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Best Practices for Shielding Analyses of Activated Metals and Spent Resins from Reactor Operation

This report investigated best practices for performing shielding evaluations of Type B waste packages, as defined in 10 CFR Part 71 regulations on packaging and transportation of radioactive material, or packages for which the contents are not defined before loading and may include a broad range of nuclides, geometries, and non-fuel materials. The following non-fuel waste streams were analyzed: Activated metals from decommissioned commercial power reactors, including Type 304 stainless steel, reactor vessel steel, and Inconel, Control blades from boiling water reactors, Neutron-activated corrosion products on surfaces of activated metals, and Spent resins from power plant operations. Measured elemental compositions, including major constituents and impurities, for steel and Inconel samples from commercial power reactors were used in activation calculations to determine radionuclide inventories in activated metals. For a simplified cask model, 60 Co contribution to the total external package dose rate at 30 days after shutdown varied from approximately 60% to 95%, depending on the activated metal, initial cobalt impurity concentration in the metal, and the thickness of the overpack gamma shield. Its maximum contribution to the total external package dose rate of approximately 100% was reached within the time interval of 2 to 5 years after shutdown and was maintained for up to 45 to 60 years after shutdown, depending on material, initial cobalt impurity concentration, and shield thickness. Thereafter, the 60 Co contribution to external package dose rate decreased with increasing decay time. Cobalt-60 is primarily produced by neutron reactions with the cobalt impurity in steel and Inconel. Other important radionuclides in activated metals contributing to package external dose rate are radionuclides with relatively short decay times, including 51 Cr, 59 Fe, 58 Co, and 54 Mn. These radionuclides may be represented as an equivalent 60 Co activity/source because 60 Co gamma ray emissions are bounding in terms of source strength and energy to other important radionuclides identified in the analyzed activated metals. Approaches for modeling the neutron-activated corrosion products that may be attached to activated reactor components were analyzed in this report. It was demonstrated that a surface source is more conservative than a uniform volumetric source for the treatment of neutron-activated corrosion products with respect to external package dose rates. An analysis of the maximum radionuclide loadings reported on spent resins identified the radionuclides 137 Cs, 60 Co, 134 Cs, 65 Zn, and 58 Co as the primary contributors to external package dose rate. For a resin cooled for 3.08 years, the external package dose rate was entirely produced by the reported 137 Cs and 60 Co inventory. The neutron sources from actinides found on spent resins or activated metals produced negligible dose rates and may be ignored in dose rate analyses. Effects of idealized waste material, source geometry, and spatial material/source distributions on external package dose rates were determined based on dose rate results for a simplified cask model under normal conditions of transport. Type 304 stainless steel, zirconium, and aluminum with adjusted mass densities based on a maximum content weight were analyzed for material modeling effects on external package dose rate. These materials produced identical external package dose rates within the statistical uncertainties of the dose rate estimates. Among four different source geometry configurations with homogeneous material of different mass densities, uniform volumetric source distribution, and the same source strength, the geometry configuration with lowest mass density (i.e., minimum self-shielding effect among the four cases) was most conservative. Spatial source distributions that better represent localized peak 60 Co activity values were more conservative than a uniform volumetric source distribution, assuming the same weight and total source strength per package. The increase in external dose rate caused by localized source peaks can be as much as the ratio between source peak activity density to average activity density, depending on the location of the activated metal with peak activity density. Therefore, the shielding analysis may be simplified if localized peak activities and the average activity per package can be measured/determined and documented at the time of cask loading. For simplicity, external package dose rates may be determined based on average source activity and a uniform volumetric source distribution. The dose rate results from that calculation model multiplied by the ratio of peak activity density to average activity density will produce maximum dose rate values for conservative estimates.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Measurement of the prompt fission neutron spectrum from 800 keV to 10 MeV for 240 Pu(sf) and for the 240 Pu($n,f$) reaction induced by neutrons of energy from 1–20 MeV

Here, the presence of 240 Pu in nuclear fuels for reactors has resulted in high uncertainties in the results of reactor and nuclear transmutation calculations because of deficiencies in 240 Pu-related nuclear data. Specifically for the prompt fission neutron spectrum (PFNS) of 240 Pu, there is only one neutron-induced, (n,f), measurement at 0.85 MeV incident neutron energy and only one complete spontaneous fission, (sf), measurement. This limited availability of data does not sufficiently guide nuclear data evaluations of these quantities. Here we report on a measurement of both the 240 Pu(sf) and the 240 Pu(n,f) PFNS, both over the emitted neutron energy range of 0.79–10.0 MeV, and from incident neutron energies of 1.0–20.0 MeV for the (n,f) reaction. Measurements were made with a hemispherical array of liquid scintillators at the high-energy Los Alamos Neutron Science Center white neutron source at the Weapons Neutron Research facility as part of the joint LANL-LLNL Chi-Nu experimental campaign to measure actinide fission neutron spectra. These measurements are the first of their kind, and provide clear experimental evidence for second-chance fission, third chance fission, and pre-equilibrium neutron emission processes in neutron-induced fission of 240 Pu, and are the first ever measurements above 1 MeV incident neutron energy.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Exploring the sensitivity of charge-exchange ( p , n ) reactions to the neutron density distribution

The determination of the nuclear neutron properties suffers from uncontrolled uncertainties, which have attracted considerable attention recently, such as in the context of the PREX experiment. Our aim is to analyze the sensitivity of charge-exchange (p,n) reactions to the neutron density distribution ρ n and constrain the neutron characteristics in the nuclear structure models. Method: By combing the folding and the mean-field models, the nucleon-nucleus (N,A) potential can be obtained from the nuclear density distribution. Further, the (p,p) and (p,n) cross sections for 48 Ca and 208 Pb are calculated following the distorted-wave Born approximation method. As a result, compared with the (p,p) cross section, the effects of ρ n variation on the (p,n) cross section are significant, which is due to the impact of isovector properties. Based on the global folding model analyses of data, it is found that 48 Ca and 208 Pb have relatively large neutron skin thickness ΔR np . Results illustrate that the charge-exchange (p,n) reaction is a sensitive probe of ρ n . The results in this paper can offer useful guides for future experiments of neutron characteristics.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Update on NNL TSL Evaluations and Validation [Slides]

12 new/revised TSL evaluations were contributed to ENDF/B-VIII.1. The thermal diffusion length $L$ is an integral property of a single material’s absorption and scattering cross sections (both differential and integral). No other neutron reactions or materials are involved. The MC21-calculated $L$ for water is consistent with the spread of experimental data and is sufficiently sensitive to different H-H 2 O TSL physics models to use the method as a TSL integral performance benchmark. Modern high-quality diffusion experiments at elevated $T$ would allow direct low-cost physics benchmarking of water TSLs when public elevated-$T$ critical benchmarks are limited. NNL is working with LLNL and RPI to develop experimental PNDA capability. An ICSBEP Fundamental Physics benchmark of the Nassar and Murphy PNDA experiment is being developed to provide an example of how to evaluate these type of benchmarks.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Measurement of the Prompt Fission Neutron Spectrum from 800 keV to 10 MeV for 240 Pu($sf$) and for the 240 Pu($n,f$) Reaction Induced by Neutrons of Energy from 1-20 MeV

The presence of 240 Pu in nuclear fuels for reactors has resulted in high uncertainties in the results of reactor and nuclear transmutation calculations because of deficiencies in 240 Pu-related nuclear data. Specifically for the prompt fission neutron spectrum (PFNS) of 240 Pu, there is only one neutron-induced, ($n,f$), measurement at 0.85 MeV incident neutron energy and only one complete spontaneous fission, ($sf$), measurement. This limited availability of data does not sufficiently guide nuclear data evaluations of these quantities. Here we report on a measurement of both the 240 Pu($sf$) and the 240 Pu($n,f$) PFNS, both over the emitted neutron energy range of 0.79–10.0 MeV, and from incident neutron energies of 1.0–20.0 MeV for the ($n,f$) reaction. Measurements were made with a hemispherical array of liquid scintillators at the high-energy Los Alamos Neutron Science Center white neutron source at the Weapons Neutron Research facility as part of the joint LANL-LLNL Chi-Nu experimental campaign to measure actinide fission neutron spectra. These measurements are the first of their kind, and provide clear experimental evidence for second-chance fission, third-chance fission, and pre-equilibrium neutron emission processes in neutron-induced fission of 240 Pu, and are the first ever measurements above 1 MeV incident neutron energy.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Updates to the n+ 63,65 Cu RRR+URR Evaluations [Slides]

This work updates neutron reactions on 63,65 Cu. It also discusses the motivations of the research which is to correct deficiencies in benchmark performance since critical assembly configurations use Cu as a reflector. This presentation discusses the incorporation of URR parameters fit to 2017 63 Cu(n, γ) measurement by Weigand et al., as well as preliminary work on angular distributions and states that validation against copper-sensitive ICSBEP benchmarks is ongoing. The presentation concludes by stating that R -matrix analysis coupled to consistent average parameters used in the URR have been performed for 63,65 Cu isotopes, that future work will focus on the angular distributions, and that an analysis of additional data measured on natural Cu sample is in progress.

07 ISOTOPE AND RADIATION SOURCES↗

Reaction-in-flight neutrons as a diagnostic for hydrodynamical mixing in double shell inertial confinement fusion capsules

We examine reaction-in-flight (RIF) neutrons as diagnostics for hydrodynamical mixing of high-Z shell material into the hotspot of double shell capsules that are designed for the National Ignition Facility. In particular, we consider the effects of different levels of mixing of tungsten shell material into the DT gas on RIF spectra. Using a set of 1D simulations from the radiation hydrodynamic code xRAGE to determine the temperature and density profiles of the mixed W-DT gas, we find that increasing the mass of mix systematically reduces the ratio of RIF neutrons to primary 14 MeV neutrons. The shape of the RIF spectrum also changes with mix, with the predicted spectrum softening in energy with increasing mix.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Microjet printing of metal salt or oxide targets for nuclear reaction studies on radionuclides

Radioactive targets for direct measurements of neutron-induced reactions are required to improve evaluated cross-section data and, ultimately, the fidelity of neutron reaction network simulations. Electrodeposition and molecular plating are the current state-of-the-art radioactive target production techniques, but not all metals can be electrodeposited or molecular plated with high yields. Alternative techniques can be expensive or may produce targets that are unsatisfactory in terms of thickness, yield, or purity. Microjet printing is a new, rather inexpensive technique that utilizes equipment with a small footprint and has the potential to produce thin, highly radioactive targets with good uniformity and minimal impurities from the target fabrication process. This study involved optimizing the process of producing microjet printed targets to allow for the fabrication of a stable vanadium(V) oxide (V 2 O 5 ) target that was compared with an analogous electrodeposition V 2 O 5 target manufactured via the application of a vanadium chemical conversion coating on aluminum (Al) foil. Finally, the results from these studies suggest microjet printing could be used to produce relatively uniform target layers with adequate film thicknesses (< 15 μm). V 2 O 5 microjet printed targets, when compared with chemical conversion coating V 2 O 5 targets, appeared to be qualitatively less uniform and quantitatively larger in thickness (11.7(27) μm vs. 5.3(18) μm). However, the conversion coating target contained more impurities and the Al backing had a higher background contribution to measurements of neutron-induced reactions as opposed to targets produced via microjet printing. Overall, the results from this study suggest microjet printing has the capability to be an excellent alternative target production technique to the electrodeposition and molecular plating methods.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Correlated $\ n-γ$ angular distributions from the $\ Q$ = 4.4398 MeV 12 C ($\ n, n' γ$) reaction for incident neutron energies from 6.5 MeV to 16.5 MeV

Neutron scattering cross sections and angular distributions represent one of the most glaring sources of uncertainty in calculations of nuclear systems. Even simple nuclei like 12 C show indications of errors in nuclear databases for scattering reactions. Measurements of inelastic neutron scattering have historically measured either the scattered neutrons or the nuclear deexcitation $\ γ$ emission. Only a very small number of experiments attempted correlated measurements of both the neutron and $\ γ$ data simultaneously, even though these $\ n-γ$ correlations could be essential for understanding particle transport in nuclear systems. In this work we describe a measurement of the $\ n, γ$, and correlated $\ n-γ$ angular distributions from the $\ Q$ = 4.4398 MeV 12 C ($\ n, n'γ$) reaction in a single experiment using an EJ-309 liquid scintillator detector array with wide angular coverage, and with a continuous incident neutron energy range from 6.5 to 16.5 MeV. We also provide a thorough covariance description of these results, including normalization of the probability distribution. While the measured n distributions agree well with the relatively large number of available literature measurements, there are comparatively very few measurements of the γ distributions from this reaction. However, our data support the presence of a nonzero α 4 Legendre polynomial component of the γ angular distribution suggested in past measurements, which is currently not incorporated in the ENDF/B-VIII.0 library despite the use of these same literature data for evaluation of the 12 C ($\ n, n'γ$) cross section. The correlated $\ n-γ$ distribution measurements are limited to three measurements at incident neutron energies near 14 MeV. Our results do not generally agree with any of these literature measurements. We observe clear indications of significant changes in the $\ n$ distribution for specific $\ γ$-detection angles and vice versa especially near thresholds for other reaction channels, which shows the potential for significant bias in experiments that, for example, tag on inelastic scattering using a single or small number of $\ γ$ -detection angles and could impact particle transport calculations.

6 ≤ A ≤ 19↗

Neutron Induced Nuclear Reaction Cross Sections for Radiochemistry in the Region of Thallium, Lead, and Bismuth

We have developed a set of modeled nuclear reaction cross sections for use in radiochemical detector diagnostics. Systematics for the input parameters required by the Hauser-Feshbach statistical model developed in the TALYS code system are used to calculate neutron induced nuclear reaction cross sections for targets ranging from Thallium (Z = 81) to Bismuth (Z = 83).

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Operando Neutron Imaging of Reaction Extent and Particle Swelling Informs Limiting Factors for Salt Hydrate Thermochemical Energy Storage

Salt hydrates are a promising thermochemical energy storage medium that stores heat through the reversible uptake (hydration) and release (dehydration) of water vapor. Our study deploys operando neutron imaging to investigate salt hydrate performance with high spatial resolution (42 μm pixels). For flow over a packed bed with diffusion-driven transport, measurements reveal the formation of a solid diffusion layer due to particle swelling for the pure SrBr2 salt. In contrast, the SrBr2–vermiculite composite exhibits significantly less swelling and more than a 2-fold increase in the apparent water vapor diffusivity. For axial flow through a packed bed, neutron imaging confirms theoretically predicted transitions from a moving reaction front to a homogeneous profile with an increase in humid air flow rate. Our study establishes neutron imaging as a powerful technique to advance fundamental understanding of thermochemical systems and help guide composite material design.

Kinzer, Bryan [ORNL] (ORCID:0000000337804910)↗

Detailed study of the eikonal reaction theory for the breakup of one-neutron halo nuclei

Background: One-neutron removal reactions are used to study the single-particle structure of unstable nuclei, and in particular the exotic halo nuclei. The eikonal reaction theory (ERT) has been developed by Yahiro, Ogata, and Minomo [Prog. Theor. Phys. 126, 167 (2011)] to include dynamical effects, which are missing in the usual eikonal description of these reactions. Encouraging results have been obtained for total breakup cross sections in comparison to more elaborate reaction models. Purpose: Here, we extend these comparisons to more differential breakup cross sections expressed as functions of the relative energy or parallel momentum between the core and halo neutron. Method: ERT predictions of these cross sections are compared to state-of-the-art calculations. Results: The hypotheses upon which the ERT is based are confirmed and their range of validity is made clearer. The actual ordering of the evolution operators affects ERT differential cross sections and a specific choice leads to excellent agreement with the reference calculation. Dynamical effects in the treatment of the neutron-target interaction can be significant in the parallel-momentum observable. Conclusions: The role of the different interactions in the dynamics of breakup reactions of one-neutron halo nuclei are better understood and improvements to the ERT are suggested.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

182 W (𝑛,2⁢𝑛)⁢ 181 W cross-section data from threshold to 15 MeV

Measurements of the 182 W(n, 2n) 181 W cross section have been performed in the neutron energy range between 8 and 15 MeV using the activation technique. Such data are needed to help interpret results of laser shots at the National Ignition Facility using a new DT capsule design, featuring a high-Z inner shell, with tungsten as the favored material, and an outer shell made of a low-Z material. Our data are in very good agreement with the previous data of Frehaut et al., which are based on a different technique, and in fair agreement with the ENDF/B-VIII.0 and the JEFF-3.3 evaluations.

150 ≤ A ≤ 189↗

Measurement of the 28 Si ⁢(𝑛,𝑛′⁢𝛾) cross section with 𝑛, 𝛾, and correlated 𝑛−𝛾 angular distributions

Silicon has become an unavoidable element in the circuitry central to everyday life. In turn, the interactions of silicon isotopes with neutrons for nuclear physics applications, among other motivations, have become increasingly important to understand. The dominant isotope of silicon, 28 Si, is thus of primary interest for enhanced understanding for neutron transport calculations and related investigations. Unfortunately, the existing measurement database for neutron scattering reactions on 28 Si is minimal, and nuclear data evaluations on this topic have not been updated for decades. This article details new measurements of the 28 Si ⁢(𝑛,𝑛′⁢𝛾) reaction utilizing multiple analysis methods available within the correlated gamma neutron array for scattering (CoGNAC). Specifically, high-precision near-threshold results and high-incident-energy results were obtained using the 𝛾-only and correlated 𝑛−𝛾 techniques. First-ever measurements of the correlated 𝑛−𝛾 angular distribution for particles emitted following population of the first excited state in 28 Si were obtained as well, which provide unique insight into theoretical descriptions of the inelastic neutron scattering reaction mechanism itself and detailed guidance for nuclear reaction models. The results agree well with literature data where they exist, and substantially expand on the current database for neutron reactions on 28 Si .

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

169 Tm(n,2n) 168 Tm and 169 Tm(n,3n) 167 Tm cross-section measurements from 15 to 21 MeV

The 169 Tm(n,2n) 168 Tm and 169 Tm(n,3n) 167 Tm cross sections have been measured in the neutron energy range between 15 and 21 MeV using the 3 H(d,n) 4 He neutron source reaction. The 169 Tm(n,3n) 167 Tm data are intended to provide an accurate database for interpreting so-called reaction-in-flight neutron yields, which provide a sensitive tool for studying properties of the deuterium-tritium plasma created in inertial confinement fusion laser shots at the National Ignition Facility at Lawrence Livermore National Laboratory. The data are compared to previous data and evaluations for the reaction studied and are found to be in good agreement with the ENDF/B-VIII.0 evaluation, although small adjustments are necessary for the 169 Tm(n,3n) 167 Tm reaction. Here, for the first time in any (n,2n) cross-section measurements to date, a comprehensive data set ranging from threshold to 21 MeV has been obtained by the same group.

150 ≤ A ≤ 189↗

Measurement of the 252 Cf ⁢(sf) prompt fission neutron spectrum utilizing 12 C ⁡(𝑛, 𝑛) and 9 Be ⁢(𝑛, 𝑛) neutron scattering reference measurements

The 252 Cf spontaneous fission (sf), prompt fission neutron spectrum (PFNS) is a fundamental quantity for nuclear physics measurements of neutron-emitting reactions. This energy distribution of neutrons emitted from fission has been considered a neutron data standard for decades and has been utilized as a reference for neutron detection efficiency, validation of Monte Carlo simulations, benchmarking of dosimetry standards, and more. A significant portion of the global collection of nuclear data on neutron-induced reactions is correlated with the 252 Cf ⁢(sf) PFNS. Despite the reliance on this quantity by the nuclear physics community, the historical collection of 252 Cf PFNS measurements display systematic disagreements that are not understood or easily explained. These experimental discrepancies could potentially bias the 252 Cf PFNS Standard evaluation. On top of this, these past experiments frequently employed correlated experimental measurement or analysis methods. The artificial intelligence (AI)/machine learning (ML)-informed californium chi-nuclear data experiment (AIACHNE) project was formed to (a) investigate these discrepancies utilizing AI/ML methods to identify outlying regions of literature data, assign these regions to features of the experiment itself, and perform an improved evaluation of the 252 Cf PFNS and (b) perform a new experimental measurement of this quantity designed to improve upon the existing literature database. Here, in this work, we report on the AIACHNE 252 Cf PFNS experiment utilizing a new analysis method uncorrelated with all previous measurements: neutron efficiency determinations based on elastic neutron scattering on 12 C and 9 Be . This new method provides an independent test of the existing literature data and evaluation of the 252 Cf ⁢(sf) PFNS. The method is described with detailed covariance quantification procedures, as well as a direct discussion of the sources of uncertainty described as requirements in the “Templates” series of papers. The 252 Cf ⁢(sf) PFNS reported in this work agrees well with the overall shape of the existing standard PFNS evaluation as well as many literature measurements, thus verifying the current evaluation utilizing new techniques. However, the results suggest that there are deficiencies in the angle-differential 12 C and 9 Be ⁢(𝑛, 𝑛) evaluated nuclear data, which produce unphysical structures in the reported result. While these structures are relatively minor, they become obvious because of the high statistical precision of the data and the expected smooth continuity of the 252 Cf ⁢(sf) PFNS.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Improved $^{95}\mathrm{Mo}$ neutron resonance parameters and astrophysical reaction rates

We report improved 95 Mo neutron resonance parameters and reaction rates are important for nuclear astrophysics, testing nuclear models, and nuclear criticality safety. However, despite many previous neutron-capture and total cross-section measurements on this nuclide, there still is much room for improvement as well as several discrepancies. For example, there are very few firm resonance spin and parity assignments; average resonance parameters are available only for each parity, the currently recommended astrophysical reaction rate results in disagreements between stellar models and meteoric isotopic anomalies, and there are substantial disagreements in the neutron-capture cross section at low energies important for nuclear criticality safety. To obtain an improved set of neutron resonance parameters and astrophysical reaction rates for 95 Mo. High-resolution neutron-capture and transmission data were measured at the Oak Ridge Electron Linear Accelerator (ORELA) using highly isotopically enriched 95 Mo samples. The neutron-capture apparatus, data reduction, and analysis were improved so that information contained in the γ-ray cascade following neutron capture were used to assign resonance J π values. Following this, simultaneous analysis of the new neutron-capture and transmission data was used to obtain resonance energies, gamma widths, and neutron widths and their uncertainties to a maximum energy of 10 keV. Accurate neutron-capture cross sections also were obtained for the unresolved resonance region to a maximum energy of 500 keV and, together with the new resonance parameters, used to calculate the astrophysical reaction rates in the temperature range from 5 to 30 keV. A vastly improved set of 95Mo neutron resonance parameters and an astrophysical reaction rate accurate to about 3% were obtained. Firm J π assignments were determined for 261 of the 314 observed resonances. This is a very large improvement over the previously published 32 firm J π assignments for 108 resonances. Also, the number of resonances having both firm J π assignments and Γ γ values was increased by almost a factor of 24—from 11 to 261. Neutron- and total-radiation-width distributions and average resonance spacings, average total radiation widths, and neutron strength functions were obtained for the six different s- and p-wave possibilities. Parameters for the lowest s-wave resonance, which is most important for criticality benchmarks, were obtained with high accuracy. Simple modification of the neutron-capture apparatus and expansion and improvement of data analysis techniques led to a large increase in firm J π assignments for 95 Mo neutron resonances. The resulting astrophysical reaction rate is 20%–30% larger than the currently recommended rate at s-process temperatures, which should lead to better agreement between stellar models and meteoric isotopic anomalies. The neutron-capture cross section at low energies is substantially larger than recommended in the latest evaluation, which is problematical for criticality benchmarks. The average resonance spacing as a function of spin and parity is significantly different from current models. The total-radiation-width distributions are significantly broader than predicted by theory and show significant departures from the expected Gaussian shapes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗