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At least 109 records · Page 6

Space-dependent calculation of the multiplicity moments for shells

In earlier work, we extended the methodology of multiplicity counting in nuclear safeguards, by elaborating the one-speed stochastic transport theory of the calculation of the so-called multiplicity moments, i.e. the factorial moments of the number of neutrons emitted from a fissile item, following a source event from an internal neutron source (spontaneous fission and (α, n) reactions). Calculations were made for spheres and cylinders of various shapes. In all our work so far, the material of the items was homogeneous, and the distribution of the internal source was assumed to be uniformly distributed within the item, with the neutron emission assumed to be isotropic. In the present work the calculations are extended to the case of a point source inside either a solid sphere or in a spherical shell. This necessitates the extension of the theory to non-homogeneous items and non-uniform and non-isotropic sources. This work describes the extension of the theory and provides some quantitative results. (authors)

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

SSA Monte Carlo and Master Equation Modeling of Neutron Leakage Distributions

Strongly stochastic neutron populations in highly subcritical multiplying media containing weak spontaneous fission sources are unique indicators of the presence of SNM. For instance, in neutron multiplicity counting, an extended tail in the count number probability distribution is observed that is a characteristic of and sensitive to the amount of SNM present. Theoretical modeling and efficient computation of stochastic neutron distributions are complementary to experimental measurements and moreover shed light on the fundamental interactions and transport processes that underlie nuclear signatures. Modeling approaches that are intermediate between gross-system level models and high-fidelity but computationally demanding Monte Carlo simulations are of particular interest in this regard. Furthermore we present three advances on existing work in point kinetic or lumped geometry: (i) implementation of the Stochastic Simulation Algorithm (SSA), a system state-updating Monte Carlo method that is more e cient than single-event Monte Carlo in lumped geometries, (ii) application of the backward Master equation to obtain time-gated count moments, and (iii) reconstructing the count number distribution from the deterministically computed moments using a generalized Laguerre polynomial expansion.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Understanding Materials Characteristics of Palladium Lanthanide Cermet Wires as a Mimic of Californium Wire Production

Californium-252 (Cf-252) has been synthesized on a large scale (mg) since the 1970s for use as a portable neutron source. With a half-life of 2.645 years and a spontaneous fission fraction of 3.09%, Cf-252 emits 2.31 × 10 12 neutrons/gram second. Today most of the Cf-252 produced in the world is made at Oak Ridge National Laboratory (ORNL) using the High Flux Isotope Reactor (HFIR) and the Radiochemical Engineering Development Center (REDC). Because of its highly radioactive nature, all manipulations of Cf-252 need to be performed in hot cell facilities by highly trained personnel. The Cf-252 produced at ORNL is done at the REDC, which is conveniently located next to the HFIR. Cf-252 is sold as bulk wire, which has been described as palladium (Pd) metal incasing californium oxide (Cf 2 O 3 ). The process was developed by Mosley et al. at Savannah River Laboratory (SRL) where it was modeled after the thorium work done by Fuschillo et al. This process has been used since the 1970s to synthesize this unique wire, but its fundamental chemistry and materials characteristics were never openly reported. Here we aim to better understand the chemistry and the materials characteristics of Cf-252 wire production for process improvements and to better our fundamental understanding of the mid-late actinides. Though there are many challenges in working with radioactive elements such as Cf, the isotope Cf-252 is even more complicated due to its neutron emission. One challenge with neutron emission is the ability of neutrons to penetrate much deeper through materials, causing radiation damage. This makes using instrumentation to characterize the chemistry and materials properties of this process difficult. For this reason, this study will first focus on terbium (Tb) as a surrogate for Cf. Currently Tb is used as a carrier or filler in Cf production when small amounts of Cf are being processed. This, along with their similar size and charge, makes Tb a reasonable surrogate for this study.

36 MATERIALS SCIENCE↗

Total Measurement Uncertainty in Neutron Coincidence Multiplicity Analysis

Neutron multiplicity counting is the most commonly used nondestructive assay technique for determining the plutonium mass within containers of scrap PuO 2 or mixed oxide (MOX). In multiplicity analysis, the 240 Pu eff mass, leakage multiplication, and alpha ratio (the ratio of [α, n]-to-spontaneous fission neutron production) are the three primary unknown sample properties. They must be determined simultaneously. To solve for these three unknowns in a multiplicity assay, three measured values are needed: the singles, doubles, and triples neutron count rates. While the analysis is limited to solving for three unknowns, there are many additional factors that impact the observed count rates and contribute to the measurement uncertainty. In this study we investigate the various uncertainty contributors for the multiplicity analysis through a combination of traditional uncertainty propagation techniques supplemented by Monte Carlo simulations to address the dependences not explicitly expressed by the point source model. Uncertainties arising from counting statistics, calibration parameters, calibration method, nuclear data, and various material characteristics (isotopic abundances, chemical form, density, and impurities) are considered. A Total Measurement Uncertainty (TMU) estimate is then developed from these uncertainty contributors. This study is confined to multiplicity analysis of items commonly encountered in international safeguards applications. That is, the study focused on Pu oxides and MOX materials for the masses ranging up to 4000 grams total Pu. Multiplicity measurements were simulated using MCNP V6 based on the Plutonium Scrap Multiplicity Counter (PSMC), Epithermal Multiplicity Counter (ENMC), Pyrochemical Multiplicity Counter, and Large Epithermal Multiplicity Counter (LEMC) for this study; however, this report focuses on the parameterization of the uncertainties for the PSMC. The performance differences between the PSMC and the other multiplicity counting systems are relatively small, primarily manifesting in the impact on measurement precision so that the evaluation developed for the PSMC can be applied to the other multiplicity counting systems. Finally an analysis tool, the Multiplicity TMU Estimator, was developed from this study to serve as an aid for evaluation of the total measurement uncertainty of multiplicity assay results obtained from the commonly used INCC acquisition and analysis software.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Delayed Critical and Subcritical Experiments with Polyethylene Moderated Unreflected Thin 15 in. Diameter HEU Metal Plates

The thin ~15 in. diameter highly enriched uranium (HEU) metal plates were assembled to delayed criticality at the Oak Ridge Critical Experiments Facility (ORCEF) in 1969 with various thicknesses of polyethylene (varying from 1/16 to 2$\frac{3}{8}$ inches) between uranium metal plates. The average 235 U enrichment was 93.27 wt. %. These unreflected critical configurations contained 4$\frac{2}{3}$ to 20$\frac{5}{6}$ thin 15 in. diameter HEU metal plates (on loan from Los Alamos National Laboratory [LANL] and shipped to Oak Ridge National Laboratory [ORNL] on June 3, 1969). Depending on the thickness of polyethylene, the enriched uranium masses varying from 28,053 to 135,148 grams. Fractional plate sections consisted of the appropriate number of 60° pie sections. In addition to the measurement at delayed criticality, subcritical measurements were also performed by the inverse kinetic rod drop method. Prompt neutron decay constant measurements were also performed by the Rossi alpha and randomly pulsed neutron method using a time-tagged spontaneous fission californium neutron source; these are briefly reported here. At the time of these measurements in 1969, the thin HEU metal plates were in near-pristine condition with extremely little oxidation, allowing better descriptions of the uranium plates than the use of these plates in a heavily oxidized and deteriorated condition in recent reflected benchmark experiments at the LANL facility at the Nevada Test Site with these same thin highly enriched uranium metal plates. This report documents the experimental information for the measurements performed so that later researchers can perform the required uncertainty and calculational analyses and documentation to use these data for an International Nuclear Criticality Safety Benchmark Evaluation Program (ICSBEP) or a Nuclear Energy Agency (NEA) benchmark. Data from the experiments described should be acceptable for use as criticality safety benchmark experiments for the ICSBEP and the NEA nuclear criticality safety benchmark program once the uncertainty analysis on the measured neutron multiplication factors is completed. Additional data—such as the dimensional inspection reports, uranium isotopic information, and other relevant particulars—should be retrieved from the Y-12 Plant or LANL and incorporated in the final ICSBEP benchmark. Based on previous ICSBEP benchmarks with this enriched uranium metal at ORCEF, the uncertainties in $k_{eff}$ could be as low as ± 0.0002 for some configurations. Other experiments with smaller-diameter than 15 in. diameter HEU metal plates have been benchmarked in HEU-METFAST-001. The prompt neutron time decay measurements could be the basis for an International Reactor Physics Benchmark Program. Preparation of the present report is part of an effort at ORNL to document more than 15 undocumented critical and subcritical experiments enumerated in ORNL/TM-2019/18 and performed by ORNL at ORCEF and other US Department of Energy critical experiments facilities using more than 500 operational days of critical facility time. This work for this report publication was supported by the Nuclear Criticality, Radiation Transport and Safety NCSP Program at ORNL.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Alpha Decay Chains as Thermal Power Sources: Analysis and Applications for RTGs

Radioactive sources can provide power in remote and environmentally harsh locations such as the arctic or space. The generators powered by such sources are rugged and can withstand extreme temperatures, lack of sunlight, and require no human intervention for multiple years. Radioisotopes are used in thermoelectric generators to provide power at remote sites and deep in space. Isotopes like Pu-238, Cm-244, and Am-241 are used in these generators by NASA for power in space probes and spacecrafts. These power sources deliver a steady supply of energy over extended periods of time. Alpha particles created during decay do not travel far in a material. Their kinetic energy is transferred to heat that we can then convert into energy. Unlike beta and gamma decay, the slower-moving alpha particles stop in the material, making their energy available for use. Energy from these natural decay processes provides a reliable source of power. Spontaneous fission is rare and unreliable, and unlike induced fission processes, alpha decay occurs naturally and does not require external management or ignition. The ideal properties of an isotope for use as a power source depend upon the intended use. For use in an Arctic research base over a period of several years, but less than a decade, an isotope that provides high power output over a shorter lifespan may be the most suitable option. Whereas, for deep space missions where a consistent power source for decades or perhaps more than 100 years is needed that would require a very different isotope. One with a much longer half-life that would provide consistent power throughout that time and survive in that state in for these extended periods of time. These examples represent two extreme sides in terms of time frames. By analyzing the power produced by different radioactive decay processes over time, we can evaluate the suitability of various isotope decay chains for specific uses. Some unstable isotopes undergo a series of radioactive decays, transforming into different isotopes at each step and resulting in a stable isotope. The lists of isotopes in these decay processes are known as decay chains. Some of these chains, illustrated in the figures below, are currently being investigated for use in radioisotope thermoelectric generators (RTGs) designed for a range of operational durations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The particle track record of the lunar surface.

Information about lunar surface history revealed by fossil particle tracks is summarized. Such tracks are the result of damage left in dielectric materials by highly ionizing charged particles including heavy solar and galactic cosmic ray nuclei, heavy nuclei recoiling from cosmic ray induced spallation reactions, and induced- and spontaneous-fission fragments. From the distribution of cosmic ray and spallation tracks in the lunar rock, surface residence times of 1 to 30 million years and rock erosion rates of 1 to 10 A/yr have been determined. Particle tracks also record surface orientation and depth history of the rocks and contain information about ancient solar activity.

Comstock, G. M.↗

Extinct lunar radio activities - Xenon from Pu-244 and I-129 in Apollo 14 breccias.

Two Apollo 14 breccias have been found to contain xenon from the spontaneous fission of 82 my Pu-244. A third contains 60 times as much fission xenon as local uranium can account for and is probably of similar character. One of the breccias shows a Xe-129 excess most likely due to the decay of 17 my I-129. That these components can be separated and identified at all implies that complete isotopic homogenization has not occurred over a period which encompasses both extinction of these radionuclides and compaction of the breccias into their final form. In this sense isotope pre-history has been preserved in some lunar breccias providing information that pre-dates the formation of the rock itself (as determined by conventional techniques).

Behrmann, C. J.↗

Irradiation history and accretionary processes in lunar and meteoritic breccias

Particle track studies reveal an abundant record of fossil solar flare tracks in breccia components. Metamorphic events govern the degree to which this record is preserved, and studies of phases with different track retentivities allow limits to be placed on temperatures reached during a rock's history. The least affected breccias have never experienced temperatures as great as 300 C. Two breccias which contain xenon from spontaneous fission of Pu-244 (14301 and 14318) and Xe-129 (14301 only) have never been heated above about 700 C. This and evidence for a surface irradiation of some of the breccia components support a surface implantation model for the origin of the xenon in these breccias. Green glass spheres in 15086 have not been heated above about 300 C during or after breccia formation yet have retained fission tracks for less than 0.7 G.y. Argon ages of about 3.5 G.y. for similar green glass are at least five times as great and may indicate that the glass was not completely outgassed at is formation.

Macdougall, D.↗

Host phase of a strange xenon component in Allende

A description is presented for the isolation and characterization of the host phase from the Allende C3V chondrite and a mass spectrometric study of the five noble gases in this phase. It is though that the Xe component may have been produced by spontaneous fission of an extinct superheavy element. The fission Xe resides in a minor fraction comprising 0.5% of the meteorite. The fraction consists of chromite, an unknown Cr, Fe-mineral, and amorphous carbon. The gas components and the progenitor of the fission Xe may have been trapped in these minerals when they formed from the solar nebula.

Lewis, R. S.↗

Extinct superheavy element in the Allende meteorite

Radiochemical neutron activation analysis of seven Allende samples for 26 trace elements were conducted. In addition, Cr and Fe were studied with the aid of instrumental neutron activation analysis. The investigation had the objective to identify the extinct superheavy element which was present in meteorites and decayed to Xe isotopes by spontaneous fission. The superheavy element was found to reside mainly in a rare mineral (probably a Fe, Ni, Cr, Al-sulfide), comprising only 0.04% of the meteorite. It is pointed out that of the nine volatile superheavy elements 111 to 119, only 115, 114, and 113 are expected to condense as sulfides in the temperature interval between 400 and 500 K corresponding to mineral formation conditions in the solar nebula.

Anders, E.↗

He, Xe and Ne isotopes in a steady-state mass transport model and implications about terrestrial volatiles

We present a model of the steady-state transport assuming three reservoirs: a lower mantle (P) with a relatively undepleted inventory of U, Th, Pu, I, He, Ne, Xe, Ar; an upper mantle that has been extensively outgassed (D); and the atmosphere. There is mass transport at a rate M(sub PD) by plumes from the lower mantle, a fraction of which is outgassed directly into the atmosphere, while the remainder feeds matter and associated nuclei into D. D is well outgassed at spreading centers and has material containing atmospheric gases added to it by subduction. In the case of He, there is no subduction component. The approach follows the treatment of Kellogg and Wasserburg. A summary of the pertinent equations and constraints was reported earlier. The U, Th and Pu in P are estimated for Earth models from refractory element abundances in meteorites. In this model the inventory of rare gases in D is governed by the simple mixing of components from P (both radiogenic and original) with distinctive atmospheric components. In addition, alpha decay and spontaneous fission of U, and (alpha, n) reaction on oxygen from energetic alpha particles produce radiogenic/nuclear daughter products in D. These include (4)He, (136)Xe and (21)Ne. (40)K in D generates excess radiogenic (40)Ar.

Wasserburg, G. J.↗

Lunar and Planetary Science XXXV: Meteorites

The session "Meteorites" included the following reports:Description of a New Stony Meteorite Find from Bulloch County, Georgia; Meteorite Ablation Derived from Cosmic Ray Track Data Dhofar 732: A Mg-rich Orthopyroxenitic Achondrite Halogens, Carbon and Sulfur in the Tagish Lake Meteorite: Implications for Classification and Terrestrial Alteration; Electromagnetic Scrape of Meteorites and Probably Columbia Tiles; Pre-Atmospheric Sizes and Orbits of Several Chondrites; Research of Shock-Thermal History of the Enstatite Chondrites by Track, Thermoluminescence and Neutron-Activation (NAA) Methods; Radiation and Shock-thermal History of the Kaidun CR2 Chondrite Glass Inclusions; On the Problem of Search for Super-Heavy Element Traces in the Meteorites: Probability of Their Discovery by Three-Prong Tracks due to Nuclear Spontaneous Fission Trace Element Abundances in Separated Phases of Pesyanoe, Enstatite Achondrite; Evaluation of Cooling Rate Calculated by Diffusional Modification of Chemical Zoning: Different Initial Profiles for Diffusion Calculation; Mineralogical Features and REE Distribution in Ortho- and Clinopyroxenes of the HaH 317 Enstatite Chondrite Dhofar 311, 730 and 731: New Lunar Meteorites from Oman; The Deuterium Content of Individual Murchison Amino Acids; Clues to the Formation of PV1, an Enigmatic Carbon-rich Chondritic Clast from the Plainview H-Chondrite Regolith Breccia ;Numerical Simulations of the Production of Extinct Radionuclides and ProtoCAIs by Magnetic Flaring.

Source record↗

Relevant capture cross sections for intentional nuclear forensics, table summary

This summary provides a brief list of capture cross section metrics for naturally occurring isotopes for review by the Intentional Forensics Venture. This introduction is a companion to the column tabulated data, available in pdf and spreadsheet form. Cross section values for this summary list are taken from ENDF/B-VIII.0 and the development library for ENDF/B-VIII.1, with abundances taken from Nuclear Wallet Cards abundance tables. The cross section metrics are thermal cross section, resonance integral (RI), Maxwellian averaged cross section at 30 keV, and 252 Cf spontaneous fission spectrum averaged cross section. The isotopes are listed in order of Z, then A, with the elemental symbol also reported. This memo gives a brief introduction and overview of the data presented.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Analysis of the MUSIC 3 He Multiplicity Data

A measurement campaign called the Measurement of Uranium Subcritical and Critical (MUSiC) was performed on a range of configurations of highly-enriched uranium (HEU) from December 2020 through April of 2021. While part of the focus was to measure reactor kinetics parameters on delayed supercritical systems, an additional focus was performing neutron noise measurements on subcritical configurations from deeply subcritical to nearly delayed critical. Multiple detector systems were used to perform these measurements, such as a 3 He multiplicity detector called the Neutron Multiplicity Array Detector (NoMAD) and a liquid scintillator system called the Rossi-α Measurement Rapid Organic Discriminating Detector (RAM-RODD). Also included were a scintillator system from the University of Michigan and a set of small 3He tubes that have previously been used to measure Rossi-α values on near-critical systems. The focus of this paper will be a comparison of prospective analysis methods for the NoMAD measurements. Previous subcritical measurements at the National Criticality Experiments Research Center (NCERC) submitted to the International Criticality Safety Benchmark Evaluation Project (ICSBEP) used the Hage-Cifarelli formalism of the Feynman Variance-to-Mean method. This relies on the time correlations of neutron detections to infer the spontaneous fission rate and neutron multiplication of a system through binning the time tagged detections and analyzing resulting histograms of the numbers of counts. However, there are other neutron noise methods that rely on similar processes, such as the Hansen-Dowdy formalism which uses a slightly different methodology to extract multiplication from the neutron multiplicity counting moments. Comparisons can be made between these experimental results and those obtained through simulations to validate or identify deficiencies in analysis, detection methods, or the underlying nuclear data. Different time gating strategies and their effects on count rate uncertainties are also investigated.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Future of nuclear fission theory

There has been much recent interest in nuclear fission, due in part to a new appreciation of its relevance to astrophysics, stability of superheavy elements, and fundamental theory of neutrino interactions. At the same time, there have been important developments on a conceptual and computational level for the theory. The promising new theoretical avenues were the subject of a workshop held at the University of York in October 2019; this report summarises its findings and recommendations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Neutron-Neutron Correlations in the Photofission of 238U

Background: In the fission of actinides, the nearly back-to-back motion of the fission fragments has a strong effect on the kinematics of fission neutrons. This leads to a favoring of opening angles near 0? and 180? in the neutron-neutron (n-n) opening angle distributions of correlated neutron pairs from the same fission event. Purpose: To measure the n-n opening angle and energy correlations in the photofission of 238U. As of this writing, measurements of correlated n-n opening angle distributions have been reported only for the spontaneous and neutron-induced fission of actinides. This work is the first to report such a measurement using photofission and will provide useful experimental input for photofission models used in codes such as MCNP and FREYA. Method: Fission is induced using bremsstrahlung photons produced via a low duty factor, pulsed, linear electron accelerator. The bremsstrahlung photon beam impinges upon a 238U target that is surrounded by a large neutron scintillation detection system capable of measuring particle position and time of flight, from which n-n opening angle and energy are measured. Neutron-neutron angular correlations are determined by taking the ratio between a correlated neutron distribution and an uncorrelated neutron distribution formed by the pairing of neutrons produced during different beam pulses. This analysis technique greatly diminishes effects due to detector efficiencies, acceptance, and experimental drifts. Results: The angular correlation of neutrons from the photofission of 238U shows a high dependence on neutron energy as well as a dependence on the angle of the emitted neutrons with respect to the incoming photon beam. Angular correlations were also measured using neutrons from the spontaneous fission of 252Cf, showing good agreement with past measurements. Conclusions: The measured angular correlations reflect the underlying back-to-back nature of the fission fragments. An anomalous decline in n-n yield was observed for opening angles near 180? for 238U.

Burggraf, Jeff↗

Revision of Fission Yields Uncertainties in ENDF/B-VIII.0

The spontaneous and neutron-induced fission yield sublibraries in the Evaluated Nuclear Data Files (ENDF/B) contain cumulative and independent fission yield values for dozens of fissioning systems, and hundreds of fission products. In this work, we report on a correction step that was undertaken after observing anomalously large uncertainties for several end-of-chain fission products. A total of 17 cumulative fission yield uncertainties and the value of 2 independent yields were corrected as a result of this revision.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗