Abstract
Bringing oxygen atoms from infinite, passing equilibrium until short enough distances, we aim to reveal the 4f5d electron bonding property and its relevance to the peculiar physical properties within PrO2 based on both accounting for electron Coulomb repulsion and spin-orbit coupling effects in combination with Wannier function methods. The microscopic mechanism of static Janh-Teller distortions and the physical insight into the dynamic Jahn-Teller effects are clarified. Peculiarly, the magnetic coupling is suggested to be via 4f-5d-O2p-5d-4f pathway in PrO2, and the coupling between spin and orbital ordering of 4f electrons is for the first time disclosed. The 5d orbitals, hybridized with 4f electrons, are found to play important roles in these processes.
Highlights
The electron correlations in transition metal oxides 3d electrons constrain the number of electrons at a given lattice site, and induce a local entanglement of the charge, spin and orbital degrees of freedom
With the combination of density functional theory (DFT) and maximally localized Wannier functions (MLWFs) results, we took an insight into intrinsic characters of the physical phenomena which originated from the electronic correlations of 4f electrons and the hybridization between Pr-4f/5d and O-2p states
We expect that systematic investigations on the strong correlated behavior of 4f electrons should be carried out considering the effect of both crystal field and the different electronic configurations using such as the group theory
Summary
The electron correlations in transition metal oxides 3d electrons constrain the number of electrons at a given lattice site, and induce a local entanglement of the charge, spin and orbital degrees of freedom. From these experimental evidences available so far it seems likely that both the static and dynamic Jahn-Teller effects are important in PrO2, but the microscopic physical insight has not been clarified Another important issue that has never been noticed is whether the spin ordering is relevant to the orbital ordering within this strong correlated 4f system since spin-orbital orderings coupling could be widely observed in 3d electron transition metal oxides as mentioned above. There are several density functional based studies describing the electronic structures based on self-interaction-corrected (SIC) local-spin-density approach[9], the Jahn-Teller distortions in PrO2 via Perdew-Burke-Ernzerhof PBE + U calculations[10], and dynamic Jahn-Teller effect by a simple model based on a vibronic Hamiltonian[6], so far there is no microscopic insight into the versatile phenomena of PrO2 using a method that truly captures the underlying local physics.
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