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At least 19 records

Rapid extraction of short-lived isotopes from a buffer gas cell for use in gas-phase chemistry experiments, Part II: On-line studies with short-lived accelerator-produced radionuclides

We report a novel combination of advanced gas-chromatography and detection systems coupled to a buffer-gas cell was characterized on-line to allow gas-phase chemical studies of accelerator-produced short-lived α -decaying mercury, francium, and astatine isotopes. These were produced in 40 Ar- and 48 Ca-induced nuclear fusion–evaporation reactions, subsequently isolated in the recoil separators MARS at Texas A&M University, USA, and TASCA at GSI Darmstadt, Germany, before being thermalized in a buffer-gas-stopping cell. From the latter, the nuclear reaction products were extracted into gas-phase chromatographic systems, suitable for registering α-decaying short-lived radionuclides, such as isotopes of superheavy elements. Efficiencies of 21(3)% for 204-209 Fr were reached for the extraction into the optimized miniCOMPACT gas-chromatography setup, indicating that this technique enables the identification of isotopes of volatile as well as non-volatile elements. These studies guide the path towards chemical investigations of superheavy elements beyond flerovium, which are out of reach with currently used setups.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Discovery of the astatine, radon, francium, and radium isotopes

Thirty-nine astatine, thirty-nine radon, thirty-five francium, and thirty-four radium isotopes have so far been observed; 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.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear Data Sheets for A = 207

Evaluated nuclear structure and decay data for all nuclei within the A=207 mass chain are presented. The experimental data are evaluated and best values for level and gamma-ray energies, quantum numbers, lifetimes, gamma-ray intensities, and other nuclear properties are recommended. Inconsistencies and discrepancies that exist in the literature are noted. This work supersedes the earlier evaluation by M.J. Martin (1993Ma73), published in Nuclear Data Sheets70, 315 (1993).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Competition between alpha-decay and spontaneous fission at isotopes of superheavy elements Rf, Db, and Sg

The most important decay modes for heavy and superheavy nuclei are their α-decay and spontaneous fission. This work investigates the evolution and the competition of these decay modes in long isotopic sequences. The partial half-lives are given by minimal sets of parameters extracted from the fit of experimental data and theoretical results. A summary of the experimental and calculated α-decay and spontaneous fission half-lives of the isotopes of elements Rf, Db, and Sg is presented. Some half-life extrapolations for nuclides not yet known are also obtained.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Final Report for research grant "Development of Methods for High Specific Activity Labeling of Biomolecules Using Astatine-211 in Different Oxidation States"

The overall objective of this research effort was to develop methods for labeling biomolecules with higher oxidation state species of At-211. This was to be done in an effort to develop reagents that had higher in vivo stability than the present carbon-bonded At-211-labeled compounds. We were unsuccessful in that effort, as none of the approaches studied provided reagents that were stable to in vivo deastatination. However, we gained a lot of information about At-211 in higher oxidation states. The studies proved to be very difficult as small changes in pH and other conditions appeared to change the nature of the species that obtained (by HPLC retention time analyses), with many of the species being unidentifiable. The fact that there are no stable isotopes of astatine, and the chemistry of the nearest halogen iodine is quite different, made it very difficult to interpret results of some experiments. With that said, we believe that a lot of valuable information was obtained from the studies. The research effort evaluated: (1) methods for chemical oxidation of At-211, (2) approaches to chelation of oxidized At-211, and (3) approaches to oxidation of astatophenyl compounds. A major hurdle that had to be surmounted to conduct the research was the development of HPLC conditions to separate and identify the various oxidized species formed. Attempts to develop conditions for separation of iodine and astatine species by normal and reversed-phase TLC and ITLC were not successful. However, we were successful in developing conditions (from a large number of attempts) to separate oxidized forms of iodine ([I-125]iodide, [I-125]iodate and [I-125]periodate) and astatine ([At-211]astatide, [At-211]astatate, [At-211]perastatate, and several unidentified At-211 species). Information on the basic oxidation and characterization of At-211 species is provided under Objective 1. Conditions were developed to obtain new At-211 labeling method where At-211 is chelated with the DOTA and NOTA chelation reagents. However, those species were unstable to isolation. Information is provided on those studies under Objective 2. We were successful in obtaining a highly oxidized form of arylastatine, but it did not appear to be stable in vivo. Information on those studies is provided under Objective 3. While we were not successful in obtaining reagents that contained oxidized forms of At-211 that were stable to in vivo deastatination, a lot of information was gained about the oxidation of At-211 and the stability of the species produced.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

β-decay and β-delayed Neutron Emission Measurements at GSI-FRS Beyond N=126, for r-process Nucleosynthesis

New measurements of very exotic nuclei in the neutron-rich region beyond N=126 have been performed at the GSI facility with the fragment separator (FRS). The aim of the experiment is to determine half-lives and β-delayed neutron emission branching ratios of isotopes of Hg, Tl and Pb in this region. This contribution summarizes final counting statistics for identification and for implantation, as well as the present status of the data analysis of the half-lives. In summary, isotopes of Pt, Au, Hg, Tl, Pb, Bi, Po, At, Rn and Fr were clearly identified and several of them ({sup 208-211}Hg, {sup 211-215}Tl, {sup 214-218}Pb) were implanted with enough statistics to determine their half-lives. About half of them are expected to be neutron emitters, in such cases it will become possible to obtain the neutron emission probabilities, Pn.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Spectroscopy of low-lying states in neutron-deficient astatine and francium nuclei

Low-lying states in neutron-deficient astatine and francium nuclei have been studied by means of in-beam and delayed spectroscopy. The 13/2{sup +} state has been observed in francium nuclei with a similar down-sloping trend as in neighbouring astatine and bismuth isotopes, as a function of decreasing neutron number. A systematic trend can also now be seen for the 1/2{sup +} state both in astatine and francium nuclei, where the level energy decreases steeply as a function of neutron number when moving further away from the neutron shell closure. This trend is very similar between astatine nuclei and their francium isotones. Moreover, shape coexistence has been observed between the 13/2{sup +} state and the spherical 9/2{sup −} ground state in {sup 203}Fr and {sup 205}Fr.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Production of Astatine-211 for Translational Science in Radiotherapy (Research Performance Progress Report)

In this proposal we outline the methods to improve the isotope production of astatine-211 at the University of Pennsylvania Cyclotron Facility. Astatine-211 is an isotope that emits alpha- radiation and has high potential for treating otherwise untreatable cancers. The goal of this proposal is two fold, 1) Optimize current production of astatine-211 and maintain routine production and 2) develop new isotope production target systems and chemical isolation systems. By completing this proposal we will ensure that the University of Pennsylvania Cyclotron Facility continues to build it’s isotope program in an effort that unites under DOE isotope network supply initiatives with the overall goal of increasing the national supply of isotopes. The University of Pennsylvania is uniquely located in the northeast corridor of the United States of America and has access to dozens of institutions that could use astatine-211 in their research. With the support of the DOE we have the opportunity to provide additional momentum to this growing field of research and will be able to provide the foundation for economical development of astatine-211 research and application in medicine.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Production and decay spectroscopy of {sup 192}Po and {sup 194}Po

A γ-ray spectroscopy study of the (11{sup −}) isomers in {sup 194}Po and {sup 192}Po was performed at the velocity filter SHIP at GSI (Germany). Nuclei were produced in fusion-evaporation reactions and investigated in the detection set-up at the focal plane after the separator. Several new γ transitions were attributed to the isomers and detailed analysis of the first γ-γ coincidences for both isomers is being prepared. For the reaction {sup 56}Fe + {sup 141}Pr → {sup 197}At*, excitation functions for astatine and polonium isotopes were measured and compared with HIVAP calculations.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Electromagnetic moments of 215,217 Bi: Probing shell evolution beyond N = 126

The nuclear properties of bismuth isotopes (Z = 83) , with just one valence proton above the closed spherical shell at (Z = 82) , are expected to be governed by a single unpaired proton. However, already in semimagic 209 Bi (Z = 83, N = 126) , , the magnetic moment (μ) strongly deviates from the single-particle Schmidt value. A near linear decrease in μ with the increase of N after the N = 126 magic number was observed up to N = 130 . In order to test whether this trend is kept at N > 130 and to reveal the underlying mechanisms, an investigation of 215,217 Bi (N = 132, 134) has been undertaken. The magnetic dipole and electric quadrupole moments of the I π = 9/2 - nuclear ground states in these isotopes have been measured for the first time using the in-source resonance-ionization spectroscopy technique at ISOLDE (CERN). It has been shown that the linearly decreasing trend of μ( 209,211,213 Bi g ) is broken in 215,217 Bi with a nearly constant value of μ observed. Experimental data have been compared to calculations in the framework of the configuration-interaction shell model with the monopole-based universal V MU +LS interaction. The peculiarities in the behavior of μ(Bi, 9/2 - ) with increasing neutron number are explained as being due to the shell evolution, change of the neutron orbitals occupancies and strong configuration mixing beyond N = 130 . Also, the difference in the μ trends for bismuth (Z = 83) and astatine (Z = 85) isotopes with N > 126 are reproduced by the shell-model calculations. It is shown that monopole interaction plays noticeable role in the description of the peculiarities of the μ behaviour. Additionally, the extension of the application of the V MU interaction to the μ isotopic trends for heavy nuclei is important for further study of the capabilities of this promising version of the shell-model calculations.

Dipole magnetic moments↗

The electron affinity of astatine

One of the most important properties influencing the chemical behavior of an element is the electron affinity (EA). Among the remaining elements with unknown EA is astatine, where one of its isotopes, 211 At, is remarkably well suited for targeted radionuclide therapy of cancer. With the At - anion being involved in many aspects of current astatine labeling protocols, the knowledge of the electron affinity of this element is of prime importance. Here we report the measured value of the EA of astatine to be 2.41578(7) eV. This result is compared to state-of-the-art relativistic quantum mechanical calculations that incorporate both the Breit and the quantum electrodynamics (QED) corrections and the electron–electron correlation effects on the highest level that can be currently achieved for many-electron systems. The developed technique of laser-photo detachment spectroscopy of radioisotopes opens the path for future EA measurements of other radioelements such as polonium, and eventually super-heavy elements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

U.S. Department of Energy Isotope Program

The National Isotope Development Center (NIDC) interfaces with the User Community and manages the coordination of isotope production across the facilities and business operations involved in the production, sale, and distribution of isotopes. A virtual center, the NIDC is funded by the Isotope Development and Production for Research and Applications (IDPRA) subprogram of the Office of Nuclear Physics in the U.S. Department of Energy Office of Science. PNNL’s Isotope Program operates in a multi-program category-2 nuclear facility, the Radiochemical Processing Laboratory (RPL), that contains 16 hot cells and 20 gloveboxes. As part of the DOE Isotope Program, the Pacific Northwest National Laboratory dispenses strontium-90, neptunium-237, radium-223, and thorium-227. PNNL’s Isotope Program uses a dedicated hot-cell for strontium-90 dispensing and a dedicated glovebox for radium-223 and thorium-227 dispensing. PNNL’s Isotope Program has access to state of the art analytical equipment in the RPL to support their research and production activities. DOE Isotope Program funded research at PNNL has advanced the application of automated radiochemistry for isotope such as zirconium-89 and astatine-211 in partnership with the University of Washington.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Laser photodetachment of radioactive 128 I -

The first experimental investigation of the electron affinity (EA) of a radioactive isotope has been conducted at the CERN-ISOLDE radioactive ion beam facility. The EA of the radioactive iodine isotope 128 I ($t$ 1/2 = 25 min) was determined to be 3.059 052(38) eV. The experiment was conducted using the newly developed Gothenburg ANion Detector for Affinity measurements by Laser PHotodetachment (GANDALPH) apparatus, connected to a CERN-ISOLDE experimental beamline. 128 I was produced in fission induced by 1.4 GeV protons striking a thorium/tantalum foil target and then extracted as singly charged negative ions at a beam energy of 20 keV. Laser photodetachment of the fast ion beam was performed in a collinear geometry inside the GANDALPH chamber. Neutral atoms produced in the photodetachment process were detected by allowing them to impinge on a glass surface, creating secondary electrons which were then detected using a channel electron multiplier. The photon energy of the laser was tuned across the threshold of the photodetachment process and the detachment threshold data were fitted to a Wigner law function in order to extract the EA. In conclusion, this first successful demonstration of photodetachment at an isotope separator on line facility opens up the opportunity for future studies of the fundamental properties of negatively charged radioactive isotopes such as the EA of astatine and polonium.

07 ISOTOPE AND RADIATION SOURCES↗

Production of Radiohalogens: Bromine and Astatine for Imaging and Therapy

Objective: This collaborative proposal between the University of Alabama at Birmingham (UAB), University of Wisconsin, Madison (UWisc) and the University of Pennsylvania (Penn) aims to research the efficient production of high purity, clinical grade radiohalogens for preclinical and translational applications by optimizing the cyclotron targetry and separation chemistry of 76,77Br and 211At for use in imaging and therapy. Proposed Research and Methods: During the course of this project, faculty and trainees at our three institutions will use the complementary infrastructure available to examine the 76Se(p,n)76Br, 77Se(p,n)77Br, 78Se(p,2n)77Br, natAs(α,2n)77Br ,80Kr(p,α)77Br and 209Bi(α, 2n)211At reactions as routes to the production of these valuable radiohalogens for imaging and therapy. Working together we aim to optimize both solid and gas targetry, including reclamation of expensive enriched material. We will develop high yielding recovery processes based on dry distillation and ion exchange techniques. We will also create a comprehensive set of quality control procedures to ensure we are producing our radioisotopes in the highest radiochemical and chemical purity possible. By bringing three institutions together to perform research and development we provide the unique opportunity to build an everlasting cooperative culture in the field of nuclear medicine research by enabling academic centers to delve into the fields of radiohalogen chemistry. In addition, each institution involved holds different skills and expertise and a collaborative grant will facilitate the cross-pollination of ideas, techniques, and build strong bonds that unite under the DOE mission. Additionally, our work does not stop at the completion of this proposal, rather this proposal allows us to gain the momentum needed to get our research and developmental efforts off the ground thereby creating a network of three institutions dedicated to the advancement of isotope production for medical research.

07 ISOTOPE AND RADIATION SOURCES↗

Compact automated apparatus for rapid astatine recovery from nitric acid media: Design, application, and impurity characterization

We report automation of irradiated bismuth target dissolution and astatine recovery from nitric acid media has been achieved at Texas A&M University. This process can be controlled remotely; it does not require any chemical treatment or evaporation of dissolution solution prior to the separation of above-mentioned elements on an extraction chromatography column, making the final product ready within 20 min. The accompanying radio-impurities have been identified and successfully separated from astatine, leading to greater than 99% radiopurity of the desired fractions. The system consists of only one pump and a set of LabVIEW controlled valves, and allows the connection of up to 10 different columns, providing the opportunity to prepare a variety of air dry columns, which can be different column geometries, containing astatine ready for further chemistry or shipment to desired facilities.

42 ENGINEERING↗

The Texas A&M Radioisotope Production and Radiochemistry Program

The main motivation of the project at Texas A&M University was to carry out the production of critically needed radioisotopes used in medicine for diagnostics and therapy, and to establish an academic program in radionuclide production and separation methods. After a lengthy battle with the Texas A&M University Radiation Safety Office, the Texas Department of State Health Services granted us a license for the production of radionuclides in July 2015, allowing us to work in earnest in our project objectives. Experiments began immediately after licensing, and we started the assembly and testing of our target systems. There were four analytical/theoretical projects and two experimental target systems. These were for At-211 production and for Zn-62/Cu-62 production. The theoretical projects were related to the production of Mo-99/Tc-99m using a) a subcritical aqueous target system and b) production of Tc-99m from accelerator-generated Mo-99 utilizing a photon-neutron interaction with enriched Mo-100 targets. The two experimental projects were the development of targetry systems and production of At-211 and Zn-62/Cu-62 generator. The targetry system for At-211 has been tested and production of At-211 is chronic depending of availability of beam time at the cyclotron. The installation and testing of the targetry system for the production of Zn-62/Cu-62 has not been finalized. A description of the systems is described. The academic program in radionuclide production and separation methods was initiated in the fall of 2011 and, due to the lack of a radiochemistry laboratory, it was suspended. We expect to re-start the academic program at the Texas A&M Institute for Preclinical Studies under the Molecular Imaging Program.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗