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Nuclear Data Sheets for A = 209

The experimental data are evaluated for known nuclides of mass number A = 209 (Au,Hg,Tl,Pb,Bi,Po,At,Rn, Fr,Ra,Ac,Th). Detailed evaluated level properties and related nuclear structure information are presented, with the best values recommended for level energies, half-lives, γ–ray energies and intensities, decay data (energies, intensities and placement of radiations), and other spectroscopic data. This work supersedes the earlier full evaluation of A = 209 by M.J. Martin (1991Ma16)

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Development of an autonomous solvent extraction system to isolate astatine-211 from dissolved cyclotron bombarded bismuth targets

Abstract Cyclotron-produced astatine-211 ( 211 At) shows tremendous promise in targeted alpha therapy (TAT) applications due to its attractive half-life and its 100% α-emission from nearly simultaneous branched alpha decay. Astatine-211 is produced by alpha beam bombardment of naturally monoisotopic bismuth metal ( 209 Bi) via the ( α, 2n ) reaction. In order to isolate the small mass of 211 At (specific activity = 76 GBq·µg −1 ) from several grams of acid-dissolved Bi metal, a manual milliliter-scale solvent extraction process using diisopropyl ether (DIPE) is routinely performed at the University of Washington. As this process is complex and time consuming, we have developed a fluidic workstation that can perform the method autonomously. The workstation employs two pumps to concurrently deliver the aqueous and organic phases to a mixing tee and in-line phase mixer. The mixed phases are routed to a phase settling reservoir, where they gravity settle. Finally, each respective phase is withdrawn into its respective pump. However, development of a phase boundary sensor, placed in tandem with the phase settling reservoir, was necessary to communicate to the system when withdrawal of the denser aqueous phase was complete (i.e., the intersection of the two phases was located). The development and optimization of the autonomous solvent extraction system is described, and the 211 At yields from several ~1.1 GBq-level 211 At processing runs are reported.

211At↗

Astatine partitioning between nitric acid and conventional solvents: indication of covalency in ketone complexation of AtO +

Astatine-211 has been produced at Texas A&M University on the K150 cyclotron, with a yield of 890 ± 80 MBq through the 209 Bi(α,2n) 211 At reaction via an 8 h bombardment with a beam current of 4–8 μA and an α-particle beam energy of 28.8 MeV. The target was then dissolved in HNO 3 and the extraction of 211 At was investigated into a variety of organic solvents in 1–3 M HNO 3 . Extraction of 211 At with distribution ratios as high as 11.3 ± 0.6, 12.3 ± 0.8, 42.2 ± 2.2, 69 ± 4, and 95 ± 6 were observed for diisopropyl ether, 1-decanol, 1-octanol, 3-octanone, and methyl isobutyl ketone, respectively, while the distribution ratios for 207 Bi were ≤0.05 in all cases. The extraction of 211 At into both methyl isobutyl ketone and 3-octanone showed a strong, linear dependence on the HNO 3 initial aqueous concentration and better extraction than other solvents. DFT calculations show stronger binding between the carbonyl oxygen of the ketone and the At metal center.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Sci-Thur AM: YIS – 01: New technologies for astatine-211 targeted alpha therapy research

Purpose: The short-range, densely ionizing α-particles emitted by {sup 211}At (t{sub 1/2}=7.2h) are well suited for the treatment of diffuse microscopic disease, using cancer targeting biomolecules. {sup 211}At availability is limited by the rarity of α-cyclotrons required for standard production. Image-based dosimetry is also limited for {sup 211}At, which emits low intensity X-rays. Our goal was to leverage state-of-the-art infrastructure at TRIUMF to produce and evaluate two related isotopes, {sup 211}Rn (t{sub 1/2}=14.6h, 73% decay to {sup 211}At) as a generator for {sup 211}At, and {sup 209}At (t{sub 1/2}=5.4h, X-ray/gamma-ray emitter) as a novel 211At surrogate for preclinical imaging studies. Methods: Produced by spallation of uranium with 480 MeV protons, mass separated ion beams of short-lived francium isotopes were implanted into NaCl targets where {sup 211}Rn or {sup 209}At were produced by radioactive decay, in situ. {sup 211}Rn was transferred to dodecane from which {sup 211}At was efficiently extracted and evaluated for clinical applicability. High energy SPECT/CT was evaluated for measuring {sup 209}At activity distributions in mice and phantoms. Results: Our small scale {sup 211}Rn/{sup 211}At generator system provided high purity {sup 211}At samples. The methods are immediately scalable to the level of radioactivity required for in vivo experiments with {sup 211}At. {sup 209}At-based high energy SPECT imaging was determined suitable for pursuing image-based dosimetry in mouse tumour models. In the future, we will utilize quantitative {sup 209}At-SPECT for image-based dose calculations. Conclusion: These early studies provided a foundation for future endeavours with {sup 211}At-based α-therapy. Canada is now significantly closer to clinical targeted α-therapy of cancer.

60 APPLIED LIFE SCIENCES↗

Development of 211-Astatine Production in the Crocker Nuclear Laboratory Cyclotron

There is a great deal of interest in the medical community in the use of the alpha-emitter 211-At as a therapeutic isotope. Among other things, its 7.2 hour half life is long enough to allow for recovery and labeling, but short enough to avoid long term activity in patients. Unfortunately, the only practical technique for its production is to bombard a 209-Bi target with a ~29 MeV alpha beam, so it is not accessible to commercial isotope production facilities, which all use fixed energy proton beams. The US Department of Energy is therefore supporting the development of a "University Isotope Network" (UIN) to satisfy this need. Our prposoal is to retrofit the variable-energy, multi-species cyclotron at the Crocker Nuclear Laboratory at the University of California Davis with an internal Bi-209 target, such that we can put at least 100 uA of 29 MeV alpha particles on target without concerns about extraction efficiency. Using very conservative assumptions, we are confident we will be able to produce 60 mCi of 211-At in solution in an eight hour shift, which includes setup, exposure, and chemical recovery. This poster will cover the design of the target, as well as the required chemical processing and reliability upgrades.

43 PARTICLE ACCELERATORS↗

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↗

Charge radii and electromagnetic moments of 214−218 Bi : Exploring the “southern” border of the 𝑍 > 82 octupole-deformation region

The changes in the mean-squared charge radii relative to 209 Bi 126 (𝛿⁢⟨𝑟 2 ⟩ 𝑁,126 ) and the magnetic dipole and electric quadrupole moments in 214−218 Bi have been measured using the in-source resonance-ionization spectroscopy technique at ISOLDE (CERN). Magnetic moments of odd-odd bismuth nuclei have been analyzed by the additivity relation. Previous tentative spin-parity and configuration assignments based on the 𝛽-decay feeding patterns have been supported. A normal odd-even staggering in charge radii of bismuth isotopes with 𝑁>126 has been observed. The new data for the 𝛿⁡⟨𝑟 2 ⟩ of bismuth isotopes allow a study of the isotonic dependencies in the charge radii, revealing jumps in 𝛿⁢⟨𝑟 2 ⟩ 132,126 and 𝛿⁢⟨𝑟 2 ⟩ 134,126 at 𝑍 = 84. This pattern could be explained by a sudden onset of octupole deformation at 𝑁 = 132 and 134 when going from polonium (𝑍 = 84) to astatine (𝑍 = 85).

fundamental symmetries↗

Production, purification and availability of 211 At: Near term steps towards global access

We report the promising characteristics of the 7.2-h radiohalogen 211 At have long been recognized; including having chemical properties suitable for labeling targeting vectors ranging from small organic molecules to proteins, and the emission of only one α-particle per decay, providing greater control over off-target effects. Unfortunately, the impact of 211 At within the targeted α-particle therapy domain has been constrained by its limited availability. Paradoxically, the most commonly used production method – via the 209 Bi(α,2n) 211 At reaction – utilizes a widely available natural material (bismuth) as the target and straightforward cyclotron irradiation methodology. On the other hand, the most significant impediment to widespread 211 At availability is the need for an accelerator capable of generating ≥28 MeV α-particles with sufficient beam intensities to make clinically relevant levels of 211 At. In this review, current methodologies for the production and purification of 211 At – both by the direct production route noted above and via a 211 Rn generator system – will be discussed. The capabilities of cyclotrons that currently produce 211 At will be summarized and the characteristics of other accelerators that could be utilized for this purpose will be described. Finally, the logistics of networks, both academic and commercial, for facilitating 211 At distribution to locations remote from production sites will be addressed.

60 APPLIED LIFE SCIENCES↗