Multipoles in Correlated Electron Materials

Electronic structure calculations constitute a valuable tool to predict the properties of materials. In this study we propose an efficient scheme to study correlated electron systems with essentially only one free parameter, the screening length of the Coulomb potential. A general reformulation of the exchange energy of the correlated electron shell is combined with this method in order to analyze the calculations. The results are interpreted in terms of different polarization channels, due to different multipoles. The method is applied to various actinide compounds, in order to increase the understanding of the complicate behaviour of 5f electrons in these systems. We studied the non-magnetic phase of δ-Pu, where the spin polarization is taken over by a spin-orbit-like term that does not break the time reversal symmetry. We also find that a non-trivial high multipole of the magnetization density, the triakontadipole, constitutes the ordering parameter in the mysterious hidden order phase of the heavy-fermion superconductor URu2Si2. This type of multipolar ordering is also found to play an essential role in the hexagonal-based superconductors UPd2Al3, UNi2Al3 and UPt3 and in the dioxide insulators UO2, NpO2 and PuO2. The triakontadipole moments are also present in all magnetic actinides we considered, except for Cm. These results led us to formulate a new set of rules for the ground state of a system, that are valid in presence of strong spin-orbit coupling interaction instead of those of Hund; the Katt's rules. Finally, we applied our method to a new class of high-Tc superconductors, the Fe-pnictides, where the Fe 3d electrons are moderately correlated. In these materials we obtain the stabilization of a low spin moment solution, in agreement with experiment, over a large moment solution, due to the gain in exchange energy in the formation of large multipoles of the spin magnetization density.Felaktigt tryckt som Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology 70