Microscopic theory of the insulating electronic ground states of actinide dioxides AnO2 (An=U, Np, Pu, Am, and Cm)

Abstract

The electronic ground states of the actinide dioxides AnO2 (with An=U, Np, Pu, Am, and Cm) are investigated employing first-principles calculations within the framework of the local density approximation +U (LDA+U) approach, implemented in a full-potential linearized augmented plane-wave scheme. A systematic analysis of the An-5f states is performed which provides intuitive connections between the electronic structures and the local crystalline fields of the f states in the AnO2 series. Particularly the mechanisms leading to the experimentally observed insulating ground states are investigated. These are found to be caused by the strong spin-orbit and Coulomb interactions of the 5f orbitals; however, as a result of the different configurations, this mechanism works in distinctly different ways for each of the AnO2 compounds. In agreement with experimental observations, the nonmagnetic states of plutonium and curium dioxide are computed to be insulating, whereas those of uranium, neptunium, and americium dioxides require additional symmetry breaking to reproduce the insulator ground states, a condition which is met with magnetic phase transitions. We show that the occupancy of the An-f orbitals is closely connected to each of the appearing insulating mechanisms. We furthermore investigate the detailed constitution of the noncollinear multipolar moments for transverse 3q magnetic ordered states in UO2 and longitudinal 3q high-rank multipolar ordered states in NpO2 and AmO2.

15 pages, 19 figures, 1 table; accepted for publication in Phys. Rev. B

References in corpus (6)

• Magnetic state of plutonium ion in metallic Pu and its compounds
• Emergent Rank-5 'Nematic' Order in URu2Si2
• Electronic structure and non-magnetic character of $\delta$-Pu-Am alloys
• A perturbative approach to J mixing in f-electron systems: Application to actinide dioxides
• Multipolar, magnetic and vibrational lattice dynamics in the low temperature phase of uranium dioxide
• First-Principles Theory of Multipolar Order in Neptunium Dioxide

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• Electronic structure and core-level spectra of light actinide dioxides in the dynamical mean-field theory
• Non-magnetic ground state of PuO${}_2$
• Towards a first-principles determination of effective Coulomb interactions in correlated electron materials: Role of intershell interactions
• On the Raman Spectrum of Plutonium dioxide: vibrational and crystal electric field modes
• Quadrupolar Superexchange Interactions, Multipolar Order and Magnetic Phase Transition in UO${}_2$
• Hidden order and multipolar exchange striction in a correlated f-electron system
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• Electronic structure and magnetism in UGa2: DFT+DMFT approach
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• Efficient Method for Prediction of Meta-stable/Ground Multipolar Ordered States and its Application in Monolayer $\alpha$-\ce{RuX3} (X=Cl,I)
• Reexaming the ground state and magnetic properties of curium dioxide
• Theory of valence-band and core-level photoemission from plutonium dioxide
• Microscopic Theory of ${\Gamma }_3$ Quadrupole Ordering in Pr Compounds on the Basis of a $j$-$j$ Coupling Scheme