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

Abstract

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 235U, 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 235U/ 30Si 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 scalemore » 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.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Inst.
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1417958
Report Number(s):
LLNL-JRNL-728825
Journal ID: ISSN 0016-7037
Grant/Contract Number:
AC52-07NA27344; NA0000979
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Geochimica et Cosmochimica Acta
Additional Journal Information:
Journal Volume: 223; Journal Issue: C; Journal ID: ISSN 0016-7037
Publisher:
The Geochemical Society; The Meteoritical Society
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEFENSE; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY

Citation Formats

Weisz, David G., Jacobsen, Benjamin, Marks, Naomi E., Knight, Kim B., Isselhardt, Brett H., and Matzel, Jennifer E. Diffusive mass transport in agglomerated glassy fallout from a near-surface nuclear test. United States: N. p., 2017. Web. doi:10.1016/j.gca.2017.12.011.
Weisz, David G., Jacobsen, Benjamin, Marks, Naomi E., Knight, Kim B., Isselhardt, Brett H., & Matzel, Jennifer E. Diffusive mass transport in agglomerated glassy fallout from a near-surface nuclear test. United States. doi:10.1016/j.gca.2017.12.011.
Weisz, David G., Jacobsen, Benjamin, Marks, Naomi E., Knight, Kim B., Isselhardt, Brett H., and Matzel, Jennifer E. 2017. "Diffusive mass transport in agglomerated glassy fallout from a near-surface nuclear test". United States. doi:10.1016/j.gca.2017.12.011.
@article{osti_1417958,
title = {Diffusive mass transport in agglomerated glassy fallout from a near-surface nuclear test},
author = {Weisz, David G. and Jacobsen, Benjamin and Marks, Naomi E. and Knight, Kim B. and Isselhardt, Brett H. and Matzel, Jennifer E.},
abstractNote = {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 235U, 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 235U/30Si 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.},
doi = {10.1016/j.gca.2017.12.011},
journal = {Geochimica et Cosmochimica Acta},
number = C,
volume = 223,
place = {United States},
year = 2017,
month =
}

Journal Article:
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  • In a near-surface nuclear explosion where the resultant fireball can interact with the surface, vaporized materials from the nuclear device can be incorporated into molten soil and other carrier materials from that surface. This mixed material becomes a source of glassy fallout upon quenching and is locally deposited. Fallout formation models 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. We observe a surface deposition layer preserved at interfaces where two aerodynamicmore » fallout glasses agglomerated and fused, and characterized 11 such boundaries using spatial analyses to better understand the vaporization and condensation behavior of species in the fireball. Using nanoscale secondary ion mass spectrometry (NanoSIMS), we identify higher enrichments of uranium from the device ( 235U/ 238U ratio >7.5) in 8 of the interface layers. Major element analysis of the interfaces reveals the deposition layer to be enriched in Fe, Ca, Mg, Mn, and Na-bearing species and depleted in Ti and Al-bearing species. Most notably, the Fe and Ca-bearing species are enriched approximately 50% at the interface layer relative to the average concentrations measured within the fallout glasses, while Ti and Al-bearing species are depleted by approximately 20%. SiO 2 is found to be relatively invariable across the samples and interfaces (~3% standard deviation). The notable depletion of Al, a refractory oxide abundant in the soil, together with the enrichment of 235U and Fe, suggests an anthropogenic source of the enriched species or an unexpected vaporization/condensation behavior. The presence of both refractory (e.g., Ca and U) and volatile (e.g., Na) species approximately co-located in most of the observed layers (within 1.5 μm) suggests a continuous condensation process may also be occurring. Lastly, these fallout formation processes deviate from historical models of fallout formation, and have not been previously recognized in the literature.« less
  • Cited by 2
  • In a near-surface nuclear explosion where the resultant fireball can interact with the surface, vaporized materials from the nuclear device can be incorporated into molten soil and other carrier materials from that surface. This mixed material becomes a source of glassy fallout upon quenching and is locally deposited. Fallout formation models 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. We observe a surface deposition layer preserved at interfaces where two aerodynamicmore » fallout glasses agglomerated and fused, and characterized 11 such boundaries using spatial analyses to better understand the vaporization and condensation behavior of species in the fireball. Using nanoscale secondary ion mass spectrometry (NanoSIMS), we identify higher enrichments of uranium from the device (235U/238U ratio >7.5) in 8 of the interface layers. Major element analysis of the interfaces reveals the deposition layer to be enriched in Fe, Ca, Mg, Mn, and Na-bearing species and depleted in Ti and Al-bearing species. Most notably, the Fe and Ca-bearing species are enriched approximately 50% at the interface layer relative to the average concentrations measured within the fallout glasses, while Ti and Al-bearing species are depleted by approximately 20%. SiO2 is found to be relatively invariable across the samples and interfaces (~3% standard deviation). The notable depletion of Al, a refractory oxide abundant in the soil, together with the enrichment of 235U and Fe, suggests an anthropogenic source of the enriched species or an unexpected vaporization/condensation behavior. The presence of both refractory (e.g., Ca and U) and volatile (e.g., Na) species approximately co-located in most of the observed layers (within 1.5 μm) suggests a continuous condensation process may also be occurring. These fallout formation processes deviate from historical models of fallout formation, and have not been previously recognized in the literature.« less
    Cited by 2