Investigating incorporation and distribution of radionuclides in trinitite

Belloni, F.; Himbert, Jérôme; Marzocchi, O.; Romanello, V.

doi:10.1016/j.jenvrad.2011.05.003

Cited by 44 publications

(32 citation statements)

References 9 publications

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“…The uranium associated with the device is likely to be ionized by the high temperatures reached at the center of the detonation, typically over 10 7 K [17,23,68]. We therefore assume that uranium initially condenses and is incorporated into the glass as U(VI), the most highly ionized state observed in solid U-O phases [69,70].…”

Section: Discussionmentioning

confidence: 99%

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

Pacold

Lukens

Booth

et al. 2016

Journal of Applied Physics

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Nuclear weapons testing generates large volumes of glassy material 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.

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Section: Discussionmentioning

confidence: 99%

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

Pacold

Lukens

Booth

et al. 2016

Journal of Applied Physics

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“…Microanalytical techniques including secondary ion mass spectrometry (SIMS) and laser ablation inductively-coupled mass spectrometry (LA-ICP-MS) have made high precision, spatially resolved analysis of U isotope ratios possible, which has yielded new insights into complex materials [8][9][10][11]. For example, the isotopes of U in glassy fallout debris from a historical nuclear test have been shown to be heterogeneously distributed [12,13]. This spatially-resolved data may provide valuable information missed via bulk analysis methods.…”

Section: Introductionmentioning

confidence: 99%

Evaluation of the Homogeneity of the Uranium Isotope Composition of NIST SRM 610/611 by MC-ICP-MS, MC-TIMS, and SIMS

et al. 2014

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Abstract:As analytical and microanalytical applications employing uranium isotope ratios increase, so does the need for reliable reference materials, particularly in the fields of geochemistry, geochronology, and nuclear forensics. We present working values for uranium isotopic data of NIST 610/611 glass, collected by multicollector inductively-coupled plasma mass spectrometry (MC-ICP-MS), multicollector thermal ionization mass spectrometry (MC-TIMS), and secondary ion mass spectrometry (SIMS). The presence of depleted U, and, in this case, measureable 236 U, makes NIST 610/611 an ideal candidate for a uranium isotopic reference material for nuclear materials. We analyzed multiple chips of three different NIST 611 wafers and found no heterogeneity in U within or between the wafers, within analytical uncertainty. We determined working values and uncertainties (using a coverage factor of two) using data from this study and the literature for the following U isotope ratios:

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“…In contrast to Cold War era research focused on the distribution and dispersion of radioactive fallout particulates, these studies are typically motivated by renewed interest in interpreting details and signatures of a device having a potentially unknown origin [43,44,45,46]. For example, a study of trinitite (fallout formed in the Trinity explosion) published in 2006 measured several activation products and fission products via gamma spectroscopy in the glass, from which device characteristics were hypothesized [43].…”

Section: Contemporary Fallout Researchmentioning

confidence: 99%

“…Such studies have motivated further interest in improving the understanding of mixing relationships between device materials and soil using modern analytical techniques including scanning electron microscopy, X-ray spectroscopy, mass spectrometry [47,48,49,50,51,52,53]. Several recent studies of trinitite have focused on formation, specifically in terms of how the device material mixed with local soil [46,51,50]. One model of trinitite glass formation was put forth by Belloni, based on gamma spectroscopy and autoradiography.…”

Section: Contemporary Fallout Researchmentioning

confidence: 99%

Mass Transport of Condensed Species in Aerodynamic Fallout Glass from a Near-Surface Nuclear Test

Weisz¹

2016

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In a near-surface nuclear explosion, vaporized device materials are incorporated into molten soil and other carrier materials, forming glassy fallout upon quenching. Mechanisms by which device materials mix with carrier materials have been proposed, however, the specific mechanisms and physical conditions by which soil and other carrier materials interact in the fireball, as well as the subsequent incorporation of device materials with carrier materials, are not well constrained. A surface deposition layer was observed preserved at interfaces where two aerodynamic fallout glasses agglomerated and fused. Eleven such boundaries were studied using spatially resolved analyses to better understand the vaporization and condensation behavior of species in the fireball. Using nano-scale secondary ion mass spectrometry (NanoSIMS), we identified higher concentrations of uranium from the device in 7 of the interface layers, as well as isotopic enrichment (>75% 235 U) in 9 of the interface layers. Major element analysis of the interfaces revealed the deposition layer to be chemically enriched in Fe-, Ca-and Na-bearing species and depleted in Ti-and Al-bearing species. The concentration profiles of the enriched species at the interface are characteristic of diffusion. Three of the uranium concentration profiles were fit with a modified Gaussian function, representative of 1-D diffusion from a planar source, to determine time and temperature parameters of mass transport. By using a historical model of fireball temperature to simulate the cooling rate at the interface, the temperature of deposition was estimated to be ∼2200 K, with 1σ uncertainties in excess of 140 K. The presence of Na-species in the layers at this estimated temperature of deposition is indicative of an oxygen rich fireball. The notable depletion of Al-species, a refractory oxide that is highly abundant in the soil, together with the enrichment of Ca-, Fe-, and 235 U-species, suggests an anthropogenic source of the enriched species, together with a continuous chemical fractionation process as these species condensed.

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Investigating incorporation and distribution of radionuclides in trinitite

Cited by 44 publications

References 9 publications

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

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

Evaluation of the Homogeneity of the Uranium Isotope Composition of NIST SRM 610/611 by MC-ICP-MS, MC-TIMS, and SIMS

Mass Transport of Condensed Species in Aerodynamic Fallout Glass from a Near-Surface Nuclear Test

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