteration of the protein matrix. Microstructural changes in skeletal texture coincide with higher C/N ratios (+0.8) and isotope-based amino acid degradation parameters (e.g. ΣV ≥ 3), indicating extensive degradation of seawater-exposed gorgonin. However, interior gorgonin (>10 mm) retained amino acid molecular compositions (with exception of major Glycine loss) and bulk and amino acid-specific isotopic values that were similar to live-collected specimens. These results indicate that compound-specific isotope analysis of amino acids can reconstruct paleo-oceanographic biogeochemical and ecosystem information in subfossil corals beyond a clear diagenetic horizon, which is easily identifiable from an evaluation of C/N ratios together with the ΣV degradation proxy.

58 GEOSCIENCES↗

DOE OSTI2020

Tracking natural CO 2 migration through a sandstone aquifer using Sr, U and C isotopes: Chimayó, New Mexico, USA

The geochemical and isotopic characteristics of groundwaters in Chimayó, New Mexico, reflect processes that affect water quality in the Tesuque Aquifer, which overlies a leaking natural CO 2 source in a structurally complex region. In this study, select isotopes (δ 13 C, 87 Sr/ 86 Sr, 234 U/ 238 U) are applied to groundwaters to better understand CO 2 transport mechanisms and related water-rock interactions that impact Chimayó groundwater. Carbon stable isotope ratios of dissolved inorganic carbon (DIC; δ 13 CDIC = -15.10‰ to 4.50‰) identify a distinct source of upward-migrating CO 2 that interacts with the groundwater. Additionally, groundwater 87 Sr/ 86 Sr compositions (0.7098 to 0.7154) reflect intrusion of varying amounts of saline water associated with the high CO 2 source, while 234 U/ 238 U ratios corroborate presence of deep groundwater and suggest impacts from distinctive natural uranium sources are affecting groundwater. Previous work proposed two CO 2 transport mechanisms at the site: (1) dissolved in deep brine that underlies the aquifer and (2) in the gas phase; this study uses isotope mixing models to identify wells that are affected by these CO 2 transport mechanisms and demonstrates that both transport mechanisms are associated with impaired groundwaters. Overall, this study demonstrates that applying multiple isotope systems (δ 13 CDIC, 87 Sr/ 86 Sr, 234 U/ 238 U) is a dynamic tool for identifying and measuring the impact of CO 2 leakage from a sequestration site.

58 GEOSCIENCES↗

DOE OSTI2021

Organic contamination detection for isotopic analysis of water by laser spectroscopy

Hydrogen and oxygen stable isotope ratios (δ 2 H, δ 17 O, and δ 18 O values) are commonly used tracers of water. These ratios can be measured by isotope ratio infrared spectroscopy (IRIS). However, IRIS approaches are prone to errors induced by organic compounds present in plant, soil, and natural water samples. A novel approach using 17 O-excess values has shown promise for flagging spectrally contaminated plant samples during IRIS analysis. A systematic assessment of this flagging system is needed to prove it useful. Errors induced by methanol and ethanol water mixtures on measured IRIS and isotope ratio mass spectrometry (IRMS) results were evaluated. For IRIS analyses both liquid- and vapour-mode (via direct vapour equilibration) methods are used. The δ 2 H, δ 17 O, and δ 18 O values were measured and compared with known reference values to determine the errors induced by methanol and ethanol contamination. In addition, the 17 O-excess contamination detection approach was tested. This is a post-processing detection tool for both liquid and vapour IRIS triple-isotope analyses, utilizing calculated 17 O-excess values to flag contaminated samples. Organic contamination induced significant errors in IRIS results, not seen in IRMS results. Methanol caused larger errors than ethanol. Results from vapour-IRIS analyses had larger errors than those from liquid-IRIS analyses. The 17 O-excess approach identified methanol driven error in liquid- and vapour-mode IRIS samples at levels where isotope results became unacceptably erroneous. For ethanol contaminated samples, a mix of erroneous and correct flagging occurred with the 17 O-excess method. Here our results indicate that methanol is the more problematic contaminant for data corruption. The 17 O-excess method was therefore useful for data quality control. Organic contamination caused significant errors in IRIS stable isotope results. These errors were larger during vapour analyses than during liquid IRIS analyses, and larger for methanol than ethanol contamination. The 17 O-excess method is highly sensitive for detecting narrowband (methanol) contamination error in vapour and liquid analysis modes in IRIS.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2019

Regionally Correlated Oxygen and Carbon Isotope Zonation in Diagenetic Carbonates of the Bakken Formation

Diagenetic minerals preserve records of burial processes that overprint records of seawater chemistry and impact reservoir porosity. The Mississippian-Devonian aged Bakken Formation in the Williston Basin is a reservoir rock of economic importance whose productivity is affected by diagenetic carbonates, particularly dolomite-ankerite-series carbonates. To investigate how diagenetic carbonate alteration manifests in the Bakken and how that might change across the basin, a combined δ18O and δ13C isotope dataset for diagenetic carbonates was collected by in situ SIMS analysis of 10-μm spots from nine drill holes covering a ~250 km transect of the middle Bakken member. Observed core-to-rim isotopic variability in these small Fe-zoned dolomites and calcites frequently exceeds 10‰ in both δ 18 O and δ 13 C, indicating significant changes in thermal and chemical conditions during cementation. Individual ankeritic growth bands can be correlated across the basin by systematic similarities in minor-element compositions and isotope ratios. In the central part of the basin, δ 18 O and δ 13 C trends at sub-mm-scale decline consistently towards the rims of ankerite-series carbonates, which is interpreted to reflect mineral growth coincident with rising temperatures and an increasing organic contribution to inorganic carbon during burial. The most abrupt shifts in δ 18 O and δ 13 C (changes as large as 12‰ for δ 18 O and 6.5‰ for δ13C within distances < 15 μm) are observed along the basin margin, and are believed to preserve signals of hydrocarbon expulsion and fluid infiltration along basin margins. Based on the data, we conclude that ankerite-series carbonates preserve records of prolonged thermal and chemical processes that operated basinwide. The isotopic trends presented here show diagenetic rock evolution from shallow dolomite formation to deep burial ankerites, as well as the isotopic responses of carbonates to changing fluids and availability of organic δ 13 C. These results provide important constraints on how carbonate isotope records may be altered during burial in organic-rich sedimentary rocks and emphasize the need for caution in using bulk powder samples for geochemical analysis in carbonate systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Preparation of 241 Am/ 243 Am gravimetric mixtures and development of Am isotopic and assay measurement techniques using thermal ionization mass spectrometry

Three gravimetric mixtures with 241 Am/ 243 Am isotope ratios at nominally 1:1, 20:1, and 200:1 were prepared for calibration of the thermal ionization mass spectrometer instruments used for americium isotopic and assay measurements by isotope dilution mass spectrometry. The total evaporation analytical technique was developed for high-accuracy and precision measurements of Am isotopic ratios. The technique was also applied to Am assay measurements using isotope dilution mass spectrometry. The Am isotope ratio and assay measurement techniques were utilized to characterize batches of americium oxide separated from plutonium materials in storage at Los Alamos National Laboratory in support of commercial use of 241 AmO 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Projected network performance for multiple isotopes using next-generation xenon monitoring systems

Since about 2000 (Bowyer et al., 1998), radioxenon monitoring systems have been under development and testing for the verification of the Comprehensive Nuclear Test-Ban Treaty (CTBT). Operation of the systems since then has resulted in development of a next-generation of systems that are nearly ready for operational deployment. By 2010, the need to screen out civilian sources was well known (Auer et al., 2010; Saey, 2009), and isotopic ratio approaches were soon considered (Kalinowski et al., 2014) to identify specific sources. New generation systems are expected to improve the ability to verify the absence of nuclear tests by using isotopic ratios when multiple isotopes are detected. In this work, thousands of releases were simulated to compute the global detection probability of 131m Xe, 133m Xe, 133 Xe, and 135 Xe at 39 noble gas systems in the International Monitoring System (IMS) for both current and next-generation systems. Three release scenarios are defined at 1 h, 1 d, and 10 d past a 1 kt TNT equivalent 235U explosion event. Multiple cases using from one part in a million to the complete release of the xenon isotopic activity are evaluated for each scenario. Coverage maps and global integrals comparing current and next-generation monitoring systems are presented showing that next-generation noble gas systems will create measurable improvements in the IMS. The global detection probability for 133 Xe is shown to be strong in all scenarios, but only modestly improved by next-generation equipment. However, the detection probability for 131m Xe and 133m Xe increased to about 50% in different scenarios, providing a second detectable isotope for many events. As anticipated from shorter sampling intervals, the expected number of detecting samples roughly doubled and the expected number of detecting stations rose by approximately 50% for all release scenarios. Thus, it might be anticipated that future events would consist of multiple 133 Xe detections and one or more second isotope detections. In conclusion, signals of this nature should increase detection confidence, tighten release location estimates, improve rejection of civilian signals, and lessen the impacts from individual systems being offline for maintenance or repair reasons.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2023

Investigation of potential polyatomic interferences on uranium isotope ratio measurements for the LS-APGD-Orbitrap MS system

The determination of actinide (e.g., U and Pu) content and isotopics is of importance to the nuclear forensics and safeguards communities. However, in the analysis of environmental samples, such as those collected by the International Atomic Energy Agency, uranium measurements can be complicated by isobaric interferences from polyatomic variants of heavy elements (e.g., Pb). This leads to complex, time-consuming sample manipulations (i.e., separations) before determining isotope ratios. An alternative strategy to sample pretreatment is to use high-resolution mass spectrometric platforms during the analysis to fully resolve the uranium isotopes from potential polyatomic interferences, negating the need for prior chemical separation. The liquid sampling - atmospheric pressure glow discharge (LS-APGD) coupled with an Orbitrap mass spectrometer provides a high-resolution (>70,000 m/Δm at m/z 200) inorganic mass spectrometry platform. Further, as a demonstration of the power of this instrumental platform, and indeed, the high-resolution approach in general, uranium isotope ratios were determined in the presence of elemental impurities (e.g., Pb, Pt, Ta, W) commonly encountered with environmental sample swipe analysis, without any prior treatment. Even at elemental impurity concentrations of 1000–5000× relative to uranium, no interference was observed with the 235 U or 238 U signal. In addition, the 235 U/ 238 U isotope ratio for the samples with the concomitants present are within 2 standard deviations of the values obtained without their addition, indicating that these impurities do not impact the determined uranium isotope ratio. These findings represent a significant first step in leveraging the high resolution of the LS-APGD-Orbitrap-MS to overcome isobaric and molecular interferences instead of relying on chemical separations.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2025

Distinguishing fissile uranium isotopes using an active well neutron coincidence counter

Proposed thorium-based nuclear fuel cycles are likely to require quantification and verification of 233 U within nuclear material. Because of their similar fission cross sections, active neutron nondestructive assay (NDA) systems may respond similarly to 233 U and 235 U. Traditional safeguards equipment has been optimized for 235 U and 238 U quantification associated with conventional uranium/plutonium fuel cycles and may not be directly applicable to 233 U quantification when mixed with other actinides. This work used models of the large volume active well coincidence counter (LV-AWCC) at Oak Ridge National Laboratory to evaluate the performance of this neutron NDA system to differentiate fissile uranium isotopes. The models were developed to simulate NDA system performance in response to a number of triangular radiation signature training device sources within the central cavity or well. This work predicted that the LV-AWCC can effectively differentiate 233 U from 235 U in certain modes of operation. In active mode, the LV-AWCC with the cadmium liner results in different doubles count rates between the fissile isotopes for a given fissile uranium mass. Without the cadmium liner, the uranium isotopes provide a statistically indistinguishable doubles count rate response for the fissile masses considered in this work (up to approximately 150 g). The cadmium liner serves to harden the neutron interrogation spectrum, which better exploits the notable difference in the 233 U and 235 U fission cross sections at approximately 1 eV. In passive mode, the two fissile isotopes exhibit different doubles and singles count rates regardless of liner presence because the passive source strength of 233 U is approximately 2 orders of magnitude stronger than that of 235 U due to the shorter half-life and correspondingly higher (α, n) yield. We conclude that using neutron interrogation in the LV-AWCC, two measurements are needed to quantify 233 U content in mixed uranium items. The first measurement is used to determine the total fissile uranium mass using a mode that cannot distinguish fissile isotopes (i.e., where a similar response is observed for both fissile uranium isotopes such as active doubles without cadmium or using a thermal neutron interrogation source). In conclusion, the second measurement is used to determine the 233 U content by using a differentiating technique (e.g., passive doubles, passive doubles to singles ratio, active doubles with cadmium).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

Coupled neutronics, thermochemistry, corrosion modeling and sensitivity analyses for isotopic evolution in molten salt reactors

This study presents a computational methodology for analyzing isotopic evolution and associated uncertainties in molten salt reactors (MSRs), focusing on both fluoride- and chloride-based fuel salts. The primary goal is to enhance the understanding of isotopic behavior in MSRs and provide data to support future experimental efforts. The methodology integrates transport-coupled depletion calculations using OpenMC, equilibrium thermodynamics modeling with Thermochimica, and a corrosion model. Sensitivity analyses are performed to evaluate the impact of power density, air ingress, and humidity content on isotopic evolution in MSR concepts. This study examines representative F- and Cl-based MSR designs, highlighting the dominant influence of power density on isotopic composition, which significantly affects isotope production and depletion rates, accounting for approximately 76% of the observed variance in element concentration. Air ingress and humidity content also affect the redox potential, solubility of heavier elements, and corrosion rates, thereby altering the expected isotopic evolution in the reactor. On average, air ingress accounts for around 17% of the variance in element concentrations, while humidity explains the remaining 7%. These variances differ significantly from element to element, depending on the element’s role in depletion, redox potential evolution, and galvanic corrosion. The findings indicate that power density, air ingress, and humidity content are all critical factors for optimizing reactor design and operational strategies. Furthermore, the study provides expected ranges for key impurities in the fuel salt, which are crucial for guiding future experimental studies and refining MSR designs. Finally, this study demonstrates the importance of modeling depletion coupled with the evolution of redox potential and chemical interactions in MSR fuel salts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Controlled Release of Hydrogen Isotopes from Hydride-Magnetic Nanomaterials

In this work, hydrogen isotopes in the form of protium and deuterium were rapidly desorbed from magnetic-hydride iron oxide-palladium (Fe 2 O 3 -Pd) hybrid nanomaterials using an alternating magnetic field (AMF). Palladium, a hydride material with a well-known hydrogen isotope effect, was deposited on Fe 2 O 3 magnetic nanoparticle support by solution chemistries and used as a hydrogen isotope storage component. The morphological, structural, optical, and magnetic studies reveal that the Fe 2 O 3 -Pd nanoparticles (NPs) are hybrid structures exhibiting both hydrogen isotope storage (Pd) and magnetic (Fe 2 O 3 ) properties. The hydrogen isotope sorption/desorption behavior of metal hydride-magnetic nanomaterials was assessed by isothermal pressure-composition response curves (isotherms). The amount and rate of hydrogen isotope gas release was tuned by simply adjusting the strength of the magnetic field strength applied. Protium and deuterium displayed a similar loading capacity, namely H/M 0.55 and H/M=0.45, but different plateau pressures. Significant differences in the kinetics of release for protium and deuterium during magnetic heating were observed. A series of magnetically induced charge-discharge cycling experiments were conducted showing that this is a highly reproducible and robust process

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Modeling Snow Dynamics and Stable Water Isotopes Across Mountain Landscapes

Abstract A coupled hydrologic and snowpack stable water isotope model assesses controls on isotopic inputs across a mountainous basin. Annually, the most depleted isotope conditions occur in the upper subalpine where snow accumulation is high, and rainfall is low. Snowmelt isotopic evolution over time indicates fractionation processes account for <25% snowmelt enrichment. Meltwater isotopic inputs are largely determined by controls on the amount, phase and isotopic mass of precipitation coincident with the ablation period. Effect of vapor loss from the snowpack on d‐excess in snowmelt is a balance between energy and snow‐availability. It is highest above treeline, and in the grass and aspen‐dominated portions of the upper montane where vegetation shading is low. Deep snowpack in conifer forests limit the influence of vapor loss in the subalpine. Wet years reduce the effects of vapor loss on snowmelt across the basin, except in the lower montane where added snowfall bolsters snow‐limited conditions.

58 GEOSCIENCES↗

DOE OSTI2020

Factors controlling the oxygen isotopic composition of lacustrine authigenic carbonates in Western China: implications for paleoclimate reconstructions

Abstract In the carbonate-water system, at equilibrium, the oxygen isotopic composition of carbonate is dependent not only on the temperature but also on the isotopic composition of host water in which the carbonate is formed. In this study, lake surface sediment and water samples were collected from 33 terminal lakes in Western China to evaluate controls on the oxygen isotopic composition of lacustrine authigenic carbonates (δ 18 O carb ) and its spatial distribution. Our results show that water oxygen isotopic composition (δ 18 O water ) rather than lake summer water temperature (T water ), is the main determinant of δ 18 O carb , irrespective of whether oxygen isotope equilibrium is achieved. There are significant linear correlations between δ 18 O carb and elevation, as well as that between δ 18 O carb and latitude for lakes located on the Tibetan Plateau. In Western China, the spatial distribution of δ 18 O carb is consistent with that of δ 18 O water , and is ultimately controlled by the isotopic composition of local precipitation (δ 18 O precipitation ) that depends on the source of water vapor. Therefore, changes in δ 18 O carb can be predominantly interpreted as variations of δ 18 O water , which in turn represent changes in δ 18 O precipitation for paleoclimate reconstructions in this region, and may be relevant to studies of other areas.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2025

Boron isotopic analysis in bulk silicate materials using the Neoma MS/MS MC-ICP-MS

Boron (B) isotopes are a valuable tracer with applications ranging from geological, environmental, and nuclear studies because B isotopic fractionation is highly sensitive to chemical processes yielding distinct isotopic trends in natural and anthropogenic systems. Despite this wide applicability, there remain relatively few measurements on well-described reference materials and in some cases, poor agreement between various methods. We report a method for boron isotope ratio measurement in solution on the Neoma MS/MS MC-ICP-MS specifically targeting bulk silicates. We evaluate the performance of the method and instrument as it relates to the measurement of the absolute boron isotope ratio ( 10 B/ 11 B). The results indicate that the method produces data in agreement with literature values and that the sample–standard bracketing technique is appropriate for the Neoma MS/MS MC-ICP-MS which has been in use for decades on previous generation instruments. Careful tuning of the MS/MS lenses is required to obtain precision comparable to non MS/MS equipped MC-ICP-MS. With careful tuning, internal and external precisions of ∼0.3‰ were achieved. However, when the MS/MS is not properly tuned external precisions exceed 3‰. Nevertheless, our results for IAEA B-6, BCR-2, BHVO-2 and W-2a reference materials overlap the 1σ range of previously reported 10 B/ 11 B. Data are reported for total boron quantities down to a few tens of nanograms. Our procedure yielded blanks as low as 3 ng but up to 29 ng, making blank corrections important for small samples sizes in the few 10s of nanogram range. We report B isotope ratios for AGV-2G, SL-1G, GSC-2G, GSD-2G, GSE-2G, RLS-132, RLS-140, NKT-1G, and T1-G glass reference materials that have not been previously reported in the literature.

Scott, Sean R. [Pacific Northwest National Laborat↗

DOE OSTI2023

Water isotopes, climate variability, and the hydrological cycle: recent advances and new frontiers

Abstract The hydrologic cycle is a fundamental component of the climate system with critical societal and ecological relevance. Yet gaps persist in our understanding of water fluxes and their response to increased greenhouse gas forcing. The stable isotope ratios of oxygen and hydrogen in water provide a unique opportunity to evaluate hydrological processes and investigate their role in the variability of the climate system and its sensitivity to change. Water isotopes also form the basis of many paleoclimate proxies in a variety of archives, including ice cores, lake and marine sediments, corals, and speleothems. These records hold most of the available information about past hydrologic variability prior to instrumental observations. Water isotopes thus provide a ‘common currency’ that links paleoclimate archives to modern observations, allowing us to evaluate hydrologic processes and their effects on climate variability on a wide range of time and length scales. Building on previous literature summarizing advancements in water isotopic measurements and modeling and describe water isotopic applications for understanding hydrological processes, this topical review reflects on new insights about climate variability from isotopic studies. We highlight new work and opportunities to enhance our understanding and predictive skill and offer a set of recommendations to advance observational and model-based tools for climate research. Finally, we highlight opportunities to better constrain climate sensitivity and identify anthropogenically-driven hydrologic changes within the inherently noisy background of natural climate variability.

Dee, Sylvia (ORCID:000000022140785X)↗

DOE OSTI2026

Shape evolution in neutron-rich odd-even 105–109 Nb isotopes

Background: Neutron-rich nuclei around 𝑍 ≈ 40 are well known for exhibiting multiple shape transitions. Here, this region shows one of the sharpest shape transitions in the nuclear chart, evolving from a spherical vibrator at 𝑁 = 58 to a strongly deformed prolate shape at 𝑁 = 60. The largest deformations are observed for 38 Sr and 40 Zr . This abrupt shape transition disappears at 𝑍 = 36 and below, where a shape transition from spherical to oblate nuclei is predicted. On the other hand, for 𝑍 ≥ 42 and 𝑁 ≥ 60, the shape is known to evolve from axial to triaxial. While the even-𝑍 nuclei in this region have already been extensively studied, new insights can be gained from the studies of odd-𝑍 isotopes for a better understanding of the underlying mechanisms driving these phenomena. Purpose: The 41 Nb nuclei lie at the boundary between axially deformed Zr and triaxially deformed Mo nuclei. This work investigates the nuclear structure of very neutron-rich Nb nuclei up to 𝑁 = 68. The goal is to understand how the nuclear shape evolves as a function of isospin in this isotopic chain and provide new insights into the emergence of triaxial deformation. Methods: The structure of the neutron-rich Nb isotopes was investigated using state-of-the-art high-resolution 𝛾-ray spectroscopy of fission fragments produced via two different fission reactions. The use of 9 Be ⁢( 238 U, 𝑓) inverse kinematics, with a detection system comprising AGATA, EXOGAM, and VAMOS++, enabled the measurement of prompt and delayed 𝛾 rays from isotopically identified fission fragments, and 𝛾−𝛾−𝛾−𝛾 highfold data were obtained from a spontaneous fission source of 252 Cf using the Gammasphere array. Results: The level scheme of 105 Nb has been significantly extended, with the addition of two negative-parity bands observed for the first time. A new level scheme is proposed for 107 Nb, which is not in agreement with an earlier measurement, and new levels and transitions have been added to the very neutron-rich 109 Nb. The degree of triaxiality of the new bands is discussed on the basis of signature splitting analysis. The recently reported level scheme of 99 Nb has been revised. Conclusions: This systematic study on the Nb isotopic chain, compared to Zr and Mo, indicates that while the ground-state band exhibits a triaxial deformation, attributed to a proton hole coupled to a triaxially deformed Mo core, the negative-parity bands, based on isomeric bandheads, display an axially symmetric deformed structure, similar to that observed in the Zr isotopes, revealing the existence of a shape coexistence in the neutron-rich Nb nuclei.

Abushawish, M. [Université Claude-Bernard Lyon 1 (↗

DOE OSTI2023

Ultra-sensitive isotope probing to quantify activity and substrate assimilation in microbiomes

Abstract Background Stable isotope probing (SIP) approaches are a critical tool in microbiome research to determine associations between species and substrates, as well as the activity of species. The application of these approaches ranges from studying microbial communities important for global biogeochemical cycling to host-microbiota interactions in the intestinal tract. Current SIP approaches, such as DNA-SIP or nanoSIMS allow to analyze incorporation of stable isotopes with high coverage of taxa in a community and at the single cell level, respectively, however they are limited in terms of sensitivity, resolution or throughput. Results Here, we present an ultra-sensitive, high-throughput protein-based stable isotope probing approach (Protein-SIP), which cuts cost for labeled substrates by 50–99% as compared to other SIP and Protein-SIP approaches and thus enables isotope labeling experiments on much larger scales and with higher replication. The approach allows for the determination of isotope incorporation into microbiome members with species level resolution using standard metaproteomics liquid chromatography-tandem mass spectrometry (LC–MS/MS) measurements. At the core of the approach are new algorithms to analyze the data, which have been implemented in an open-source software ( https://sourceforge.net/projects/calis-p/ ). We demonstrate sensitivity, precision and accuracy using bacterial cultures and mock communities with different labeling schemes. Furthermore, we benchmark our approach against two existing Protein-SIP approaches and show that in the low labeling range used our approach is the most sensitive and accurate. Finally, we measure translational activity using 18 O heavy water labeling in a 63-species community derived from human fecal samples grown on media simulating two different diets. Activity could be quantified on average for 27 species per sample, with 9 species showing significantly higher activity on a high protein diet, as compared to a high fiber diet. Surprisingly, among the species with increased activity on high protein were several Bacteroides species known as fiber consumers. Apparently, protein supply is a critical consideration when assessing growth of intestinal microbes on fiber, including fiber-based prebiotics. Conclusions We demonstrate that our Protein-SIP approach allows for the ultra-sensitive (0.01 to 10% label) detection of stable isotopes of elements found in proteins, using standard metaproteomics data.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Oxygen isotope evidence for input of magmatic fluids and precipitation of Au-Ag-tellurides in an otherwise ordinary adularia-sericite epithermal system in NE China

Abstract Tellurium-rich (Te) adularia-sericite epithermal Au-Ag deposits are an important current and future source of precious and critical metals. However, the source and evolution of ore-forming fluids in these deposits are masked by traditional bulk analysis of quartz oxygen isotope ratios that homogenize fine-scale textures and growth zones. To advance understanding of the source of Te and precious metals, herein, we use petrographic and cathodoluminescence (CL) images of such textures and growth zones to guide high spatial resolution secondary ion mass spectroscopy (SIMS) oxygen isotope analyses (10 µm spot) and spatially correlated fluid inclusion microthermometric measurements on successive quartz bands in contemporary Te-rich and Te-poor adularia-sericite (-quartz) epithermal Au-Ag vein deposits in northeastern China. The results show that large positive oxygen isotope shifts from –7.1 to +7.7‰ in quartz rims are followed by precipitation of Au-Ag telluride minerals in the Te-rich deposit, whereas small oxygen isotope shifts of only 4‰ (–2.2 to +1.6‰) were detected in quartz associated with Au-Ag minerals in the Te-poor deposits. Moreover, fluid-inclusion homogenization temperatures are higher in comb quartz rims (avg. 266.4 to 277.5 °C) followed by Au-Ag telluride minerals than in previous stages (~250 °C) in the Te-rich deposit. The Te-poor deposit has a consistent temperature (~245 °C) in quartz that pre- and postdates Au-Ag minerals. Together, the coupled increase in oxygen isotope ratios and homogenization temperatures followed by precipitation of Au-Ag tellurides strongly supports that inputs of magmatic fluid containing Au, Ag, and Te into barren meteoric water-dominated flow systems are critical to the formation of Te-rich adularia-sericite epithermal Au-Ag deposits. In contrast, Te-poor adularia-sericite epithermal Au-Ag deposits show little or no oxygen isotope or fluid-inclusion evidence for inputs of magmatic fluid.

Geochemistry & Geophysics↗