电荷-晶格耦合和 UO2+x 中 U-O 分布的动态结构

J.C. Lewis, Ross Springell, Christopher Bell, Rebecca Nicholls, Jacek Wasik, L. Harding, Mahima Gupta, Janne Pakarinen, G. Baldinozzi, David Andersson, Xiaofeng Guo, S. Conradson
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引用次数: 0

摘要

通过扩展 X 射线吸收精细结构 (EXAFS) 测量原始 UO2.0、p+ 和 He2+ 辐照 UO2.0,以及在多个温度下测量块状 U4O9 和 U3O7 以及外延基底上的薄膜 U4O9-δ,研究了在晶体学和局部结构测量中观察到的 UO2+x 的不同结构和行为。辐照造成的无序主要局限于现有 U-O/U 对分布宽度的增加,任何新的邻壳都是次要的。正如之前所报道的,氧化添加到 U4O9 和 U3O7 中造成的紊乱要广泛得多,导致多位点 U-O 分布和 U-U 振幅的更大减小,在块状 U4O9 和薄膜 U4O9 中具有不同的分布。这包括所有 U4O9 和 U3O7 样品在 R = 1.2 Å 附近的重要光谱特征,该特征与 U-O 间距约为 1.7 Å 的 U-oxo 类型分子相吻合。除了表明这些异常现象只发生在混合价材料中,这项研究还证实了从 10 到 250 K U-O 分布的持续重新排列。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Charge-lattice coupling and the dynamic structure of the U–O distribution in UO2+x
The different structures and behaviors of UO2+x observed in crystallographic and local structure measurements were examined by extended X-ray absorption fine structure (EXAFS) measurements of pristine UO2.0, p+ and He2+ irradiated UO2.0, and, at multiple temperatures, bulk U4O9 and U3O7 and thin film U4O9-δ on an epitaxial substrate. The disorder caused by irradiation is mostly limited to increased widths of the existing U–O/U pair distributions, with any new neighbor shells being minor. As has been previously reported, the disorder caused by oxidative addition to U4O9 and U3O7 is much more extensive, resulting in multisite U–O distributions and greater reduction of the U–U amplitude with different distributions in bulk and thin-film U4O9. This includes the significant spectral feature near R = 1.2 Å for all U4O9 and U3O7 samples fit with a U-oxo type moiety with a U–O distance around 1.7 Å. In addition to indicating that these anomalies only occur in mixed valence materials, this work confirms the continuous rearrangement of the U–O distributions from 10 to 250 K. Although these variations of the structure are not observed in crystallography, their prominence in the EXAFS indicates that the dynamic structure underlying these effects is an essential factor of these materials.
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