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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

An approach to separating Pu, U, and Ti from high-purity graphite for isotopic analysis by MC-ICP-MS

Information about elemental and isotopic systematics of ultra-trace level actinides (e.g. U and Pu) and main group elements (e.g. Ti) present within nuclear grade graphite is vital to the nuclear community for improved reactor operation and security. In support of this, extensive effort has been placed on improving analysis methods (i.e., inductively coupled plasma-mass spectrometry). However, significantly less effort has been devoted to the optimization of chemical separation methods. Within the separation community, commercially available Eichrom™ resins are often employed, as their elution characteristics for various elements have been well studied, but the direct optimization of actinides and trace metal separations from a single sample have not been widely investigated. Here, methods using various Eichrom pre-packed cartridges were explored to achieve separation of ultra-trace levels of U, Pu, and Ti from a variety of graphite samples. Once the validity of the combined separation scheme was established using certified reference materials, the method was applied to historic, unirradiated and irradiated, graphite samples. For all samples investigated, precise isotope ratio measurements for the titanium isotope systems were made.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

A new highly enriched 233 U reference material for improved simultaneous determination of uranium amount and isotope amount ratios in trace level samples

A highly-enriched 233 U reference material (>0.99987 n( 233 U)/n(U)) has been prepared and characterized for use as an isotope dilution mass spectrometry spike. An ion exchange separation was performed on 1 g of high purity 233 U to further reduce trace amounts of contaminant Pu in the material. The purified 233 U was then prepared as a master solution which was analyzed for molality of uranium by modified Davies and Gray titration. A portion of the master solution was quantitatively diluted and dispensed for reference material units. Selected units were analyzed for verification of uranium amount and to characterize uranium isotope amount ratios by multi-collector inductively couple plasma mass spectrometry. Furthermore, modelling of spike-corrected isotopic data show that the new spike will enable simultaneous measurements of uranium amount and isotope amount ratios with resulting uncertainties that are substantially less sensitive to over spiking than widely used 233 U certified reference materials.

233U↗
DOE OSTI2020

Characterization of Uranium Foil Irradiations at the WSU TRIGA Reactor Using a New Reactor Model in SCALE [Slides]

A depleted uranium foil and a highly enriched uranium foil that were irradiated at the Washington State University TRIGA reactor were used to measure the relative production of 237 U and 239 U, two key isotopes of interest in nuclear forensics, as well as their decay daughters 237 Np and 239 Pu. Total fissions in the two foils were also estimated using 99 Mo measurement. A reactor model of the TRIGA was built in the SCALE neutron transport code using dimensions obtained from an existing MCNP geometry. The model was successfully used to simulate foil fissions and the reaction rate ratios in 238 U, using the laboratory-measured isotope ratios as a benchmark. The flux distribution in the foils was determined. Finally, using the continuous energy Tsunami-3d module of SCALE, a sensitivity/uncertainty analysis was performed to determine the effects on the reaction ratio caused by other reactions in the reactor and by uncertainties in the known cross-sections.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2020

Particulate plutonium released from the Fukushima Daiichi meltdowns

Traces of Pu have been detected in material released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) in March of 2011; however, to date the physical and chemical form of the Pu have remained unknown. Here we report the discovery of particulate Pu associated with cesium-rich microparticles (CsMPs) that formed in and were released from the reactors during the FDNPP meltdowns. The Cs-pollucite-based CsMP contained discrete U(IV)O 2 nanoparticles, <~10 nm, one of which is enriched in Pu adjacent to fragments of Zr-cladding. The isotope ratios, 235 U/ 238 U, 240 Pu/ 239 Pu, and 242 Pu/ 239 Pu, of the CsMPs were determined to be ~0.0193, ~0.347, and ~0.065, respectively, which are consistent with the calculated isotopic ratios of irradiated-fuel fragments. Thus, considering the regional distribution of CsMPs, the long-distance dispersion of Pu from FNDPP is attributed to the transport by CsMPs that have incorporated nanoscale fuel fragments prior to their dispersion up to 230 km away from the Fukushima Daiichi reactor site.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
NASA NTRS2013

Constraining the Flux of Impactors Postdating Heavy Bombardment Using U-Pb Ages of Impact Glasses

Spherules of glass varying in size from a few micrometres to a few millimetres are common in the lunar regolith. While some of these glass beads are products of pyroclastic fire fountains others originate as impact melt ejected from the target that breaks into small droplets and solidifies as spherical particles while raining back to the lunar surface. These glasses preserve information about the chemical composition of the target and often contain sufficient amount of radioactive nuclides such as 40K to enable Ar-40-Ar-39 dating of individual beads. Studies measuring the age of glass beads have been used in attempts to establish variations in the flux of impactors hitting the Moon, particularly during the period that postdates the formation of major impact basins [1,2]. These studies proposed a possibility of spike in the impact flux about 800 Ma [2] and over the last 400 Ma [1]. More recently U-Th-Pb isotopic systems have been also utilized to determine the age of impact glasses from the Apollo 17 regolith [3]. Our aim is to extend the application of the U-Pb system in impact glasses to spherules isolated from Apollo 14 soil 14163 in an attempt to further investigate the applicability of this isotopic system to the chronology of impact glass beads and gain additional information on the impact flux in the inner Solar system.

Nemchin, A. A.↗
DOE OSTI2025

ATONA TE-TIMS of minor uranium isotopes (FY25 Mid-Year Report)

Isotopic measurements of the minor isotopes of uranium ( 233 U, 234 U, 236 U) are indispensable measures for material accountability and processing history but can be particularly challenging to accurately measure due to the very low abundance of the minor isotopes relative to 238 U, or 235 U in the case of highly enriched uranium (HEU). The goal of this project is to quantify detection limits for minor uranium isotope species at environmental levels (e.g 236 U/ 238 U < 10 -7 ) utilizing an ATONA-outfitted instrument and the Total Evaporation Thermal Ionization Mass Spectrometry (TE-TIMS) method. In the first half of Fiscal Year 2025, we set out to identify a suitable experimental material (Task 1) and to optimize our TE-TIMS measurement routine (Task 2). We have successfully identified a material and are in the process of getting an aliquot shipped to LANL. Simultaneously, we began working on our measurement routine utilizing CRM 112A. The results of each task are discussed in detail below.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Developing Methodology to Determine Pu Isotopic Composition by Laser Ablation MC-ICP-MS

This project will develop methodology to analyze the Pu isotope ratio in mixed U-Pu particles by laser ablation MC-ICP-MS. This will involve: 1) testing and validation of the Pu analytical method using mixed U-Pu solutions and Pu doped glasses, 2) isotopic analysis of mixed U-Pu particles by laser ablation MC-ICP-MS, and 3) continued development of the R-based data reduction program. Details regarding the analytical method development and results of QC testing will be output as a deliverable to the IAEA, along with an updated version of the LARA data reduction software.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1975

Pb loss from Apollo 17 glassy samples and Apollo 16 revisited

U-Th-Pb analyses of bulk samples of soil breccia 70019, when compared to KREEP data, indicate that different lunar samples are sometimes characterized by distinctly different initial Pb isotopic compositions. U-Th-Pb analyses on nonglassy samples and a glassy separate of soil breccia 70019, and bulk and agglutinate samples of soil 72701 showed that the glassy samples did lose considerable Pb relative to U less than 200 million years ago. These data support the contention of other investigators that vaporization of volatile elements owing to impact events significantly alters the chemistry of the lunar regolith. Metaclastic rock 60315 was reanalyzed and was found to be concordant at 3.93 billion years rather than slightly discordant, as was previously reported.

Nunes, P. D.↗
DOE OSTI2025

New NDA Methods for Thorium Fuel Cycle Safeguards (Final Report)

This project developed portable Neutron Resonance Transmission Analysis (pNRTA) as a new non-destructive assay (NDA) method for thorium fuel cycles safeguards and other applications where multiple isotopes must be measured when present together. pNRTA leverages epithermal neutron resonances to assay multiple safeguards-relevant isotopes (e.g., 233 U and 235 U) when they are present together in a sample. Existing techniques are challenged by this task, driving the need for new active interrogation methods. With selected detectors, pNRTA works in high gamma-ray backgrounds from fission and activation products and 232 U progeny expected in thorium fuel cycle samples. This project leveraged a pNRTA system developed at Pacific Northwest National Laboratory (PNNL) and collaboration with the Massachusetts Institute of Technology (MIT). The system uses a commercially available deuterium-tritium (DT) neutron generator at short standoff (2 m). Key achievements in this project included: first-of-a-kind pNRTA quantitative measurements of 233 U oxide samples, an assessment of neutron detector technologies suitable for pNRTA in high gamma-ray background environments, experimentally demonstrating quantitative assay of samples containing 233 U and 235 U, and modeling studies showing the applicability of pNRTA to a wide range of material forms. Further, a custom algorithm was developed at MIT, which provided mean bias of 9% and relative standard deviation of 36% in assaying 233 U, 235 U, 238 U, and 232 Th content in eight measured samples. These outcomes form a solid technical basis for pNRTA as a new promising capability for international safeguards verification that is portable, non-destructive, quantitative, and isotopic specific.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1992

U-Th-Pb, Rb-Sr, and Sm-Nd isotopic systematics of lunar troctolitic cumulate 76535 - Implications on the age and origin of this early lunar, deep-seated cumulate

The U-Th-Pb, Rb-Sr, and Sm-Nd isotopic systematics of four lightly leached residues of pristine, high-Mg, troctolitic cumulate 76535 were analyzed in order to determine their ages and magma sources. The data indicate that the cumulate was in isotopic equilibrium with a fluid or magma characterized by a high U-238/Pb-204 (mu) value of 600 at 4.236 Ga. Two and three stage Pb evolution calculations define even greater source mu values of about 1000, assuming low lunar initial mu values between 5 and 40 prior to about 4.43 Ga. These results are similar to mu values for KREEP sources and are also consistent with values from 78235, suggesting that at least some high-Mg suite rocks were derived from magma sources with high-mu values similar to KREEP, and support that idea that these rocks postdate primary lunar differentiation and formation of ferroan anorthosites.

Premo, Wayne R.↗
DOE OSTI2020

Discriminating Uranium Isotopes Based on Fission Signatures Induced by Delayed Neutrons

The use of active interrogation to induce delayed neutron emission is a well-established technique for the characterization of special nuclear materials. Delayed neutrons have isotope-characteristic spectral and temporal signatures, which provide the basis for isotope identification. However, in bulk materials that contain an appreciable fissile (e.g., 235 U or 233 U) fraction, such as highly enriched uranium (HEU), delayed neutrons have a high probability of inducing additional fissions. As a result, the overall delayed neutron signature consists of two distinct components: the “primary” delayed neutrons (emitted directly by fission fragments) and the “secondary prompt” fission neutrons produced in fission induced by primary delayed neutrons. These prompt products differ from “primary” delayed neutrons both in their energy spectra and in the presence of coincident radiation released by the parent fission event. The presence and relative quantity of prompt products from delayed fission depend on the cross section of the material in the energy range of delayed neutrons, which may differ significantly between isotopes, thus providing an exploitable means for isotope differentiation. Here, we demonstrate two experimental approaches for discriminating between 235 U and 238 U isotopes based on the measurement of delayed neutron-induced fission products. First, HEU and depleted uranium objects are differentiated through the detection of high-energy prompt neutrons from delayed fission using both recoil-based organic liquid scintillators and thermalization spectra from a custom-built capture-gated composite detector. Secondly, coincident radiation measurements are used as the basis for discrimination by comparing the overall rates and time evolution of fission events when delayed neutrons are present.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2026

Exploration of Neutron-Rich Isotopes around N = 50 via the In-Flight Fission of a 345 MeV/Nucleon 238 U Beam

A search for new neutron-rich isotopes beyond $Z=28$ and $N=50$ was performed using a 345 MeV/nucleon $^{238}$U beam at RI Beam Factory in RIKEN Nishina Center. The BigRIPS separator and state-of-the-art radiation detectors were used to efficiently separate and identify the produced nuclei. For the first time, we have observed and determined the production cross sections for eight neutron-rich isotopes $^{72}$Cr, $^{74,75}$Mn, $^{77}$Fe, $^{79,80}$Co, $^{85}$Cu, and $^{90}$Ga. This study broadens our understanding of nuclear existence and paves the way for investigating the properties of neutron-rich medium-mass nuclei.

Shimizu, Yohei [RIKEN, Saitama (Japan); et al.]↗
NASA NTRS2015

Investigation of Benthic Foraminiferal Non-Traditional Stable Isotopes to Reconstruct Methane Fluxes in Sedimentary Environments

Methane (CH4) is an important greenhouse gas, with a global warming potential much higher than carbon dioxide (CO2) on a short time scale. Even if the residence time of CH4 in the atmosphere is relatively short (tens of years), one of the products of CH4 oxidation is CO2, a greenhouse gas with a much longer residence time in the atmosphere (tens to hundreds of years). CH4 has been proposed as one of the trigger mechanisms for rapid global climate change today and in the geological past. With regards to the geological past, numerous studies proposed the benthic foraminiferal carbon isotope ratio (Delta13C) as a tool to reconstruct the impact of marine CH4 on rapid climate changes; however, the investigation of modern benthic foraminiferal Delta13C have produced inconclusive results. CH4 has a distinctive hydrogen isotope (Delta(D)) and Delta13C signature compared to seawater, and sulfate reduction, often coupled to CH4 anaerobic oxidation in sediments, changes the sulfur isotope signature (Delta34S) of the remaining sulfate in porewater. Therefore, we hypothesize that the Delta(D) and Delta34S signature of infaunal benthic foraminiferal species can provide a complementary approach to Delta13C to study CH4 dynamics in sedimentary environments. Here, we present the preliminary results obtained analyzing Uvigerina peregrina Delta(D) and Delta34S from three different locations at Hydrate Ridge, offshore Oregon. Unfortunately, the lack of chemical data related to the moment of foraminiferal calcification makes difficult to build a robust relationship among the U. peregrina stable isotopes and the CH4 fluxes at the sampling sites. However, our results look very promising, as each site is characterized by a different Delta(D) and Delta34S signature. We emphasize that this study represents the first step in the development of new proxies (Delta(D)) and Delta34S), which may complement the more traditional benthic foraminiferal Delta13C values, to reconstruct marine CH4 fluxes in the geological past.

Borrelli, C.↗
DOE OSTI2020

Characterization of Uranium Foil Irradiations at the WSU TRIGA Reactor Using a New Reactor Model in Scale

A new reactor model of the Washington State University TRIGA was developed in the SCALE neutron transport code, and its fidelity was verified by comparison to MCNP and available data for several reactor parameters. The model was used to characterize irradiations designed to produce the short-lived actinides 237 U and 239 U, two key isotopes for nuclear forensics. These short-lived actinides, their decay daughters 237Np and 239Pu, and total fissions (via 99 Mo) were measured in irradiated foils at Los Alamos National Laboratory and other labs with good agreement among parent/daughter pairs and among labs. The laboratory-measured isotope ratios were used as a benchmark for the model determination of reaction rates. The flux distribution in the foils was also determined. Finally, using the continuous energy TSUNAMI-3D module of SCALE, a sensitivity/uncertainty analysis was performed to determine the effects on foil reactions caused by other system-wide reactions and by uncertainties in the known cross-sections.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2024

Timescales of mafic magmatic fractionation documented by paleosecular variation in basaltic drill core, Snake River Plain volcanic province, Idaho, USA

Abstract The timescales over which fractional crystallization and recharge work in mafic volcano-plutonic provinces is subject to great uncertainty. Currently modeled processes are subject to the scale of measurement: monogenetic basaltic fields accumulate over hundreds of thousands of years, consistent with U-Th-Ra isotopic variations that imply 50% crystallization of basic magmas on timescales of 100,000 years or more, whereas crystal diffusion modeling implies phenocryst residence times of ~1–1000 years. Monogenetic basalts of the Snake River Plain in southern Idaho, USA, are up to 2 km thick and postdate passage over the Yellowstone–Snake River Plain hotspot. Detailed lithologic and geophysical logging of core from deep drill holes, along with chemical stratigraphy and high-resolution paleomagnetic inclination measurements, document individual eruptive units, compound lava flows, and basaltic flow groups that accumulated over 1–6 m.y. Hiatuses are commonly marked by loess or fluvial interbeds that vary from ~0.1 m thick to 20 m thick. Radiometric (40Ar-39Ar, detrital zircon U-Pb) and paleomagnetic timescale ages show that the deepest hole (Kimama drill hole, 1912 m total depth) accumulated over ~6 m.y. Cycles of fractional crystallization and recharge are recognized in the chemical stratigraphy as up-section shifts in major and trace elements; these fractionation cycles commonly represent 40%–50% fractionation. Individual fractionation cycles may comprise 20–40 eruptive units (8–17 lava flows) with little to no change in paleomagnetic inclination (0°–1°), whereas adjacent cycles may differ by several degrees from one another or reflect changes in polarity. Rates of paleosecular variation in Holocene lavas and sediments dated using 14C document significant shifts in magnetic inclination over short timescales, ranging from ~0.05° to 2°/decade, with an average of ~0.5°/decade and a minimum rate of 0.05°/decade. This implies that fractionation cycles with ≤1° variation in magnetic inclination formed on timescales of a few decades up to a few centuries (20–200 years). Thus, the lavas collectively represent only a few thousand years of eruptive activity, with major flow groups separated in time by tens to hundreds of thousands of years. We suggest that the rates defined by paleosecular variation capture the timescales of magmatic chamber evolution (fractionation/recharge) in the seismically imaged mid-crustal sill complex; in contrast, we suggest that crystal diffusion modeling captures the residence times in shallow subvolcanic magmatic chambers that underlie individual monogenetic volcanoes.

Geology↗
NASA NTRS2005

Lunar and Planetary Science XXXVI, Part 19

The topics include: 1) The abundances of Iron-60 in Pyroxene Chondrules from Unequilibrated Ordinary Chondrites; 2) LL-Ordinary Chondrite Impact on the Moon: Results from the 3.9 Ga Impact Melt at the Landing Site of Appolo 17; 3) Evaluation of Chemical Methods for Projectile Identification in Terrestrial and Lunar Impactites; 4) Impact Cratering Experiments in Microgravity Environment; 5) New Achondrites with High-Calcium Pyroxene and Its implication for Igneous Differentiation of Asteroids; 6) Climate History of the Polar Regions of Mars Deduced form Geologic Mapping Results; 7) The crater Production Function for Mars: A-2 Cumulative Power-Law Slope for Pristine Craters Greater than 5 km in Diameter Based on Crater Distribution for Northern Plains Materials; 8) High Resolution Al-26 Chronology: Resolved Time Interval Between Rim and Interior of a Highly Fractionated Compact Type a CAI from Efremovka; 9) Assessing Aqueous Alteration on Mars Using Global Distributions of K and Th; 10) FeNi Metal Grains in LaPaz Mare Basalt Meteorites and Appolo 12 Basalts; 11) Unique Properties of Lunar Soil for In Situ Resource Utilization on the Moon; 12) U-Pb Systematics of Phosphates in Nakhlites; 13) Measurements of Sound Speed in Granular Materials Simulated Regolith; 14) The Effects of Oxygen, Sulphur and Silicon on the Dihedral Angles Between Fe-rich Liquid Metal and Olivine, Ringwoodite and Silicate Perovskite: Implications for Planetary Core Formation; 15) Seismic Shaking Removal of Craters 0.2-0.5 km in Diameter on Asteroid 433 Eros; 16) Focused Ion Beam Microscoopy of ALH84001 Carbonate Disks; 17) Simulating Micro-Gravity in the Laboratory; 18) Mars Atmospheric Sample Return Instrument Development; 19) Combined Remote LIBS and Raman Spectroscopy Measurements; 20) Unusual Radar Backscatter Properties Along the Northern Rim of Imbrium Basin; 21) The Mars Express/NASAS Project at JPL; 22) The Geology of the Viking 2 Lander Site Revisited; 23) An Impact Genesis for Loki Patera? 24) Mars Polar Cap Edges Tracked over 3 Full Mars Years; 25) Elemental Abundance in Presolar SiC: Comparing Grains Separated by Acid Residue and Gently Separation Procedures; 26) First Results from the Descent Imager/Spectral Radiometer (DISR) Experiment on the Huygens Entry Probe of Titan; 27) Minor Element Behavior of Pallasite Olivine: Understanding Pallasite Thermal History and Chronology; 28) Canonical Anorthite in a Grosnaja Forsterite-bearing CAI; 29) Experimental Evidence for Condensation of 'Astrophysical' Carbonate; 30) Distribution and Classification of Multiple Coronae on Venus; 31) Recognition of Rayed Craters on Mars in THEMIS Thermal Infrared Imagery: Implications for Martian Meteorite Source Regions; 32) Geochemical Modeling of Evaporites on Mars: Insight from Meridiani Planum; 33) Hadean Crustal Processes Revealed from Oxygen Isotopes and U-Th-Pb Depth Profiling of Pre-4.0 Ga Detrital Zircons from Western Australia; 34) On Modeling the Seepage of Water into the Martian Subsurface; 35) Martial Gullies and Groundwater: A Series of Unfortunate Exceptions; 36) Olivine and Carbonate Globules in ALH84001: A Terrestrial Analog, and Implications for Water on Mars; 37) A Reevaluation of Mass Movements Within the Valles Marineris Region of Mars Using MOLA and MOC Data; 38) Evidence of Hydrated 109P/Swift-Tuttle Meteoroids from Meteor Spectroscopy; 39) Cr-54 Anomalies in the Solar System: Their Extent and Origin; 40) Reevaluation of the Mn-53-Cr-53 Systematic in the Basaltic Achondrites; 41) Effective Liquid Metal-Silicate Mixing Upon Shock by Power-Law Droplet Size Scaling in Richtmyer-Meshkov Like Perturbations; 42) Post-Impact Deformation of Impact Craters: Towards a Better Understanding Through the Study of Mjolnir Crater; 43) Cutting Silica Aerogel for Particle Extraction; 44) Liquid Hydrocarbons on Titan's Surface? How Cassini ISS Observations Fit into the Story (So Far); and 45) Mesoscale Simulations of Polar Circulations: Late Spring to Late Summe

Source record↗
NASA NTRSDate not supplied

Modeling 238U/204Pb (μ) and Initial Pb of Lunar Meteorite Northwest Africa 12593

Apatite Ca 5 (PO 4 ) 3 (F, Cl, OH) serves as a valuable analytical resource. It is the only nominally hydrous phase on the moon and possesses the capacity to concentrate elements like U, Th, Pb, and rare earth elements (REE). This characteristic facilitates its use in U-Pb and Pb-Pb geochronology, allowing for the determination of the initial isotopic Pb and the -238 U/ -204 Pb ratio (μ) of the parent melt. In situ analysis of apatite grains can provide a detailed record of geochemical changes, revealing the broader petrogenetic and volatile history of the source material. This mineral is particularly informative in understanding the developmental history of its source. In situ analyses are crucial for lunar samples, predominantly composed of breccias, where correlating distinct grains with whole rock analyses poses challenges. This study utilizes in situ apatite isotopic analysis of apatite grains in lunar meteorite Northwest Africa 12593 and model the initial Pb isotopic composition and -238 U/ -204 Pb (μ) of the source. We present in situ Secondary Ionization Mass Spectrometry (SIMS) Pb-Pb analyses of 12 apatite grains in Northwest Africa (NWA) 12593 to test two hypotheses: 1) NWA 12593 clasts and matrix are closely related and from the same source, and 2) the matrix material previously documented as having a highland affinity has a lower modeled μ then KREEP.

K M Lehman Franco↗
DOE OSTI2026

High sensitivity measurement of femtogram-level 238 Pu by thermal ionization mass spectrometry with correction of background 238 U

Low-concentration plutonium isotopic measurements provide a valuable fingerprint to identify possible material origins in the context of environmental contamination monitoring, environmental tracing, nuclear safeguards, nuclear forensics, and treaty monitoring. Thermal ionization mass spectrometry (TIMS) has long been recognized as one of the most sensitive techniques for plutonium isotopic measurement, but has not generally been utilized for 238 Pu determination, especially at low concentrations, due to an isobaric interference from 238 U, prevalent as background. Here, this work demonstrates a new analytical technique for correction of background 238 U from the 238 Pu counts collected during a TIMS analysis. The technique takes advantage of the higher ionization temperature of U relative to Pu and uses a 235 U tracer added after plutonium purification chemistry for 238 U semi-quantitative determination. This technique has been successfully applied to the determination of 238 Pu concentration and the 238 Pu/ 239 Pu ratio in sample types including single-isotope standards, isotopic certified reference materials, matrix-containing environmental reference materials, and simulated nuclear detonation debris. The results have been directly compared on a sample-by-sample basis to alpha spectrometry results. The detection limit by this new technique is 0.23 fg 238 Pu, which was previously unachievable by mass spectrometry and is possible in around 1 h of analysis time post-chemistry compared to weeks of required counting time by alpha spectrometry (at the same atom amount). We also present original, high precision data for Pu isotope concentrations in IAEA-384, Fangataufa Sediment, including 242 Pu results for the first time. The new technique allows measurement of a key isotope, 238 Pu, that was previously not measured in small environmental or nuclear forensics collections.

238Pu↗