Improved 235U, 238U, 239Pu, and 240Pu Photofission Cross Sections Across the GDR
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Silano, Jack [Lawrence Livermore National Laborato↗
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Single particle – MC-ICP-MS for isotopic analysis of uranium particles
Single particle – multi-collector – inductively coupled plasma – mass spectrometry (SP-MC-ICP-MS) was employed to measure a suspension of 1 µm U3O8 particles (∼1.3 pg total U/particle) to determine their individual isotopic compositions of 234U/238U, 235U/238U, and 236U/238U. The effects of different detector combinations for 235U and 238U, including secondary electron multipliers (SEM) and Faraday detectors (1011 and 1013 Ω amplifiers), were explored for accuracy and precision optimization on the observed 235U/238U. The minor isotopic ratios (i.e., 234U/238U and 236U/238U) were analyzed such that the 234U and 236U were monitored on SEM detectors and the 238U was monitored on a Faraday (1011 Ω) detector. Various integration times (5, 10, 25, and 50 ms) were investigated in all detector configurations to gain a better understanding of their impact on sensitivity, accuracy, and precision. For 235U/238U ratios of 1 µm U3O8 particles, a dual Faraday detector measurement with 1011 Ω was the optimal choice; measurement of 1021 particles yielded an average 235U/238U ratio of 0.00170 (14), a −1.8% relative difference (% RD) from the reference value. The minor isotopic compositions were determined to be 0.0000070 (14) and 0.0000758 (48) for the 234U/238U and 236U/238U, respectively. These measurements correspond to <8% and <1% RD from their reference value for the 234U/238U and 236U/238U, respectively. SP-MC-ICP-MS was also able to provide insight into measurement sensitivity. In these individual particles, merely 15 and 165 atto-grams (ag) of 234U and 236U were present (calculated). Initial limits of detection for SP-MC-ICP-MS were determined to be ∼1.0 ag (when measured via SEM detectors). This valuable approach is applicable to areas including nuclear forensics, nuclear safeguards, and geochemical analysis, which require high-precision measurements of uranium within micron-sized particles.
Manard, Benjamin [ORNL] (ORCID:0000000207400627)↗
Measurements of short-lived fission product yields from photofission of 238 U using 13.0 MeV monoenergetic photons
Photon-induced fission product yield (FPY) measurements were conducted on the isotope 238U. Fission was induced using Eγ = 13.0 MeV monoenergetic photons produced by the Triangle Universities Nuclear Laboratory’s (TUNL’s) High Intensity γ-ray Source (HIγS) facility. Short-lived FPYs were measured by performing cyclic activation of the sample using a rapid target transfer system. Following activation, the 238U target was rapidly (0.4 s) transferred to a counting station consisting of two well-shielded high-purity germanium (HPGe) detectors. The irradiation-counting cycle was repeated until the summed data had sufficient statistical accuracy. Twenty-eight unique fission products with half-lives ranging from 1 s to 450 s were identified, and their cumulative FPYs determined. Furthermore, the results are compared with previous independent FPY measurements using inverse kinematics. Good agreement between the data sets is found despite the different excitation energy distributions of the fissioning nucleus in the experiments.
Physics - Nuclear physics and radiation physics↗
Molten Salt Lattice Confinement Fusion (LCF) Fast Fission Reactor for Lunar and Planetary Surface Power
Molten salt fission reactors (MSR) have been suggested for lunar and planetary surface power systems. They have the advantage of operating at high temperature, for efficient thermal-electrical conversion, low pressure, long-lived with high nuclear fuel burnup. MSR are often designed to breed fissile 233U from natural 232Th by neutron capture and decay via: 232Th(n,)233Th(,)233Pa(,)233U Unfortunately, this process requires 233Pa isotope separation and segregation to decay to 233U. This requirement prevents additional neutron capture that interferes with 233U breeding. Instead, Wooley’s sub-critical, fast fission, molten salt reactor would use externally generated tokamak fusion neutrons1,2 to fission all actinides.We propose a simpler fusion-fast-fission sub-critical reactor that generates fast neutrons in situ from lattice confinement fusion (LCF) to fission fertile and fissile actinides. This hybrid reactor doesn't require enriched 235U fissile pins to initiate fis-sion reactions, nor 233Pa separation and segregation during operation. Like Wooley’s, this hybrid reactor “burns” natural uranium (238U) or thorium (232Th) which avoids uranium enrichment and additional fissile material launch safety and security costs. The LCF neutron source is initiated by bremsstrahlung photoneutrons (Fig. 1)3 or isotopic neutron sources in electron-screened lattices (Fig. 2)4,5. Alternatively, the electrolytic Pd-deuterium co-deposition6protocol fast fissions7 both 232Th and 238U. However, an aqueous electrolyte-based system, without pressurization similar to conventional pressurized water fission reactors, is incapable of high temperatures due to the boiling point of the electrolyte slightly over 100 C. Molten salts can be used instead as was demonstrated at the University of Hawaii8 using a variety of Ni and Pd cathodes in lithiated, hydrided and deuterated salts. These salts have melting points often exceeding 500C making them suitable to efficiently produce electrical power9 through either Advanced Stirling Genera-tors (< 100 kWe) or closed-Brayton Cycle (> 100 kWe). This hybrid reactor could power a wide range of lunar or Martian applications from unmanned in-struments, to charging vehicles and entire facilities such as human habitats or in situ resource utilization. The power conversion cycles are Carnot Cycle limited, but generally 30% efficient at best. However, waste heat on the moon or Mars is important to surviving either two-week lunar nights or Martian nights as well as providing process heat for mineral extraction and “living off the land”
Lawrence Forsley↗
Efficient Computation of Doppler-Broadened Elastic Scattering Kernel Moments Using Ladder-Operator Formulation
Anefficient routine for computing Legendre moments of the Doppler-broadened elastic scattering kernel, including resonance scattering effects, has been implemented in the ISOXML module of Griffin. Isotropic scattering in the center-of-mass system and the ideal gas model for target motion are assumed. A ladder-operator formulation is introduced to compute all Legendre moments from order 0 to N simultaneously, enabling near-linear scaling of computational cost with respect to the maximum Legendre order. A physics-based strategy for constructing outgoing energy grids has also been developed, in which a tailored base grid is combined with adaptive refinement to maintain accuracy while limiting the number of outgoing energy points. For energies between resonances, a constant cross-section model is employed to further reduce computational cost. In addition, a quantitative criterion is derived to determine isotope-wise cut-off incident energies based on a prescribed up-scattering probability coverage. For 238U, up to incident energies of approximately 75, 230, and 661 eV at 294, 900, and 2500 K (corresponding to a 2% up-scattering probability threshold), computation of P0 kernels requires 1–8 s and computation of P0–P5 kernels requires 0.4–4 min using a single thread, while maintaining 1–3% relative error in up-scattering probability. These results demonstrate that the proposed formulation enables accurate and computationally practical Doppler-broadened kernel generation for online multigroup cross-section production in Griffin.
Doppler-broadening↗
ENDF/B-VIII.1
The ENDF/B-VIII.1 release is the newest evaluated nuclear data library produced, distributed, and recommended by CSEWG for use in nuclear science and technology applications. Among the many key advances, relative to the previous version ENDF/B-VIII.0, are: re-evaluation of 239Pu file by a joint international effort; updated 16,18O, 19F, 28-30Si, 50-54Cr, 55Mn, 54,56,57Fe, 63,65Cu, 139La, 233,235,238U, and 240,241Pu neutron nuclear data by the IAEA-coordinated INDEN collaboration; significant changes for 3He, 6Li, 9Be, 51V, 88Sr, 103Rh, 140,142Ce, Dy, 181Ta, Pt, 206-208Pb, and 234,236U neutron data; new nuclear data for the photo-nuclear, being 196 adopted from the IAEA2019 Photonuclear Data Library and one new file from JENDL-5; and new evaluations for the charged-particle and atomic sublibraries. Numerous thermal neutron scattering kernels were re-evaluated or provided for the very first time. Additionally, new covariance testing was implemented. ENDF/B-VIII.1 reduced bias in the simulations of many integral experiments with particular progress noted for fluorine, copper and stainless steel containing benchmarks. Data issues which had hindered the deployment of ENDF/B-VIII.0 for commercial nuclear power applications in high burn-up situations, were addressed. ENDF/B-VIII.1 data are distributed in both ENDF-6 and GNDS formats.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Fluid dynamical description of relativistic nuclear collisions
On the basis of both a conventional relativistic nuclear fluid dynamic model and a two fluid generalization that takes into account the interpenetration of the target and projectile upon contact, collisions between heavy nuclei moving at relativistic speeds are calculated. This is done by solving the relevant equations of motion numerically in three spatial dimensions by use of particle in cell finite difference computing techniques. The effect of incorporating a density isomer, or quasistable state, in the nuclear equation of state at three times normal nuclear density, and the effect of doubling the nuclear compressibility coefficient are studied. For the reaction 20Ne + 238U at a laboratory bombarding energy per nucleon of 393 MeV, the calculated distributions in energy and angle of outgoing charged particles are compared with recent experimental data both integrated over all impact parameters and for nearly central collisions.
Nix, J. R.↗
Neutron fluences and dose equivalents measured with passive detectors on LDEF
Neutron fluences were measured on LDEF in the low energy (< 1 MeV) and high energy (> 1 MeV) ranges. The low energy detectors used the 6Li(n,alpha)T reaction with Gd foil absorbers to separate thermal (< 0.2 eV) and resonance (0.2 eV-1 MeV) neutron response. High energy detectors contained sets of fission foils (181Ta, 209Bi, 232Th, 238U) with different neutron energy thresholds. The measured neutron fluences together with predicted spectral shapes were used to estimate neutron dose equivalents. The detectors were located in the A0015 and P0006 experiments at the west and Earth sides of LDEF under shielding varying from 1 to 19 g/cm2. Dose equivalent rates varied from 0.8 to 3.3 microSv/d for the low energy neutrons and from 160 to 390 microSv/d for the high energy neutrons. This compares with TLD measured absorbed dose rates in the range of 1000-3000 microGy/d near these locations and demonstrates that high energy neutrons contribute a significant fraction of the total dose equivalent in LEO. Comparisons between measurements and calculations were made for high energy neutrons based on fission fragment tracks generated by fission foils at different shielding depths. A simple 1-D slab geometry was used in the calculations. Agreement between measurements and calculations depended on both shielding depth and threshold energy of the fission foils. Differences increased as both shielding and threshold energy increased. The modeled proton/neutron spectra appeared deficient at high energies. A 3-D model of the experiments is needed to help resolve the differences.
LDEF Project↗
Radiogenic heating of comets by 26Al and implications for their time of formation
The effect of radiogenic heating on the thermal evolution of spherical icy bodies with radii 1 km < R < 100 km was investigated. The radioisotopes considered were 26Al, 40K, 232Th, 235U, and 238U. Except for the 26Al abundance, which was varied, the other initial abundances were kept fixed, at values derived from those of chondritic meteorites and corresponding to a gas-to-dust ratio of 1. The initial models were homogeneous and isothermal (To = 10 K) amorphous ice spheres, in a circular orbit at 10(4) AU from the Sun. The main object of this study was to examine the conditions under which the transition temperature from amorphous into cubic ice (Ta = 137 K) would be reached. It was shown that the influence of the short-lived radionuclide 26Al dominates the effect of other radioactive species for bodies of radii up to approximately 50 km. Consequently, if we require comets to retain their ice in amorphous form, as suggested by observations, an upper limit of approximately 4 x 10(-9) is obtained for the initial 26Al abundance in comets, a factor of 100 lower than that of the inclusions in the Allende meteorite. A lower limit for the formation time of comets may thus be derived. The possibility of a coexistence of molten cometary cores and extended amorphous ice mantles is ruled out. Larger icy spheres (R > 100 km) reached Ta even in the absence of 26Al, due to the decay of the other radionuclides. As a result, a crystalline core formed whose relative size depended on the composition assumed. Thus the outermost icy satellites in the solar system, which might have been formed of ice in the amorphous state, have probably undergone crystallization and may have exhibited eruptive activity when the gas trapped in the amorphous ice was released (e.g., Miranda).
Non-NASA Center↗
Heating and melting of small icy satellites by the decay of 26Al
We study the effect of radiogenic heating due to 26Al on the thermal evolution of small icy satellites. Our object is to find the extent of internal melting as a function of the satellite radius and of the initial 26Al abundance. The implicit assumption, based on observations of young stars, is that planet and satellite accretion occurred on a time scale of approximately 10(6) yr (comparable with the lifetime of 26Al). The icy satellites are modeled as spheres of initially amorphous ice, with chondritic abundances of 40K, 232Th, 235U, 238U, corresponding to an ice/dust mass ratio of 1. Evolutionary calculations are carried out, spanning 4.5 x 10(9) yr, for different combinations of the two free parameters. Heat transfer by subsolidus convection is neglected for these small satellites. Our main conclusion is that the initial 26Al abundance capable of melting icy bodies of satellite size to a significant extent is more than 10 times lower than that prevailing in the interstellar medium (or that inferred from the Ca-Al rich inclusions of the Allende meteorite, approximately 7 x 10(-7) by mass). We find, for example, that an initial 26Al mass fraction of approximately 4 x 10(-8) is sufficient for melting almost completely icy spheres with radii of 800 km, typical of the larger icy planetary satellites. We also find that for any given 26Al abundance, there is a narrow range of radii below which only marginal melting occurs and above which most of the ice melts (and refreezes later). Since extensive melting may have important consequences, such as differentiation, gas release, and volcanic activity, the effect of 26Al should be included in future studies of satellite interiors.
Non-NASA Center↗
Impact Shocking of a Zircon-Sanidine Mixture and Investigations of Pb Mobility
The purpose of this project is to explore the mobility, mixing, and possible clumping of Pb isotopes during laboratory impact shock experiments. Impact events are a common planetary occurrence and their effect on istotope systematics and subsequent geochronology is not fully understood. By artificially shocking mixtures of zircon and sanidine and investigating the sample products, it may be possible to understand if and how Pb is mobilized during impact shock. Isotopes of Pb are the final daughter products of the decay chains of 238U, 235U and 232Th and therefore understanding how mobile the daughter product is during impact events could have consequences for dating impact events. These investigations will also reveal if Pb isotopes can be mixed between minerals
Szumila, I.↗
Impact Shocking of a Zircon-Sanidine Mixture and Investigations of Pb Mobility
The purpose of this project is to explore the mobility, mixing, and possible clumping of Pb isotopes during laboratory impact shock experiments. Impact events are a common planetary occurrence and their effect on istotope systematics and subsequent geochronology is not fully understood. By artificially shocking mixtures of zircon and sanidine and investigating the sample products, it may be possible to understand if and how Pb is mobilized during impact shock. Isotopes of Pb are the final daughter products of the decay chains of 238U, 235U and 232Th and therefore understanding how mobile the daughter product is during impact events could have consequences for dating impact events. These investigations will also reveal if Pb isotopes can be mixed between minerals.
Szumila, I.↗
Accessing Icy Worlds using Lattice Confinement Fusion (LCF) Fast Fission
NASA proposed the Ocean Worlds Exploration Program to search for extraterrestrial life. The challenge is that up to 40 kilometer-thick ice must first be broken through to reach sub-surface oceans. These icy ocean worlds include Ceres, Europa, Enceladus, and Pluto. Each world may have a liquid water ocean beneath their ice crust. These oceans are likely heated by the parent planet’s tidal forces, or in the case of Pluto or Ceres, by residual radioactive decay. A robotic probe exploring the oceans beneath must either melt or bore through the ice crust first. Consequently, the proposed probe needs to contend with hydrostatic ice pressure, ice phase and density changes, then water pressure. Such a mission requires a small, but robust and long lived, electrical energy and heat source. Instead, we propose a novel, compact, scalable nuclear energy source using neither highly enriched uranium (HEU) nor 238Pu similar to the hybrid fusion-fission generator described by Forsley and Mosier-Boss. This nuclear energy source uses Lattice Confinement Fusion (LCF) neutrons to fast-fission thorium or depleted uranium where neither 232Th nor 238U isotopes are fissile
Theresa L Benyo↗
Recovery of Neptunium-236g from Photon and Proton-Irradiated Actinide Targets
Neptunium-236g is a rare radionuclide used as a tracer for neptunium-237 analyses. The availability of 236gNp is limited and the viable production routes are costly, time consuming, and only produce trace quantities of the desired product. For this work, two known production methods were tested to determine product recovery, purity, and viability for use as a tracer. The first method utilizes a photon-irradiated 237Np target to produce 236gNp by the 237Np(?,n)?236Np reaction. The second method utilizes the 238U(d,4n) ?236Np reaction. These production routes were evaluated previously, and the former was considered ineffective without isotope separation and the latter was not well-characterized for the 236mNp/236gNp production ratio. Recent resurgence of electromagnetic isotope separation technology has enabled at least partial recovery of 236gNp from part-per-million abundance feeds produced by the photonuclear reaction. To address the lack of production data for the second method, a deuteron-irradiated depleted uranium target was chemically processed to recover and purify the Np for abundance and ratio analyses. The status and current analytical results for each production method are presented.
07 ISOTOPE AND RADIATION SOURCES↗
Evaluating the 238 U PFNS Including Chi-Nu Experimental Data
This report documents an evaluation of 238 U prompt fission neutron spectra (PFNS) which is a deliverable for a FY2024 Q4 NCSP (Nuclear Criticality Safety Program) milestone. This evaluation is new; its prior input is based on extended Los Alamos and exciton models implemented in the code CoH. Experimental covariances were estimated for five experimental data sets. One of these data sets that was measured by the Chi-Nu team of LANL and LLNL. It covers the 238 U PFNS for continuous incident-neutron energies of 1–20 MeV and outgoing-neutron energies from 10 keV– 10 MeV with high precision. Contrary to Chi-Nu data, previous data sets were measured in a limited energy range. The resulting evaluated data correspond well to the experimental PFNS taken into account for the evaluation. The evaluated PFNS also produce average mean energies in agreement with associated Chi-Nu data. If one uses the new evaluated data to predict the neutron multiplication factor, k eff , of the Flattop, Flattop-Pu and BigTen ICSBEP critical assemblies (which all have thick reflectors with high percentages of 238 U), the differences of simulated values compared to those using ENDF/B-VIII.1β3 is modest (less than 25 pcm). In addition to that, the new PFNS predict on average 238 U LLNL pulsed-sphere neutron-leakage spectra slightly better than ENDF/BVIIII.0 and ENDF/B-VIII.1β3 PFNS. The differences are, however, well within the experimental uncertainties.
238U↗