Average structure and local configuration of excess oxygen in UO2+x

Wang, Jianwei; Ewing, Rodney C.; Becker, Udo

doi:10.1038/srep04216

Title: Average structure and local configuration of excess oxygen in UO2+x

Journal Article · Wed Mar 19 00:00:00 EDT 2014 · Scientific Reports

DOI:https://doi.org/10.1038/srep04216· OSTI ID:1385695

Wang, Jianwei; Ewing, Rodney C.; Becker, Udo

Determination of the local configuration of interacting defects in a crystalline, periodic solid is problematic because defects typically do not have a long-range periodicity. Uranium dioxide, the primary fuel for fission reactors, exists in hyperstoichiometric form, UO2+x. Those excess oxygen atoms occur as interstitial defects, and these defects are not random but rather partially ordered. The widely-accepted model to date, the Willis cluster based on neutron diffraction, cannot be reconciled with the first-principles molecular dynamics simulations present here. We demonstrate that the Willis cluster is a fair representation of the numerical ratio of different interstitial O atoms; however, the model does not represent the actual local configuration. The simulations show that the average structure of UO2+x involves a combination of defect structures including split di-interstitial, di-interstitial, mono-interstitial, and the Willis cluster, and the latter is a transition state that provides for the fast diffusion of the defect cluster. The results provide new insights in differentiating the average structure from the local configuration of defects in a solid and the transport properties of UO2+x.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

DOE Contract Number:: SC0001089

OSTI ID:: 1385695

Journal Information:: Scientific Reports, Vol. 4, Issue 1; Related Information: MSA partners with University of Notre Dame (lead); University of California, Davis; Florida State University; George Washington University; University of Michigan; University of Minnesota; Oak Ridge National Laboratory; Oregon state University; Rensselaer Polytechnic Institute; Savannah River National Laboratory; ISSN 2045-2322

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

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