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تسجيل مستخدم جديدItinerant Nature of U 5f States in Uranium Mononitride UN Revealed by Angle Resolved Photoelectron Spectroscopy
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The electronic structure of the antiferromagnet uranium nitride (UN) has been studied by angle resolved photoelectron spectroscopy using soft X-rays (hn=420-520 eV). Strongly dispersive bands with large contributions from the U 5f states were observed in ARPES spectra, and form Fermi surfaces. The band structure as well as the Fermi surfaces in the paramagnetic phase are well explained by the band-structure calculation treating all the U 5f electrons as being itinerant, suggesting that itinerant description of the U 5f states is appropriate for this compound. On the other hand, changes in the spectral function due to the antiferromagnetic transition were very small. The shapes of the Fermi surfaces in a paramagnetic phase are highly three-dimensional, and the nesting of Fermi surfaces is unlikely as the origin of the magnetic ordering.
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The electronic structure of the ferromagnetic superconductor URhGe in the paramagnetic phase has been studied by angle-resolved photoelectron spectroscopy using soft x rays (hn=595-700 eV). Dispersive bands with large contributions from U 5f states w
ere observed in the ARPES spectra, and form Fermi surfaces. The band structure in the paramagnetic phase is partly explained by the band-structure calculation treating all U 5f electrons as being itinerant, suggesting that an itinerant description of U 5f states is a good starting point for this compound. On the other hand, there are qualitative disagreements especially in the band structure near the Fermi level (E_B < 0.5 eV). The experimentally observed bands are less dispersive than the calculation, and the shape of the Fermi surface is different from the calculation. The changes in spectral functions due to the ferromagnetic transition were observed in bands near the Fermi level, suggesting that the ferromagnetism in this compound has an itinerant origin.
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We have elucidated the nature of the electron correlation effect in uranium compounds by imaging the partial $mathrm{U}~5f$ density of states (pDOS) of typical itinerant, localized, and heavy fermion uranium compounds by using the $mathrm{U}~4d-5f$ r
esonant photoemission spectroscopy. Obtained $mathrm{U}~5f$ pDOS exhibit a systematic trend depending on the physical properties of compounds. The coherent peak at the Fermi level can be described by the band-structure calculation, but an incoherent peak emerges on the higher binding energy side ($lesssim 1~mathrm{eV}$) in the Uf pDOS of localized and heavy fermion compounds. As the $mathrm{U}~5f$ state is more localized, the intensity of the incoherent peak is enhanced and its energy position is shifted to higher binding energy. These behaviors are consistent with the prediction of the Mott metal-insulator transition, suggesting that the Hubbard-$U$ type mechanism takes an essential role in the $5f$ electronic structure of actinide materials.
Uranium and plutoniums 5f electrons are tenuously poised between strongly bonding with ligand spd-states and residing close to the nucleus. The unusual properties of these elements and their compounds (eg. the six different allotropes of elemental pl
utonium) are widely believed to depend on the related attributes of f-orbital occupancy and delocalization, for which a quantitative measure is lacking. By employing resonant x-ray emission spectroscopy (RXES) and x-ray absorption near-edge structure (XANES) spectroscopy and making comparisons to specific heat measurements, we demonstrate the presence of multiconfigurational f-orbital states in the actinide elements U and Pu, and in a wide range of uranium and plutonium intermetallic compounds. These results provide a robust experimental basis for a new framework for understanding the strongly-correlated behavior of actinide materials.
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