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We report gamma ray spectroscopy measurements of trinitite samples and analogous samples obtained from detonation sites in Nevada and Semipalatinsk, as well as in situ measurements of topsoil at the Trinity site. We also report the first isotopic composition measurements of trinitite using the novel forensics technique of decay energy spectroscopy (DES) as a complement to traditional forensics techniques. Our gamma spectroscopy and DES measurements are compared to other published results.

A rapid method for the separation and qualitative analysis of several neutron activation products (198Au, 192Ir, 72Ga, 51Cr, 191/195m/197Pt, 54Mn, 57Co, and 59Fe) from fission products and soil matrixes has been developed. Analytes were isolated within 20 h using ion exchange chromatography. After separation, the activation products were characterized by γ-spectroscopy and inductively coupled plasma-optical emission spectroscopy. Validation experiments demonstrated versatility of the method, showing that the activation products could be isolated from fresh fission products and other contaminants associated with complex soil matrixes.

Understanding actinide(III) (AnIII = CmIII, AmIII, AcIII) solution-phase speciation is critical for controlling many actinide processing schemes, ranging from medical applications to reprocessing of spent nuclear fuel. Unfortunately, in comparison to most elements in the periodic table, AnIII speciation is often poorly defined in complexing aqueous solutions and in organic media. This neglect – in large part – is a direct result of the radioactive properties of these elements, which make them difficult to handle and acquire. Herein, we surmounted some of the handling challenges associated with these exotic 5f-elements and characterized CmIII, AmIII, and AcIII using AnIII L3-edge X-ray absorption spectroscopy (XAS) as a function of increasing nitric acid (HNO3) concentration. Our results revealed that actinide aquo ions, An(H2O)x3+ (x = 9.6 ± 0.7, 8.9 ± 0.8, and 10.0 ± 0.9 for CmIII, AmIII, and AcIII), were the dominant species in dilute HNO3 (0.05 M). In concentrated HNO3 (16 M), shell-by-shell fitting of the extended X-ray fine structure (EXAFS) data showed the nitrate complexation increased, such that the average stoichiometries of Cm(NO3)4.1±0.7(H2O)5.7±1.3(1.1±0.2)−, Am(NO3)3.4±0.7(H2O)5.4±0.5(0.4±0.1)−, and Ac(NO3)2.3±1.7(H2O)8.3±5.2(0.7±0.5)+ were observed. Data obtained at the intermediate HNO3 concentration (4 M) were modeled as a linear combination of the 0.05 and 16 M spectra. For all three metals, the intermediate models showed larger contributions from the 0.05 M HNO3 spectra than from the 16 M HNO3 spectra. Additionally, these efforts enabled the Cm–NO3 and Ac–NO3 distances to be measured for the first time. Moreover, the AnIII L3-edge EXAFS results, contribute to the growing body of knowledge associated with CmIII, AmIII, and AcIII coordination chemistry, in particular toward advancing understanding of AnIII solution phase speciation.

Characterizing how actinide properties change across the f-element series is critical for improving predictive capabilities and solving many nuclear problems facing our society. Unfortunately, it is difficult to make direct comparisons across the 5f-element series because so little is known about trans-plutonium elements. Results described herein help to address this issue through isolation of An(S2CNEt2)3(N2C12H8) (Am, Cm, and Cf). These findings included the first single crystal X-ray diffraction measurements of Cm-S (mean of 2.86 ± 0.04 Å) and Cf-S (mean of 2.84 ± 0.04 Å) bond distances. Furthermore, they highlight the potential of An(S2CNEt2)3(N2C12H8) for providing a test bed for comparative analyses of actinide versus lanthanide bonding interactions.

The alpha-emitter 225Ac (t1/2 = 9.92 d) is currently under development for targeted alpha-particle therapy of cancer, and accelerator production of 225Ac via proton irradiation of thorium targets requires robust separations of 225Ac from chemically similar fission product lanthanides. Additionally, the lanthanide elements represent critical components in modern technologies, and radiolanthanides such as 140Nd (t1/2 = 3.37 d) also have potential application in the field of nuclear medicine. The ionic liquid, 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([Bmim][NTf2]), combined with the diglycolamide extractant, N,N-dioctyldiglycolamic acid (DODGAA), was adsorbed on macroporous resin support to produce a solvent impregnated resin (SIR) that was investigated for separations of 225Ac and lanthanides. The equilibrium distribution coefficients (Kd) of the rare earth elements (Sc(III), Y(III), Ln(III)), 225Ac(III), Th(IV), and U(VI) on the prepared DODGAA/[Bmim][NTf2]-SIR were determined from batch adsorption experiments in HCl and HNO3 media. The DODGAA/[Bmim][NTf2]-SIR exhibited preferential uptake of the heavier lanthanide elements while allowing for the separation of the lighter lanthanides. Column separations utilizing the DODGAA/[Bmim][NTf2]-SIR were effective at separating the lighter lanthanides from each other, and separating 225Ac from a mixture of lanthanides, 213Bi, and 225Ra without the need for additional complexing agents.

The rare earth isotope 163Ho is of interest for neutrino mass measurements. This report describes the isolation of 163Ho from a proton-irradiated dysprosium target and its purification. A Dy metal target was irradiated with 16 MeV protons for 10 h. After target dissolution, 163Ho was separated from the bulk Dy via cation-exchange high performance liquid chromatography using 70 mmol dm –3 α-hydroxyisobutyric acid as the mobile phase. Subsequent purification of the collected Ho fraction was performed to remove the α-hydroxyisobutyrate chelating agent and to concentrate the Ho in a low ionic strength aqueous matrix. The final solution was characterized by MC-ICP-MS to determine the 163Ho/165Ho ratio, 163Ho and the residual Dy content. The HPLC purification process resulted in a decontamination factor 1.4E5 for Dy. The isolated Ho fraction contained 24.8 ± 1.3 ng of 163Ho corresponding to holmium recovery of 72 ± 3%.

We demonstrate very high–resolution photon spectroscopy with a microwave-multiplexed 4-pixel transition edge sensor (TES) array. The readout circuit consists of superconducting microwave resonators coupled to radio frequency superconducting-quantum-interference devices (RF-SQUIDs) and transduces changes in input current to changes in phase of a microwave signal. We used a flux-ramp modulation to linearize the response and avoid low-frequency noise. The result is a very high-resolution photon spectroscopy with a microwave-multiplexed 4-pixel transition edge sensor array. We performed and validated a small-scale demonstration and test of all the components of our concept system, which encompassed microcalorimetry, microwave multiplexing, RF-SQUIDs, and software-defined radio (SDR). We shall display data we acquired in the first simultaneous combination of all key innovations in a 4-pixel demonstration, including microcalorimetry, microwave multiplexing, RF-SQUIDs, and SDR. We present the energy spectrum of a gadolinium-153 ( 153 Gd) source we measured using our 4-pixel TES array and the RF-SQUID multiplexer. For each pixel, one can observe the two 97.4 and 103.2 keV photopeaks. We measured the 153 Gd photon source with an achieved energy resolution of 70 eV, full width half maximum (FWHM) at 100 keV, and an equivalent readout system noise of 90 pA/pHz at the TES. This demonstration establishes a path for the readout of cryogenic x-ray and gamma ray sensor arrays with more elements and spectral resolving powers. We believe this project has improved capabilities and substantively advanced the science useful for missions such as nuclear forensics, emergency response, and treaty verification through the explored TES developments.