I will describe collaborative efforts combining synthesis, characterization and theory in order to assess the predictions of various many-body approaches for the strongly correlated actinide dioxides.    A particular focus will be the counterintuitive prediction from hybrid density functional theory (DFT) that while UO2 is a classic Mott insulator and quite ionic, the PuO2 analogue, also insulating, shows significant Pu5f/O2p orbital mixing and band dispersion, indicative of covalent interactions. This has spurred efforts to synthesize high quality thin films of UO2, NpO2, and PuO2 using the technique of polymer assisted deposition (PAD), and to characterize them with optical spectroscopy, angle-resolved photoemission, and X-ray absorption spectroscopy.  I will discuss the results of the experiments, and compare them with predictions of several many-body theories including screened hybrid DFT, the widely used DFT+U approximations, and dynamic mean-field theory (DMFT).  As time permits I will sketch the direction we are taking to address the strongly correlated metals.

Covalency and strong correlations in actinide materials

247th National Meeting (2014)

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