XPS Study of Ion Irradiated and Unirradiated UO2 Thin Films

Teterin, Yuri A. and Popel, Aleksej J. and Maslakov, Konstantin I. and Teterin, Anton Yu. and Ivanov, Kirill E. and Kalmykov, Stepan N. and Springell, Ross and Scott, Thomas B. and Farnan, Ian (2016) XPS Study of Ion Irradiated and Unirradiated UO2 Thin Films. Inorganic Chemistry. ISSN 0020-1669, ESSN: 1520-510X

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Abstract

XPS determination of the oxygen coefficient k O =2+x and ionic (U 4+ , U 5+ and U 6+ ) composition of oxides UO 2+x formed on the surfaces of differently oriented (hkl) planes of thin UO 2 films on LSAT (Al 10 La 3 O 51 Sr 14 Ta 7 ) and YSZ (yttria-stabilized zirconia) substrates was performed. The U 4f and O 1s core-electron peak intensities as well as the U 5f relative intensity before and after the 129 Xe 23+ and 238 U 31+ irradiations were employed. It was found that the presence of uranium dioxide film in air results in formation of oxide UO 2+x on the surface with mean oxygen coefficients k O in the range 2.07-2.11 on LSAT and 2.17-2.23 on YSZ substrates. These oxygen coefficients depend on the substrate and weakly on the crystallographic orientation. On the basis of the spectral parameters it was established that uranium dioxide films AP2,3 on the LSAT substrates have the smallest k O values, and from the XRD and EBSD results it follows that these samples have a regular monocrystalline structure. The XRD and EBSD results indicate that samples AP5-7 on the YSZ substrates have monocrystalline structure, however, they have the highest k O values. The observed difference in the k O values, probably, caused by the different nature of the substrates: the YSZ substrates provide 6.4% compressive strain, whereas (001) LSAT substrates result only in 0.03% tensile strain in the UO 2 films. 129 Xe 23+ irradiation (92 MeV, 4.8 × 10 15 ions/cm 2 ) of uranium dioxide films on the LSAT substrates was shown to destroy both long range ordering and uranium close environment, which results in increase of uranium oxidation state and regrouping of oxygen ions in uranium close environment. 238 U 31+ (110 MeV, 5 × 10 10 , 5 × 10 11 , 5 × 10 12 ions/cm 2 ) irradiations of uranium dioxide films on the YSZ substrates were shown to form the lattice damage only with partial destruction of the long range ordering.

Item Type: Article
Uncontrolled Keywords: 2016AREP; IA71
Subjects: 03 - Mineral Sciences
Divisions: 03 - Mineral Sciences
Journal or Publication Title: Inorganic Chemistry
Depositing User: Sarah Humbert
Date Deposited: 28 Jul 2016 12:42
Last Modified: 11 Apr 2017 21:03
URI: http://eprints.esc.cam.ac.uk/id/eprint/3706

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