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At least 415 records · Page 23

Generation of Enrichment-Dependent Thermal Neutron Scattering Data

This work details the generation of enrichment-dependent thermal neutron scattering cross sections for several crucial uranium fuel compounds. The evaluations of the thermal scattering law (TSL) and associated cross sections for uranium dioxide (UO 2 ), uranium carbide (UC), and uranium nitride (UN) were performed using standard ab initio lattice dynamics (AILD) methods. The data for uranium metal was produced using a novel hybrid approach of molecular dynamics combined with lattice dynamics methods. 235 U enrichments of 5%, 10% (LEU+), 19.75% (HALEU), 93% (HEU), and 100% were considered, in addition to natural uranium. The enrichment-dependent masses and free atom cross sections were used in the generation of elastic and inelastic thermal neutron scattering cross sections, while the calculation of the phonon density of states (DOS) and resulting TSL considered only the natural isotopic composition of uranium. The use of an identical DOS for all enrichments is expected to have minimal impact on the final data, as the small change in uranium mass should not significantly affect lattice vibrations. The cross sections are shown to exhibit significant dependence on 235 U enrichment. The submission of this data to the National Nuclear Data Center (NNDC) for release in the ENDF/B-VIII.1 database should support the design of advanced reactor concepts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Automated reactor physics analysis framework of High Flux Isotope Reactor low-enriched uranium silicide dispersion fuel designs

The High Flux Isotope Reactor (HFIR) is a versatile research reactor that provides one of the highest steady-state neutron fluxes of any reactor in the world. The HFIR reactor physics team investigated the conversion of the current 93 wt% highly enriched uranium U 3 O 8 -Al dispersion fuel to a 19.75% low-enriched uranium (LEU) U 3 Si 2 -Al dispersion fuel. The team continuously develops a Python module to streamline the analysis steps required for an LEU core design to ensure reproducible and agile design iteration. The Python module automates the data processing between analysis steps and automates the input perturbation for branch calculations and design changes. The automated framework has proven to significantly increase the efficiency and reproducibility of the reactor physics team to design High Flux Isotope Reactor (HFIR) LEU cores and thoroughly analyze performance metrics, safety metrics, and thermal safety margins. Consequently, the team can now respond rapidly to fuel fabrication engineer and thermal-hydraulic-structural analyst requests. Numerous combinations of LEU fuel designs are explored, of which two LEU fuel designs are presented here in this paper: a low density silicide design, and a high-density silicide design. Results show that both designs meet or exceed safety and performance metrics with exception for minor differences caused by the hardened spectrum from LEU.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

U-238-U-234-Th-230-Th-232 systematics and the precise measurement of time over the past 500,000 years

A method is presented for the high-precision measurement of the Th-230 abundance in corals by isotope-dilution mass spectrometry using techniques developed by Chen and Wasserburg (1980, 1981) and Chen et al. (1986). It is shown that 6 x 10 to the 8th atoms of Th-230 can be measured to + or - 30 percent (2 sigma) and 2 x 10 to the 10th atoms of Th-230 to + or - 2 percent. The time over which useful age data on corals can be obtained ranges from a few years to about 500 ky, with the uncertainty in age ranging from 5 y for a 180-y-old coral, to 44 y for a 8294-y-old coral, to 1.1 ky for a 123.1-ky-old coral. Ages were determined with high analytical precision for several corals that grew during high sea-level stands about 120 ky ago, supporting the view that the dominant cause of Pleistocene climate change was Milankovitch forcing.

Edwards, R. Lawrence↗

Microscopic-macroscopic level densities for low excitation energies

Level density ρ(E,Q) is derived within the micro-macroscopic approximation (MMA) for a system of strongly interacting Fermi particles with the energy E and additional integrals of motion Q , in line with several topics of the universal and fruitful activity of A. S. Davydov. Within the extended Thomas Fermi and semiclassical periodic orbit theory beyond the Fermi-gas saddle-point method, we obtain ρ ∝ I ν (S)/S ν , where I ν (S) is the modified Bessel function of the entropy S . For small shell-structure contribution, one finds ν = κ/2 + 1, where κ is the number of additional integrals of motion. This integer number is a dimension of Q, Q = { N, Z , …} for the case of two-component atomic nuclei, where N and Z are the numbers of neutrons and protons, respectively. For much larger shell structure contributions, one obtains ν = κ /2 + 2. The MMA level density ρ reaches the well-known Fermi gas asymptote for large excitation energies and the finite micro-canonical combinatoric limit for low excitation energies. Further, the additional integrals of motion can also be the projection of the angular momentum of a nuclear system for nuclear rotations of deformed nuclei, number of excitons for collective dynamics, and so on. Fitting the MMA total level density ρ( E , Q) for a set of the integrals of motion Q = { N, Z }, to experimental data on a long nuclear isotope chain for low excitation energies, one obtains the results for the inverse level-density parameter K , which differs significantly from those of neutron resonances due to shell, isotopic asymmetry, and pairing effects.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

As-Built Simulation of the High Flux Isotope Reactor

The Oak Ridge National Laboratory High Flux Isotope Reactor (HFIR) is an 85 MWt flux trap-type research reactor that supports key research missions, including isotope production, materials irradiation, and neutron scattering. The core consists of an inner and an outer fuel element containing 171 and 369 involute-shaped plates, respectively. The thin fuel plates consist of a U 3 O 8 -Al dispersion fuel (highly enriched), an aluminum-based filler, and aluminum cladding. The fuel meat thickness is varied across the width of the involute plate to reduce thermal flux peaks at the radial edges of the fuel elements. Some deviation from the designed fuel meat shaping is allowed during manufacturing. A homogeneity scan of each fuel plate checks for potential anomalies in the fuel distribution by scanning the surface of the plate and comparing the attenuation of the beam to calibration standards. While typical HFIR simulations use homogenized fuel regions, explicit models of the plates were developed under the Low-Enriched Uranium Conversion Program. These explicit models typically include one inner and one outer fuel plate with nominal fuel distributions, and then the plates are duplicated to fill the space of the corresponding fuel element. Therefore, data extracted from these simulations are limited to azimuthally averaged quantities. To determine the reactivity and physics impacts of an as-built outer fuel element and generate azimuthally dependent data in the element, 369 unique fuel plate models were generated and positioned. This model generates the three-dimensional (i.e., radial–axial–azimuthal) plate power profile, where the azimuthal profile is impacted by features within the adjacent control element region and beryllium reflector. For an as-built model of the outer fuel element, plate-specific homogeneity data, 235 U loading, enrichment, and channel thickness measurements were translated into the model, yielding a much more varied azimuthal power profile encompassed by uncertainty factors in analyses. These models were run with the ORNL-TN and Shift Monte Carlo tools, and they contained upwards of 500,000 cells and 100,000 unique tallies.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Factors controlling precision and accuracy in isotope-ratio-monitoring mass spectrometry

The performance of systems in which picomole quantities of sample are mixed with a carrier gas and passed through an isotope-ratio mass spectrometer system was examined experimentally and theoretically. Two different mass spectrometers were used, both having electron-impact ion sources and Faraday cup collector systems. One had an accelerating potential of 10kV and accepted 0.2 mL of He/min, producing, under those conditions, a maximum efficiency of 1 CO2 molecular ion collected per 700 molecules introduced. Comparable figures for the second instrument were 3 kV, 0.5 mL of He/min, and 14000 molecules/ion. Signal pathways were adjusted so that response times were <200 ms. Sample-related ion currents appeared as peaks with widths of 3-30 s. Isotope ratios were determined by comparison to signals produced by standard gases. In spite of rapid variations in signals, observed levels of performance were within a factor of 2 of shot-noise limits. For the 10-kV instrument, sample requirements for standard deviations of 0.1 and 0.5% were 45 and 1.7 pmol, respectively. Comparable requirements for the 3-kV instrument were 900 and 36 pmol. Drifts in instrumental characteristics were adequately neutralized when standards were observed at 20-min intervals. For the 10-kV instrument, computed isotopic compositions were independent of sample size and signal strength over the ranges examined. Nonlinearities of <0.04%/V were observed for the 3-kV system. Procedures for observation and subtraction of background ion currents were examined experimentally and theoretically. For sample/ background ratios varying from >10 to 0.3, precision is expected and observed to decrease approximately 2-fold and to depend only weakly on the precision with which background ion currents have been measured.

NASA Discipline Exobiology↗

Lead in Martian Meteorites-- Observations and Inconsistencies: I. Chassigny

The history of Pb isotope analyses of the martian meteorites (SNC) and their interpretations is laden with difficulties. Two different analytical groups have interpreted their ancient (≥ 4 Ga) shergottite Pb ages as primary [1-5]. A Nakhla age of approximately 4.3 Ga has been interpreted to be primary as well [2]. This is in stark contrast to the young (≤ 1.4 Ga) crystallization ages defined by the Rb-Sr, Sm-Nd, Lu-Hf, and KAr systems [6]. Possibly, a better interpretation for the ancient Pb ages is that they reflect the formation times of the various SNC source regions [7]. A difficulty in dealing with Pb is that terrestrial contamination is ubiquitous, unlike the other chronometer systems noted above. This issue is complicated by the fact that radioactive decay causes localized mineral damage. So washing and leaching to remove Pb contamination tends to remove in situ radiogenic Pb. This issue is further compounded because U and Th are often concentrated in phosphates and other minor phases, so the leaching process tends to remove these, especially phosphates. Another difficulty is that it is not clear whether the observed Pb isotopic variation in leachates, residues, and ion-microprobe analyses is due to terrestrial or to indigenous martian Pb contamination [e.g., 8]. A third difficulty is that the shergottites on the one hand, and the nakhlites and chassignites on the other, appear to have come from separate source regions with different chemical compositions [e.g., 7]. Thus, it is expected that their Pb isotopic characteristics would be different. And even if all these meteorite types came from the same source region, their igneous ages differ considerably. The nakhlites and chassignites are ~1.4 Ga and the shergottites are ≤ 600 Ma [e.g., 6]. This age difference alone should assure that the two distinct SNC groups have differing Pb isotopic signatures.

Jones, J. H.↗

Mini-99 Experiment Design and Target Assembly

Qualification of nuclear fuels requires an understanding of a myriad of fuel performance variables, which requires time-consuming irradiations in test reactors. Accelerating burnup accumulation to reduce the irradiation time has historically been accomplished by increasing the 235 U enrichment in integral fuel tests, which inherently couples the fuel’s temperature and fission heat generation. Separate effects irradiation testing of nuclear fuel, using the MiniFuel target in the Oak Ridge National Laboratory’s (ORNL’s) High Flux Isotope Reactor (HFIR), offers an approach for decoupling fuel temperature and fission rate by reducing the quantity of the fuel and relying primarily on gamma heating in the surrounding components to drive fuel temperatures. However, if the fission rate is high enough, the fuel temperature will still vary over time as the fission heating changes, primarily due to poor heat conduction between the fuel and the surrounding components. This work details the design, analysis, and fabrication of a MiniFuel target which utilizes sodium bonding to improve the heat rejection from the fuel specimen, enabling the testing of higher 235 U enrichments (~8wt.%) to further accelerate burnup accumulation without prohibitively large temperature variations throughout the course of the irradiation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Integrated chronostratigraphy of Proterozoic-Cambrian boundary beds in the western Anabar region, northern Siberia

Carbonate-rich sedimentary rocks of the western Anabar region, northern Siberia, preserve an exceptional record of evolutionary and biogeochemical events near the Proterozoic/Cambrian boundary. Sedimentologically, the boundary succession can be divided into three sequences representing successive episodes of late transgressive to early highstand deposition; four parasequences are recognized in the sequence corresponding lithostratigraphically to the Manykal Formation. Small shelly fossils are abundant and include many taxa that also occur in standard sections of southeastern Siberia. Despite this coincidence of faunal elements, biostratigraphic correlations between the two regions have been controversial because numerous species that first appear at or immediately above the basal Tommotian boundary in southeastern sections have first appearances scattered through more than thirty metres of section in the western Anabar. Carbon- and Sr-isotopic data on petrographically and geochemically screened samples collected at one- to two-metre intervals in a section along the Kotuikan River, favour correlation of the Staraya Reckha Formation and most of the overlying Manykai Formation with sub-Tommotian carbonates in southeastern Siberia. In contrast, isotopic data suggest that the uppermost Manykai Formation and the basal 26 m of the unconformably overlying Medvezhya Formation may have no equivalent in the southeast; they appear to provide a sedimentary and palaeontological record of an evolutionarily significant time interval represented in southeastern Siberia only by the sub-Tommotian unconformity. Correlations with radiometrically dated horizons in the Olenek and Kharaulakh regions of northern Siberia suggest that this interval lasted approximately three to six million years, during which essentially all 'basal Tommotian' small shelly fossils evolved.

Non-NASA Center↗

Sm-Nd dating of Fig Tree clay minerals of the Barberton greenstone belt, South Africa

Sm-Nd isotopic data from carbonate-derived clay minerals of the 3.22-3.25 Ga Fig Tree Group, Barberton greenstone belt, South Africa, form a linear array corresponding to an age of 3102 +/- 64 Ma, making these minerals the oldest dated clays on Earth. The obtained age is 120-160 m.y. younger than the depositional age determined by zircon geochronology. Nd model ages for the clays range from approximately 3.39 to 3.44 Ga and almost cover the age variation of the Barberton greenstone belt rocks, consistent with independent evidence that the clay minerals are derived from material of the belt. The combined isotopic and mineralogical data provide evidence for a cryptic thermal overprint in the sediments of the belt. However, the highest temperature reached by the samples since the time of clay-mineral formation was <300 degrees C, lower than virtually any known early Archean supracrustal sequence.

Non-NASA Center↗

The carbon-isotopic composition of Proterozoic carbonates: Riphean successions from northwestern Siberia (Anabar Massif, Turukhansk Uplift)

Thick carbonate-dominated successions in northwestern Siberia document secular variations in the C-isotopic composition of seawater through Mesoproterozoic and early Neoproterozoic (Early to early Late Riphean) time. Mesoproterozoic dolomites of the Billyakh Group, Anabar Massif, have delta 13C values that fall between 0 and -1.9 permil versus PDB, with values in the upper part of the succession (Yusmastakh Formation) consistently higher than those of the lower (Ust'-Il'ya and Kotuikan formations). Consistent with available biostratigraphic and radiometric data, delta 13C values for Billyakh carbonates compare closely with those characterizing early Mesoproterozoic carbonates (about 1600-1200 Ma) worldwide. In contrast, late Mesoproterozoic to early Neoproterozoic limestones and dolomites in the Turukhansk Uplift exhibit moderate levels of secular variation. Only the lowermost carbonates in the Turukhansk succession (Linok Formation) have delta 13C values that approximate Billyakh values. Higher in the Turukhansk succession, delta 13C values vary from -2.7 to +4.6 permil (with outliers as low as -5.0 permil interpreted as diagentically altered). Again, consistent with paleontological and radiometric data, these values compare well with isotopic values from 1200 to 850 Ma successions elsewhere. Five sections measured in different parts of the Turukhansk basin show nearly identical patterns of variation, confirming that carbonate delta 13C correlates primarily with time and not facies. The Siberian sections illustrate the potential of integrated biostratigraphic and chemostratigraphic data in the intra- and interbasinal correlation of Mesoproterozoic and early Neoproterozoic rocks.

NASA Discipline Exobiology↗

Millimeter-scale variations of stable isotope abundances in carbonates from banded iron-formations in the Hamersley Group of Western Australia

Several diamond drill cores from formations within the Hamersley Group of Western Australia have been studied for evidence of short-range variations in the isotopic compositions of the carbonates. For a set of 32 adjacent microbands analyzed in a specimen from the Marra Mamba Iron Formation, carbon isotope compositions of individual microbands ranged from -2.8 to -19.8 per mil compared to PDB and oxygen isotope compositions ranged from 10.2 to 20.8 per mil compared to SMOW. A pattern of alternating abundances was present, with the average isotopic contrasts between adjacent microbands being 3.0 per mil for carbon and 3.1 per mil for oxygen. Similar results were obtained for a suite of 34 microbands (in four groups) from the Bruno's Band unit of the Mount Sylvia Formation. Difficulties were experienced in preparing samples of single microbands from the Dales Gorge Member of the Brockman Iron Formation, but overall isotopic compositions were in good agreement with values reported by previous authors. Chemical analyses showed that isotopically light carbon and oxygen were correlated with increased concentrations of iron. The preservation of these millimeter-scale variations in isotopic abundances is interpreted as inconsistent with a metamorphic origin for the isotopically light carbon in the BIF carbonates. A biological origin is favored for the correlated variations in 13C and Fe, and it is suggested that the 13C-depleted carbonates may derive either from fermentative metabolism or from anaerobic respiration. A model is presented in which these processes occur near the sediment-water interface and are coupled with an initial oxidative precipitation of the iron.

NASA Program Exobiology↗

Nitrogen metabolism in Lignifying Pinus taeda cell cultures

The primary metabolic fate of phyenylalanine, following its deamination in plants, is conscription of its carbon skeleton for lignin, suberin, flavonoid, and related metabolite formation. Since this accounts for approximately 30-40% of all organic carbon, an effective means of recycling the liberated ammonium ion must be operative. In order to establish how this occurs, the uptake and metabolism of various 15N-labeled precursors (15N-Phe, 15NH4Cl, 15N-Gln, and 15N-Glu) in lignifying Pinus taeda cell cultures was investigated, using a combination of high performance liquid chromatography, 15N NMR, and gas chromatograph-mass spectrometry analyses. It was found that the ammonium ion released during active phenylpropanoid metabolism was not made available for general amino acid/protein synthesis. Rather it was rapidly recycled back to regenerate phenylalanine, thereby providing an effective means of maintaining active phenylpropanoid metabolism with no additional nitrogen requirement. These results strongly suggest that, in lignifying cells, ammonium ion reassimilation is tightly compartmentalized.

NASA Discipline Number 40-50↗

Isotopic and Fuel Lattice Parameter Trends in Extended Enrichment and Higher Burnup LWR Fuel Vol I: PWR fuel

Commercial light water reactor (LWR) operators and fuel vendors in the United States are pursuing changes to nuclear fuel that include extended enrichment (EE) and accident-tolerant fuel (ATF) designs. The term EE (8% > 235 U > 5%) is used in this report to refer to a subset of high assay low-enriched uranium (HALEU) that is considered usable in commercial US LWRs in the near term. ATF features are designed to improve fuel system performance under accident conditions. One goal of EE is to improve fuel cycle economy by enabling fuel to be depleted to higher burnup than the typical current maximum pin burnup limits (62 gigawatt-days per metric ton of uranium [GWd/MTU]). Adoption of EE, ATF, and high burnup (HBU) fuels in the US commercial fleet requires a clear understanding of the effects on core physics parameters and used fuel isotopic content, as well as confidence in the accuracy of computer code predictions over an expanded range of materials, enrichment, and burnup. A thorough understanding of the applicability and adequacy of benchmark data (e.g., criticality, decay heat, isotopic content) for computer code validation is necessary to ensure that appropriate safety margins are maintained. To prepare for and support these potential changes, the effects of EE, ATF, and HBU are being assessed for selected representative LWR fuel designs. The project is divided into phases: this report summarizes the findings of Phase 1, which focuses on the lattice physics parameter and used fuel isotopic changes for a conventional Westinghouse 17×17 pressurized water reactor (PWR) design. The primary investigation tool is the SCALE Polaris code using the SCALE 56-group Evaluated Nuclear Data File (ENDF)/B-VII.1 cross sections. The goal of the current work is to (1) identify and explain important effects of EE and HBU (reactivity, lattice physics, and isotopic effects) assuming that PWR fuel design and usage remain similar to those for current enrichment fuel, (2) provide limited code-to-code comparisons with higher order cross section libraries and/or codes, and (3) identify any apparent anomalous trends in the results for further investigation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Organic sulfur fluxes and geomorphic control of sulfur isotope ratios in rivers

Pyrite oxidation plays a critical role in the relationship between weathering and climate, and its impact on the global carbon cycle has previously been constrained through inversion models utilizing observations of river sulfate ($SO^{2–}_{4}$) and its 34 S/ 32 S isotope ratio (δ 34 S SO4 ). However, measurements from some rivers have suggested that SSO4 can be substantially impacted by processes such as microbial sulfate reduction and/or sulfur assimilation and cycling, rather than simply reflecting a weighted mixture of lithologic sulfur sources. To study the prevalence and controls on $SO^{2–}_{4}$ transformations, in this study we measured dissolved major element concentrations and δ 34 S SO4 in river water samples from throughout western Iceland. Our analyses focused on samples from a small catchment hosting the Efri Haukadalsá river, a system with relatively uniform and isotopically constrained basaltic bedrock. We also measured sediment δ 34 S and sulfur speciation using sulfur K-edge X-ray absorption spectroscopy on sediment and vegetation samples from this catchment. Values of dissolved δ 34 S SO4 in the Efri Haukadalsá ranged from 2.5‰ to 23.7‰ and had a linear relationship with Cl – /$SO^{2–}_{4}$ ratios, indicating that $SO^{2–}_{4}$ predominantly derived from basalt weathering and meteoric precipitation. The lower δ 34 S SO4 values were found in fluvial valleys with V-shaped cross sections, while higher values of δ 34 S SO4 occurred in U-shaped, glacially eroded valleys with thick alluvial fills blanketing the valley floor. Spectroscopic observations identified organic sulfur phases in suspended river sediment, floodplain deposits, and vegetation. Mass balance calculations quantified the organic sulfur flux as less than 10% of $SO^{2–}_{4}$ export, and sediment δ 34 S values were comparable to river δ 34 S SO4 . We interpreted these isotopic and chemical patterns as reflecting differences in the availability of unweathered bedrock across the Efri Haukadalsá catchment, with V-shaped valleys having greater access to fresh sulfide-bearing minerals than alluviated U-shaped valleys; this interpretation is in contrast to one in which the elevated δ 34 S SO4 values reflect fractionation during sulfur transformations along alluvial reaches. These results validated the application of river inversion models for constraining weathering fluxes and affirmed that pyrite oxidation globally, even in the presence of river sulfur cycling, modulates the abundance of atmospheric carbon dioxide.

54 ENVIRONMENTAL SCIENCES↗

Determination of the C-12/C-13 and O-16/O-18 ratio in the Martian atmosphere by 10 micron heterodyne spectroscopy

The planetary atmosphere of Mars was studied during the opposition of May, 1984, by means of a 10-micron heterodyne receiver mounted at the Cassegrain focus of a 3-m telescope. On the basis of a model of the Martian atmosphere, the isotopic ratios derived from the fully resolved absorption spectra obtained were compared with the results of Viking probe in situ measurements and terrestrial values; agreement is obtained within statistical errors. It is shown that highly resolving spectroscopy allows for the determination of isotopic ratios in remote sensing with a precision that is comparable to that of in situ mass spectroscopy.

Schrey, U.↗

Sizing up the sub-Tommotian unconformity in Siberia

Sedimentary rocks in the western Anabar region, northwestern Siberia, preserve an exceptional record of evolution and biogeochemical events near the Proterozoic-Cambrian boundary. Carbon isotopic data on petrographically and geochemically screened samples collected at 1 to 2 m intervals support correlation of the lower Anabar succession (Staraya Reckha and lower Manykai Formations) with sub-Tommotian carbonates of the Ust'-Yu-doma Formation in southeastern Siberia. In contrast, the upper Manykai and most of the overlying Medvezhya Formation appear to preserve a sedimentary and paleontological record of an evolutionary important time interval represented in southeastern Siberia only by the sub-Tommotian unconformity. Correlation of the Anabar section with other northern Siberian successions that contain well-dated volcanic rocks permits the estimate that the sub-Tommotian unconformity in southeastern Siberia spans approximately 3 to 6 m.y. Diverse small shelly fossils (but not archaeocyathans) previously thought to mark the base of the Tommotian Stage evolved sequentially throughout this earlier interval.

NASA Discipline Exobiology↗

Lead isotope systematics of three Apollo 17 mare basalts

The paper deals with new and more accurate determinations of uranium, thorium, and isotopic lead data for five bulk samples and separate pyroxene, ilmenite, and plagioclase from basalt 71055. In a concordia diagram, the samples suggest a postcrystallization disturbance of the U-Pb systems of the rock. There is no compelling reason, from U-Pb data, to believe that the moon is younger than 4.55 AE.

Tilton, G. R.↗