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Chromium isotopes in an acidic fluvial system: Implications for modern and ancient Cr isotope records
Chromium is an important redox-active element, with significant Cr isotope fractionations driven by redox transformations in the natural environment and quantified through laboratory experiments. Recent work has demonstrated that non-redox-driven transformations can also produce small variations in Cr isotopes, but the role of these processes in controlling environmental Cr isotope variations remains unclear. The highly acidic but biologically diverse acid rock drainage system in Río Tinto, Spain (and affiliated rivers) provides a unique opportunity to examine how non-redox-related processes can substantially affect the isotopic composition of Cr in a natural system. Our results suggest that under conditions where Cr redox transformations are obviated, Cr cycling is largely controlled by formation of Fe-oxyhydroxides and Fe-hydroxysulfates, Cr adsorption, and Cr speciation, with little apparent Cr isotope fractionation between source materials, waters, and sediments. Moderate Cr isotope shifts, however, may be the result of non-redox processes, including adsorption to organic ligands and potentially biological uptake. These results add to a growing body of evidence for the importance of non-redox transformations in contributing to environmental Cr isotope variations, with implications for the use of chromium isotopes in studies of sedimentary Cr isotope records. In particular, this study is a validation of the potential for sulfide weathering in the Proterozoic to deliver relatively unfractionated Cr isotopes to the ocean, despite rising and sustained high oxygen levels.
Chromium isotope fractionation during reduction of Chromium(VI) by Iron(II/III)-bearing clay minerals
Chromium stable isotope ratios are used to trace the reduction of Cr(VI) to Cr(III) in both ancient and modern systems. However, quantitative interpretation of Cr isotopic signatures has been stymied by the large variability in isotopic fractionation factors for Cr(VI) reduction by different reductants. Here we determine Cr isotope fractionation factors during Cr(VI) reduction by Fe(II/III)-bearing clay minerals, which are abundant in subsurface environments. Several variables were tested: pH, total Fe content of the clay, and the fraction of reduced Fe within the clay (Fe(II)/Fe(total)). The latter controls the standard reduction potential of the clay. Our results demonstrate that neither pH nor total Fe content of the clay have major effects on isotopic fractionation. In contrast, as the effective standard reduction potential of the clay and thus the standard free energy of Cr(VI) reduction become more negative, Cr isotope fractionation factors decrease in magnitude from - 4.9 to -1.3‰ according to a linear free energy relationship. This linear free energy relationship can be predicted from Marcus electron transfer theory and allows first-order predictions of Cr isotope fractionation factors to be made from the standard reduction potential or Fe(II)/Fe(total) of a clay, potentially improving our ability to model Cr isotope signatures in geochemical systems. Chromium is the first isotope system to show such a linear free energy relationship over a diverse range of reductants, including both aqueous and solid-phase reductants, and may provide a model for determining other redox-driven kinetic isotope effects in environmentally important isotope systems.
Chromium isotopes as indicators of hexavalent chromium reduction
This is the final report for a university research project which advanced development of a new technology for identifying chemical reduction of hexavalent chromium contamination in groundwater systems. Reduction renders mobile and toxic hexavalent chromium immobile and less toxic. The new method uses stable isotope ratio measurements, which are made using multicollector ICP-mass spectrometry. The main objectives of this project were completed during the project period and two peer-reviewed articles were published to disseminate the information gained.
Time-of-flight mass measurements of neutron-rich chromium isotopes up to N = 40 and implications for the accreted neutron star crust
Here, we present the mass excesses of 59-64 Cr, obtained from recent time-of-flight nuclear mass measurements at the National Superconducting Cyclotron Laboratory at Michigan State University. The mass of 64Cr is determined for the first time, with an atomic mass excess of -33.48(44) MeV. We find a significantly different two-neutron separation energy S 2n trend for neutron-rich isotopes of chromium, removing the previously observed enhancement in binding at N = 38. Additionally, we extend the S 2n trend for chromium to N = 40, revealing behavior consistent with the previously identified island of inversion in this region. We compare our results to state-of-the-art shell-model calculations performed with a modified Lenzi-Nowacki-Poves-Sieja interaction in the fp shell, including the g 9/2 and d 5/2 orbits for the neutron valence space. We employ our result for the mass of 64 Cr in accreted neutron star crust network calculations and find a reduction in the strength and depth of electron-capture heating from the A = 64 isobaric chain, resulting in a cooler than expected accreted neutron star crust. This reduced heating is found to be due to the >1-MeV reduction in binding for 64 Cr with respect to values from commonly used global mass models.
Chromium Isotope Fractionation During Reduction of Cr(VI) Under Saturated Flow Conditions
Chromium isotopes are potentially useful indicators of Cr(VI) reduction reactions in groundwater flow systems; however, the influence of transport on Cr isotope fractionation has not been fully examined. Laboratory batch and column experiments were conducted to evaluate isotopic fractionation of Cr during Cr(VI) reduction under both static and controlled flow conditions. Organic carbon was used to reduce Cr(VI) in simulated groundwater containing 20 mg L{sup -1} Cr(VI) in both batch and column experiments. Isotope measurements were performed on dissolved Cr on samples from the batch experiments, and on effluent and profile samples from the column experiment. Analysis of the residual solid-phase materials by scanning electron microscopy (SEM) and by X-ray absorption near edge structure (XANES) spectroscopy confirmed association of Cr(III) with organic carbon in the column solids. Decreases in dissolved Cr(VI) concentrations were coupled with increases in {delta}{sup 53}Cr, indicating that Cr isotope enrichment occurred during reduction of Cr(VI). The {delta}{sup 53}Cr data from the column experiment was fit by linear regression yielding a fractionation factor ({alpha}) of 0.9979, whereas the batch experiments exhibited Rayleigh-type isotope fractionation ({alpha} = 0.9965). The linear characteristic of the column {delta}{sup 53}Cr data may reflect the contribution of transport on Cr isotope fractionation.
Titanium and chromium isotopic compositions of calcium-aluminum-rich inclusions: Implications for the sources of isotopic anomalies and the formation of distinct isotopic reservoirs in the early Solar System
As the earliest-dated solids in our Solar System, calcium-aluminum-rich inclusions (CAIs) provide a record of their formation environment near the young Sun and hold clues to the formation of planetary-scale isotopic reservoirs in the solar protoplanetary disk. Although CAIs from several CV, CK, CM, CO, and ordinary chondrites have been analyzed previously for their Ti isotopic compositions, CAIs from just three CV chondrites have been analyzed for their Cr isotopic compositions, and only a handful of CAIs have been measured for both their Ti and Cr isotopic compositions. We report mass-independent Ti and Cr isotopic anomalies in several CAIs from CV and CK chondrites; this is the first report of the Cr isotopic composition of a CAI from a CK chondrite. With this data, we aim to better constrain the compositional range of CAIs in ε 50 Ti versus ε 54 Cr space, thereby facilitating the isotopic characterization of the material inherited by the solar protoplanetary disk and the role of CAIs in the formation of distinct planetary-scale isotopic reservoirs in our early Solar System. The narrow range in isotopic anomalies in CAIs when compared to other early-formed refractory inclusions such as platy hibonite crystals (PLACs) and spinel-hibonite inclusions (SHIBs) suggests that CAIs record the mixing of these precursor materials and the averaging of their larger isotopic anomalies. The isotopic composition of CAIs is therefore likely the result of a combination of factors, including mixing of material inherited from their formation region, heterogeneous carrier phase distribution, and thermal processing in the disk. The ε 50 Ti and ε 54 Cr isotopic compositions of CAIs are not correlated, further demonstrating that these isotopic anomalies have different carrier phases. The Ti and Cr isotopic compositions of CAIs additionally show that CAIs alone cannot be responsible for the compositional difference between the non-carbonaceous chondritic (NC) and carbonaceous chondritic (CC) isotopic reservoirs but nevertheless do play a role in the formation of these large-scale isotopic reservoirs in the early Solar System.
Newly Evaluated Neutron Reaction Data on Chromium Isotopes
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Reduced transition strengths of low-lying yrast states in chromium isotopes in the vicinity of N = 40
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Chromium Isotopic Evidence for Mixing of NC and CC Reservoirs in Polymict Ureilites: Implications for Dynamical Models of the Early Solar System
Nucleosynthetic isotope anomalies show that the first few million years of solar system history were characterized by two distinct cosmochemical reservoirs, CC (carbonaceous chondrites and related differentiated meteorites) and NC (the terrestrial planets and all other groups of chondrites and differentiated meteorites), widely interpreted to correspond to the outer and inner solar system, respectively. At some point, however, bulk CC and NC materials became mixed, and several dynamical models offer explanations for how and when this occurred. We use xenoliths of CC materials in polymict ureilite (NC) breccias to test the applicability of such models. Polymict ureilites represent regolith on ureilitic asteroids but contain carbonaceous chondrite-like xenoliths. We present the first 54 Cr isotope data for such clasts, which, combined with oxygen and hydrogen isotopes, show that they are unique CC materials that became mixed with NC materials in these breccias. It has been suggested that such xenoliths were implanted into ureilites by outer solar system bodies migrating into the inner solar system during the gaseous disk phase ~3–5 Myr after CAI, as in the "Grand Tack" model. However, combined textural, petrologic, and spectroscopic observations suggest that they were added to ureilitic regolith at ~50–60 Myr after CAI, along with ordinary, enstatite, and Rumuruti-type chondrites, as a result of the breakup of multiple parent bodies in the asteroid belt at this time. This is consistent with models for an early instability of the giant planets. The C-type asteroids from which the xenoliths were derived were already present in inner solar system orbits.
Chromium isotope systematics of martian meteorites: Implications for Mars' early differentiation
Abstract not provided
ORNL Resolved Resonance Covariance Generation for ENDF/B-VII.1
Resonance-parameter covariance matrix (RPCM) evaluations in the resolved resonance regionwere done at the Oak Ridge National Laboratory (ORNL) for the chromium isotopes, titanium isotopes, {sup 19}F, {sup 58}Ni, {sup 60}Ni, {sup 35}Cl, {sup 37}Cl, {sup 39}K, {sup 41}K, {sup 55}Mn, {sup 233}U, {sup 235}U, {sup 238}U, and {sup 239}Pu using the computer code SAMMY. The retroactive approach of the code SAMMY was used to generate the RPCMs for {sup 233}U. For {sup 235}U, the approach used for covariance generation was similar to the retroactive approach with the distinction that real experimental data were used as opposed to data generated from the resonance parameters. RPCMs for {sup 238}U and {sup 239}Pu were generated together with the resonance parameter evaluations. The RPCMs were then converted in the ENDF format using the FILE32 representation. Alternatively, for computer storage reasons, the FILE32 was converted in the FILE33 cross section covariance matrix (CSCM). Both representations were processed using the computer code PUFF-IV. This paper describes the procedures used to generate the RPCM and CSCM in the resonance region for ENDF/B-VII.1. The impact of data uncertainty in nuclear reactor benchmark calculations is also presented.
Thermodynamic controls on redox-driven kinetic stable isotope fractionation
Stable isotope fractionation arising from redox reactions has the potential to illuminate the oxygenation of Earth's interior, oceans, and atmosphere. However, reconstruction of past and present redox conditions from stable isotope signatures is complicated by variable fractionations associated with different reduction pathways. Here we demonstrate a linear relationship between redox-driven kinetic fractionation and the standard free energy of reaction for aqueous chromium(VI) reduction by iron(II) species. We also show that the intrinsic kinetic fractionation factor is log-linearly correlated with the rate constant of reaction, which is in turn a function of the free energy of reaction. The linear free energy relationship for kinetic fractionation describes both our experimental results and previous observations of chromium isotope fractionation and allows the magnitude of fractionation to be directly linked to environmental conditions such as pH and oxygen levels. By demonstrating that the magnitude of kinetic fractionation can be thermodynamically controlled, this study systematically explains the large variability in chromium(VI) isotope fractionation and provides a conceptual framework that is likely applicable to other isotope systems.
Ab Initio Limits of Atomic Nuclei
We predict the limits of existence of atomic nuclei, the proton and neutron drip lines, from the light through medium-mass regions. Starting from a chiral two- and three-nucleon interaction with good saturation properties, we use the valence-space in-medium similarity renormalization group to calculate ground-state and separation energies from helium to iron, nearly 700 isotopes in total. Here, we use the available experimental data to quantify the theoretical uncertainties for our ab initio calculations towards the drip lines. Where the drip lines are known experimentally, our predictions are consistent within the estimated uncertainty. For the neutron-rich sodium to chromium isotopes, we provide predictions to be tested at rare-isotope beam facilities.
Nuclear Data Sheets for A = 44
The experimental data are evaluated for known nuclides of mass number A=44 (Si,P,S,Cl,Ar,K,Ca,Sc,Ti,V, Cr,Mn). Detailed evaluated level properties and related information are presented, including adopted values of level and {gamma}-ray energies, decay data (energies, intensities and placement of radiations), and other spectroscopic data. This work supersedes earlier full evaluations of A=44 published by 1999Ca45 and 1990En08 (also 1998En04 update). No excited states are known in {sup 44}Si, {sup 44}P, {sup 44}Cr, {sup 44}Mn. Only one excited state is known in 44V and its Isobaric Analog State (IAS) has been observed but with the level energy not known. Information for {sup 44}S, {sup 44}Cl and {sup 44}Ar is limited and their radioactive decay schemes seem incomplete in view of large Q values and known excitations much below than allowed by Q values. The {sup 44}Ca, {sup 44}Sc and {sup 44}Ti nuclides remain as the most extensively studied from many different reactions and decays.
{sup 58}Fe AND {sup 54}Cr IN EARLY SOLAR SYSTEM MATERIALS
Stepwise dissolution of primitive meteorites exhibits large {sup 54}Cr anomalies but no collateral effects on {sup 58}Fe and {sup 48}Ca, two other neutron-rich nuclides from the iron peak. These results suggest that {sup 54}Cr must have been produced in particular zones of the rare Type Ia supernovae or that {sup 48}Ca and/or {sup 58}Fe were produced together in Type II supernovae and were chemically separated into some mineral phase that favors Cr over Ca and Fe, and it is the dissolution properties of that phase that is driving the isotopic effect in leaching. The recent findings of nanometer-size oxide grains with very large {sup 54}Cr excesses favored the latter scenario for the origin of the mono-isotopic Cr isotopic effect. In addition, the absence of isotopic variations in the {sup 58}Fe/{sup 54}Fe ratio at the mineral scale confirms that the short-lived nuclide {sup 60}Fe (T {sub 1/2} = 2.62 Myr) was homogeneously distributed to a less than 15% dispersion in the early solar nebula.
Giant halos in medium nuclei within modified relativistic mean field (MRMF) model
The large number of neutrons in a region beyond a closed shell core indicates the presence of giant halos in nuclei. In this work, by using the Rotival method within a modified relativistic mean field (MRMF) model, we predict theoretically the formation of giant halos in Cr and Zr isotopes. The MRMF model is a modification of standard RMF model augmented with isoscalar and isovector tensor terms, isovector-isoscalar vector cross coupling term and electromagnetic exchange term for Coulomb interaction in local density approximation (LDA).
Differential Isotopic Fractionation during Cr(VI) Reduction by an Aquifer-Derived Bacterium under Aerobic versus Denitrifying Conditions
We studied Cr isotopic fractionation during Cr(VI) reduction by Pseudomonas stutzeri strain RCH2. Finally, despite the fact that strain RCH2 reduces Cr(VI) cometabolically under both aerobic and denitrifying conditions and at similar specific rates, fractionation was markedly different under these two conditions (ε was ~2‰ aerobically and ~0.4‰ under denitrifying conditions).