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Element 117

An international team of scientists from Russia and the United States, including two Department of Energy national laboratories and two universities, has discovered the newest superheavy element, element 117. The team included scientists from the Joint Institute of Nuclear Research (Dubna, Russia), the Research Institute for Advanced Reactors (Dimitrovgrad), Lawrence Livermore National Laboratory, Oak Ridge National Laboratory, Vanderbilt University, and the University of Nevada, Las Vegas.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Calculation of the evaporation residue cross sections for the synthesis of the superheavy element Z=119 via the {sup 50}Ti+{sup 249}Bk hot fusion reaction

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.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear Data Sheets for A = 230

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).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Application of a Dual-Column Method to Selectively Extract and Purify Berkelium-249 from Other Actinides and Impurities

The super heavy element (SHE) Tennessine (Ts, Element 117) was discovered in 2016 a collaboration of US and Russian scientists vis bombardment reaction of 249 Bk + 48 Ca $\rightarrow$ 117 Ts, while the target element 249 Bk (half-life 330d) was produced and provided by the Radiochemical Engineering Development Center (REDC), Oak Ridge National Laboratory (ORNL). The production of 249 Bk at REDC, ORNL requires a multi-step chemical process of irradiated curium feedstock target to remove all fission product (FP) elements and to separate 249 Bk from other actinide (An) elements (Am, Cm, Cf, Fm and Es), including: Caustic Dissolution, Acid Dissolution, Cleanex, two LiCl Anion Exchanges, LiOH Precipitation, Cation Exchange with AHIB, and with Bk Finishing as the final Bk purification step. The major product of this campaign is 252 Cf, while 249 Bk is one of important by-products. The current Cf campaign for recovery of c.a. 15 mg of 249 Bk per campaign (not including the time for Finishing of Cf, Fm and Es) takes 6 or 7 months, including ~3 months spent on Bk Finishing. Bk Finishing includes two major processes: (1) BERKEX, operated inside a hot cell with two cycles of batch solvent extraction (SX) using di-2-ethylhexyl phosphoric acid (HDEHP) as the extractant for tetravalent 249 Bk from an 8 $M$ HNO 3 -0.3 $M$ NaBrO 3 solution; and (2) Cation Exchange (CX) with AHIB (α-Hydroxy isobutyric acid), operated inside a glove box laboratory. Entire Bk Finishing takes five SX, more than five column runs and several drying down processes for aqueous solutions including one from 500 mL to 1 mL for volume reduction. To shorten the Bk Finishing period and simplify the Bk purification operation steps, possibilities of using other resin columns were explored.Recent trials using columns of either $LN$ resin or $MP$-1 anion exchange resin adsorbing the tetravalent 249 Bk 4+ in 8 $M$ HNO 3 -0.5 $M$ NaBrO 3 , followed by eluting impurities (e.g. Ce 4+ ,Cf 3+ ) and stripping 249 Bk resulted in a new Dual Column Method of selectively separating 249 Bk from other trans-plutonium elements and fission product (FP) impurities. This new method is proposed to replace the current Bk Finishing and provide increased Bk purification effeciency and a shorter processing period of 4 to 5 months (less decay loss for higher 249 Bk productivity). This TM Report discusses the trial experimental results, describes the dual column method with relevant chemistry issues and possibilities being used in further process steps ahead of the Bk Finishing.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

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↗

Discovery of element 117: Super-heavy elements and the “island of stability”

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.

07 ISOTOPE AND RADIATION SOURCES↗

Separation and Purification of Berkelium-249 and Einsteinium-254

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.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Production of Cf-252 and other transplutonium isotopes at Oak Ridge National Laboratory

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.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Dynamics of quasifission

Quasifission is the primary reaction mechanism that limits the formation of superheavy nuclei and consequently an important ingredient for choosing the best target-projectile combinations for the heavy element searches. Quasifission is characterized by nuclear contact-times that are much longer than those found in deep-inelastic reactions, resulting in a substantial mass and charge transfer. In this manuscript we employ the fully microscopic time-dependent Hartree-Fock (TDHF) theory to study quasifission. New results are presented for the {sup 48}Ca+{sup 249}Bk system.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

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↗

2010 Neutron Review: ORNL Neutron Sciences Progress Report

During 2010, the Neutron Sciences Directorate focused on producing world-class science, while supporting the needs of the scientific community. As the instrument, sample environment, and data analysis tools at High Flux Isotope Reactor (HFIR ) and Spallation Neutron Source (SNS) have grown over the last year, so has promising neutron scattering research. This was an exciting year in science, technology, and operations. Some topics discussed are: (1) HFIR and SNS Experiments Take Gordon Battelle Awards for Scientific Discovery - Battelle Memorial Institute presented the inaugural Gordon Battelle Prizes for scientific discovery and technology impact in 2010. Battelle awards the prizes to recognize the most significant advancements at national laboratories that it manages or co-manages. (2) Discovery of Element 117 - As part of an international team of scientists from Russia and the United States, HFIR staff played a pivotal role in the discovery by generating the berkelium used to produce the new element. A total of six atoms of ''ununseptium'' were detected in a two-year campaign employing HFIR and the Radiochemical Engineering Development Center at Oak Ridge National Laboratory (ORNL) and the heavy-ion accelerator capabilities at the Joint Institute for Nuclear Research in Dubna, Russia. The discovery of the new element expands the understanding of the properties of nuclei at extreme numbers of protons and neutrons. The production of a new element and observation of 11 new heaviest isotopes demonstrate the increased stability of super-heavy elements with increasing neutron numbers and provide the strongest evidence to date for the existence of an island of enhanced stability for super-heavy elements. (3) Studies of Iron-Based High-Temperature Superconductors - ORNL applied its distinctive capabilities in neutron scattering, chemistry, physics, and computation to detailed studies of the magnetic excitations of iron-based superconductors (iron pnictides and chalcogenides), a class of materials discovered in 2008. This research is yielding new insights into the relationship between magnetism and superconductivity and has established several key features of this family of high-temperature superconducting (HTS ) materials: the maximum magnetic field at which they can function, the nature of the electrons involved in the superconductivity, the dependence of the properties upon chemical substitution, and the character of the magnetic fluctuations in the material. The results suggest that despite important differences between these materials and the HTS copper oxides, a universal mechanism may be responsible for the unconventional superconductivity. (4) Coal Sequestration Research: A New Home for Greenhouse Gases - One possibility for slowing down the increasing levels of carbon dioxide (CO{sub 2}) in the atmosphere is to capture the gas in natural underground features such as coal seams. Critical to the feasibility of this technology is determining how much CO{sub 2} can be stored, no method for which has been found - until now. (5) Accelerator Reliability Passes 92% - In December 2010, SNS set a new record for itself when the accelerator ran at 1 MW with 100% reliability. Target Performance Exceeds All Expectations - The mercury target used at SNS is the first of its kind. During the design and planning for SNS, many people were skeptical that the target would work. In 2010, it was confirmed that the target was working not only well but much better than anyone would have imagined. (6) Changing the World of Data Acquisition - Researchers at SNS are starting to benefit from event-based data analysis. Event data mode captures and stores an individual data set for every single neutron that strikes a detector - precisely when and where the neutron is detected. This technique provides numerous advantages over traditional methods. Event data mode allows researchers to process their data at the highest resolution possible with no loss of data. This method of data collection provides a much more efficient way for users to gather data and get the most from their beam time. (7) New Laboratories for Users - The HFIR and SNS user communities continue to grow dramatically. In 2010, HFIR hosted 862 users and SNS 796, outpacing projections for both facilities. To meet the needs of those users, a new complex of 13 laboratories is now open for users at SNS. (8) Innovative Detectors Provide Relief from Helium-3 Shortage - Helium-3 ({sup 3}He) has been the gas of choice for gaseous detectors since the early days of neutron science. About two years ago, detector scientists worldwide faced the reality that stockpiles of {sup 3}He are dwindling rapidly, while demand for it has risen by a factor of five. The Neutron Sciences Detectors Group has developed two new types of detectors that don't rely on {sup 3}He: the Anger camera and the wavelength shifting fiber neutron detector, both of which use lithium ({sup 6}Li).

High Flux isotope reactor↗