New Insights into the 243 Am+ 48 Ca Reaction Products Previously Observed in the Experiments on Elements 113, 115, and 117
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Oganessian, Yu. Ts.↗
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Investigation of the 243 Am+ 48 Ca reaction products previously observed in the experiments on elements 113, 115, and 117
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Oganessian, Yu. Ts.↗
Discovery of Elements 113- 118
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Physics - Nuclear physics and radiation physics, C↗
Tennessine Announced As Provisional Name For Superheavy Element 117
The International Union of Pure and Applied Chemistry (IUPAC) Inorganic Chemistry Division has published a Provisional Recommendation for the names and symbols of the recently discovered superheavy elements 113, 115, 117, and 118. Tennessine (Ts) is proposed for element 117, recognizing the contribution of Tennessee research centers ORNL, Vanderbilt and the University of Tennessee to superheavy element research.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Active Correlation Technique: Status and Development
During the recent years, at the FLNR (JINR) a successful cycle of experiments has been accomplished on the synthesis of the superheavy elements with Z = 112-118 with {sup 48}Ca beam. From the viewpoint of the detection of rare decays and background suppression, this success was achieved due to the application of a new radical technique--the method of active correlations. The method employs search in a real-time mode for a pointer to a probable correlation like recoil-alpha for switching the beam off. In the case of detection in the same detector strip an additional alpha-decay event, of 'beam OFF' time interval is prolonged automatically.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Upper Limit for the 248 Cm( 50 Ti, x n) 298− x Og Reaction Cross Section
After the synthesis of element 113, nihonium (Nh) via the 209 Bi( 70 Zn,n) 278 Nh cold fusion reaction using the RIKEN heavy-ion Linear ACcelerator (RILAC) and the GAs-filled Recoil Ion Separator (GARIS), the search for the heaviest isotopes of oganesson was initiated with GARIS-II by means of the 248 Cm( 50 Ti,xn) 298−x Og fusion evaporation reaction. The optimal bombarding energy for the 50 Ti + 248 Cm reaction was determined from the quasielastic barrier distribution extracted from the excitation function of quasielastic backscattering. Here, this method optimizes the compound nucleus formation. The search for Og was conducted for 39 days on the basis of the experimentally derived 50 Ti beam energy of 227.9(5) MeV at the middle of 248 Cm target. A precise analysis of the dataset based on multiple event search strategies revealed no decay chains with a total dose on 248 Cm target of 4.93 × 10 18 50 Ti projectiles, reaching a sensitivity of 0.27 pb and a 1σ upper cross section limit of 0.50 pb.
Gall, Benoît Jean-Paul [University of Strasbourg (↗
Decay Properties of {sup 266}Bh and {sup 262}Db Produced in the {sup 248}Cm+{sup 23}Na Reaction - Further Confirmation of the {sup 278}113 Decay Chain
Decay properties of an isotope {sup 266}Bh and its daughter nucleus {sup 262}Db produced by the {sup 248}Cm({sup 23}Na,5n) reaction were studied by using a gas-filled recoil separator coupled with a position-sensitive semiconductor detector. {sup 266}Bh was clearly identified from the correlation of the known nuclide, {sup 262}Db. The obtained decay properties of {sup 266}Bh and {sup 262}Db are consistent with those observed in the {sup 278}113 chain by RIKEN collaboration, which provided further confirmation of the discovery of {sup 278}113.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Electronic Structure and Gas-Phase Behaviour of the Heaviest Elements
Electronic structures and gas-phase adsorption behaviour of the heaviest elements 112, 113 and 114 and of their lighter homologs Hg, Tl and Pb is studied on the basis of ab initio Dirac-Coulomb atomic and four-component Density Functional Theory molecular and cluster calculations. The heaviest elements were shown to have low adsorption enthalpies on Teflon and should, therefore, be well transported through Teflon capillaries from the target chamber to the chemistry set up. Adsorption enthalpies of these elements on the Au(111) surface are predicted as -44.5 kJ/mol, -158.6 kJ/mol and -68.5 kJ/mol, respectively, giving the following sequence in the adsorption temperatures 113>114>112.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Comparing the fluorination of Pb+ and Po+: insights into p-block relativistic effects for superheavy elements
It is expected that the chemical properties of the heaviest of the superheavy elements (SHEs, = 113 – 118) do not align with what is suggested by their current positions on the periodic table. Specifically, the onset of significant relativistic effects, including increased spin–orbit splitting of the p-orbitals may lead to enhanced stability of low-oxidation states. Notably, it is predicted that flerovium ( = 114) may exhibit pseudo-noble gas behavior from a electron configuration that acts as an ‘inert pair’. Even though it is expected that the – splitting becomes pronounced toward the end of the p-block’s sixth row, there is currently limited experimental evidence to confirm its extent or impact. Here, the production of gas-phase lead ( = 82) and polonium ( = 84) fluoride cations (PbF and PoF ) were compared to elucidate differences in accessible oxidation states. The PoF and PbF species were produced and identified with the FIONA spectrometer at the Lawrence Berkeley National Laboratory 88-Inch Cylctron Facility. Polonium showed notably different fluorination chemistry than lead, producing PoF and PoF as primary products compared to lead’s PbF and PbF . The distribution of PoF products observed offer insights as to the role of spin–orbit splitting for polonium. Similar studies of superheavy elements would elucidate the accessibility of their low-oxidation states as well as to inform chemical predictions for eighth-row elements not yet discovered.
Pore, Jennifer L [Nuclear Science Division, Lawren↗
Calculation of Transactinide Homolog Isotope Production Reactions Possible with the Center for Accelerator Mass Spectrometry (CAMS) at Lawrence Livermore National Laboratory
The LLNL heavy element group has been investigating the chemical properties of the heaviest elements over the past several years. The properties of the transactinides (elements with Z > 103) are often unknown due to their low production rates and short half-lives, which require lengthy cyclotron irradiations in order to make enough atoms for statistically significant evaluations of their chemistry. In addition, automated chemical methods are often required to perform consistent and rapid chemical separations on the order of minutes for the duration of the experiment, which can last from weeks to months. Separation methods can include extraction chromatography, liquid-liquid extraction, or gas-phase chromatography. Before a lengthy transactinide experiment can be performed at an accelerator, a large amount of preparatory work must be done both to ensure the successful application of the chosen chemical system to the transactinide chemistry problem being addressed, and to evaluate the behavior of the lighter elemental homologs in the same chemical system. Since transactinide chemistry is literally performed on one single atom, its chemical properties cannot be determined from bulk chemical matrices, but instead must be inferred from the behavior of the lighter elements that occur in its chemical group and in those of its neighboring elements. By first studying the lighter group homologs in a particular chemical system, when the same system is applied to the transactinide element under investigation, its decay properties can be directly compared to those of the homologues, thereby allowing an inference of its own chemistry. The Center for Accelerator Mass Spectrometry (CAMS) at Lawrence Livermore National Laboratory (LLNL) includes a 1 MV Tandem accelerator, capable of accelerating light ions such as protons to energies of roughly 15 MeV. By using the CAMS beamline, tracers of transactinide homolog elements can be produced both for development of chemical systems and for evaluation of homolog chemical properties. CAMS also offers an environment for testing these systems 'online' by incorporating automated chemical systems into the beamline so that tracers can be created, transported, and chemically separated all on the shorter timescales required for transactinide experiments. Even though CAMS is limited in the types and energies of ions they can accelerate, there are still a wide variety of reactions that can be performed there with commercially available target materials. The half-lives of these isotopes vary over a range that could be used for both online chemistry (where shorter half-lives are required) and benchtop tracers studies (where longer lived isotopes are preferred). In this document, they present a summary of tracer production reactions that could be performed at CAMS, specifically for online, automated chemical studies. They are from chemical groups four through seven, 13, and 14, which would be appropriate for studies of elements 104-107, 113, and 114. Reactions were selected that had (a) commercially available target material, (b) half-lives long enough for transport from a target chamber to an automated chemistry system, and (c) cross-sections at CAMS available projectile energies that were large enough to produce enough atoms to result in a statistically relevant signal after losses for transport and chemistry were considered. In addition, the resulting product atoms had to decay with an observable gamma-ray using standard Ge gamma-ray detectors. The table includes calculations performed for both metal targets and their corresponding oxides.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Studies of Flerovium and Element 115 Homologs with Macrocyclic Extractants
Study of the chemistry of the heaviest elements, Z ≥ 104, poses a unique challenge due to their low production cross-sections and short half-lives. Chemistry also must be studied on the one-atom-at-a-time scale, requiring automated, fast, and very efficient chemical schemes. Recent studies of the chemical behavior of copernicium (Cn, element 112) and flerovium (Fl, element 114) together with the discovery of isotopes of these elements with half-lives suitable for chemical studies have spurred a renewed interest in the development of rapid systems designed to study the chemical properties of elements with Z ≥ 114. This dissertation explores both extraction chromatography and solvent extraction as methods for development of a rapid chemical separation scheme for the homologs of flerovium (Pb, Sn, Hg) and element 115 (Bi, Sb), with the goal of developing a chemical scheme that, in the future, can be applied to on-line chemistry of both Fl and element 115. Carrier-free radionuclides, used in these studies, of the homologs of Fl and element 115 were obtained by proton activation of high-purity metal foils at the Lawrence Livermore National Laboratory (LLNL) Center for Accelerator Mass Spectrometry (CAMS): nat In(p,n) 113 Sn, nat Sn(p,n) 124 Sb, and Au(p,n) 197m,g Hg. The carrier-free activity was separated from the foils by novel separation schemes based on ion exchange and extraction chromatography techniques. Carrier-free Pb and Bi isotopes were obtained from development of a novel generator based on cation exchange chromatography using the 232 U parent to generate 212 Pb and 212 Bi. Macrocyclic extractants, specifically crown ethers and their derivatives, were chosen for these studies; crown ethers show high selectivity for metal ions. Finally. a potential chemical system for Fl was established based on the Eichrom Pb resin, and insight to an improved system based on thiacrown ethers is presented.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Actinide targets for the synthesis of super-heavy elements
Since 2000, six new super-heavy elements with atomic numbers 113 through 118 have been synthesized in hot fusion reactions of 48Ca beams on actinide targets. These target materials, including 242 Pu, 244 Pu, 243 Am, 245 Cm, 248 Cm, 249 Cf, and 249 Bk, are available in very limited quantities and require specialized production and processing facilities resident in only a few research centers worldwide. This report describes the production and chemical processing of heavy actinide materials for super-heavy element research, current availabilities of these materials, and related target fabrication techniques. The impact of actinide materials in super-heavy element discovery is reviewed, and strategies for enhancing the production of rare actinides including 249 Bk, 251 Cf, and 254 Es are described.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
The limits of nuclear mass and charge
Four new elements with atomic numbers Z = 113, 115, 117 and 118 have recently been added to the periodic table. The questions pertaining to these superheavy systems are at the forefront of research in nuclear and atomic physics, and chemistry. Here, this Perspective offers a high-level view of the field and outlines future challenges.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Online chemical adsorption studies of Hg, Tl, and Pb on SiO 2 and Au surfaces in preparation for chemical investigations on Cn, Nh, and Fl at TASCA
Online gas-solid adsorption studies with single-atom quantities of Hg, Tl, and Pb, the lighter homologs of the superheavy elements (SHE) copernicium (Cn, Z=112), nihonium (Nh, Z=113), and flerovium (Fl, Z=114), were carried out using short-lived radioisotopes. The interaction with Au and SiO 2 surfaces was studied and the overall chemical yield was determined. Here, suitable radioisotopes were produced in fusion-evaporation reactions, isolated in the gas-filled recoil separator TASCA, and flushed rapidly to an adjacent setup of two gas chromatography detector arrays covered with SiO 2 (first array) and Au (second array). While Tl and Pb adsorbed on the SiO 2 surface, Hg interacts only weakly and reached the Au-covered array. Our results contribute to elucidating the influence of relativistic effects on chemical properties of the heaviest elements by providing experimental data on these lighter homologs.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Rare earth element enrichment in coal and coal-adjacent strata of the Uinta Region, Utah and Colorado
This study aims to quantify rare earth element enrichment within coal and coal-adjacent strata in the Uinta Region of central Utah and western Colorado. Rare earth elements are a subset of critical minerals as defined by the U.S. Geological Survey. These elements are used for a wide variety of applications, including renewable energy technology in the transition toward carbon-neutral energy. While rare earth element enrichment has been associated with Appalachian coals, there has been a more limited evaluation of western U.S. coals. Here, samples from six active mines, four idle/historical mines, four mine waste piles, and seven stratigraphically complete cores within the Uinta Region were geochemically evaluated using portable X-ray fluorescence ( n = 3,113) and inductively coupled plasma-mass spectrometry ( n = 145) elemental analytical methods. Results suggest that 24%–45% of stratigraphically coal-adjacent carbonaceous shale and siltstone units show rare earth element enrichment (>200 ppm), as do 100% of sampled igneous material. A small subset (5%–8%) of coal samples display rare earth element enrichment, specifically in cases containing volcanic ash. This study proposes two multi-step depositional and diagenetic models to explain the enrichment process, requiring the emplacement and mobilization of rare earth element source material due to hydrothermal and other external influences. Historical geochemical evaluations of Uinta Region coal and coal-adjacent data are sparse, emphasizing the statistical significance of this research. These results support the utilization of active mines and coal processing waste piles for the future of domestic rare earth element extraction, offering economic and environmental solutions to pressing global demands.
Coe, Haley H.↗
Structural analysis of nested neutralizing and non-neutralizing B cell epitopes on ricin toxin's enzymatic subunit
In this report, we describe the X–ray crystal structures of two single domain camelid antibodies (V H H), F5 and F8, each in complex with ricin toxin's enzymatic subunit (RTA). F5 has potent toxin–neutralizing activity, while F8 has weak neutralizing activity. F5 buried a total of 1760 Å 2 in complex with RTA and made contact with three prominent secondary structural elements: α–helix B (Residues 98–106), β–strand h (Residues 113–117), and the C–terminus of α–helix D (Residues 154–156). F8 buried 1103 Å 2 in complex with RTA that was centered primarily on β–strand h. As such, the structural epitope of F8 is essentially nested within that of F5. All three of the F5 complementarity determining regions CDRs were involved in RTA contact, whereas F8 interactions were almost entirely mediated by CDR3, which essentially formed a seventh β–strand within RTA's centrally located β–sheet. A comparison of the two structures reported here to several previously reported (RTA–VHH) structures identifies putative contact sites on RTA, particularly α–helix B, associated with potent toxin–neutralizing activity. Here, this information has implications for rational design of RTA–based subunit vaccines for biodefense.
59 BASIC BIOLOGICAL SCIENCES↗
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↗