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Nuclear Data Sheets for A = 249

The evaluated spectroscopic data are presented for known nuclides of mass 249 (Cm, Bk, Cf, Es, Fm, Md, No). {sup 249}No has not been identified as yet. Significant amounts of new data have been added since the last evaluation of A=249 nuclides. This work supersedes earlier full evaluations of A=249 published by 1999Ar21.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Formation of Superheavy Elements: Study Based on Dynamical Approach

Using multi-dimensional Langevin equations for the probability distribution of the distance between the surfaces of two approaching nuclei, we have studied the formation of superheavy elements via calculation of evaporation and fission cross sections of these elements. Evaporation residue cross sections have been calculated for the 1n, 2n, 3n, 4n, and 5n evaporation channels using one and four dimensional Langevin equations for the {sup 48}Ca+{sup 226}Ra, {sup 232}Th, {sup 238}U, {sup 237}Np, {sup 239,240,242,244}Pu, {sup 243}Am, {sup 245,248}Cm, {sup 249}Bk, and {sup 249}Cf reactions. Our results show that with increasing dimension of Langevin equations the evaporation residue cross section is increased. Also, obtained results based on fourdimensional Langevin are in better agreement with experimental data in comparison with one-dimensional model.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Disposition Options for Mk-42 Materials - 17072

In the late 1980s, the DOE Defense Programs identified a need to recover special isotopes of americium, curium, and plutonium (Am/Cm/Pu) from Mark-42 (Mk-42) targets that had been irradiated at the SRS. Eighty Mk-42 target segments were transferred from SRS to ORNL for recovery of these special isotopes. Approximately 65% of the target materials has been processed and converted to solids. The remaining Mk-42 materials are either targets stored in their irradiated forms or target material stored from various stages of processing. The Pu, Am-243 and Cm-244 in these targets are valuable materials; for example, the Am/Cm materials are potential feedstocks for production of heavy actinides (Cf-252, Bk-249, etc.). Although the isotopes in the Mk-42 materials have value, there is continual pressure to look at de-inventorying material in storage to only retain the most valuable materials needed to meet mission needs and to allow other materials to be added to the inventory as they become available. Evaluations are underway for potential disposition options for the Mk-42 materials. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Evaluation of Options for Disposition of Mk-42 Materials - 18034

In the late 1980's, the DOE defense programs identified a need to recover special isotopes of americium, curium, and plutonium from Mark-42 (Mk-42) targets that had been irradiated at the SRS. Eighty Mk-42 target segments were transferred from SRS to ORNL for recovery of these special isotopes. Approximately 65% of the target material has been processed, and the recovered material converted to solids. The remaining Mk-42 materials are stored either as targets in their irradiated forms or as target material from various stages of processing. The Pu, Am-243 and Cm-244 in these targets are valuable materials; for example, the Am/Cm materials are potential feedstocks for production of heavy actinides (Cf-252, Bk-249, etc.). In addition, rare long-lived fission product (LLFP) isotopes present in the targets in much smaller quantities, such as Zr-93, also have value to the research community. Although the isotopes in the Mk-42 materials have value, there is continual pressure to de-inventory the material in storage and only retain the most valuable materials needed to meet mission needs and provide inventory space for other materials to be added as they become available. Evaluations are underway for potential disposition options for the Mk-42 materials. Previous studies have included identification and evaluation of disposition options for the various Mk-42 materials in storage at ORNL [1]. Evaluations have included options for recovering the major isotopes and evaluating the waste that would be sent to disposal facilities. This paper summarizes the next steps in the evaluation process to develop an optimum path forward for the disposition of the Mk-42 materials. It includes an evaluation of the future programmatic need for the materials, the impact of storage on facility operations, and additional evaluations of options for dispositioning the materials. In addition to recovery of the major isotopes previously evaluated, it also looks at the potential to recover rare LLFP isotopes present in the targets in small quantities. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Extraction of americium, curium, and californium with LN resin from HCl and HNO 3

The uptake of 241 Am, 244 Cm and 249 Cf with LN resin was studied in HCl and HNO3 solutions with concentrations ranging from 0.02 to 2.5 M. There is high uptake at concentrations < 0.1 M in both acids for all three isotopes with decreasing uptake at higher concentrations and negligible extraction at ≥ 0.6 M. Californium has a higher extraction than americium and curium, which are extremely similar. Kinetics studies showed rapid uptake of all three isotopes. Here, column studies were performed to demonstrate the separation of 241 Am and 249 Cf, and a bulk separation including nine stable lanthanides along with 241 Am, 249 Cf, and 88 Y.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Nuclear Data Sheets for A = 248

Detailed level schemes, decay schemes, and the experimental data on which they are based are presented for all nuclei with mass number A=248. The experimental reaction and decay data are evaluated; inconsistencies and discrepancies are noted; and adopted values are given for various level properties (including spin and parity, halflife, and configuration), γ properties (including energy, intensity, and multipole character) and α properties (including energy, intensity, and hindrance factor). This evaluation replaces the A=248 evaluation published by A. Akovali in Nuclear Data Sheets 87, 249 (1999)

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Isolation and characterization of a californium metallocene

Californium (Cf) is currently the heaviest element accessible above microgram quantities. Cf isotopes impose severe experimental challenges due to their scarcity and radiological hazards. Consequently, chemical secrets ranging from the accessibility of 5f/6d valence orbitals to engage in bonding, the role of spin–orbit coupling in electronic structure, and reactivity patterns compared to other f elements, remain locked. Organometallic molecules were foundational in elucidating periodicity and bonding trends across the periodic table, with a twenty-first-century renaissance of organometallic thorium (Th) through plutonium (Pu) chemistry, and to a smaller extent americium (Am), transforming chemical understanding. Yet, analogous curium (Cm) to Cf chemistry has lain dormant since the 1970s. Here, we revive air-/moisture-sensitive Cf chemistry through the synthesis and characterization of [Cf(C 5 Me 4 H) 2 Cl 2 K(OEt 2 )] n from two milligrams of 249 Cf. This bent metallocene motif, not previously structurally authenticated beyond uranium (U), contains the first crystallographically characterized Cf–C bond. Analysis suggests the Cf–C bond is largely ionic with a small covalent contribution. Lowered Cf 5f orbital energy versus dysprosium (Dy) 4f in the colourless, isoelectronic and isostructural [Dy(C 5 Me 4 H) 2 Cl 2 K(OEt 2 )] n results in an orange Cf compound, contrasting with the light-green colour typically associated with Cf compounds.

Chemical bonding↗

Minimum critical masses and their uncertainties for several fissile nuclides and reflectors - 14296

A systematic effort was undertaken to reevaluate the minimum critical mass for several fissile nuclides and reflectors. This was done using MCNP6 in combination with several modern nuclear data libraries, viz. ENDF/B-VII.1, JENDL-4.0 and JEFF-3.1.1. This combination was benchmarked extensively against criticality safety benchmarks. The procedure to extract the minimum critical mass from the MCNP6 calculations was carefully implemented, so that it would have a negligible impact on the accuracy of the end results. All parts of the calculation, i.e. nuclear data processing, MCNP6 models, and post-processing, were applied consistently for all cases, involving varying fissile nuclides and reflectors. Results for the minimum critical mass were generated for {sup 233,235}U, {sup 236,239,241}Pu, {sup 242m}Am, {sup 243,245,247}Cm, and {sup 249,251}Cf, for the case of water moderation and water reflection. For {sup 235}U, the minimum critical mass was also calculated for cases with other reflectors, such as beryllium, heavy water, graphite, lead, and concrete. The results for the water reflection cases are in good agreement with most of the literature values, but for the cases with reflectors such as graphite, lead, or concrete, there are sizable differences. The accuracy of the results was assessed in two ways. First, a comparison was made with criticality safety benchmark results, by selecting benchmarks that resemble the minimum mass systems the most. It was clear that for {sup 233,235}U and {sup 239}Pu with water reflection, the differences in minimum critical masses between the libraries are consistent with the differences obtained for benchmark cases. The difference between the benchmark calculations and the benchmark values is then an indication of the accuracy with which one can simulate comparable systems. Secondly, sensitivity runs were performed with the new MCNP6 sensitivity option, based on ENDF/B-VII.1 nuclear data. For each fissile nuclide, the sensitivity of k{sub eff} to cross sections such as capture, fission, elastic, inelastic was calculated for the minimum critical mass case. The same was done for the {sup 1}H and {sup 16}O cross sections in the moderator and reflector. The uncertainty in k{sub eff} was calculated by combining the sensitivity profiles with the appropriate ENDF/B-VII.1 covariance matrix, using the SUSD code. As a final step, the uncertainty in k{sub eff} can be translated to an uncertainty in the minimum critical mass. (author)

42 ENGINEERING↗