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Castro, Alonso

Publications and source records attributed to Castro, Alonso.

Sensitive Detection of an Erbium Isotope in an Atomic Beam Using Cavity Ring-Down Spectroscopy

Here, we have applied cavity ring-down spectroscopy (CRDS) to the study of the 166Er isotope in an atomic beam. These measurements were realized with an external cavity diode laser tuned to the 400.9 nm atomic transition of erbium and a customized high-finesse ring-down optical cavity under vacuum. Erbium atomic beams of different number densities were generated in a tantalum foil micro-crucible within the cavity. Absorbance values of the 166Er isotope between 3 × 10–6 and 7 × 10–5 were measured with a best-case precision on the order of 10–6, which is remarkable when considering the extreme temperatures at which the measurements were conducted, and the short detection path which is characteristic of collimated atomic beams. Number densities of erbium atoms were inferred to be between 2 × 106 and 6 × 107 cm–3. This work demonstrates for the first time the ability of studying dilute atomic beams of refractory materials with high accuracy utilizing CRDS. In these initial studies, we used erbium as a model system, but we expect to extend the proposed approach to the measurement of isotopes of uranium and plutonium for nuclear non-proliferation applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Application of saturation absorption spectroscopy to study the hyperfine structure of 235U and accurate 235U/238U isotope ratio determinations at 861.031 nm

The uranium transition 5f 3 6d7s 2 ( 5 L 6 ) → 5f 3 7s 2 7p ( 5 K 5 ) at 861.031 nm was studied using saturation absorption spectroscopy. The hyperfine structure of the 235 U isotope was determined by measuring the Doppler-suppressed absorption spectrum, and the hyperfine structure constants were obtained by employing transition-specific line strength theory and spectral fitting. The magnetic-dipole and electric-quadrupole constants were determined to be A = -3.2887 ± 0.1957 mK and B = 31.8712 ± 8.0789 mK for the upper state 5f 3 7s 2 7p ( 5 K 5 ). A theoretical calculation for the hyperfine structure constants of the 235 U isotope was also carried out by the relativistic configuration-interaction (RCI) method, and the obtained values were found to be in agreement with the measured values. In addition, the line profile of 238 U was experimentally investigated for different excitation intensities and modeled using the RCI method for estimating the transition probability and oscillator strength, with various residual broadening mechanisms considered beyond the radiative decay. Finally, we show that these results allow us to make improvements on the precision of spectral measurements using our previously developed technique for isotope ratio determinations in atomic beams.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Actinide Isotopic Analysis by Atomic Beam Laser Absorption Spectroscopy

The isotopic analysis of nuclear materials in the field has important applications in nuclear forensics for non-proliferation. In the area of safeguards, the rapid detection of isotopic signatures and ratios of uranium and plutonium reveals whether or not nuclear materials are as declared for a given facility.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Isotopic spectroscopy of uranium atomic beams produced by thermal reduction of uranium compounds

We present a method for producing atomic beams of uranium from molecular uranium precursors in a micro-crucible. In previous work, we have shown that uranium in an atomic beam can be analyzed for isotopic abundances down to enrichment levels of 0.7%. Here in this paper, we show that the same method can be utilized to analyze samples of any of the most common uranium-containing compounds to obtain the same quality of analytical results. This technique relies only on the addition of a metal species capable of reducing the uranium compound of interest. This work presents a brief discussion of the necessary criteria for thermal reduction, development and proof-of-principle of the technique using Er 2 O 3 as a non-radioactive surrogate material, and application to samples of the uranium compounds UO 2 , U 3 O 8 , UO 2 (NO 3 ) 2 , UO 2 F 2 , and UF 4 , to obtain isotope-resolved absorption spectra from an atomic beam produced from these molecular precursors.

Bartlett, Joshua H.↗

Nuclear recoil spectroscopy of levitated particles

Here, we propose a method for the detection and characterization of nuclear decay processes. Specifically, we describe how nuclear decay recoil can be observed within small particles levitated in an optical trap with high positional resolution. Precise measurements of the magnitude of each recoil as well as their rate of occurrence can provide accurate information about the isotopic composition of a radioactive sample. We expect that this technique for nuclear material characterization will be especially useful in the area of nuclear forensic analysis.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Isotope-resolved atomic beam laser spectroscopy of natural uranium

Here, we present our results on the development of a technique for conducting laser absorption spectroscopy of uranium in a collimated atomic beam using a compact and potentially fieldable device. A solid natural uranium metal sample is vaporized in a modest vacuum of several mTorr via resistive heating of a tantalum foil micro-crucible. A temperature of over 2000 °C is reached by applying only 200 W of electrical power to the crucible. At this temperature, the vapor pressure of uranium is large enough to generate a stable atomic beam. A diode laser is tuned around the 861.031 nm uranium transition, which allows the observation of absorption bands from both the 238 U and 235 U isotopes. The isotopic composition of uranium Standard Reference Material 960 is obtained from the absorption signal, in excellent agreement with the nominal value. In conclusion, our approach can be readily applied to the isotopic analysis of other actinides, and it is expected to lead to the development of compact, fieldable instrumentation.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Note: Micro-channel array crucible for isotope-resolved laser spectroscopy of high-temperature atomic beams

Here, we present a novel compact design for a multichannel atomic oven which generates collimated beams of refractory atoms for fieldable laser spectroscopy. Using this resistively heated crucible, we demonstrate spectroscopy of an erbium sample at 1300 °C with improved isotopic resolution with respect to a single-channel design. In addition, our oven has a high thermal efficiency. By minimizing the surface area of the crucible, we achieve 2000 °C at 140 W of applied electrical power. As a result, the design does not require any active cooling and is compact enough to allow for its incorporation into fieldable instruments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Solid-phase extraction microfluidic devices for matrix removal in trace element assay of actinide materials

Advances in sample nebulization and injection technology have significantly reduced the volume of solution required for trace impurity analysis in plutonium and uranium materials. Correspondingly, we have designed and tested a novel chip-based microfluidic platform, containing a 100-µL or 20-µL solid-phase microextraction column, packed by centrifugation, which supports nuclear material mass and solution volume reductions of 90% or more compared to standard methods. Quantitative recovery of 28 trace elements in uranium was demonstrated using a UTEVA chromatographic resin column, and trace element recovery from thorium (a surrogate for plutonium) was similarly demonstrated using anion exchange resin AG MP-1. Of nine materials tested, compatibility of polyvinyl chloride (PVC), polypropylene (PP), and polytetrafluoroethylene (PTFE) chips with the strong nitric acid media was highest. Finally, the microcolumns can be incorporated into a variety of devices and systems, and can be loaded with other solid-phase resins for trace element assay in high-purity metals.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Atomic Beam Laser Spectrometer for In-field Isotopic Analysis

This is a powerpoint presentation for the DTRA quarterly program review that goes into detail about the atomic beam laser spectrometer for in-field isotopic analysis. The project goals are the following: analysis of post-detonation debris, determination of U and Pu isotopic composition, and fieldable prototype: < 2ft 3 , < 1000W.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Analytical Chemistry and Materials Characterization Results for Debris Recovered from Nitrate Salt Waste Drum S855793

Solid debris was recovered from the previously-emptied nitrate salt waste drum S855793. The bulk sample was nondestructively assayed for radionuclides in its as-received condition. Three monoliths were selected for further characterization. Two of the monoliths, designated Specimen 1 and 3, consisted primarily of sodium nitrate and lead nitrate, with smaller amounts of lead nitrate oxalate and lead oxide by powder x-ray diffraction. The third monolith, Specimen 2, had a complex composition; lead carbonate was identified as the predominant component, and smaller amounts of nitrate, nitrite and carbonate salts of lead, magnesium and sodium were also identified. Microfocused x-ray fluorescence (MXRF) mapping showed that lead was ubiquitous throughout the cross-sections of Specimens 1 and 2, while heteroelements such as potassium, calcium, chromium, iron, and nickel were found in localized deposits. MXRF examination and destructive analysis of fragments of Specimen 3 showed elevated concentrations of iron, which were broadly distributed through the sample. With the exception of its high iron content and low carbon content, the chemical composition of Specimen 3 was within the ranges of values previously observed in four other nitrate salt samples recovered from emptied waste drums.

Inorganic, Organic, Physical, & Analytical Chemist↗

Analytical Chemistry Developmental Work Using a 243 Am Solution

This project seeks to reestablish our analytical capability to characterize Am bulk material and develop a reference material suitable to characterizing the purity and assay of 241 Am oxide for industrial use. The tasks associated with this phase of the project included conducting initial separations experiments, developing thermal ionization mass spectrometry capability using the 243 Am isotope as an isotope dilution spike , optimizing the spike for the determination of 241 Pu- 241 Am radiochemistry, and, additionally, developing and testing a methodology which can detect trace to ultra- trace levels of Pu (both assay and isotopics) in bulk Am samples .

Inorganic, Organic, Physical, & Analytical Chemist↗