Plutonium segregation in glassy aerodynamic fallout from a nuclear weapon test.

This study combines electron microscopy equipped with energy dispersive spectroscopy to probe major element composition and autoradiography to map plutonium in order to examine the spatial relationships between plutonium and fallout composition in aerodynamic glassy fallout from a nuclear weapon test. A sample set of 48 individual fallout specimens were interrogated to reveal that the significant chemical heterogeneity of this sample set could be described compositionally with a relatively small number of compositional endmembers. Furthermore, high concentrations of plutonium were never associated with several endmember compositions and concentrated with the so-called mafic glass endmember. This result suggests that it is the physical characteristics of the compositional endmembers and not the chemical characteristics of the individual component elements that govern the un-burnt plutonium distribution with respect to major element composition in fallout.

Spatially-resolved analyses of aerodynamic fallout from a uranium-fueled nuclear test.

Five silicate fallout glass spherules produced in a uranium-fueled, near-surface nuclear test were characterized by secondary ion mass spectrometry, electron probe microanalysis, autoradiography, scanning electron microscopy, and energy-dispersive x-ray spectroscopy. Several samples display compositional heterogeneity suggestive of incomplete mixing between major elements and natural U ((238)U/(235)U = 0.00725) and enriched U. Samples exhibit extreme spatial heterogeneity in U isotopic composition with 0.02 < (235)U/(238)U < 11.84 among all five spherules and 0.02 < (235)U/(238)U < 7.41 within a single spherule. In two spherules, the (235)U/(238)U ratio is correlated with changes in major element composition, suggesting the agglomeration of chemically and isotopically distinct molten precursors. Two samples are nearly homogenous with respect to major element and uranium isotopic composition, suggesting extensive mixing possibly due to experiencing higher temperatures or residing longer in the fireball. Linear correlations between (234)U/(238)U, (235)U/(238)U, and (236)U/(238)U ratios are consistent with a two-component mixing model, which is used to illustrate the extent of mixing between natural and enriched U end members.

A combined theoretical and experimental investigation of uranium dioxide under high static pressure.

We have investigated the behavior of uranium dioxide (UO2) under high static pressure using a combination of experimental and theoretical techniques. We have made Raman spectroscopic measurements up to 87 GPa, electrical transport measurements up to 50 GPa from 10 K to room temperature, and optical transmission measurements up to 28 GPa. We have also carried out theoretical calculations within the GGA + U framework. We find that Raman frequencies match to a large extent, theoretical predictions for the cotunnite (Pnma) structure above 30 GPa, but at higher pressures some behavior is not captured theoretically. The Raman measurements also imply that the low-pressure fluorite phase coexists with the cotunnite phase up to high pressures, consistent with earlier reports. Electrical transport measurements show that the resistivity decreases by more than six orders of magnitude with increasing pressure up to 50 GPa but that the material never adopts archetypal metallic behavior. Optical transmission spectra show that while UO2 becomes increasingly opaque with increasing pressure, a likely direct optical band gap of more than 1 eV exists up to at least 28 GPa. Together with the electrical transport measurements, we conclude that the high pressure electrical conductivity of UO2 is mediated by variable-range hopping.

When the dust settles: stable xenon isotope constraints on the formation of nuclear fallout.

Nuclear weapons represent one of the most immediate threats of mass destruction. In the event that a procured or developed nuclear weapon is detonated in a populated metropolitan area, timely and accurate nuclear forensic analysis and fallout modeling would be needed to support attribution efforts and hazard assessments. Here we demonstrate that fissiogenic xenon isotopes retained in radioactive fallout generated by a nuclear explosion provide unique constraints on (1) the timescale of fallout formation, (2) chemical fractionation that occurs when fission products and nuclear fuel are incorporated into fallout, and (3) the speciation of fission products in the fireball. Our data suggest that, in near surface nuclear tests, the presence of a significant quantity of metal in a device assembly, combined with a short time allowed for mixing with the ambient atmosphere (seconds), may prevent complete oxidation of fission products prior to their incorporation into fallout. Xenon isotopes thus provide a window into the chemical composition of the fireball in the seconds that follow a nuclear explosion, thereby improving our understanding of the physical and thermo-chemical conditions under which fallout forms.

Solid debris collection for radiochemical diagnostics at the National Ignition Facility.

Radiochemical analysis of post-ignition debris inside the National Ignition Facility (NIF) target chamber can help determine various diagnostic parameters associated with the implosion efficiency of the fusion capsule. This technique is limited by the ability to distinguish ablator material from other debris and by the collection efficiency of the capsule debris after implosion. Prior to designing an on-line collection system, the chemical nature and distribution of the debris inside the chamber must be determined. The focus of our current work has been on evaluating capture of activated Au hohlraum debris on passive foils (5 cm diameter, 50 cm from target center) post-shot. Preliminary data suggest that debris distribution is locally heterogeneous along the equatorial and polar line-of-sights.

Improving precision in resonance ionization mass spectrometry: influence of laser bandwidth in uranium isotope ratio measurements.

The use of broad bandwidth lasers with automated feedback control of wavelength was applied to the measurement of (235)U/(238)U ratios by resonance ionization mass spectrometry (RIMS) to decrease laser-induced isotopic fractionation. By broadening the bandwidth of the first laser in a three-color, three-photon ionization process from a bandwidth of 1.8 GHz to about 10 GHz, the variation in sequential relative isotope abundance measurements decreased from 10% to less than 0.5%. This procedure was demonstrated for the direct interrogation of uranium oxide targets with essentially no sample preparation.

Constraints on the formation age of cometary material from the NASA Stardust mission.

We measured the 26Al-26Mg isotope systematics of a approximately 5-micrometer refractory particle, Coki, returned from comet 81P/Wild 2 in order to relate the time scales of formation of cometary inclusions to their meteoritic counterparts. The data show no evidence of radiogenic 26Mg and define an upper limit to the abundance of 26Al at the time of particle formation: 26Al/27Al < 1 x 10(-5). The absence of 26Al indicates that Coki formed >1.7 million years after the oldest solids in the solar system, calcium- and aluminum-rich inclusions (CAIs). The data suggest that high-temperature inner solar system material formed, was subsequently transferred to the Kuiper Belt, and was incorporated into comets several million years after CAI formation.

53Mn-53Cr dating of fayalite formation in the CV3 chondrite Mokoia: evidence for asteroidal alteration.

Fayalite grains in chondrules in the oxidized, aqueously altered CV3 chondrite Mokoia have large excesses of radiogenic chromium-53. These excesses indicate the in situ decay of short-lived manganese-53 (half-life = 3.7 million years) and define an initial 53Mn/55Mn ratio of 2.32 (+/-0.18) x 10(-6). This ratio is comparable to values for carbonates in CI and CM chondrites and for several classes of differentiated meteorites. Mokoia fayalites formed 7 to 16 million years after Allende calcium-aluminum-rich inclusions, during hydrothermal activity on a geologically active asteroid after chondritic components had ceased forming in the solar nebula.

Water on Mars: Clues from Deuterium/Hydrogen and Water Contents of Hydrous Phases in SNC Meteorites.

Ion microprobe studies of hydrous amphibole, biotite, and apatite in shergottite-nakhlite-chassignite (SNC) meteorites, probable igneous rocks from Mars, indicate high deuterium/hydrogen (D/H) ratios relative to terrestrial values. The amphiboles contain roughly one-tentn as much water as expected, suggesting that SNC magmas were less hydrous than previously proposed. The high but variable D/H values of these minerals are best explained by postcrystallization D enrichment of initially D-poor phases by martian crustal fluids with near atmospheric D/H (about five times the terrestrial value). These igneous phases do not directly reflect the D/H ratios of martian "magmatic" water but provide evidence for a D-enriched martian crustal water reservoir.

Correlated Si isotope anomalies and large 13C enrichments in a family of exotic SiC grains.

A suite of morphologically distinctive silicon carbide (SiC) grains from the Orgueil and Murchison carbonaceous chondrite meteorites contains Si and C of highly anomalous isotopic composition. All of the SiC grains in this suite are characterized by a distinctive platy morphology and roughly developed hexagonal crystal forms that allow them to be distinguished from other types of SiC found in the host meteorites. The delta 29Si and delta 30Si values of individual SiC crystals deviate from those of normal solar material by more than 100%, while the delta 13C values range from 150 to 5200%. Isotopically normal C and Si are not found in any of these SiC crystals. The SiC grains belonging to this morphological suite are isotopically distinct from fine-grained SiC aggregates and other morphological types of SiC in unequilibrated meteorites. The 29Si/28Si and 30Si/28Si ratios of these platy grains are well correlated and define a linear array that does not pass through the composition of normal, solar Si. This behavior contrasts sharply with the diverse and poorly correlated Si isotopic compositions shown by the total SiC population. We suggest that the distinctive morphological characteristics and comparatively simple Si isotope systematics identify the platy SiC crystals as a genetically related family, formed around a single, isotopically heterogeneous presolar star or an association of related stars. The enrichments in 13C and the Si isotope systematics of the platy SiC are broadly consistent with theoretical models of nucleosynthesis in low-mass, carbon stars on the asymptotic giant branch. The Si isotope array most plausibly reflects mixing between 28Si-rich material, inherited from a previous generation of stars, and material enriched in 29Si and 30Si, produced in intershell regions by neutron capture during He-burning. 13C is also produced in intershell regions by proton reactions on 12C seed nuclei and is carried with s-process nuclei to the stellar envelope by convection which penetrates down to the He shell. The absence of a correlation between the Si and C isotopic compositions of the SiC suggests either episodic condensation of SiC, extending over several thermal pulses, in the atmosphere of a single star, or derivation of the SiC from several stars characterized by different rates of 13C production. In the multiple star scenario, the linear correlation of the 29Si/28Si and 30Si/28Si ratios among the platy SiC indicates that these stars evolved from a common Si seed composition under similar conditions of neutron-capture nucleosynthesis. The 29Si/30Si ratio of the SiC, inferred by us to be produced by neutron capture in the stellar interior, is distinct from values calculated from models of nucleosynthesis in AGB stars.

Plutonium-244 fission tracks: evidence in a lunar rock 3.95 billion years old.

Tracks attributed to the spontaneous fission of plutonium-244 and of uranium-238 were detected in a large whitlockite crystal in the lunar breccia 14321 from the Fra Mauro formation. For a track-retention age of 3.95 x 10(9) years the number of plutonium tracks relative to the number of uranium tracks is 0.51 +/- 0.15, provided that the rock was not heavily neutron-irradiated 3.95 X 10(9) years ago.