Cyclotron production and cyclometallation chemistry of 192Ir

Introduction To explore new questions and techniques in nuclear medicine, new isotopes with novel chemical and nuclear properties must be developed. We are interested in the small cyclotron production of new radiometals for the development of new radiopharmaceuticals (RX). In an example of RX multifunctionality, Luminescence Cell Imaging (LCI) has been combined with radio-isotopes to allow compounds that can be imaged with both optical microscopy and nuclear techniques [1]. Within this field, iridium cy-clometalates have good potential with excellent photophysical properties [2]. As well, low specific activity iridium-192 has found use in brachy-therapy as a high-intensity beta emitter [3]. Despite this, iridium radioisotopes have yet to be applied to cyclometalation chemistry, or a radiochemical isolation method developed for carrier free production on a medical cyclotron. Our goal is to demonstrate the feasibility of the production and isolation of radio-iridium, and its application to cyclometalate chemistry as a potentially interesting tool for nuclear medicine research. Materials and Methods Following literature precedent [4], natural osmium was electroplated onto a silver disc from basic media containing osmium tetroxide and sulphamic acid. The thin deposits obtained (15–20 mg cm−2) were weighed and characterized with scanning electron microscopy. Targets were irradiated using the TRIUMF TR13 cyclotron, delivering 12.5 MeV protons to the target disc. Initial bombardments were per-formed at 5 μA; gamma spectra of the targets were collected 24 hours after end of bombardment. The irradiated material was oxidized, dissolved from the target backing, and separated via anion exchange. In parallel to the isotope production work, non-radioactive iridium was used to define a chemical procedure suitable for the synthesis of model iridium cyclometalate compounds given low concentrations of radioiridium. These experiments will be performed with radioactive iridium in the next step of the research project. Results and Conclusion Proton bombardment of natural osmium yielded a range of iridium isotopes, with characteristic spectral lines corresponding to 186-190Ir, and 192Ir; no other characteristic radiation was observed. The EOB activity of each isotope was then used in thin target calculations to approximate their (p,n) cross section. Preliminary cross section measurements of the 192Os(p,n)192Ir reaction (53 ± 13 mb @ 12.5 MeV) confirm published data (52.3 ± 5.7 mb @ 12.2 MeV) [6], and provide as-yet unpublished data on the lower mass number isotopes. The progress of radioactive iridium through the radiochemical separation was tracked with a dose calibrator; the osmium complex formed was brightly coloured and could be seen retained on the column. The overall efficiency of the process is estimated at 80 %. Radioactive cyclometallation chemistry is currently under-way. The production and isolation of a range of iridium isotopes in a chemically useful form was demonstrated, and is ready to be applied to a cyclometalate model compound. Future work will investigate the production of 192Ir from enriched 192Os

Highly charged ions in Penning traps, a new tool for resolving low lying isomeric states

The use of highly charged ions increases the precision and resolving power, in particular for short-lived species produced at on-line radio-isotope beam facilities, achievable with Penning trap mass spectrometers. This increase in resolving power provides a new and unique access to resolving low-lying long-lived ($T_{1/2} > 50$ ms) nuclear isomers. Recently, the $111.19(22)$ keV (determined from $\gamma$-ray spectroscopy) isomeric state in $^{78}$Rb has been resolved from the ground state, in a charge state of $q=8+$ with the TITAN Penning trap at the TRIUMF-ISAC facility. The excitation energy of the isomer was measured to be $108.7(6.4)$ keV above the ground state. The extracted masses for both the ground and isomeric states, and their difference, agree with the AME2003 and Nuclear Data Sheet values. This proof of principle measurement demonstrates the feasibility of using Penning trap mass spectrometers coupled to charge breeders to study nuclear isomers and opens a new route for isomer searches.Comment: 8 pages, 6 figure

Extinction of the N=20 neutron-shell closure for 32Mg examined by direct mass measurements

The 'island of inversion' around $^{32}$Mg is one of the most important paradigm for studying the disappearance of the stabilizing 'magic' of a shell closure. We present the first Penning-trap mass measurements of the exotic nuclides $^{29-31}$Na and $^{30-34}$Mg, which allow a precise determination of the empirical shell gap for $^{32}$Mg. The new value of 1.10(3) MeV is the lowest observed shell gap for any nuclide with a canonical magic number.Comment: 6 pages, 4 figures, submitted to Physical Review

Low-Background In-Trap Decay Spectroscopy with TITAN at TRIUMF

An in-trap decay spectroscopy setup has been developed and constructed for use with the TITAN facility at TRIUMF. The goal of this device is to observe weak electron-capture (EC) branching ratios for the odd-odd intermediate nuclei in the $\beta\beta$ decay process. This apparatus consists of an up-to 6 Tesla, open-access spectroscopy ion-trap, surrounded radially by up to 7 planar Si(Li) detectors which are separated from the trap by thin Be windows. This configuration provides a significant increase in sensitivity for the detection of low-energy photons by providing backing-free ion storage and eliminating charged-particle-induced backgrounds. An intense electron beam is also employed to increase the charge-states of the trapped ions, thus providing storage times on the order of minutes, allowing for decay-spectroscopy measurements. The technique of multiple ion-bunch stacking was also recently demonstrated, which further extends the measurement possibilities of this apparatus. The current status of the facility and initial results from a $^{116}$In measurement are presented.Comment: Proceedings for the 2nd International Conference on Advances in Radioactive Isotope Science (ARIS2014

Precision mass measurements of magnesium isotopes and implications on the validity of the Isobaric Mass Multiplet Equation

If the mass excess of neutron-deficient nuclei and their neutron-rich mirror partners are both known, it can be shown that deviations of the Isobaric Mass Multiplet Equation (IMME) in the form of a cubic term can be probed. Such a cubic term was probed by using the atomic mass of neutron-rich magnesium isotopes measured using the TITAN Penning trap and the recently measured proton-separation energies of $^{29}$Cl and $^{30}$Ar. The atomic mass of $^{27}$Mg was found to be within 1.6$\sigma$ of the value stated in the Atomic Mass Evaluation. The atomic masses of $^{28,29}$Mg were measured to be both within 1$\sigma$, while being 8 and 34 times more precise, respectively. Using the $^{29}$Mg mass excess and previous measurements of $^{29}$Cl we uncovered a cubic coefficient of $d$ = 28(7) keV, which is the largest known cubic coefficient of the IMME. This departure, however, could also be caused by experimental data with unknown systematic errors. Hence there is a need to confirm the mass excess of $^{28}$S and the one-neutron separation energy of $^{29}$Cl, which have both come from a single measurement. Finally, our results were compared to ab initio calculations from the valence-space in-medium similarity renormalization group, resulting in a good agreement.Comment: 7 pages, 3 figure

Breakdown of the Isobaric Multiplet Mass Equation for the A = 20 and 21 Multiplets

Using the Penning trap mass spectrometer TITAN, we performed the first direct mass measurements of 20,21Mg, isotopes that are the most proton-rich members of the A = 20 and A = 21 isospin multiplets. These measurements were possible through the use of a unique ion-guide laser ion source, a development that suppressed isobaric contamination by six orders of magnitude. Compared to the latest atomic mass evaluation, we find that the mass of 21Mg is in good agreement but that the mass of 20Mg deviates by 3{\sigma}. These measurements reduce the uncertainties in the masses of 20,21Mg by 15 and 22 times, respectively, resulting in a significant departure from the expected behavior of the isobaric multiplet mass equation in both the A = 20 and A = 21 multiplets. This presents a challenge to shell model calculations using either the isospin non-conserving USDA/B Hamiltonians or isospin non-conserving interactions based on chiral two- and three-nucleon forces.Comment: 5 pages, 2 figure

Far From \u27Easy\u27 Spectroscopy with the 8π and GRIFFIN Spectrometers at TRIUMF-ISAC

The 8π spectrometer, installed at the TRIUMF-ISAC facility, was the world\u27s most sensitive γ-ray spectrometer dedicated to β-decay studies. A description is given of the 8π spectrometer and its auxiliary detectors including the plastic scintillator array SCEPTAR used for β-particle tagging and the Si(Li) array PACES for conversion electron measurements, its moving tape collector, and its data acquisition system. The recent investigation of the decay of 124Cs to study the nuclear structure of 124Xe, and how the β-decay measurements complemented previous Coulomb excitation studies, is highlighted, including the extraction of the deformation parameters for the excited 0+ bands in 124Xe. As a by-product, the decay scheme of the (7+) 124Cs isomeric state, for which the data from the PACES detectors were vital, was studied. Finally, a description of the new GRIFFIN spectrometer, which uses the same auxiliary detectors as the 8π spectrometer, is given

In-beam internal conversion electron spectroscopy with the SPICE detector

The SPectrometer for Internal Conversion Electrons (SPICE) has been commissioned for use in conjunction with the TIGRESS $\gamma$-ray spectrometer at TRIUMF's ISAC-II facility. SPICE features a permanent rare-earth magnetic lens to collect and direct internal conversion electrons emitted from nuclear reactions to a thick, highly segmented, lithium-drifted silicon detector. This arrangement, combined with TIGRESS, enables in-beam $\gamma$-ray and internal conversion electron spectroscopy to be performed with stable and radioactive ion beams. Technical aspects of the device, capabilities, and initial performance are presented