Optical spectroscopy and modeling of uranium gas-phase oxidation: Progress and perspectives

Abstract In order to model the fate and transport of particles following a nuclear explosion, there must first be an understanding of individual physical and chemical processes that affect particle formation. One interaction pertinent to fireball chemistry and resultant debris formation is that between uranium and oxygen. In this study, we use laser ablation of uranium metal in different concentrations of oxygen gas, either 16 O 2 or 18 O 2 , to determine the influence of oxygen on rapidly cooling uranium. Analysis of recovered particulates using infrared absorption and Raman spectroscopies indicate that the micrometer-sized particulates are predominantly amorphous UO x (am-UO x , where 3 ≤ x ≤ 4) and UO 2 after ablation in 1 atm of pure O 2 and a 1% O 2 /Ar mixture, respectively. Energy dispersive X-ray spectroscopy (EDS) of particulates formed in pure O 2 suggest an O/U ratio of ~ 3.7, consistent with the vibrational spectroscopy analysis. Both am-UO x and UO 2 particulates convert to α-U 3 O 8 when heated. Lastly, experiments performed in 18 O 2 environments show the formation of 18 O-substituted uranium oxides; vibrational frequencies for am-U 18 O x are reported for the first time. When compared to literature, this work shows that cooling timescales can affect the structural composition of uranium oxides (i.e., crystalline vs. amorphous). This indicator can be used in current models of nuclear explosions to improve our predicative capabilities of chemical speciation. 

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The effect of oxygen concentration on the speciation of laser ablated uranium

This work reports the experimental characterization of detonation initiation modes in a confined chamber in respect to the different types of reacting waves generated in various small-diameter ignition tubes. Depending on the length of the tube and mixtures composition, four types of reacting waves can be generated and utilized to initiate detonation in the main chamber, namely the over-driven detonation ignition wave, CJ detonation ignition wave, high-speed deflagration ignition wave and deflagration ignition wave. Based on the mechanisms of detonation initiation in the main chamber, four initiation modes can be observed: the direct initiation, the local explosion initiation, and the fast and slow deflagration-to-detonation transition (DDT) initiation. By comparing the detonation initiation positions and flame-tip velocities, the first two modes show appreciably shorter initiation distances compared to the DDT modes. The over-driven detonation ignition wave is shown to yield a high probability of direct initiation, while contrary to expectation, the high-speed deflagration ignition wave exhibits superior initiation performance compared to the CJ detonation ignition wave. It is illustrated that the energy decay through diffraction and the effect of precursor shock wave reflection on the wall of the rectangular chamber are viable factors responsible for this observation. The deflagration ignition wave is also shown to be able to rapidly initiate the detonation near the inlet of the chamber, albeit with a lower success rate.

Experimental characterization of detonation initiation modes in a confined chamber flush-mounted with small-diameter ignition tubes

Surrogate nuclear explosive debris was synthesized and characterized for major, minor, and trace elemental composition as well as uranium isotopics. The samples consisted of an urban glass matrix, equal masses soda lime and cement, doped with 500 ppm uranium with varying enrichments. The surface and cross section morphology were measured with SEM, and the major elemental composition was determined by XPS. LA-ICP-MS was used to measure the uranium isotopic abundance comparing different sampling techniques. The results provide an example of the utility of LA-ICP-MS for forensics applications.

Synthesis and characterization of surrogate nuclear explosion debris: urban glass matrix

The measurement of Kr and Xe isotope ratios in nuclear explosion debris can be performed requiring little sample preparation Fragments of debris are simply crushed or heated to release trapped gases Kr and Xe arising from fission product decay As a suitable test material for this measurement, 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

The preparation of non-radioactive glassy surrogate nuclear explosion debris (SNED) loaded with isotopically altered Xe

We report a study of materials recovered from a uranium-containing plasma generated by an electric arc. The device used to generate the arc is capable of sustaining temperatures of an eV or higher for up to 100 μs. Samples took the form of a 4 μm-thick U238 film deposited onto 8 pairs of 17 μm-thick Cu electrodes supported on a 25 μm-thick Kapton backing and sandwiched between glass plates. Materials recovered from the glass plates and around the electrode tips after passage of an arc were characterized using scanning and transmission electron microscopy. Recovered materials included a variety of crystalline compounds (e.g., UO2, UC2, UCu5,) as well as mixtures of uranium and amorphous glass. Most of the materials collected on the glass plates took the form of spherules having a wide range of diameters from tens of nanometers to tens of micrometers. The composition and size of the spherules depended on location, indicating different chemical and physical environments. A theoretical analysis we have carrie...

Exploring high temperature phenomena related to post-detonation using an electric arc

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Exploring high temperature phenomena related to post-detonation using an electric arc