Abstract
Our works shows that the americium pyrochlore (241)Am(2)Zr(2)O(7) undergoes a phase transition to a defect-fluorite structure along with an unusual volume contraction when subjected to internal radiation from alpha-emitting actinides. Disorder relaxation proceeds through the simultaneous formation of cation antisites and oxygen Frenkel pairs. X-ray absorption spectroscopy at the Am-L(II) and the Zr-K edges reveals that Am-O polyhedra show an increasing disorder with increasing exposure. In contrast, the Zr-O polyhedral units remain highly ordered, while rotating along edges and corners, thereby reducing the structural strain imposed by the growing disorder around americium. We believe it is this particular property of the compound that provides the remarkable resistance to radiation (>9.4 x 10(18) alpha-decay events g(-1) or 0.80 dpa).
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