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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Precision Mass Measurements of Neutron-Rich Neodymium and Samarium Isotopes and Their Role in Understanding Rare-Earth Peak Formation

The Canadian Penning Trap mass spectrometer at the Californium Rare Isotope Breeder Upgrade (CARIBU) facility was used to measure the masses of eight neutron-rich isotopes of Nd and Sm. These measurements are the first to push into the region of nuclear masses relevant to the formation of the rare-earth abundance peak at A similar to 165 by the rapid neutron-capture process. We compare our results with theoretical predictions obtained from "reverse engineering" the mass surface that best reproduces the observed solar abundances in this region through a Markov chain Monte Carlo technique. Our measured masses are consistent with the reverse-engineering predictions for a neutron star merger wind scenario.

Orford, R.↗
DOE OSTI2020

Samarium isotope compositions of uranium ore concentrates: A novel nuclear forensic signature

Uranium ore is mined and milled to produce uranium ore concentrate (UOC), a regulated product of the nuclear fuel cycle. Additionally, diversion of UOC from the fuel cycle into possible weapons production is a key concern in global nonproliferation efforts. As such, the ability to trace the origin of seized nuclear materials is imperative to law enforcement efforts. Although isotopic signatures of UOCs have proven fruitful to pinpoint sample provenance, new isotopic signatures are needed because most existing isotopic signatures are not indicative of the original ore body from which the U is derived. In this work, we developed a new method to separate samarium (Sm) from a U-rich sample matrix and report the first Sm isotope compositions of 32 UOCs derived from a variety of worldwide uranium mines. Relative to terrestrial standards, approximately half the UOCs have resolved and anticorrelated 149 Sm- 150 Sm isotope compositions, consistent with the capture of thermal neutrons by 149 Sm in the ore body. The UOCs with anomalous Sm isotope compositions tend to derive from older (~>1.5Ga) and higher-grade ore bodies, although other factors, such as the presence of neutron moderators like water, also play a role. Nonetheless, the Sm isotope compositions of UOCs directly reflects the neutron fluence over the history of the original ore body and can be used to discern different geologic conditions associated with that ore body. Overall, this work demonstrates the potential use of Sm isotopes as a novel nuclear forensics signature for origin assessment of UOCs.

58 GEOSCIENCES↗
DOE OSTI2018

Entry-level spin distributions and relative γ -neutron branching ratios of samarium isotopes populated by the ( p , t ) reaction

The spin distribution populated in the $^{150}\mathrm{Sm}(p,t)$ reaction with 25 MeV protons has been investigated here using the silicon telescope and high-purity germanium array Hyperion. Angular distributions of outgoing tritons and relative intensities of ${\gamma}$ rays from low-lying levels are used to deduce the initial spin distribution using statistical calculations and are compared with a semiclassical model of the $(p,t)$ reaction. Experimental and theoretical results suggest a peak strength near $4{\hbar}$ when gated on outgoing tritons detected in Hyperion, while the full $4{\pi}$ distribution may peak near $2{\hbar}$. Additionally, the average ${\gamma}$-neutron branching ratio is determined from the data with the aid of one of two new codes presented in this work. Finally, the analysis is extended to other recent studies of $^{152,154}\mathrm{Sm}(p,t)$ to form systematics of the spin-dependence of the surrogate method applied to heavy nuclei in the transitional to deformed region.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2019

Nuclear level densities and γ -ray strength functions in samarium isotopes

The γ-strength functions and level densities in the quasicontinuum of 147,149 Sm isotopes have been extracted from particle-γ coincidences using the Oslo method. The nuclei of interest were populated via (p,d) reactions on pure 148,150 Sm targets and the reaction products were recorded by the Hyperion array. An upbend in the low-energy region of the γSF has been observed. The systematic analysis of the γSF for a range of Sm isotopes highlights the interplay between scissors mode and the upbend. In conclusion, shell-model calculations show reasonable agreement with the experimental γSFs and confirm the correspondence between the upbend and scissors mode.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2015

Reactor Fuel Isotopics and Code Validation for Nuclear Applications

Experimentally measured isotopic concentrations of well characterized spent nuclear fuel (SNF) samples have been collected and analyzed by previous researchers. These sets of experimental data have been used extensively to validate the accuracy of depletion code predictions for given sets of burnups, initial enrichments, and varying power histories for different reactor types. The purpose of this report is to present the diversity of data in a concise manner and summarize the current accuracy of depletion modeling. All calculations performed for this report were done using the Oak Ridge Isotope GENeration (ORIGEN) code, an internationally used irradiation and decay code solver within the SCALE comprehensive modeling and simulation code. The diversity of data given in this report includes key actinides, stable fission products, and radioactive fission products. In general, when using the current ENDF/B-VII.0 nuclear data libraries in SCALE, the major actinides are predicted to within 5% of the measured values. Large improvements were seen for several of the curium isotopes when using improved cross section data found in evaluated nuclear data file ENDF/B-VII.0 as compared to ENDF/B-V-based results. The impact of the flux spectrum on the plutonium isotope concentrations as a function of burnup was also shown. The general accuracy noted for the actinide samples for reactor types with burnups greater than 5,000 MWd/MTU was not observed for the low-burnup Hanford B samples. More work is needed in understanding these large discrepancies. The stable neodymium and samarium isotopes were predicted to within a few percent of the measured values. Large improvements were seen in prediction for a few of the samarium isotopes when using the ENDF/B-VII.0 libraries compared to results obtained with ENDF/B-V libraries. Very accurate predictions were obtained for 133 Cs and 153 Eu. However, the predicted values for the stable ruthenium and rhodium isotopes varied as much as 10% of the measured values, and 109 Ag was consistently over-predicted by as much as 170%. In general, there is a larger uncertainty for modeling radioactive fission products when compared to either the actinides or the stable fission products in SNF. The relative C/E ratios ranged from a few percent for 137 Cs up to 60% and 100% for 106 Ru and 125 Sb, respectively. Limited or no radioactive fission products data exist in the current data sets for reactor types other than PWRs and BWRs. More work is needed in obtaining a greater diversity of radioactive fission product data. While performing this survey, issues leading to inconsistencies in nuclear fission yield data were discovered that specifically impacted the fission product noble gases. Emphasis was given to this legacy data, and corrective actions were taken as described in this report. After the fission yield data were corrected, the stable xenon and krypton fission products were predicted to within 5% of their measurements. However, preliminary results not explicitly given in this report indicate that the relative C/E ratio for the radioactive isotope 85 Kr varied as much as 10%. Due to the complex migration and the difficulty in measuring noble gases in the fuel, a more thorough investigation is needed to understand how accurately depletion codes can calculate these gas concentrations.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
NASA NTRS1979

On isotopic anomalies in samarium

The solar isotopic composition of Sm is decomposed into s, r, and p components. The anomaly pattern discovered by Lugmair et al. (1978) in EK1-04 Allende inclusion can be presented as a fractionation of the average s-pattern from the average r-pattern. This representation requires a fractionation of 0.029%/(amu) and either (1) a 0.42% deficiency of s relative to r and a 0.15% deficiency of p relative to r, or (2) a 0.42% excess of r relative to s and a 0.27% excess of p relative to s. The nature of this anomaly suggest a systematic physical fractionation of r, s, and p nuclei from each other in the initial condition leading to EK1-04. A neighboring supernova injection would not be expected to produce this anomaly.

Clayton, D. D.↗
NASA NTRS1989

Rhenium-osmium and samarium-neodymium isotopic systematics of the Stillwater complex

The role of magma mixing in the formation of strategic platinum-group element ore deposits is examined using isotopic data from the Stillwater Complex, Montana. Nd and Os isotopic data show that the intrusion formed from at least two distinct magmas: ultramafic (U-type) affinity magmas and anorthositic (A-type) affinity magmas. The U-type magmas formed from a lithospheric mantle source containing recycled crustal materials and the A-type magmas originated either by crustal contamination of basaltic magmas or by partial melting of basalt in the lower crust. The results also suggest that the platinum-group element ore deposits were derived from A-type magmas which were injected into the U-type magma chamber at several stages during the development of the ultramafic series.

Lambert, David D.↗
NASA NTRS2021

The effects of terrestrial weathering on samarium-neodymium isotopic composition of ordinary chondrites

Following their fall to Earth, meteorites experience weathering. In this systematic study, we evaluate the trace element composition of ordinary chondrites from the Antarctic cold desert, and Atacama (Chile) and Lut (Iran) hot deserts, with an emphasis on rare earth elements (REE). Our data confirms that terrestrial weathering of meteorites in hot deserts changes their trace element (Sr, Ba, REE, Hf, Th, and U) concentrations. However, weathering effects in majority of Antarctic samples are limited to slight Ba, REE, Hf, and Th depletions and in some case to U enrichment. In comparison to the Antarctic meteorites, hot desert samples show greater disturbances and REE fractionation relative to the average fall values. We measured the Sm-Nd isotopic composition of the hot desert meteorites that have heavily affected REE compositions. Our Sm-Nd isotopic data show a significant effect of terrestrial weathering evidenced by non-CHUR (147)Sm/(144)Nd and (143)Nd/(144)Nd ratios. Measurements show a higher variation and lower values of (147)Sm/(144)Nd for the Atacama samples than those from the Lut Desert. Deviations from CHUR (147)Sm/(144)Nd value are in positive accordance with the degree of La/Lu fractionation caused by weathering. The ɛNd values of Atacama and Lut deserts meteorites range from −2.20 to +1.61, which is wider than the −1.07 to +0.64 range for falls. We suggest that disturbance of primary Sm/Nd ratios resulting from mixing with terrestrial components originating from soil during weathering is responsible for lower (147)Sm/(144)Nd ratio in these meteorites. The majority of the Atacama meteorites regardless of their weathering degrees have their REE compositions and ɛNd affected by terrestrial contamination. Both (147)Sm/(144)Nd ratio and ɛNd values show no straightforward relationship with weathering degree. However, in both cases the samples with the highest negative isotopic disturbances are H chondrites from the Atacama and Lut deserts. In addition, Ba concentration shows a negative correlation with (147)Sm/(144)Nd ratio. Care must be taken into account while dealing with samples collected from hot deserts, even fresh-looking ones.

Isotope geochemistry↗
DOE OSTI2015

Absolute photoneutron cross sections of Sm isotopes

Photoneutron cross sections for seven samarium isotopes, {sup 144}Sm, {sup 147}Sm, {sup 148}Sm, {sup 149}Sm, {sup 150}Sm, {sup 152}Sm and {sup 154}Sm, have been investigated near neutron emission threshold using quasimonochromatic laser-Compton scattering γ-rays produced at the synchrotron radiation facility NewSUBARU. The results are important for nuclear astrophysics calculations and also for probing γ-ray strength functions in the vicinity of neutron threshold. Here we describe the neutron detection system and we discuss the related data analysis and the necessary method improvements for adapting the current experimental method to the working parameters of the future Gamma Beam System of Extreme Light Infrastructure - Nuclear Physics facility.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2014

High Specific Activity Sm-153 By Post Irradiation Isotope Separation (Final Scientific Technical Report)

The isotope, samarium-153 ( 153 Sm) has ideal nuclear properties well suited for a variety of therapeutic applications; however, it is only available with low specific activity (radioactivity per unit mass) due to the method of production. Commercially useful quantities can be made by the 152 Sm (n,γ) 153 Sm reaction in a nuclear reactor, but typical irradiation parameters result in less than 2% of the 152 Sm target material being converted, leading to a very diluted end product. Since chemical processing methods cannot be used to perform isotopic separation, this means that >98% of the resultant pharmaceutical molecules are labeled with “cold” target atoms and are incapable of providing any radiation-induced therapeutic effect. The goals of this project were to introduce a new approach to the production of high specific activity (HSA) 153 Sm utilizing electromagnetic isotope separation (EMIS), and to perform biodistribution and chemistry studies with such HSA 153 Sm to test labeling capability with targeting molecules. Included in these studies was the successful development of a collection substrate that would allow the efficient deposit and removal of 153 Sm; to this end, DLC (diamond like carbon) foils were successfully employed. In the first year of this project a surface ion source was developed, leading to the successful production of a mass separated beam of stable Sm ions. Studies were then performed using similar apparatus at the Oak Ridge National Laboratory, leading to a well-separated beam of isotopically pure samarium ions. This was followed by the successful production of four 15 mCi samples (over a 7 month period) of HSA 153 Sm which were delivered to the IsoTherapeutics Group for biodistribution and chemical labeling studies. Such samples were produced by neutron irradiation of 5 mg metal samples of 152 Sm at the HFIR (ORNL High Flux Isotope Reactor), followed by manual transfer of the samples from the irradiation capsule to the chamber of a surface ion source. Isotopic beams were then extracted using the IRIS2 EMIS facility, and collected onto 10 μm thick DLC foils. The samples were irradiated for 10 h periods, with typical collection periods lasting 12 - 16 h. Employing appropriate chemical approaches, these HSA 153 Sm samples were evaluated for labeling with small, medium and large molecules. The ability to label a variety of targeting molecules is important to demonstrate the potential therapeutic capabilities. Biodistribution studies, using HSA 153 Sm with the bone agent DOTMP, in rodents demonstrated that the biodistribution is similar to what is observed with LSA 153 Sm. Labeling was successfully achieved with peptides, and large protein molecules.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2017

Isotopic Ratios of Samarium by TIMS for Nuclear Forensic Application

The isotopic ratio of Nd, Sm, and Gd can provide important information regarding fissile material (nuclear devices, reactors), neutron environment, and device yield. These studies require precise measurement of Sm isotope ratios, by either TIMS or MC-ICP-MS. There has been an increasing trend to measure smaller and smaller quantities of Sm bearing samples. In nuclear forensics 10-100 ng of Sm are needed for precise measurement. To measure sub-ng Sm samples using TIMS for nuclear forensic analysis.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

State densities of heavy nuclei in the static-path plus random-phase approximation

We report that nuclear state densities are important inputs to statistical models of compound-nucleus reactions. State densities are often calculated with self-consistent mean-field approximations that do not include important correlations and must be augmented with empirical collective enhancement factors. Here, we benchmark the static-path plus random-phase approximation (SPA + RPA) to the state density in a chain of samarium isotopes 148–155 Sm against exact results (up to statistical errors) obtained with the shell-model Monte Carlo (SMMC) method. The SPA + RPA method incorporates all static fluctuations beyond the mean field together with small-amplitude quantal fluctuations around each static fluctuation. Using a pairing plus quadrupole interaction, we show that the SPA + RPA state densities agree well with the exact SMMC densities for both the even- and odd-mass isotopes. For the even-mass isotopes, we also compare our results with mean-field state densities calculated with the finite-temperature Hartree-Fock-Bogoliubov (HFB) approximation. We find that the SPA + RPA repairs the deficiencies of the mean-field approximation associated with broken rotational symmetry in deformed nuclei and with the violation of particle-number conservation in the pairing condensate. In particular, in deformed nuclei the SPA + RPA reproduces the rotational enhancement of the state density relative to the mean-field state density.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Low-energy enhancement in the magnetic dipole γ-ray strength functions of heavy nuclei

A low-energy enhancement (LEE), which was observed experimentally in the gamma-ray strength function (γSF) describing the decay of compound nuclei, would have profound effects on r-process nucleosynthesis if it persists in heavy neutron-rich nuclei. The LEE was shown to be a feature of the magnetic dipole (M1) strength function in configuration-interaction shell-model calculations in medium-mass nuclei. However, its existence in heavy open-shell nuclei remains an open question. Here, using a combination of many-body methods, we identify a LEE in the M1 γSFs of heavy samarium nuclei. In particular, we use the static-path plus random-phase approximation (SPA+RPA), which includes static and small-amplitude quantal fluctuations beyond the mean field. Using the SPA+RPA strength as a prior, we apply the maximum-entropy method (MEM) to obtain finite-temperature M1 γSFs from exact imaginary-time response functions calculated with the shell model Monte Carlo (SMMC) method. We find that the slope of the LEE in samarium isotopes is roughly independent of the average initial energy over a wide range below the neutron separation energy. As the neutron number increases, strength transfers to a low-energy excitation, which we interpret as the scissors mode built on top of excited states.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Markov Chain Monte Carlo Predictions of Neutron-rich Lanthanide Properties as a Probe of r -process Dynamics

Lanthanide element signatures are key to understanding many astrophysical observables, from merger kilonova light curves to stellar and solar abundances. To learn about the lanthanide element synthesis that enriched our solar system, we apply the statistical method of Markov Chain Monte Carlo to examine the nuclear masses capable of forming the r-process rare-earth abundance peak. We describe the physical constraints we implement with this statistical approach and demonstrate the use of the parallel chains method to explore the multidimensional parameter space. We apply our procedure to three moderately neutron-rich astrophysical outflows with distinct types of r-process dynamics. We show that the mass solutions found are dependent on outflow conditions and are related to the r-process path. We describe in detail the mechanism behind peak formation in each case. We then compare our mass predictions for neutron-rich neodymium and samarium isotopes to the latest experimental data from the CPT at CARIBU. Here, we find our mass predictions given outflows that undergo an extended (n,γ)⇌(γ,n) equilibrium to be those most compatible with both observational solar abundances and neutron-rich mass measurements.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS1995

Shapes and stability of algebraic nuclear models

A generalization of the procedure to study shapes and stability of algebraic nuclear models introduced by Gilmore is presented. One calculates the expectation value of the Hamiltonian with respect to the coherent states of the algebraic structure of the system. Then equilibrium configurations of the resulting energy surface, which depends in general on state variables and a set of parameters, are classified through the Catastrophe theory. For one- and two-body interactions in the Hamiltonian of the interacting Boson model-1, the critical points are organized through the Cusp catastrophe. As an example, we apply this Separatrix to describe the energy surfaces associated to the Rutenium and Samarium isotopes.

Lopez-Moreno, Enrique↗
DOE OSTI2013

Discovery of samarium, europium, gadolinium, and terbium isotopes

Currently, thirty-four samarium, thirty-four europium, thirty-one gadolinium, and thirty-one terbium isotopes have been observed and the discovery of these isotopes is described here. For each isotope a brief synopsis of the first refereed publication, including the production and identification method, is presented.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2011

{sup 149}Sm(n,{alpha}){sup 146}Nd Cross Sections in the MeV Region

We have measured the {sup 149}Sm(n,{alpha}){sup 146}Nd cross section at 4.5, 5.0, 5.5, 6.0, and 6.5 MeV. Measurements were performed at the 4.5 MV Van de Graaff accelerator of Peking University with monoenergetic neutrons produced via the {sup 2}H(d,n){sup 3}He reaction using a deuterium gas target. Alpha particles were detected with a double-section gridded ionization chamber having two back-to-back {sup 149}Sm{sub 2}O{sub 3} samples attached to the common cathode. Absolute neutron flux was measured using a small {sup 238}U fission chamber and monitored by a BF{sub 3} long counter. These are the first reported cross sections for this reaction at these energies, except at 6.0 eV, where our new data are in good agreement with our earlier result. The present results help to much better constrain the {sup 149}Sm(n,{alpha}){sup 146}Nd cross section in a region where its energy dependence is changing fairly rapidly and there are large differences between evaluated nuclear data libraries.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

New loading method for high precision Sm isotope analysis of nuclear materials using thermal ionization mass spectrometry

This work demonstrates an analytical protocol for high precision Sm isotope analysis by thermal ionization mass spectrometry (TIMS) using a Pt activator. Here, the method permits precise measurements of small aliquots (1–20 ng) of Sm on single Re filament using a modified static-total evaporation technique. This study represents the first attempt to use such protocols for Sm isotope analyses while reducing the loading size of Sm for TIMS. The method could potentially be deployed to study geological, meteorites and lunar samples containing low Sm concentrations, to monitor neutron irradiation exposure based on 149,150 Sm, or to measure Sm isotopic composition in other types of nuclear samples.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗