Laura E. Wolfsberg

Proton-induced cross sections relevant to production of 225Ac and 223Ra in natural thorium targets below 200 MeV

Cross sections for (223,)(225)Ra, (225)Ac and (227)Th production by the proton bombardment of natural thorium targets were measured at proton energies below 200 MeV. Our measurements are in good agreement with previously published data and offer a complete excitation function for (223,)(225)Ra in the energy range above 90 MeV. Comparison of theoretical predictions with the experimental data shows reasonable-to-good agreement. Results indicate that accelerator-based production of (225)Ac and (223)Ra below 200 MeV is a viable production method.

225Ac and 223Ra production via 800 MeV proton irradiation of natural thorium targets

Cross sections for the formation of (225,227)Ac, (223,225)Ra, and (227)Th via the proton bombardment of natural thorium targets were measured at a nominal proton energy of 800 MeV. No earlier experimental cross section data for the production of (223,225)Ra, (227)Ac and (227)Th by this method were found in the literature. A comparison of theoretical predictions with the experimental data shows agreement within a factor of two. Results indicate that accelerator-based production of (225)Ac and (223)Ra is a viable production method.

Ac, La, and Ce radioimpurities in 225Ac produced in 40–200 MeV proton irradiations of thorium

Abstract Accelerator production of 225Ac addresses the global supply deficiency currently inhibiting clinical trials from establishing 225Acs therapeutic utility, provided that the accelerator product is of sufficient radionuclidic purity for patient use. Two proton activation experiments utilizing the stacked foil technique between 40 and 200 MeV were employed to study the likely co-formation of radionuclides expected to be especially challenging to separate from 225Ac. Foils were assayed by nondestructive γ-spectroscopy and by α-spectroscopy of chemically processed target material. Nuclear formation cross sections for the radionuclides 226Ac and 227Ac as well as lower lanthanide radioisotopes 139Ce, 141Ce, 143Ce, and 140La whose elemental ionic radii closely match that of actinium were measured and are reported. The predictions of the latest MCNP6 event generators are compared with measured data, as they permit estimation of the formation rates of other radionuclides whose decay emissions are not clearly discerned in the complex spectra collected from 232Th(p,x) fission product mixtures.

Cross sections from proton irradiation of thorium at 800 MeV

Nuclear formation cross sections are reported for 65 nuclides produced from 800-MeV proton irradiation of thorium foils. These data are useful as benchmarks for computational predictions in the ongoing process of theoretical code development and also to the design of spallation-based radioisotope production currently being considered for multiple radiotherapeutic pharmaceutical agents. Measured data are compared with the predictions of three MCNP6 event generators and used to evaluate the potential for 800-MeV productions of radioisotopes of interest for medical radiotherapy. In only a few instances code predictions are discrepant from measured values by more than a factor of two, demonstrating satisfactory predictive power across a large mass range. Similarly, agreement between measurements presented here and those previously reported is good, lending credibility to predictions of target yields and radioimpurities for high-energy accelerator-produced radionuclides.

Measurement of the 240Pu/239Pu mass ratio using a transition-edge-sensor microcalorimeter for total decay energy spectroscopy.

We have developed a new category of sensor for measurement of the (240)Pu/(239)Pu mass ratio from aqueous solution samples with advantages over existing methods. Aqueous solution plutonium samples were evaporated and encapsulated inside of a gold foil absorber, and a superconducting transition-edge-sensor microcalorimeter detector was used to measure the total reaction energy (Q-value) of nuclear decays via heat generated when the energy is thermalized. Since all of the decay energy is contained in the absorber, we measure a single spectral peak for each isotope, resulting in a simple spectral analysis problem with minimal peak overlap. We found that mechanical kneading of the absorber dramatically improves spectral quality by reducing the size of radioactive inclusions within the absorber to scales below 50 nm such that decay products primarily interact with atoms of the host material. Due to the low noise performance of the microcalorimeter detector, energy resolution values of 1 keV fwhm (full width at half-maximum) at 5.5 MeV have been achieved, an order of magnitude improvement over α-spectroscopy with conventional silicon detectors. We measured the (240)Pu/(239)Pu mass ratio of two samples and confirmed the results by comparison to mass spectrometry values. These results have implications for future measurements of trace samples of nuclear material.

Sensor and Method Development for Analysis of Alpha- and Beta-Decaying Radioisotopes Embedded InsideMicrocalorimeter Detectors

We discuss sensor and method development for the analysis of alphaand beta-decaying radioisotopes encapsulated within superconducting transition-edge sensor microcalorimeter absorbers. For alpha-decaying isotopes, e.g., 238Pu, 241Am, and 210Po, this is a measurement of the total nuclear reaction energy (Q) and the spectra consist of sharp, narrow peaks. The primary peak is at the Q value, with secondary peaks corresponding to gamma-ray-escape peaks. In contrast, for beta-decaying isotopes, e.g., 241Pu, the spectrum is a low energy continuum ending at E=Q. We are developing transition edge-sensor (TES) microcalorimeters to measure these spectra simultaneously in a single sample, hence allowing quantitative analysis of all Pu isotopes from 238 to 242. We have developed and used TES microcalorimeter detectors for this purpose, and it represents a new quantitative analysis tool for nuclear forensics and safeguards. Due to the high efficiency of the embedded source geometry, measurement times can be minimized. The high dynamic range of our sensors creates the opportunity to measure the relatively low energy beta-decay spectrum of 241Pu (Q = 20.78 keV) simultaneously with the Q ~ 5-6 MeV of alpha-decaying actinides. Finally, the technique could also be effective for determining the time since chemical purification of Pu using the 241Pu/241Am isotopic ratio via simultaneous measurement of the low-energy 241Pu beta particles and the high-energy 241Am Q-value.