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DOE OSTI2023

Differential charge radii: Proton-neutron interaction effects

The analysis of self-consistency and proton-neutron interaction effects in the buildup of differential charge radii were carried out in covariant density functional theoretical calculations without pairing interaction on the example of selected configurations in the Pb isotopes. The proton-neutron interaction of neutron(s) added to the neutron 𝑁 = 126 core and the protons forming the 𝑍 = 82 proton core is responsible for a major contribution to the buildup of differential charge radii. It depends on the products of proton and neutron wave functions and thus on their nodal structure. This interaction leads to a redistribution of single-particle density of occupied proton states which in turn modifies the charge radii. Furthermore, the microscopic origin of this redistribution and its consequences for differential charge radii were investigated for the first time. Self-consistency effects affecting the shape of proton potential, total proton densities and the energies of the single-particle proton states provide only minor contribution to differential charge radii.

190 ≤ A ≤ 219↗

NASA NTRS2017

Shergottite Lead Isotope Signature in Chassigny and the Nakhlites

The nakhlites/chassignites and the shergottites represent two differing suites of basaltic martian meteorites. The shergottites have ages less than or equal to 0.6 Ga and a large range of initial Sr-/Sr-86 and epsilon (Nd-143) ratios. Conversely, the nakhlites and chassignites cluster at 1.3-1.4 Ga and have a limited range of initial Sr-87/Sr-86 and epsilon (Nd-143). More importantly, the shergottites have epsilon (W-182) less than 1, whereas the nakhlites and chassignites have epsilon (W-182) approximately 3. This latter observation precludes the extraction of both meteorite groups from a single source region. However, recent Pb isotopic analyses indicate that there may have been interaction between shergottite and nakhlite/chassignite Pb reservoirs.Pb Analyses of Chassigny: Two different studies haveinvestigated 207Pb/204Pb vs. 206Pb/204Pb in Chassigny: (i)TIMS bulk-rock analyses of successive leaches and theirresidue [3]; and (ii) SIMS analysis of individual minerals[4]. The bulk-rock analyses fall along a regression of SIMSplagioclase analyses that define an errorchron that is olderthan the Solar System (4.61±0.1 Ga); i.e., these define amixing line between Chassigny’s principal Pb isotopic components(Fig. 1). Augites and olivines in Chassingy (notshown) also fall along or near the plagioclase regression [4].This agreement indicates that the whole-rock leachateslikely measure indigenous, martian Pb, not terrestrial contamination[5]. SIMS analyses of K-spars and sulfides definea separate, sub-parallel trend having higher 207Pb/206Pbvalues ([4]; Fig. 1). The good agreement between the bulkrockanalyses and the SIMS analyses of plagioclases alsoindicates that the Pb in the K-spars and sulfides cannot be amajor component of Chassigny.The depleted reservoir sampled by Chassigny plagioclaseis not the same as the solar system initial (PAT) andrequires a multi-stage origin. Here we show a two-stagemodel (Fig. 1) with a 238U/204Pb (μ) of 0.5 for 4.5-2.4 Gaand a μ of 7 for 2.4-1.4 Ga. This is not a unique model butdoes produce a Pb composition that falls on the plagioclaseregression at 1.4 Ga, the approximate igneous age of Chassigny [1]. It should be noted that low-μ single-stage modelsare not capable of producing sufficiently radiogenic 206Pb/204Pb at 1.4 Ga.Relation to Shergottites: The Chassigny K-spars and sulfides fall along a second mixing line defined by leachesand residues of depleted and intermediate shergottites [6]. This mixing line falls above the plagioclase regression.Therefore, we also interpret the radiogenic component of this mixing line to represent indigenous martian Pb. It ispossible that the depleted and intermediate shergottites and the Chassigny plagioclases sample radiogenic Pb from thethe same source, i.e., the mixing lines may intersect at high 206Pb/204Pb.Both K-spar and sulfide are late-stage phases. At the time of their crystallization, the Chassigny system appearsto have remained open to a depleted shergottite Pb reservoir. The depleted component of the shergottite mixing linecan be generated by a single-stage evolution from PAT (4.5 to 1.4 Ga) in a reservoir having a μ ~2. A similar modelfor the most depleted shergottites is also possible: μ = 1.5 for 4.5 to 0.3 Ga.Nakhlites: Nakhlite analyses plot between the shergottite and Chassigny plagioclase regressions [3]. So again,members of the nakhlite/chassignite suite show affinities to shergottite Pb.

Jones, J. H.↗

NASA NTRS1981

The isotopic composition of uranium and lead in Allende inclusions and meteoritic phosphates

The isotopic compositions of uranium and lead in Ca-Al-rich inclusions from the Allende chondrite and in whitlockite from the St. Severin chondrite and the Angra dos Reis achondrite are reported. Isoptopic analysis of acid soluble fractions of the Allende inclusions and the meteoritic whitlockite, which show isotopic anomalies in other elements, reveals U-235/U-238 ratios from 1/137.6 to 1/138.3, within 20 per mil of normal terrestrial U abundances. The Pb isotopic compositions of five coarse-grained Allende inclusions give a mean Pb-207/Pb-206 model age of 4.559 + or - 0.015 AE, in agreement with the U results. Pb isotope ratios of two fine-grained inclusions and a coarse-grained inclusion with strong mass fractionation and some nonlinear isotopic anomalies indicate that the U-Pb systems of these inclusions have evolved differently from the rest of Allende. Th/U abundance ratios in the Allende inclusions and meteoritic phosphate are found to range from 3.8 to 96, presumably indicating an optimal case for Cm/U fractionation, although the normal U concentrations do not support claims of abundant live Cm-247 or Cm-247/U-238 fractionation at the time of meteorite formation, in contrast to previous results. A limiting Cm-247/U-235 ratio of 0.004 at the time of meteorite formation is calculated which implies that the last major r process contribution at the protosolar nebula was approximately 100 million years prior to Al-26 formation and injection.

Chen, J. H.↗

NASA NTRS1975

The source of sublimates on the Apollo 15 green and Apollo 17 orange glass samples

Elemental analyses of the thin film of micromounds which coat the surfaces of Apollo 15 green glass and Apollo 17 orange glass are reported. It is thought that Zn, Ga, Pb, Cu, Tl, S, F, and Cl condensed as a sublimate on the outside surface of these glass particles in lava fountains about 3.4 and 3.6 b.y. ago (Apollos 15 and 17, respectively). The heavy metals enriched in these samples may have been mobilized in a halide- and sulfide-rich vapor, while the source of these elements and of the glass may be a sulfide- and halide-rich pyroxenite inside the moon. The isotopic composition of lead on the surface of individual particles was determined, and the composition is considered with respect to the evolution of the source region. The lead on the surfaces is similar to lead that has been mixed into other soils and breccias at nearby sites.

Meyer, C., Jr.↗

NASA NTRS1986

Speculations on nature and extent of Archean basement in Labrador as indicated by SR, ND and PB isotopic systematics of proterozoic intrusives

The Sm-Nd and Rb-Sr isotopic compositions of mid to late Proterozoic (approximately 1.6 to 1.1 Ga) massif-type anorthosites and mafic intrusives in the eastern Canadian shield are correlated with geographic location. Complexes in the Grenville province have positive epsilon sub Nd values and initial Sr-87/Sr-86 (I sub Sr) generally less than 0.703, suggesting derivation from depleted mantle. In Labrador, similar complexes close to or northwest of a line roughly corresponding to the Grenville Front have negative epsilon sub Nd values and I sub Sr 0.703. This contrast was intrepreted as reflecting either enriched mantle under the Nain Province, or contamination of the Nain intrusives with older crustal components. Lead isotopic compositions, however, favor the latter. The possibility of using these Proterozoic intrusives as tracers to characterize the nature and extent of older basement types in Labrador is discussed.

Ashwal, L. D.↗

DOE OSTI2023

Bioinspired stability enhancement in deuterium-substituted organic–inorganic hybrid perovskite solar cells

Abstract In hybrid perovskite solar cells (PSCs), the reaction of hydrogens (H) located in the amino group of the organic A-site cations with their neighboring halides plays a central role in degradation. Inspired by the retarded biological activities of cells in heavy water, we replaced the light H atom with its abundant, twice-as-heavy, nonradioactive isotope, deuterium (D) to hamper the motion of H. This D substitution retarded the formation kinetics of the detrimental H halides in Pb-based PSCs, as well as the H bond-mediated oxidation of Sn2+ in Sn–Pb-based narrow-bandgap PSCs, evidenced by accelerated stability studies. A computational study indicated that the zero point energy of D-based formamidinium (FA) is lower than that of pristine FA. In addition, the smaller increase in entropy in D-based FA than in pristine FA accounts for the increased formation free energy of the Sn2+ vacancies, which leads to the retarded oxidation kinetics of Sn2+. In this study, we show that substituting active H with D in organic cations is an effective way to enhance the stability of PSCs without sacrificing photovoltaic (PV) performance. This approach is also adaptable to other stabilizing methods.

14 SOLAR ENERGY↗

DOE OSTI2022

A refined assessment of nuclear data target accuracy requirements for ALFRED

The interest in target accuracy assessment has been recently renewed within the OECD/NEA Working Party on International Nuclear Data Evaluation Cooperation with an update exercise, thanks to the invaluable initiative of Massimo Salvatores. This work, moving from evaluations on the main core integral parameters of the Advanced Lead-cooled Fast Reactor European Demonstrator (ALFRED), and the identification of the associated target accuracies needed for improving its design, approaches the retrieval of target accuracy requirements for nuclear data, as the inverse problem of uncertainty quantification. The preliminary results obtained in a previous work are here refined by explicitly taking into account the total contribution due to correlations among variables in the optimization constraint, while its various components are evaluated individually. Moreover, three different sets of cost parameters are considered to introduce a bias in the solution in order to take in due account the relative difficulties in the execution of new differential experiments as needed for achieving the proposed target accuracies. By this, the obtained results are deemed usefully informative, and proposed for the update of a High Priority List which identifies the isotopes-reaction couples of most interest for future refinement experiments, especially when integrated with further analogous information collected on other advanced nuclear systems. Among the cross-sections whose refinement contributes the most to the reduction of the multiplication factor, the fission of Pu{sup 239} was found, which needs to be fixed below 1% in the range of interest for ALFRED (2 keV-4 MeV). Another contribution for the amelioration of the multiplication factor calculation accuracy, is due to the capture channel of Pu{sup 239}, for which the initial high uncertainty (around 15%) can be significantly reduced resorting to easily practicable experiments. The same occurs for the inelastic of Pb{sup 207}, for which the initial uncertainty value of around 50% can be drastically reduced up to target values between 4% and 7%.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

NASA NTRS2015

Lead Isotope Compositions of Acid Residues from Olivine-Phyric Shergottite Tissint: Implications for Heterogeneous Shergottite Source Reservoirs

Geochemical studies of shergottites suggest that their parental magmas reflect mixtures between at least two distinct geochemical source reservoirs, producing correlations between radiogenic isotope compositions and trace element abundances. These correlations have been interpreted as indicating the presence of a reduced, incompatible element- depleted reservoir and an oxidized, incompatible- element-enriched reservoir. The former is clearly a depleted mantle source, but there is ongoing debate regarding the origin of the enriched reservoir. Two contrasting models have been proposed regarding the location and mixing process of the two geochemical source reservoirs: (1) assimilation of oxidized crust by mantle derived, reduced magmas, or (2) mixing of two distinct mantle reservoirs during melting. The former requires the ancient Martian crust to be the enriched source (crustal assimilation), whereas the latter requires isolation of a long-lived enriched mantle domain that probably originated from residual melts formed during solidification of a magma ocean (heterogeneous mantle model). This study conducts Pb isotope and trace element concentration analyses of sequential acid-leaching fractions (leachates and the final residues) from the geochemically depleted olivine-phyric shergottite Tissint. The results suggest that the Tissint magma is not isotopically uniform and sampled at least two geochemical source reservoirs, implying that either crustal assimilation or magma mixing would have played a role in the Tissint petrogenesis.

Moriwaki, R.↗

DOE OSTI2024

NSUF BOILER Pre-Irradiation Characterization and High Flux Isotope Reactor Experiment Design

Alumina-forming austenitic (AFA) stainless steels have emerged as a candidate alloy because of their high-temperature strength, formability, cost, and compatibility with primary coolants for lead-cooled fast reactors (LFRs). This class of steels has exceptional high-temperature oxidation performance; however, a high concentration of Ni is required to stabilize the austenite phase and to provide sufficient creep strength. AFA stainless steels are also susceptible to liquid metal embrittlement (LME). Additionally, under neutron irradiation, Ni will enrich at grain boundaries due to radiation-induced segregation (RIS). Nickel RIS can increase the LME under these coupled effects. Oak Ridge National Laboratory (ORNL) and the NSUF program have leveraged its High Flux Isotope Reactor (HFIR) and experience with complex irradiation experiments to design experiment capsules that test the aforementioned coupled effects. These capsules are designed for insertion in the central flux trap, the highest flux region, of HFIR. The experiment capsules will be filled with Pb, designed to passively melt from the gamma heating in HFIR. The specimens were fabricated into miniature tensile specimens from two different alloys, GA05-25Ni and GA05-20Ni, varying Ni concentrations. The experiment capsules are designed to achieve target temperatures of 400 °C and 650 °C with accumulated dosage of 3 dpa. This report documents the specimen alloy characterization, experimental design, and expected performance of the capsules.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

NASA NTRS1972

U-Th-Pb systematics in three Apollo 14 basalts and the problem of initial Pb in lunar rocks.

The isotopic composition of Pb and the elemental concentration of U, Th and Pb were measured on 'total' rock samples 14053, 14073 and 14310 and on mineral separates of 14310 and 14053. These are the first Pb-U isochrons obtained for lunar basalts and indicate a reasonable solution to the previous discrepancy between the different methods of 'absolute' age determination. The resulting U-Pb isochron ages are compatible with the Rb-Sr and K-Ar ages on the same rocks. However, it is not possible to establish a precise time of 'crystallization' from the Pb-U data because of the small angle of intersection between the linear arrays and the concordia curve. These data show that total rock model ages do not in general yield crystallization ages. The data on 14310 and 14053 show that these rocks were formed containing a highly radiogenic initial lead which accounts for the excessively high total rock model ages by the U-Th-Pb method. The data prove that at the time of extrusion of some basalts, unsupported lead with extremely high Pb-207/Pb-206 ratios was added to the lunar surface.

Tera, F.↗

DOE OSTI2022

Preparation & shipping of ten neutron irradiated Eurofer97 steel variants to HFIR for SANS experiments

At ORNL, ten variants of Eurofer97 steel were irradiated in the high flux isotope reactor (HFIR) to ~2.94 – 3.24 dpa at 300 ± 30 °C, as part of the EUROfusion Lot-IV collaboration. The irradiations were performed in non-instrumented rabbit capsules in the flux trap region, which included SS-J3 type tensile samples and M4-CVN multi-notch bend bars. Their full set of microstructure and mechanical properties were previously reported in multiple previous publications. In this project, half-broken irradiated and nonirradiated SS-J3 tensile samples from ten alloys, code-named H, I, J, K, L, M, N, O, P and E, were prepared and shipped for facilitating small angle neutron scattering (SANS) experiments at the HFIR general purpose (GP)-SANS beam line. This report summarizes the completed tasks which included canister moves at the Irradiated Materials Examination and Testing (IMET) hot-cell facility to retrieve the samples from long-term storage, loading of the ten irradiated samples at IMET inside lead (Pb) piglets that were specifically provided by ORNL for SANS experiments and radiological shipment from IMET facility to the HFIR hot cells for performing SANS experiments. In addition to the irradiated samples, ten nonirradiated half-broken pieces from the Eurofer97 variants were also provided to HFIR for SANS.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Deformation and Collectivity in Doubly Magic 208 Pb

Lead-208 is the heaviest known doubly magic nucleus and its structure is therefore of special interest. Despite this magicity, which acts to provide a strong restorative force toward sphericity, it is known to exhibit both strong octupole correlations and some of the strongest quadrupole collectivity observed in doubly magic systems. In this Letter, we employ state-of-the-art experimental equipment to conclusively demonstrate, through four Coulomb-excitation measurements, the presence of a large, negative, spectroscopic quadrupole moment for both the vibrational octupole 3$^{−}_{1}$ and quadrupole 2$^{+}_{1}$ state, indicative of a preference for prolate deformation of the states. The observed quadrupole moment is discussed in the context of the expected splitting of the 3 − ⊗3 − two-phonon states, due to the coupling of the quadrupole and octupole motion. These results are compared with theoretical values from three different methods, which are unable to reproduce both the sign and magnitude of this deformation. Thus, in spite of its well-studied nature, 208 Pb remains a puzzle for our understanding of nuclear structure.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗