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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

A geochemical approach to constraining the formation of glassy fallout debris from nuclear tests

Reprocessed earth material is a glassy nuclear fallout debris from near-surface nuclear tests. A geochemical approach to analysis of glassy fallout is uniquely suited to determine the means of reprocessing and shed light on the mechanisms of fallout formation. An improved understanding of fallout formation is of interest both for its potential to guide post-detonation nuclear forensic investigations and in the context of possible affinities between glassy debris and other glasses generated by high-energy natural events, such as meteorite impacts and lightning strikes. Our study presents a large major-element compositional dataset for glasses within aerodynamic fallout from the Trinity nuclear test (“trinitite”) and a geochemically based analysis of the glass compositional trends. Silica-rich and alkali-rich trinitite glasses show compositions and textures consistent with formation through melting of individual mineral grains—quartz and alkali feldspar, respectively—from the test-site sediment. Furthermore, the volumetrically dominant glass phase—called the CaMgFe glass—shows extreme major-element compositional variability. Compositional trends in the CaMgFe glass are most consistent with formation through volatility-controlled condensation from compositionally heterogeneous plasma. Radioactivity occurs only in CaMgFe glass, indicating that co-condensation of evaporated bulk ground material and trace device material was the main mechanism of radioisotope incorporation into trinitite. CaMgFe trinitite glasses overlap compositionally with basalts, rhyolites, fulgurites, tektites, and microtektites but display greater compositional diversity than all of these naturally formed glasses. Indeed, the most refractory CaMgFe glasses compositionally resemble early solar system condensates—specifically, CAIs.

58 GEOSCIENCES↗
DOE OSTI2023

Laser Driven Hydrothermal Processing (LDHP) for Rapid Dissolution of Glassy Nuclear Debris

Discovered in 2009 on the SLAB laser system at LLNL, Laser-Driven Hydrothermal Processing (LDHP) both spalls and transiently dissolves a wetted surface (e.g., rock, concrete, paint) when that surface is struck by a laser beam pulse under specific conditions. Previous projects have explored the application of LDHP to expediting sample dissolution for post-detonation nuclear forensics. Early results were very promising, indicating that this method could decrease material dissolution time by a factor of 10 or more. However, the large and complicated lasers previously used are impractical for this application. Under the R^3 venture we aimed to benchmark the LDHP capabilities of turn-key commercial off-the-shelf (COTS) lasers, and to establish how this process could be integrated into an analytical workflow for nuclear forensic analysis. We demonstrated that geological rock standards could be quickly processed into fine powder by LDHP followed by complete acid digestion in 15 minutes, without elemental fractionation that would skew analytical results. We determined that the COTS laser can be used for LDHP that could potentially reduce dissolution time for solid nuclear debris samples in post detonation nuclear forensics. One downside to this approach, however, is that the laser interactions are different with every material, so extensive method validation would be required for all likely material compositions. The LDHP processing rates of several materials were tested and determined to be favorable in the beginning with significant slowdown due to particulate scattering. This could be mitigated either by stopping and centrifuging the sample at specific intervals, or through design of a continuous solvent flow through mechanism.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Measurements of extinct fission products in nuclear bomb debris: Determination of the yield of the Trinity nuclear test 70 y later

This study describes an approach to measuring extinct fission products that would allow for the characterization of a nuclear test at any time. The isotopic composition of molybdenum in five samples of glassy debris from the 1945 Trinity nuclear test has been measured. Nonnatural molybdenum isotopic compositions were observed, reflecting an input from the decay of the short-lived fission products 95 Zr and 97 Zr. By measuring both the perturbation of the 95 Mo/ 96 Mo and 97 Mo/ 96 Mo isotopic ratios and the total amount of molybdenum in the Trinity nuclear debris samples, it is possible to calculate the original concentrations of the 95 Zr and 97 Zr isotopes formed in the nuclear detonation. Together with a determination of the amount of plutonium in the debris, these measurements of extinct fission products allow for new estimates of the efficiency and yield of the historic Trinity test.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

U-Pu and Ba-Cs isotopic measurements on Trinitite by laser ablation sampling on the Neoma MC-ICP-MS

In this study we present the results of combined U-Pu and Ba-Cs isotope measurements obtained by laser ablation (LA) sampling of two glassy debris fragments (‘Trinitite’) from the world's first atomic bomb detonation conducted in New Mexico on July 16, 1945. Our primary goal in conducting these measurements was to understand whether examination of the U-Pu and Ba-Cs systematics by direct sampling (e.g. without any chemical separation or purification prior to isotope ratio measurement) could yield meaningful information that would differentiate the Trinitite fragments from glassy material lacking a nuclear fission signature. These measurements were conducted on a ThermoFisher Scientific Neoma multi collector – inductively coupled plasma – mass spectrometer (MC-ICP-MS), which is a relatively new MC-ICP-MS platform, so we also examine the behavior of these isotope systems in standards sampled in solution and via LA. Unsurprisingly, the measurements made on purified solutions of the U, Pu, and Ba isotopic standards produce high precision isotope ratios. Furthermore, this extends to the U-Pu measurements made by LA sampling, with the expected degradation in precision and accuracy related to matrix effects and signal intensity fluctuation. However, the Ba-Cs data acquired by LA is of low precision across all of the matrices examined and bears evidence of complex mass fractionation that will require further investigation to resolve. In total, our results indicate that the observed U-Pu isotope data are of sufficient quality to accurately constrain the U and Pu isotopic composition of glass containing sub-ppm levels of these elements which in turn could be used to differentiate glass containing anthropogenic fission products from natural glass whereas the Ba-Cs LA data cannot be used for this purpose until further methodological refinement is performed.

Ba-Cs↗
DOE OSTI2019

Interpreting mixing relationships in energetic melts to estimate vapor contribution and composition

Heterogeneous, glassy debris can be produced by energetic events such as near surface nuclear explosions and asteroid impacts. In these events, the resultant debris comprises a rapidly-cooled mixture of the projectile or bomb material with proximate materials such as soil and anthropogenic structures. Glasses formed in these events preserve inter and/or intra sample compositional variation reflecting complex mixtures of the precursor materials or their chemically fractionated products. Understanding formation mechanisms and chemical processes relating to energetic glass formation based on study of the end products requires an objective method for calculating the precursor components that mixed together to produce the final product. Here, we compare a set of multivariate linear-least squares approaches to address the unmixing problem of heterogeneous glasses including classical least squares (CLS), principal component analysis (PCA) and two multivariate curve resolution – alternating least squares (MCR-ALS) approaches. We generate a synthetic data set representing spatially resolved, compositional data in a set of heterogeneously mixed glasses to understand model sensitivity to precursor abundance and composition. We explore the impact of incomplete knowledge of the system prior to the formation of the melts on the resulting confidence and accuracy of the solution (i.e., the number, composition, and abundances of the precursor materials). We conclude that a closure and equality constrained MCR-ALS approach succeeds in identifying unrecognized precursor components and is a suitable alternative to CLS approaches when the investigator has incomplete knowledge of the starting precursor chemical compositions. Finally, we demonstrate application of this MCR-ALS approach to measurements of Trinitite.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2016

The Preparation of Non-radioactive Glassy Surrogate Nuclear Explosion Debris (SNED) Loaded with an Isotopically Altered Noble Gas

The measurement of the Kr and Xe isotope ratios in nuclear explosion debris is an important forensic tool as the method requires very little sample preparation. Fragments of debris are simply crushed or heated to release the trapped gases Kr and Xe arising from fission product decay. As suitable test materials are not readily available we have been investigating a method to incorporate isotopically enriched 129Xe in glassy materials that mimic nuclear explosion debris. The approach used to prepare these materials will be described along with some of the example results obtained.

Trinitite, Nuclear forensics, Fission Xe, Surrogat↗
DOE OSTI2017

Tracking Radionuclide Fractionation in the First Atomic Explosion Using Stable Elements

Compositional analysis of postdetonation fallout is a tool for forensic identification of nuclear devices. However, the relationship between device composition and fallout composition is difficult to interpret because of the complex combination of physical mixing, nuclear reactions, and chemical fractionations that occur in the chaotic nuclear fireball. By using a combination of in situ microanalytical techniques (electron microprobe analysis and secondary ion mass spectrometry), we show that some heavy stable elements (Rb, Sr, Zr, Ba, Cs, Ba, La, Ce, Nd, Sm, Dy, Lu, U, Th) in glassy fallout from the first nuclear test, Trinity, are reliable chemical proxies for radionuclides generated during the explosion. Stable-element proxies show that radionuclides from the Trinity device were chemically, but not isotopically, fractionated by condensation. Moreover, stable-element proxies delineate chemical fractionation trends that can be used to connect present-day fallout composition to past fireball composition. Stable-element proxies therefore offer a novel approach for elucidating the phenomenology of the nuclear fireball as it relates to the formation of debris and the fixation of device materials within debris.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1972

Mineralogy and origin of Fra Mauro fines and breccias.

Textural features, glassy spherule and glassy aggregate contents, and size-frequency distributions of lithic components of the regolith fines indicate that the Fra Mauro regolith of the smooth terrain is a highly reworked accumulation of debris derived primarily by impact comminution of annealed breccias. Analyses of the glassy spherules suggest that mare-derived debris must amount to less than 5% of the regolith, but exotic materials having the composition of the Fra Mauro breccias (highland-like) cannot be recognized. Breccia samples from the Fra Mauro site include (1) regolith breccias derived by lithification of local regolith material, (2) texturally and compositionally unique white rock breccias that may have been derived from ancient ejecta buried beneath the Fra Mauro formation, and (3) annealed breccias that are excavated samples of the Fra Mauro formation. The latter were deposited as heated impact ejecta, probably by avalanches produced by the Imbrian event and were annealed in situ in a thermal regime perhaps equivalent to that responsible for the pyroxene-hornfels facies of metamorphism in terrestrial rocks.

Quaide, W.↗
DOE OSTI2016

Synthesis and Analysis of Glass Analogs for Solid Fallout Debris

Following a nuclear detonation, radiochemists and post-detonation debris diagnosticians are tasked with performing high-quality analysis of fallout debris samples and accurate device interpretation. Debris formed following a nuclear detonation commonly consists of a heterogeneous glassy matrix containing uranium, plutonium, neptunium, americium, and fission/activation products. Homogeneous and well-characterized reference materials are critical for accurate post-detonation debris analysis. Such reference materials can include aged nuclear explosion debris from the Nevada Test Site (e.g., Trinitite) as well as 'fresh' doped-glass material. Recent work has highlighted the often heterogeneous nature of historical debris, which presents a problem from the aspects of safeguards accountancy and verification as well as micro-scale characterization (i.e., microbeam analysis). In this regard, our work focuses on the creation of homogeneous, 'fresh' doped-glassy standards containing uranium, plutonium, surrogate fission products (e.g., Sr, Cs, Pm, Sm, Eu), and urban material (e.g., Fe and Ca from construction material, stainless steel, aluminosilicates phases as a surrogate for dirt). (authors)

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2017

Nominations for the 2017 NNSA Pollution Prevention Awards

In the field of nuclear forensics, one of the biggest challenges is to dissolve postdetonation debris for analysis. Debris generated after a nuclear detonation is a glassy material that is difficult to dissolve with chemicals. Traditionally, concentrated nitric acid, hydrofluoric acid, or sulfuric acid are employed during the dissolution. These acids, due to their corrosive nature, are not suitable for in-field/on-site sample preparations. Uranium oxides are commonly present in nuclear fuel processing plants and nuclear research facilities. In uranium oxides, the level of uranium isotope enrichment is a sensitive indicator for nuclear nonproliferation and is monitored closely by the International Atomic Energy Agency (IAEA) to ensure there is no misuse of nuclear material or technology for nuclear weapons. During an IAEA on-site inspection at a facility, environmental surface swipe samples are collected and transported to the IAEA headquarters or network of analytical laboratories for further processing. Uranium oxide particles collected on the swipe medium are typically dissolved with inorganic acids and are then analyzed for uranium isotopic compositions. To improve the responsiveness of on-site inspections, in-field detection techniques have been recently explored. However, in-field analysis is bottlenecked by time-consuming and hazardous dissolution procedures, as corrosive inorganic acids must be used. Corrosive chemicals are difficult to use in the field due to personnel safety considerations, and the transportation of such chemicals is highly regulated. It was therefore necessary to develop fast uranium oxide dissolution methods using less hazardous chemicals in support of the rapid infield detection of anomalies in declared nuclear processes.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2012

HD 172555: Detection of 63 micrometers [OI] Emission in a Debris Disc

Context. HD 172555 is a young A7 star belonging to the Beta Pictoris Moving Group that harbours a debris disc. The Spitzer IRS spectrum of the source showed mid-IR features such as silicates and glassy silica species, indicating the presence of a warm dust component with small grains, which places HD 172555 among the small group of debris discs with such properties. The IRS spectrum also shows a possible emission of SiO gas. Aims. We aim to study the dust distribution in the circumstellar disc of HD 172555 and to asses the presence of gas in the debris disc. Methods. As part of the GASPS Open Time Key Programme, we obtained Herschel-PACS photometric and spectroscopic observations of the source. We analysed PACS observations of HD 172555 and modelled the Spectral Energy Distribution (SED) with a modified blackbody and the gas emission with a two-level population model with no collisional de-excitation. Results. We report for the first time the detection of [OI] atomic gas emission at 63.18 micrometers in the HD 172555 circumstellar disc.We detect excesses due to circumstellar dust toward HD 172555 in the three photometric bands of PACS (70, 100, and 160 m). We derive a large dust particle mass of (4.8 plus-minus 0.6)x10(exp -4) Mass compared to Earth and an atomic oxygen mass of 2.5x10(exp -2)R(exp 2) Mass compared to Earth, where R in AU is the separation between the star and the inner disc. Thus, most of the detected mass of the disc is in the gaseous phase.

Riviere-Marichalar, P.↗
NASA NTRS1993

A discontinuous melt sheet in the Manson impact structure

Petrologic studies of the core recovered from holes drilled in the Manson, Iowa, buried impact structure may unravel the thermal history of the crater-fill debris. We made a cursory examination of about 200 m of core recovered from the M-1 bore hole. The M-1 bore hole was the first of 12 holes drilled as part of a cooperative drilling program between the U.S. Geological Survey and the Iowa Geological Survey Bureau. The M-1 core hole is about 6 km northeast of the center of the impact structure, apparently on the flank of its central peak. We developed a working hypothesis that a 30-m-thick breccia unit within a 53-m-thick unit previously termed the 'crystalline clast breccia with glassy matrix' is part of a discontinuous melt sheet in the crater-fill impact debris. The 30-m-thick breccia unit reached temperatures sufficient to partially melt some small breccia clasts and convert the fine-grained breccia matrix into a silicate melt that cooled to a greenish-black, flinty, microcrystalline rock. The results of the investigation of this unit are presented.

Izett, G. A.↗
DOE OSTI2016

Chemical speciation of U, Fe, and Pu in melt glass from nuclear weapons testing

Nuclear weapons testing generates large volumes of glassy materials that influence the transport of dispersed actinides in the environment and may carry information on the composition of the detonated device. We determine the oxidation state of U and Fe (which is known to buffer the oxidation state of actinide elements and to affect the redox state of groundwater) in samples of melt glass collected from three U.S. nuclear weapons tests. For selected samples, we also determine the coordination geometry of U and Fe, and we report the oxidation state of Pu from one melt glass sample. We find significant variations among the melt glass samples and, in particular, find a clear deviation in one sample from the expected buffering effect of Fe(II)/Fe(III) on the oxidation state of uranium. In the first direct measurement of Pu oxidation state in a nuclear test melt glass, we obtain a result consistent with existing literature that proposes Pu is primarily present as Pu(IV) in post-detonation material. In addition, our measurements imply that highly mobile U(VI) may be produced in significant quantities when melt glass is quenched rapidly following a nuclear detonation, though these products may remain immobile in the vitrified matrices. The observed differences in chemical state among the three samples show that redox conditions can vary dramatically across different nuclear test conditions. The local soil composition, associated device materials, and the rate of quenching are all likely to affect the final redox state of the glass. The resulting variations in glass chemistry are significant for understanding and interpreting debris chemistry and the later environmental mobility of dispersed material.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1980

Hypervelocity impacts on Skylab IV/Apollo windows

A description is presented of some new observations of crater morphology on the Skylab IV/Apollo windows. Aluminum is detected as the only foreign component in six of the seven lined glassy pit craters so far examined by EDS analysis. The most probable source is from aluminum oxide spherules, exhaust effluent of solid fuel rocket motors. The seventh crater contains titanium which may have been derived from an impact of a chip of thermal paint. The size distribution of the lined glassy pit craters appears to be compatible with an origin by hypervelocity impacts of aluminum spherules. If the aluminum oxide spherules are in earth orbit, impact velocities largely in the range of 7 to 10 km/s should be expected. Thus, the impact velocities are well below those expected for most impacts by micrometeorites and these lower velocities may be significant in the development of the lined glassy pit craters. The results indicate that there is a significant population of man-induced micro-debris in earth orbit.

Clanton, U. S.↗
DOE OSTI2020

Spatially-Resolved Characterization Techniques and Their Implications for Nuclear Debris Formation.

Debris from nuclear tests has a complex formation process and can inform multiple fields of study such as geology, atmospheric science, shock physics, and chemistry under extreme conditions. Macroscopic nuclear debris forms as the result of fireball interaction with surrounding materials (e.g., structural and environmental component), which rapidly undergo melting and vaporization followed by condensation, convective/diffusive mixing, and solidification over the course of seconds. In atmospheric events, some of this material may disperse over long distances, but much of the material is deposited close-in to ground zero, often in multicomponent, partially (or entirely) amorphous debris formations. During the U.S. nuclear testing program, this material was collected and analyzed, particularly for radionuclide composition. Fallout formation models were developed from nuclear test data based on such radionuclide compositional analyses. These models were not just used to understand fallout dispersion (i.e. the spread of radioactivity over geographical regions) but also guide radiochemical interpretations of historical nuclear tests.6 Developments in analytical techniques over the past several decades have made it possible to make new analyses on historical debris, some of which may be more than a half-century old. For example, inductively-coupled plasma mass spectrometry (ICP-MS) has been used to look at the trace elements in glassy fallout material from aboveground nuclear tests (including the Trinity test). Advanced analyses using X-ray absorption allowed for the measurement of oxidation state of fallout constituents, including actinides. The ability to measure trace actinides and their subsequent oxidation state is important to understanding how the surrounding environment may have influenced the resultant fallout composition and may have implications for why certain fractionation trends have been observed. Here we present data from historic nuclear test debris illustrating the power of spatially resolved methods to connect interaction of the near-field environment with the explosion and provide new insights into nuclear debris formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Generating aerodynamic surrogate nuclear explosion debris (SNED)

So called “aerodynamic debris” has often been observed from explosion debris collected on the fringe of surface nuclear tests, and is assumed to result from ejection of melted and re-condensing ground materials drawn up into the rising explosion fireball. The material forms small glassy particulates measuring ~1mm, ranging in shape from near perfectly spherical glassy beads to more elongated forms and occasionally agglomerates of two or more particles displaying some degree of fusion. Producing material with a similar range of characteristics in the laboratory may be quite challenging, as the temperatures required can exceed 1500°C while keeping the particulates suspended in constant motion. In this paper we describe an apparatus that can heat lofted sediment particulates up to 1mm very rapidly above their melting points, allowing extended interactions times from seconds to minutes. Examples of the different material forms produced will be compared to real aerodynamic debris recovered from nuclear explosions described in the literature.

Liezers, M.↗
DOE OSTI2017

Diffusive mass transport in agglomerated glassy fallout from a near-surface nuclear test

Aerodynamically-shaped glassy fallout is formed when vapor phase constituents from the nuclear device are incorporated into molten carriers (i.e. fallout precursor materials derived from soil or other near-field environmental debris). The effects of speciation and diffusive transport of condensing constituents are not well defined in models of fallout formation. Previously we reported observations of diffuse micrometer scale layers enriched in Na, Fe, Ca, and 235 U, and depleted in Al and Ti, at the interfaces of agglomerated fallout objects. Here in this paper, we derive the timescales of uranium mass transport in such fallout as it cools from 2500 K to 1500 K by applying a 1-dimensional planar diffusion model to the observed 235 U/ 30 Si variation at the interfaces. By modeling the thermal transport between the fireball and the carrier materials, the time of mass transport is calculated to be <0.6 s, <1 s, <2 s, and <3.5 s for fireball yields of 0.1 kt, 1 kt, 10 kt, and 100 kt respectively. Based on the calculated times of mass transport, a maximum temperature of deposition of uranium onto the carrier material of ~2200 K is inferred (1σ uncertainty of ~200 K). We also determine that the occurrence of micrometer scale layers of material enriched in relatively volatile Na-species as well as more refractory Ca-species provides evidence for an oxygen-rich fireball based on the vapor pressure of the two species under oxidizing conditions. These results represent the first application of diffusion-based modeling to derive material transport, thermal environments, and oxidation-speciation in near-surface nuclear detonation environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗