[PDF] Chemical bonding in americium oxides: x-ray spectroscopic view-论文阅读讨论-ReadPaper

摘要

The electronic structure and the chemical state in Am binary oxides andAm-doped UO$_2$ were studied by means of x-ray absorption spectroscopy atshallow Am core ($4d$ and $5d$) edges. In particular, the Am $5f$ states wereprobed and the nature of their bonding to the oxygen states was analyzed. Theinterpretation of the experimental data was supported by the Anderson impuritymodel (AIM) calculations which took into account the full multiplet structuredue to the interaction between $5f$ electrons as well as the interaction withthe core hole. The sensitivity of the branching ratio of the Am $4d_{3/2}$ and$4d_{5/2}$ x-ray absorption lines to the chemical state of Am was shown usingAm binary oxides as reference systems. The observed ratio for Am-doped UO$_2$suggests that at least at low Am concentrations, americium is in the Am(III)state in the UO$_2$ lattice. To confirm the validity of the applied AIMapproach, the analysis of the Am $4f$ x-ray photoelectron spectra of AmO$_2$and Am$_2$O$_3$ was also performed which revealed a good agreement betweenexperiment and calculations. As a whole, AmO$_2$ can be classified as thecharge-transfer compound with the $5f$ occupancy ($n_f$) equal to 5.73electrons, while Am$_2$O$_3$ is rather a Mott-Hubbard system with $n_f$=6.05.

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