Investigating the electronic structure of fluorite-structured oxide compounds: comparison of experimental EELS with first principles calculations

被引:7
作者
Aguiar, J. A. [1 ,2 ]
Ramasse, Q. M. [3 ]
Asta, M. [1 ,4 ]
Browning, N. D. [1 ,5 ,6 ]
机构
[1] Univ Calif Davis, Dept Chem Engn & Mat Sci, Davis, CA 95616 USA
[2] Lawrence Livermore Natl Lab, Phys & Life Sci Directorate, Livermore, CA 94550 USA
[3] SuperSTEM Lab, Daresbury WA4 4AD, England
[4] Univ Calif Berkeley, Dept Mat Sci, Berkeley, CA 94720 USA
[5] Univ Calif Davis, Dept Mol & Cellular Biol, Davis, CA 95616 USA
[6] Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA
关键词
DENSITY-FUNCTIONAL-THEORY; PHOTOEMISSION SPECTRA; URANIUM-DIOXIDE; FINE-STRUCTURE; AB-INITIO; SPECTROSCOPY; ABSORPTION; ZIRCONIA; ELNES; CEO2;
D O I
10.1088/0953-8984/24/29/295503
中图分类号
O469 [凝聚态物理学];
学科分类号
070205 ;
摘要
Energy loss spectra from fluorite-structured ZrO2, CeO2, and UO2 compounds are compared with theoretical calculations based on density functional theory (DFT) and its extensions, including the use of Hubbard-U corrections (DFT + U) and hybrid functionals. Electron energy loss spectra (EELS) were obtained from each oxide using a scanning transmission electron microscope (STEM). The same spectra were computed within the framework of the full-potential linear augmented plane-wave (FLAPW) method. The theoretical and experimental EEL spectra are compared quantitatively using non-linear least squares peak fitting and a cross-correlation approach, with the best level of agreement between experiment and theory being obtained using the DFT + U and hybrid computational approaches.
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页数:9
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