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At least 271 records · Page 15

Correlations between energy and $\gamma$-ray emission in 239 Pu($n, f$)

Here, we study $\gamma$-ray emission following $^{239}\mathrm{Pu}(n,\mathrm{f})$ over an incident neutron energy range of $2 < E_i < 40$ MeV. We present the first experimental evidence for positive correlations between the total angular momentum generated in fission and the excitation energy of the compound nucleus prior to fission. The $\gamma$-ray multiplicity increases linearly with incident energy below the 2\textsuperscript{nd}-chance fission threshold with a slope of $0.085 \pm 0.010$~MeV$^{-1}$. This linear trend appears to hold for the average excitation energy of the compound nucleus between $9 < \langle E_x \rangle < 19$ MeV. Most of the multiplicity increase comes from an enhancement around a $\gamma$-ray energy of 0.7 MeV, which we interpret as stretched quadrupole $\gamma$ rays that indicate an increase in total fission-fragment angular momentum with excitation energy.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Employing ternary fission of Pu 242 as a probe of very neutron-rich matter

Detailed assessments of the ability of recent theoretical approaches to modeling existing experimental data for ternary fission confirm earlier indications that the dominant mode of cluster formation in ternary fission is clusterization in very neutron rich, very low density, essentially chemically equilibrated, nucleonic matter. An extended study and comparison of these approaches applied to ternary fission yields in the thermal neutron induced reaction 241 Pu(n th ,f) has been undertaken to refine the characterization of the source matter. Here, the resonance gas approximation has been improved taking in-medium effects on the binding energies into account. A temperature of 1.29 MeV, density of 6.7 × 10 -5 nucleons/fm 3 and proton fraction Y p = 0.035 are found to provide a good representation of yields of the ternary emitted light particles and clusters. In particular, results for Z = 1 and 2 isotopes are presented. Isotopes with larger Z are discussed, and the roles of medium and continuum effects, even at very low density are illustrated.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Fission of 240 Pu with Symmetry-Restored Density Functional Theory

Nuclear fission plays an important role in fundamental and applied science, from astrophysics to nuclear engineering, yet it remains a major challenge to nuclear theory. Theoretical methods used so far to compute fission observables rely on symmetry-breaking schemes where basic information on the number of particles, angular momentum, and parity of the fissioning nucleus is lost. In this letter, we analyze the impact of restoring broken symmetries in the benchmark case of 240 Pu.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Quantifying the resonant photoemission of radiation damaged Pu

Here, the resonant photoelectron spectroscopy (ResPes) of new and aged δ-Pu(Ga) is reassessed by using the small oxygen contaminant peaks as an independent and quantitative check upon conventional cross-photon-energy normalization. Good agreement is found between the measured oxygen intensities and the atomic cross section calculations. Consistent with earlier analyses, the radiation induced damage in the aged samples is found to compress and sharpen the 5f peaks. This is associated with increased localization of the 5f bands, corresponding to the 5f density of states calculations that show a narrowing of 5f bandwidth with cluster size diminishment.

36 MATERIALS SCIENCE↗

Data Testing of Polyethylene Thermal Scattering Law with New Thermal Epithermal eXperiments (TEX) Plutonium Baseline Benchmark, PU-MET-MIXED-002

Five plutonium baseline experiments completed in September of 2018 from the Thermal Epithermal eXperiments (TEX) program have been accepted by the International Criticality Safety Benchmark Evaluation Project as PU-MET-MIXED-002 and will be included in the 2020 version of the handbook. The experiments were made up of stacked layers of plutonium Zero Power Physics Reactor (ZPPR) plates moderated by polyethylene (PE, chemical formula C2H4) to varying degrees to create configurations with five different neutron spectra, including one fast configuration, one thermal configuration, and three mixed configurations. Calculations of the benchmark show overprediction of k eff when using the most recent release of the Evaluated Nuclear Data File Version B (ENDF/B) library release (VIII.0) cross sections, particularly when compared to the previous ENDF/B-VII.1 results. One potential source of overprediction was hypothesized to be the new Molecular Dynamics (MD) generated PE Thermal Scattering Law (TSL). The overprediction was shown via calculation to not be caused by the new ENDF/B-VIII.0 thermal scattering law, and in fact the overprediction was mitigated by the new PE TSL.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Hotspot 2.07.1 doses (FGR-13) from releases of 1 g Pu-239 (SBK Calcs)

This calculation is to be used for accident analysis at B239, B331, B332, and B334. The objective of this analysis is to determine: The dose per gram of Pu-239 Solubility Class S (FGR-13) for various release heights, receptor heights and distances from 100 to 1000 meters. This calculation can be used to evaluate particulate plume dispersion releases for the co-located worker and public receptors.

61 RADIATION PROTECTION AND DOSIMETRY↗

Systematic Calculation of Pu Pourbaix Diagrams: Modelling Support for the LANL ACRSP Team

The report enclosed entitled “Systematic Calculation of Pu Pourbaix Diagrams: Modelling Support of the LANL ACRSP Team” was prepared by Amphos21 under contract to the Los Alamos National Laboratory Actinide Chemistry and Repository Science Program (ACRSP) team to support an enhanced understanding of the actinide and brine chemistry in the Waste Isolation Pilot Plant (WIPP) transuranic repository. In this report, the ThermoChimie chemistry model and database, with some slight modifications, were used to calculate Pourbaix diagrams to investigate the effects of ionic strength, organic complexation, and metal competition on the predominance diagrams for aqueous and solid plutonium species under the anoxic and reducing conditions expected in the repository. These diagrams were connected to iron chemistry phase diagrams since this iron chemistry is expected to define and control redox properties in the WIPP repository concept.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

239 Pu(n,f) Neutron Multiplicity Evaluation with CGMF-Very First Release Candidate [Slides]

239 Pu(n,f) nu-bar evaluated with CGMF from E inc = 0.1-20 MeV. Changes compared to VIII.0: Prior: CGMF model included via Kalman and sensitivities of CGMF model parameters to nu-bar. Evaluation technique: Kalman including correction for PPP. Experimental data: Nearly all data that Phil took into account (I rejected: Huanqiao, Johnstone, Leroy, Nesterov, Smirenkin); New UQ for all experimental data; Marini; No correlations between unc. of different exp., except for Cf-252(sf) nu-bar uncertainty cross-correlating all uncertainties.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Measuring Neptunium Concentration using Optical Spectrometry for the Pu-238 Supply Program

Targets containing 237 Np are irradiated at the High Flux Isotope Reactor at Oak Ridge National Laboratory to produce 238 Pu, as plutonium dioxide (PuO 2 ), a heat source material for use in future NASA space missions. Kilogram quantities of Np are processed yearly and developing methods to efficiently characterize and monitor the Np processing streams with optical spectroscopy and real-time monitoring software is a critical aspect of this effort. Here, we evaluate how ultraviolet/visible/near-infrared (UV-Vis-NIR) absorbance and Raman spectroscopic techniques are applicable to characterizing concentrated Np solutions and provide proof-of-principle and proof-of-concept results for each technique. Both techniques were tested in lab-scale studies and should improve the timeliness of production efforts. However, spectrophotometry is the more mature option and has been successfully demonstrated in a hot cell environment. An overview of the initial findings, a brief demonstration, and areas for future work will be highlighted in this report.

07 ISOTOPE AND RADIATION SOURCES↗

How does Ga doping of δ-Pu affect the phonons? [Slides]

As part of the LDRD-DR project “Aging and Metastability of Delta-Phase Plutonium,” largescale density functional theory calculations were performed to reveal details of how Ga doping affects the phonons of deltaphase Pu.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

LANL update to 239 Pu in the fast energy range [Slides]

Researchers are in the process of updating the Pu cross sections in the fast energy range (complementing the work of IAEA / INDEN / ORNL lower energy work in the resonance range). LANL is overhauling its evaluation tools (CoH, CGMF, DeCE, Kalman, NEXUS, PySOK, SOK) and focusing on consistency throughout evaluation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

LANL/LLNL 240 Pu( n,f ) Prompt Fission Neutron Spectrum Measurement (Q4 FY2022 Progress Report)

The report details the joint LANL/LLNL measurement of the 240 Pu( n,f ) prompt fission neutron spectrum (PFNS) for incident neutron energies from 1–20 MeV. A summary of the experimental setup, including details of the parallel-plate avalanche counter (PPAC) used for this experiment, beam time awarded and received, and adaptations made for specifically for this experiment are described in Sec. II. Some preliminary results obtained with a portion of the total available statistics from the executed experiment are then described in Sec. III with a discussion of potential benefits and losses if more data were collected. Finally, some primary tasks remaining to convert these data to final results are discussed in Sec. IV.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

239 Pu(n,f) Neutron Multiplicity Evaluation with CGMF-Very First Release Candidate. [Slides]

239 Pu(n,f) nu-bar evaluated with CGMF from E inc = 0.1-20 MeV. Changes compared to VIII.0: Prior: CGMF model included via Kalman and sensitivities of CGMF model parameters to nu-bar. Evaluation technique: Kalman including correction for PPP. Experimental data: Nearly all data that Phil took into account (I rejected: Huanqiao, Johnstone, Leroy, Nesterov, Smirenkin); New UQ for all experimental data; Marini; No correlations between unc. of different exp., except for Cf-252(sf) nu-bar uncertainty cross-correlating all uncertainties.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Validation of Recent Changes in Actinide Evaluations U-235, U-233, Pu-239 [Slides]

This presentation discusses U-235 updates, including fluctuations in the fission cross section in the URR range that were refined to represent measured data following the Paradela et al. evaluation. There were small changes to the low-energy resonances to improve the fit to measured capture data from RPI (capture reduced by 5% from 0.06-7.8 eV, by 7.7% from 7.8-11 eV) and there was a very small change to the thermal nu-bar within uncertainties. Discrete level data are stored in MF=6 (format requirement, no impact on calculations) and issues leading to negative eigenvalues in cross-covariances in the RR have been sorted out. In conclusion, many improvements were made to evaluated nuclear data of actinides in the resonance region and above, such as minor changes to U-235 including assessment of changes that depend on the finalization of the O-16 evaluation. U-233 improvements show significant progress in performance and some further improvement might be needed at intermediate energies. Pu-239 ORNL/IAEA evaluation is promising; however, more work is needed.

07 ISOTOPE AND RADIATION SOURCES↗

ENDF/B-VIII.1 Validation (Preliminary Release 2 + New 239 Pu)

This document should serve as a reference for validation testing of nuclear data files included in the second preliminary release of ENDF/B-VIII.1 and the newly evaluated 239 Pu nuclear data file to be included in the third preliminary release of ENDF/B-VIII.1. Experiment names listed in this report are based on International Criticality Safety Benchmark Evaluation Project (ICSBEP) Handbook designations. Additional information on ICSBEP handbook designations can be found at https://www.oecd-nea.org/jcms/pl_20291/icsbep-handbook. The validation metrics used in this report include the effective neutron multiplication factor, k eff , and tritium production. All validation metrics were calculated using the radiation transport code Monte Carlo N-Particle (MCNP).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Correct symmetry in density functional theory calculations of δ-Pu [Slides]

Density functional theory (DFT) calculations in the delta-phase of Pu have long relied on the antiferromagnetic (AFM) spin structure to approximate the material’s unique electronic structure. The resulting tetragonal distortion away from the correct cubic symmetry was believed to be a necessary consequence of allowing an ordered spin structure.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Covariance Testing and Update on 239 Pu and 235 U PFNS Covariances [Slides]

This presentation discusses in detail how covariances were obtained and tested. Along with a look into some of the mathematical checks that were performed. Possible "physics issues" in covariances were highlighted and addressed. Covariances for Dysprosium and Erbium-169 were touched on along with various uncertainties and issues. An update on Uranium-235 and Plutonium-239 Pu PFNS covariances was given.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗