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At least 145 records · Page 8

A New Era of Nuclear Criticality Experiments: The First 10 Years of Radiation Test Object Operations at NCERC

The work presented in this paper focuses on the first 10 years (2011–2020) of radiation test object (RTO) operations at the National Criticality Experiments Research Center. RTOs are subcritical configurations of special nuclear material that are built by hand. These configurations are utilized for benchmark experiments, detector testing/characterization, and training. An overview of the types of measurements used in RTO operations is given as well as a history of RTO operations at Los Alamos National Laboratory from 1944–2011.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The Role of Pulse Radiolysis in Advanced Nuclear Fuel Cycles

The effects of ionizing radiation are ubiquitous throughout all aspects of a nuclear fuel cycle. The complexity and intensity of these effects are greatest during reactor operations and in the management of used nuclear fuel and waste. Radiation-induced processes typically promote the chemical transformation of molecules and materials with the formation of potentially detrimental degradation products and corresponding changes in physical and chemical properties, which ultimately impact the effectiveness and longevity of nuclear technologies. Consequently, a molecular-level understanding of radiation effects over multiple time, distance, and material domains is essential for the innovation and deployment of next generation nuclear technologies. Attaining this knowledge necessitates a firm grasp of radiation-induced reaction kinetics, for which pulsed electron radiolysis is the methodology of choice. Presented here are several recent studies from our group that demonstrate the critical role of pulsed electron radiolysis techniques in the advancement of our understanding of radiation-induced chemistry under advanced nuclear fuel cycle conditions. Research topics include late actinide redox chemistry, radiation robustness of used nuclear fuel reprocessing complexants, and the behavior of metal cations in high temperature molten salt media.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Thermonuclear reaction rate of 29 Si(p,γ) 30 P

The thermonuclear rate of the 29 Si(p,γ) 30 P reaction impacts the 29 Si abundance in classical novae. A reliable reaction rate is essential for testing the nova paternity of presolar stardust grains. At present, the fact that no classical nova grains have been unambiguously identified in primitive meteorites among thousands of grains studied is puzzling, considering that classical novae are expected to be prolific producers of dust grains. We investigated the 29 Si + p reaction at center-of-mass energies of 200–420 keV, and present improved values for resonance energies, level excitation energies, resonance strengths, and branching ratios. One new resonance was found at a center-of-mass energy of 303 keV. For an expected resonance at 215 keV, an experimental upper limit could be determined for the strength. We evaluated the level structure near the proton threshold, and present new reaction rates based on all the available experimental information. Our new reaction rates have much reduced uncertainties compared with previous results at temperatures of T ≥ 140 MK, which are most important for classical nova nucleosynthesis. Furthermore, future experiments to improve the reaction rates at lower temperatures are discussed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Assessment of Modeling and Nuclear Data Needs for Active Neutron Interrogation

This document is the primary deliverable for a scoping study proposed to DOE National Laboratory Announcement Number LAB 19-2114 in the NNSA research area. The study supports user applications employing active neutron interrogation by providing a science plan to improve the modeling capability and the nuclear data that radiation transport codes use. Users rely on the accuracy of the elastic scattering and non-elastic cross-sections spanning thermal energies to 14 MeV (and higher in some cases) for modeling the neutron transport through complex geometries of materials potentially composed of many elements. While the elastic scattering cross-section data are accepted for all commonly occurring elements, the non-elastic cross-section data and the associated emission data include reaction channels that require attention. The study focused on the non-elastic reactions that emit secondary, also known as prompt, gammas with the premise that many users would benefit from improved modeling of these reactions. Many users develop material assay technologies based upon gamma signatures from radiative capture, inelastic scattering, and reactions on low-Z isotopes emitting multiple particles, so the nuclear data gaps, modeling deficiencies, and recommendations for addressing the shortfalls were assessed for these reactions. Fission gammas were excluded from this study because there are other efforts underway to address known shortfalls. Follow-on efforts that successfully execute the recommendations will tangibly improve to the ability to model gamma signatures and backgrounds for user applications, such as controlled substance detection, oil-well logging, and space exploration.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Measurement of the 25 Al(𝑑,𝑛)⁢ 26 Si reaction and impact on the 25 Al⁢(𝑝,𝛾)⁢ 26 Si reaction rate

The 25 Al(p,γ) 26 Si reaction plays a key role in nucleosynthesis pathways that influence the galactic abundance of 26 Al. A more precise determination of the proton strength of the lowest ℓ = 0 proton resonance in 26 Si is needed to improve reaction-rate calculations. This work measures the 25 Al(d,n) 26 Si proton-transfer reaction in inverse kinematics using a radioactive ion beam at RESOLUT, determining excitation energies and cross sections for the lowest ℓ = 0 resonance associated with the 3 + 3 state at 5.92(2) MeV. Coupled-reaction-channels calculations (FRESCO) are used to extract the ℓ = 0 spectroscopic factor and the corresponding proton width, yielding Γₚ = 2.19(45) eV and a (p,γ) resonance strength of 26(10) meV. This resonance is found to dominate the 25 Al(p,γ) 26 Si reaction rate above 0.2 GK.

20 ≤ A ≤ 38↗

Search for Nova Presolar Grains: $γ$-Ray Spectroscopy of 34 Ar and its Relevance for the Astrophysical 33 Cl($p,γ$) Reaction

The discovery of presolar grains in primitive meteorites has launched a new era of research in the study of stellar nucleosynthesis. However, the accurate classification of presolar grains as being of specific stellar origins is particularly challenging. Recently, it has been suggested that sulfur isotopic abundances may hold the key to definitively identifying presolar grains with being of nova origins and, in this regard, the astrophysical Cl 33 ( p , γ ) Ar 34 reaction is expected to play a decisive role. As such, we have performed a detailed γ -ray spectroscopy study of Ar 34 . Excitation energies have been measured with high precision and spin-parity assignments for resonant states, located above the proton threshold in Ar 34 , have been made for the first time. Uncertainties in the Cl 33 ( p , γ ) reaction have been dramatically reduced and the results indicate that a newly identified ℓ = 0 resonance at E r = 396.9 ( 13 ) keV dominates the entire rate for T = 0.25 – 0.40 GK . Furthermore, nova hydrodynamic simulations based on the present work indicate an ejected S 32 / S 33 abundance ratio distinctive from type-II supernovae and potentially compatible with recent measurements of a presolar grain.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Countdown to perovskite space launch: Guidelines to performing relevant radiation-hardness experiments

Perovskite photovoltaics (PVs) are under intensive development for promise in terrestrial energy production. Soon, the community will find out how much of that promise may become reality. Perovskites also open new opportunities for lower cost space power. However, radiation tolerance of space environments requires appropriate analysis of relevant devices irradiated under representative radiation conditions. We present guidelines designed to rigorously test the radiation tolerance of perovskite PVs. We review radiation conditions in common orbits, calculate nonionizing and ionizing energy losses (NIEL and IEL) for perovskites, and prioritize proton radiation for effective nuclear interactions. Low-energy protons (0.05-0.15 MeV) create a representative uniform damage profile, whereas higher energy protons (commonly used in ground-based evaluation) require significantly higher fluence to accumulate the equivalent displacement damage dose due to lower scattering probability. Furthermore, high-energy protons may "heal" devices through increased electronic ionization. These procedural guidelines differ from those used to test conventional semiconductors.

14 SOLAR ENERGY↗

Radioisotope dating of nuclear materials using cryogenic decay energy spectrometry

Cryogenic decay energy spectrometry provides high energy resolution and enables absolute decay counting, offering an alternative measurement technique for radiochronometry. A cryogenic decay energy spectrometry experiment was conducted using a magnetic microcalorimeter to determine the age of a plutonium sample. The energy resolution was measured at 0.05% from 5 to 6 MeV. The time since sample purification was determined using the measured concentration ratio of the 241 Am/ 241 Pu radiochronometer. Sample age estimates based on 241 Pu alpha-decay and beta-decay counts, along with 241 Am decay counts, align with the expected sample age within expanded uncertainty (k = 2), supporting the accuracy of cryogenic decay energy spectrometry as a radiochronometric method.

and nuclear chemistry↗

Neutron Leakage Spectra Sensitivities for ICSBEP Benchmarks

Neutron leakage spectra have been measured, simulated, and investigated by many groups. These spectra have many uses, including determining shielding requirements and calculating dose for radiation protection purposes, validating nuclear data, and determining material composition. It has even been proposed to use measurements of neutron leakage spectra to determine the soil composition of Mars. As part of the Los Alamos National Laboratory (LANL) Experiments Underpinned by Computational Learning for Improvements in nuclear Data (EUCLID) Laboratory Directed Research Development (LDRD) project, the authors are working on developing methods to calculate sensitivities to neutron leakage spectra. This may allow nuclear data evaluators to better use neutron leakage spectra data to constrain or adjust nuclear data. This may also be particularly useful as many neutron leakage spectra measurements do not require fissile material and can be performed with well characterized neutron sources. Neutron leakage spectra measurements are usually performed by placing a detector at the outside of a nuclear system. This may be a reactor, a neutron generator, or a neutron source. Certain detection systems can use pulse height data to infer neutron energies, other detector systems rely on other ways of determining neutron energy (for example, a Bonner sphere with multiple moderator thicknesses can be used to measure neutron spectrum). These measurements typically rely on some unfolding of the measured results. For pulsed systems like the "Livermore Pulsed Spheres," time-of-flight information can also help to constrain the neutron energy spectra data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Radiation-Induced Dark Counts for Silicon Single-Photon Detectors in Space

Single-photon detectors operating on satellites for use in a quantum communications network can incur large dark-count-rate increases from the natural radiation environment of space. Displacement damage to the material lattice of a detector from the ionizing radiation can result in a permanent dark-count increase in the detector. In this work, we analyze the radiation-induced dark-count rate of a silicon single-photon avalanche diode onboard a satellite at different orbiting altitudes, as well as, the additional radiation from a nuclear-disturbed environment caused by a high-altitude nuclear explosion. For detectors on low Earth orbit satellites, protons are the biggest source of radiation damage and are best mitigated by choosing an orbit that minimizes exposure when passing through the South Atlantic Anomaly and Polar Cusps. Detectors on medium Earth orbit and geostationary orbit satellites, if shielded by more than 10 mm of aluminum, provide the best platform in terms of the least amount of radiation damage to the detectors. In the event of a high-altitude nuclear explosion, the artificial radiation belts produced by the explosion will cause too much damage to silicon single-photon detectors on low Earth orbit satellites and render them unfit for quantum communications in less than a day. Higher orbit satellites will only suffer minor dark-count-rate increases from the artificial radiation belts.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

PLA Renewable Bio Polymer Based Solid-State Gamma Radiation Detector-Dosimeter for Biomedical and Nuclear Industry Applications

Polylactic acid (PLA) as a “green,” renewable corn-soy based polymer resin was assessed as a novel solid-state detector for rapid-turnaround gamma radiation dosimetry in the 1–100 kGy range–of significant interest in biomedical and general nuclear industry applications. Co-60 was used as the source of gamma photons. It was found that PLA resin responds well in terms of rheology and porosity metrics with an absorbed gamma dose (Dg). In this work, rheological changes were ascertained via measuring the differential mass loss ratio (MLR) of irradiated PLA placed within PTFE-framed (40 mm × 20 mm × 0.77 mm) cavities bearing ~0.9 g of PLA resin and pressed for 12–16 min in a controlled force hot press under ~6.6 kN loading and platens heated to 227 °C for the low Dg range: 0–11 kGy; and to 193 °C for the extended Dg range: 11–120 kGy. MLR varied quadratically from 0.05 to ~0.2 (1σ ~ 0.007) in the 0–11 kGy experiments, and from 0.05 to ~0.5 (1σ ~0.01) in the 0–120 kGy experiments. Rheological changes from gamma irradiation were modeled and simultaneously correlated with void-pocket formations, which increase with Dg. A single PLA resin bead (~0.04 g) was compressed 5 min at 216 °C in 0–16 kGy experiments, and compressed 2 min at 232 °C in the 16–110 kGy experiments, to form sturdy ~100 µm thick wafers in the same press. Aggregate coupon porosity was then readily measurable with conventional optical microscope imaging and analyzed with standard image processing; this provided complementary data to MLR. Average porosity vs. dose varied quadratically from ~0 to ~15% in the 0–16 kGy range and from ~0 to ~18% over the 16–114 kGy range. These results provide evidence for utilizing “green”/renewable (under $0.01) PLA resin beads for rapid and accurate (+/-5–10%) gamma dosimetry over a wide 0–120 kGy range, using simple to deploy mass and void measuring techniques using common laboratory equipment.

61 RADIATION PROTECTION AND DOSIMETRY↗

Detection of Anomalies in Environmental Gamma Radiation Background with Hopfield Artificial Neural Network - Consortium on Nuclear Security Technologies (CONNECT) Q3 Report

Environmental screening of gamma radiation consists of detecting weak nuisance and anomaly signal in the presence of strong and highly varying background. In a typical scenario, a mobile detector-spectrometer continuously measures gamma radiation spectra in short, e.g., one-second, signal acquisition intervals. The measurement data is a 2D matrix, where one dimension is gamma ray energy, and the other dimension is the number of measurements or total time. In principle, gamma radiation sources can be detected and identified from the measured data by their unique spectral lines. Detecting sources from data measured in a search scenario is difficult due to the highly varying background because of naturally occurring radioactive material (NORM), and low signal-to-noise ratio (S/N) of spectral signal measured during one-second acquisition intervals. The objective of this work is to investigate performance of a Hopfield Neural Network (HNN) in in detection and identification of weak nuisances and anomalies events in the presence of a highly fluctuating background. Performance of HNN algorithm is benchmarked using search data from an environmental screening campaign. One data set contained a 137 Cs source, and another dataset contained a 131 I source.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Forward modeling approach to nuclear reaction cross sections: Applications in neutron inelastic scattering

The development of nuclear reaction models for the production of evaluated nuclear data has traditionally been performed by comparing measured cross sections with predictions from reaction model codes whose physical input parameters are adjusted to obtain the best agreement between measured and modeled results. To more directly probe reaction model inputs, this work introduces a forward modeling approach to experimental reaction cross-section determination, where the most important physical input parameters to reaction model calculations are obtained via 𝜒 2 minimization between measured and calculated observables. This was demonstrated using data collected by the Gamma Energy Neutron Energy Spectrometer for Inelastic Scattering (GENESIS) at the 88-inch cyclotron at Lawrence Berkeley National Laboratory, a detection array consisting of organic liquid scintillators and high-purity germanium (HPGe) detectors. Using a broad-spectrum neutron beam and a 99.98%-enriched 56 Fe target, GENESIS was used to perform a simultaneous measurement of 56 Fe 𝛾-ray production cross sections and secondary neutron energy and angle distributions. The results of the forward modeling approach to the determination of energy-differential 𝛾-ray production cross sections for the yrast 4 + → 2 + and 6 + → 4 + transitions, as well as eight other off-yrast transitions, were compared against those obtained using conventional techniques, and the results are in good agreement. In addition to discrete 𝛾-ray yield total scattered neutron energy-angular distributions as a function of incident neutron energy were also obtained using forward modeling and found to agree with evaluated data, with the exception of elastic scattering at small angles. The fitted reaction model parameters obtained through forward modeling were also used to calculate the cross section for the unobserved (𝑛, 2⁢𝑛) reaction; excellent agreement with the current evaluation was obtained, providing a validation of the predictive capabilities of the forward model approach. This work bridges the gap between nuclear data experiment and evaluation by providing a new means for extracting inelastic neutron-scattering cross sections and neutron-induced 𝛾-ray production data while directly probing reaction model physics.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Measurable radiation levels around individuals externally contaminated by nuclear fallout

During the early response to large-scale radioactive contamination events, people who are potentially affected need to be screened for radioactive contamination and public health staff need to triage individuals who may need immediate decontamination. This is typically done by screening individuals for external contamination using ionising radiation detection equipment. In this study, spatially and temporally dependent isotopic compositions from a simulated nuclear detonation and Monte Carlo methods were used to relate contamination activity levels to the measurable radiation levels at select distances away from an individual with whole-body contamination. Radionuclide-specific air kerma rate coefficients and Geiger–Mueller instrument response coefficients at five select distances from contaminated individuals are presented for 662 radionuclides. Temporally and spatially dependent incident-specific coefficients are presented for a hypothetical surface detonation of a 235 U-fueled device.

61 RADIATION PROTECTION AND DOSIMETRY↗