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Expanded Intercomparison of Nuclear Data Libraries Using Jupiter and Jupiter High-240 Experiments

There is a limited availability of plutonium experiments with sensitivity to lead in the ICSBEP (International Handbook of Evaluated Criticality Safety Benchmark Experiments) Handbook. The Jupiter and Jupiter High-240 experiments were performed at the National Criticality Experiments Research Center as a collaborative effort between Los Alamos National Laboratory and the Japan Atomic Energy Agency to assess lead void coefficients in a plutonium-lead system containing weapons- and reactor-grade plutonium, respectively. Concurrent with benchmark development, an intercomparison of calculations using different nuclear data libraries has been performed to assess the usability of the experimental data for nuclear data adjustment in a “softer-that-fast” neutron energy spectrum. Eigenvalue calculations using MCNP with the ENDF/B-VIII.0 and TENDL-2021 nuclear data libraries calculate closest to the benchmark values for Jupiter. Calculations using JENDL-5 and ENDF/B-VIII.1 match best with the Jupiter High-240 values. Lead void worth calculations using the various nuclear data libraries are all within 3σ of their respective measured values. Perturbation studies between ENDF/B-VIII.0 and ENDF/B-VIII.1 demonstrate an approximate increase in calculated eigenvalues for the Jupiter series experiments by ~240 pcm for plutonium (mostly 239 Pu) and ~120 pcm for lead accompanied by a decrease contributed by ~113 pcm for copper and ~13 pcm for stainless steel. Nuclear data sensitivities and uncertainties investigated using Whisper show slightly lower sensitivity to scatter than a lead-reflected plutonium sphere but greater sensitivity to neutron capture. The sensitivities between Jupiter and Jupiter High-240 for lead are very similar for both ENDF/B-VIII.0 and ENDF/B-VIII.1 nuclear data. These benchmarks are more sensitive to neutron capture in lead than other plutonium benchmark experiments and would be useful for both lead and 240 Pu validation. In conclusion, with the high degree of compensating effects between copper, lead, and plutonium cross sections, additional isolated Pb-Pu and Cu-Pu benchmarks would be beneficial in improving these nuclear data.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Materials Data on PuCu2 by Materials Project

PuCu2 crystallizes in the orthorhombic Imma space group. The structure is three-dimensional. Pu is bonded in a 12-coordinate geometry to twelve equivalent Cu atoms. There are a spread of Pu–Cu bond distances ranging from 2.95–3.12 Å. Cu is bonded in a 10-coordinate geometry to six equivalent Pu and four equivalent Cu atoms. There are a spread of Cu–Cu bond distances ranging from 2.52–2.55 Å.

36 MATERIALS SCIENCE↗

Materials Data on PuCu6 by Materials Project

PuCu6 is Bergman Structure: Mg32(Al,Zn)49 Bergman-derived structured and crystallizes in the orthorhombic Pnma space group. The structure is three-dimensional. Pu is bonded in a 6-coordinate geometry to nineteen Cu atoms. There are a spread of Pu–Cu bond distances ranging from 2.86–3.38 Å. There are five inequivalent Cu sites. In the first Cu site, Cu is bonded in a 10-coordinate geometry to four equivalent Pu and ten Cu atoms. There are a spread of Cu–Cu bond distances ranging from 2.47–3.02 Å. In the second Cu site, Cu is bonded to three equivalent Pu and nine Cu atoms to form a mixture of edge, face, and corner-sharing CuPu3Cu9 cuboctahedra. There are a spread of Cu–Cu bond distances ranging from 2.45–2.59 Å. In the third Cu site, Cu is bonded in a 11-coordinate geometry to three equivalent Pu and eight Cu atoms. There are two shorter (2.50 Å) and one longer (2.82 Å) Cu–Cu bond lengths. In the fourth Cu site, Cu is bonded in a 12-coordinate geometry to three equivalent Pu and nine Cu atoms. There are a spread of Cu–Cu bond distances ranging from 2.44–3.00 Å. In the fifth Cu site, Cu is bonded to three equivalent Pu and nine Cu atoms to form a mixture of edge, face, and corner-sharing CuPu3Cu9 cuboctahedra. There are one shorter (2.45 Å) and one longer (2.57 Å) Cu–Cu bond lengths.

36 MATERIALS SCIENCE↗