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Register a new userRole of Ce 4f hybridization in the origin of magnetism in nanoceria
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Nanoscale CeO2 (nanoceria) is a prototypical system that presents d0 ferromagnetism. Using a combination of x-ray absorption spectroscopy, x-ray magnetic circular dichroism and modelling, we show that nanostructure, defects and disorder, and non-stoichiometry create magnetically polarized Ce 4f and O 2p hybridized states captured by the vacancy orbitals (Vorb) that are vital to ferromagnetism. Further, we demonstrate that foreign ions (Fe and Co) enhance the moment at Ce 4f sites while the number of Vorb is unchanged, pointing clearly to the mechanism of orbital hybridization being key missing ingredient to understanding the unexpected ferromagnetism in many nanoscale dilute magnetic oxides and semiconductors.
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Ce 3d-4f resonant angle-resolved photoemission measurements on CeCoGe$_{1.2}$Si$_{0.8}$ and CeCoSi$_{2}$ have been performed to understand the Fermi surface topology as a function of hybridization strength between Ce 4$f$- and conduction electrons in heavy-fermion systems. We directly observe that the hole-like Ce 4$f$-Fermi surfaces of CeCoSi$_{2}$ is smaller than that of CeCoGe$_{1.2}$Si$_{0.8}$, indicating the evolution of the Ce 4$f$-Fermi surface with the increase of the hybridization strength. In comparision with LDA calculation, the Fermi surface variation cannot be understood even though the overall electronic structure are roughly explained, indicating the importance of strong correlation effects. We also discuss the relation between the Ce 4$f$-Fermi surface variation and the Kondo peaks.
Spin- and angle-resolved resonant (Ce $4dto4f$) photoemission spectra of a monolayer Ce on Fe(110) reveal spin-dependent changes of the Fermi-level peak intensities. That indicate a spin-dependence of $4f$ hybridization and, thus, of $4f$ occupancy and local moment. The phenomenon is described in the framework of the periodic Anderson model by $4f$ electron hopping into the exchange split Fe 3d derived bands that form a spin-gap at the Fermi energy around the $bar{Gamma}$ point of the surface Brillouin zone.
One year after their initial discovery, two schools of thought have crystallized regarding the electronic structure and magnetic properties of ferropnictide systems. One postulates that these are itinerant weakly correlated metallic systems that become magnetic by virtue of spin-Peierls type transition due to near-nesting between the hole and the electron Fermi surface pockets. The other argues these materials are strongly or at least moderately correlated, the electrons are considerably localized and close to a Mott-Hubbard transition, with the local magnetic moments interacting via short-range superexchange. In this paper we argue that neither picture is fully correct. The systems are moderately correlated, but with correlations driven by Hunds rule coupling rather than by the on-site Hubbard repulsion. The iron moments are largely local, driven by Hunds intra-atomic exchange. Superexchange is not operative and the interactions between the Fe moments are considerably long-range and driven mostly by one-electron energies of all occupied states.
Based on first principles calculations, this study reveals that magnetism in otherwise non-magnetic materials can originate from the partial occupation of antibonding states. Since the antibonding wavefunctions are spatially antisymmetric, the spin wavefunctions should be symmteric according to the exchange antisymmetric principle of quantum mechanics. We demonstrate that this phenomenon can be observed in a graphitic carbon nitride material, $g$-C$_4$N$_3$, which can be experimentally synthesized and seen as a honeycomb structure with a vacancy. Three dangling bonds of N atoms pointing to the vacancy site interact with each other to form one bonding and two antibonding states. As the two antibonding states are near the Fermi level, and electrons should partially occupy the antibonding states in spin polarization, this leads to 1~$mu_B$ magnetic moment.
Magnetocrystalline anisotropy (MCA) in doped Ce$_{2}$Co$_{17}$ and other competing structures was investigated using density functional theory. We confirmed that the MCA contribution from dumbbell Co sites is very negative. Replacing Co dumbbell atoms with a pair of Fe or Mn atoms greatly enhance the uniaxial anisotropy, which agrees quantitatively with experiment, and this enhancement arises from electronic-structure features near the Fermi level, mostly associated with dumbbell sites. With Co dumbbell atoms replaced by other elements, the variation of anisotropy is generally a collective effect and contributions from other sublattices may change significantly. Moreover, we found that Zr doping promotes the formation of 1-5 structure that exhibits a large uniaxial anisotropy, such that Zr is the most effective element to enhance MCA in this system.
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