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 (238U/235U = 0.00725) and enriched U. Samples exhibit extreme spatial heterogeneity in U isotopic composition with 0.02 < 235U/238U < 11.84 among all five spherules and 0.02 < 235U/238U < 7.41 within a single spherule. In two spherules, the 235U/238U 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 234U/238U, 235U/238U, and 236U/238U 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.