Biogeochemistry of Actinides: Recent Progress and Perspective
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The total kinetic energy (TKE) release in fission is an important observable, constituting over 80% of the energy released in fission (E f ≈ 200MeV). While the TKE release in the 239 Pu(n,f) reaction was previously measured up to 50 MeV incident neutron energy (E n ), there were features in TKE release at the highest values of E n that were puzzling. There was a marked flattening of TKE release from E n = 30 to 50 MeV, in disagreement with the clearly decreasing TKE observed from E n = 0.5 to 30 MeV. To verify and clarify this trend, TKE measurements at higher values of E n were made. We present absolute measurements of TKE release in 239 Pu(n,f) from E n = 2.4 to 100 MeV. Here, we used silicon PIN detectors to measure the fragment energies and deduce mass-yield curves using the 2E-method. We also discuss fission asymmetry and the relationships between approx. fission fragment mass and distortion.
At Lawrence Livermore National Laboratory, we focus on science and technology research to ensure our nation’s security. We also apply that expertise to solve other important national problems in energy, bioscience, and the environment. Science & Technology Review is published eight times a year to communicate, to a broad audience, the Laboratory’s scientific and technological accomplishments in fulfilling its primary missions. The publication’s goal is to help readers understand these accomplishments and appreciate their value to the individual citizen, the nation, and the world.
Progress this quarter: All technical work on this project had been completed in Q2. In Q3, we only worked on summarizing the results of this 4-year project for the final report. It will be submitted separately.
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Presentation for DOE-NE Aqueous Separation 2021 PIs’ Meeting updating on the FY21 research activities of the INL Center for Radiation Chemistry Research.
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This is the poster put together for the FY 2020 LDRD Poster Session for the concluding LDRD# 19P43-006FP: Spectroscopic Studies of Covalency in Minor Actinide-Soft Donor Ligand Complexes.
Neptunium-236g is a rare radionuclide used as a tracer for neptunium-237 analyses. The availability of 236gNp is limited and the viable production routes are costly, time consuming, and only produce trace quantities of the desired product. For this work, two known production methods were tested to determine product recovery, purity, and viability for use as a tracer. The first method utilizes a photon-irradiated 237Np target to produce 236gNp by the 237Np(?,n)?236Np reaction. The second method utilizes the 238U(d,4n) ?236Np reaction. These production routes were evaluated previously, and the former was considered ineffective without isotope separation and the latter was not well-characterized for the 236mNp/236gNp production ratio. Recent resurgence of electromagnetic isotope separation technology has enabled at least partial recovery of 236gNp from part-per-million abundance feeds produced by the photonuclear reaction. To address the lack of production data for the second method, a deuteron-irradiated depleted uranium target was chemically processed to recover and purify the Np for abundance and ratio analyses. The status and current analytical results for each production method are presented.
A method for depositing actinides directly onto a 4H-SiC Schottky barrier diode (SBD) detector as a field deployable actinides sensor was developed to enable off-site analysis, shortening the time to obtain critical information such as elements, concentration, and/or isotopic ratio related to the radiological situation. A thin film of Hg was first electrodeposited onto the Pt contact of the SiC diode, followed by chronoamperometric deposition of microgram levels of actinides under conventional control conditions. The 4H-SiC diode maintained consistent functionality through the electrodeposition process and showed resolved alpha-energy spectra that contained accurate isotopic information demonstrating the feasibility of a combined chemical and radiological sensor for field actinide detection and quantification.
The separation of actinium ( 228 Ac) from radium ( 223,228 Ra) on cation exchange resin with a diethylenetriaminpentaacetic acid-lactate buffer solution is demonstrated with series of columns. High yield, high radiopurity (~ 100%) separations of Ac from Ra are feasible with small columns in biologically compatible conditions and pHs. As Ac is eluted before Ra on these columns, further studies were performed to determine if this separation system could be applied to Ra/Ac isotope generators, but these were not successful. In conclusion, the separations presented in this work may be relevant for radiopharmaceutical purifications of 225 Ac which is typically obtained from its 225 Ra parent isotope.
X-ray radiography offers the ability to noninvasively inspect the internal structure and material composition of objects. Dual-energy radiography allows material discrimination but is limited in quantitative material measurements due to the broad nature of the interrogating x-ray spectrum. Spectral radiography detectors provide an observation of not just the number of x rays that are transmitted through a sample but also the spectrum. Here, experimental validations of a method to use spectral x-ray radiography to accurately quantify the uranium mass in a powder are presented. An accurate system response model was developed, which includes a model of the incident x-ray source spectrum and a pixel-wise detector response that describes how the transmitted x rays were observed. Further, a calibration to account for the effect of partial x-ray attenuation was developed. As a result, the method is demonstrated to be capable of estimating the uranium mass in a variety of uranium oxide powders to a bias of –0.01±0.62%.
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Presentation highlight the INL Center for Radiation Chemistry Research's contributions the Material Recovery & Waste Form Development Campaign on sulfur chloride processing technologies.
The Astrobiology Primer 3.0 (ABP3.0) is a concise introduction to the field of astrobiology for students and others who are new to the field of astrobiology. It provides an entry into the broader materials in this supplementary issue of Astrobiology and an overview of the investigations and driving hypotheses that make up this interdisciplinary field. The content of this chapter was adapted from the other 10 articles in this supplementary issue and thus represents the contribution of all the authors who worked on these introductory articles. The content of this chapter is not exhaustive and represents the topics that the authors found to be the most important and compelling in a dynamic and changing field.
A study was conducted to determine if individual particle characteristics could be used to identify particles of interest, sub-samples, from bulk post-detonation debris. Three archived post-detonation debris samples were used for this effort. Particles from these samples were identified as active (produced fission tracks), and inactive (did not produce fission tracks), as the first defining characteristic. Morphology was the secondary characteristic to select particles for further study, i.e. spherical/non-spherical. Once particles were identified and isolated, they were characterized by optical microscopy for size in µm, number of fission tracks, morphology, transmitted light color, and reflected light color. Particles were then analyzed by scanning electron microscopy for morphology, elemental content, and compound identification. Raman spectroscopy was attempted on five particles with indeterminate results due to environmental mixing (heterogeneity) during the events of particle formation. Once all non-destructive analyses were completed all particles were analyzed by thermal ionization mass spectrometry to determine isotopic atom percents of plutonium and uranium, and an estimate of atoms of plutonium and uranium in each particle. An estimate of the ratio of uranium to plutonium was also obtained (U/Pu). Data analytics of the data from the particles showed that combining characteristics of the particles have a high probability of identifying particles of interest from bulk post-detonation debris samples. Please note that this version of the report is an abridged version of the full report (Wagnon et al. 2025) that has been edited to be appropriate for public release.
This milestone highlights the successful upgrade and deployment of the Radiochemical Analysis of Gaseous Samples (RAGS) system, which delivers high-quality measurements (<20% uncertainty) of activated gaseous species from NIF implosions. These measurements are critical for supporting Stockpile Stewardship Program (SSP) relevant platforms, including LANL’s Double Shell and LLNL’s Pushered Single Shell campaigns. The RAGS diagnostic technique enables analysis of short-range mixing in implosions using high-Z shells, which are otherwise inaccessible to conventional x-ray diagnostic methods. By facilitating the investigation of high-Z material mixing into fusion burn, this system provides essential data for quantifying and interpreting results in high-energy density (HED) experiments. This report details the physics motivation, diagnostic fundamentals, planned and enacted upgrade work, and the quantification of uncertainty for the upgraded system.