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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.
The evaluators present in this publication spectroscopic data and level schemes from radioactive decay and nuclear reactions for all isobars with mass number A=230. This evaluation includes the first experimental evidence of 230Am, produced through the 197Au(40Ar,3n)234Bk (α decay to 230Am) reaction, E(40Ar)=188.4 MeV (2003MoZX).
One hundred and five isotopes of the transuranium elements neptunium, plutonium, americium, curium, berkelium, and californium have been observed so far; the discovery of these isotopes is described. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.
Berkelium-249 ( 249 Bk) and einsteinium-254 ( 254 Es) are isotopes of great importance for the investigation of berkelium and einsteinium chemical properties and super heavy element research. Therefore, it is necessary to be able to isolate acceptable, pure quantities of both isotopes to further research capabilities. These isotopes, along with californium-252 ( 252 Cf), are synthesized through the irradiation of mixed-curium targets in the High Flux Isotope Reactor (HFIR), which has the highest continuous thermal neutron flux in the world. Once irradiated, the targets are transferred to the Radiochemical Engineering Development Center for further chemical processing and final purification to separate 249 Bk and 254 Es from the remainder of isotopes present. Several methods of separation, such as the Berkex batch solvent extraction along with cation-exchange and alpha-hydroxy-isobutyrate (AHIB) columns, are employed to achieve a clean separation of the isotopes. Production Campaigns 74–77 are discussed in depth for 252 Cf, 249 Bk, and 254 Es production and isolation of 249 Bk and 254 Es. An attempt to isolate 257 Fm in Campaign 77 is discussed as well. Table 1 summarizes the total amount of material isolated in each campaign.
Interest in actinide–carbon bonds has persisted since actinide organometallics were first investigated for applications in isotope separation during the Manhattan Project. Transplutonium organometallics are rarely isolated and structurally characterized, likely owing to limited isotope inventories, a scarcity of suitable laboratory infrastructure, and intrinsic difficulties with the anaerobic conditions required. In this paper, we report the discovery of an organometallic “berkelocene” complex prepared from 0.3 milligrams of berkelium-249. Single-crystal x-ray diffraction shows a tetravalent berkelium ion between two substituted cyclooctatetraene ligands, resulting in the formation of berkelium–carbon bonds. The coordination in berkelocene resembles that of uranocene, and calculations show that the berkelium 5f orbitals engage in covalent overlap with the δ-symmetry orbitals of the cyclooctatetraenide ligand π system. Charge transfer from the ligands is diminished relative to uranocene and other actinocenes, which maximizes contributions from the stable, half-filled 5f 7 configuration of tetravalent berkelium.
The merging of small-scale syntheses and rapid crystallization methods have provided access to crystalline samples of berkelium (Z=97) and californium (Z=98) coordination complexes and compounds that can be interrogated with a suite of spectroscopic tools and structural elucidation approaches that have come online over the last 20 years. The combination of this experimental data with relativistic theoretical methods that capture the effects of spin-orbit coupling and scalar relativistic effects have allowed us to understand the electronic structure of berkelium and californium compounds at a level of detail that was not previously possible. The harbinger of this new era of post-curium chemistry was the synthesis and characterization of [Cf{B 6 O 8 (OH) 5 }]. This compound possesses a structure type that is distinct from earlier actinide borates, a reduction in coordination number for californium, contracted Cf-O bond lengths, a substantially reduced magnetic moment with respect to the calculated free-ion moment and, most importantly, vibronically coupled broadband photoluminescence. Ligand-field analysis also showed that the splitting of the ground state was larger than typically found in the f-block elements, and when taken together places its overall electronic structure as a hybrid of d- and f-block components. The discovery of the unusual properties of this compound has led to the development of large families of 4f and 5f coordination complexes, in an effort to uncover the underlying origin of the electronic structure oddities, and whether there really is a sharp onset of these changes at californium. This in turn pushed the development of far more challenging berkelium chemistry (from a radiologic standpoint) because the half-life of the isotopes decreases from 351 years for 249 Cf to 330 days for 249 Bk. This short review details some of the chemistry that has been reported over the last 15 years, and its consequences for understanding the periodic table.
The evaporation residue (ER) cross sections for 3n and 4n evaporation channels in the {sup 50}Ti + {sup 249}Bk reaction leading the formation of {sup 296}119 and {sup 295}119 isotopes are evaluated by means of a modified fusion-by-diffusion model. In the model, the dynamic evolution from dinucleus to mononucleus is taken into account with the two-dimensional coupled Langenvin equations. The calculated maximum ER cross sections in 3n and 4n evaporation channels of the {sup 50}Ti + {sup 249}Bk reaction are 0.17 and 0.57 pb, respectively. The cross section of 0.57 pb is close to the present experimental limit for the registration of the evaporation residual nuclei. Therefore, superheavy element 119 may be the most hopeful new element with Z>118 to be synthesized under somehow improved experimental conditions in the near future.
Element 117 (tennessine) joined the periodic table in November 2016. Two tennessine isotopes were synthesized by bombarding 249 Bk from Oak Ridge National Laboratory with 48 Ca ions at the Joint Institute of Nuclear Research, Russia, and 11 new heaviest isotopes of odd-Z elements were observed in subsequent decay chains. These isotopes exhibit increasing lifetimes as the closed nuclear shell at neutron number N = 184 is approached, providing evidence for the “island of stability” for super-heavy elements. Here, this article summarizes recent super-heavy element research with a focus on element 117, the role of actinide targets, and opportunities to synthesize elements 119 and 120.
In 1957 Glenn T. Seaborg conceived and advocated for the construction of the High Flux Isotope Reactor (HFIR) and the Transuranium Processing Plant (since then renamed the Radiochemical Engineering Development Center, or REDC) at Oak Ridge National Laboratory. There, heavily shielded hot cells, glove boxes, and laboratories allow recovery of transuranium elements produced in substantial quantities. Seaborg’s vision of HFIR and REDC producing milligram quantities of berkelium, californium, and einsteinium has been fulfilled beginning in 1966 through May 2019 with 78 production campaigns yielding a cumulative totals of 1.2 g of 249 Bk, 10.2 g of 252 Cf, 39 mg of 253 Es, and 15 pg of 257 Fm. Notably, 252 Cf is a neutron source used in many industrial applications including oil exploration; process control systems for the cement industry, coal analysis, and power production; sources to start nuclear reactors and perform nondestructive materials analyses; homeland security and national defense detection devices; and medical research. Isotopes made available through transplutonium production at HFIR/REDC have enabled scientists to study the nuclear properties and reactions, chemical properties, optical properties, and solid-state properties of transplutonium elements. Long-lived isotopes have served as targets in heavy ion accelerators to produce heavier elements leading to the discovery of 104 Rf, 105 Db, 106 Sg, 113 Nh, 114 Fl, 115 Mc, 116 Lv, 117 Ts, and 118 Og. This paper reviews the evolution of the processing flowsheets to produce, separate, and purify transplutonium isotopes, which have evolved over 50 years of operation at HFIR and REDC, and summarizes directions of future work to improve the efficiency of the production operations.
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)
We present available information pertaining to the nuclear structure of all nuclei with mass numbers A=243. Various decay and reaction data are evaluated and compared. Adopted data, levels, spin, parity and configuration assignments are given. When there are insufficient data, expected values from systematics of nuclear properties or/and theoretical calculations are quoted. Unexpected or discrepant experimental results are also noted. A summary and compilation of the discovery of various isotopes in this mass region is given in 2013Fr02 ( 243 Np, 243 Pu, 243 Am, 243 Cm, 243 Bk, and 243 Cf), 2011Me01 ( 243 Es), and 2013Th02 ( 243 Fm).
Available information pertaining to the nuclear structure of all nuclei with mass numbers A=247 is presented. Various decay and reaction data are evaluated and compared. Adopted data, levels, spin, parity and configuration assignments are given. When there are insufficient data, expected values from systematics of nuclear properties or/and theoretical calculations are quoted. Unexpected or discrepant experimental results are also noted. A summary and compilation of the discovery of various isotopes in this mass region is given in 2013Fr02 ({sup 247}Pu, {sup 247}Am, {sup 247}Cm, {sup 243}Bk, {sup 247}Cf), 2011Me01 ({sup 247}Es), and 2013Th02 ({sup 247}Fm, {sup 247}Md)
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)