Using a combination of techniques in synthesis, theory and spectroscopy there has been major progress in elucidating the electronic structure of actinide oxides. Central to this improved understanding of actinide oxides is the use of hybrid functionals in calculating the electronic structure of these actinides. The hybrid functional calculations are coupled with the epitaxial thin film deposition technique of polymer assisted deposition which subsequently enables angle-resolved photoelectron spectroscopy measurements. Within the series of Mott/charge-transfer insulators which constitute the actinide dioxides, one observes a crossing point at Pu where there is a substantial increase in hybridization compared to the neighboring elements. This increase in hybridization was first predicted theoretically and later observed experimentally. In PuO2, the observed hybridization between the Pu 5f and O 2p electrons is an order of magnitude larger than in UO2 in spite of the radial 5f wavefunction in Pu being smaller than in U. A direct comparison between theory and spectroscopy reveals the significant improvement in understanding actinide oxides from Th to Pu which emphasize the role of hybridization in determining the electronic structure of these materials.

Electronic structure of actinide oxides from hybrid functionals and photoemission

251st National Meeting (2016)

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