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Register a new userThe dual nature of 5f electrons and origin of heavy fermions in U compounds
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We develop a theory for the electronic excitations in UPt$_3$ which is based on the localization of two of the $5f$ electrons. The remaining $f$ electron is delocalized and acquires a large effective mass by inducing intra-atomic excitations of the localized ones. The measured deHaas-vanAlphen frequencies of the heavy quasiparticles are explained as well as their anisotropic heavy mass. A model calculation for a small cluster reveals why only the largest of the different $5f$ hopping matrix elements is operative causing the electrons in other orbitals to localize.
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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 $mathrm{U}~4d-5f$ resonant 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.
We present specific heat measurements of 4% Rh-doped U(Ru,Rh)2Si2 at magnetic fields above the proposed metamagnetic transition field Hm~34 T, revealing striking similarities to the isotructural Ce analog CeRu2Si2, suggesting that strongly renormalized hybridized band models apply equally well to both systems. The vanishing bandwidths as H --> Hm are consistent with a putative quantum critical point close to Hm. The existence of a phase transition into an ordered phase in the vicinity of Hm for 4% Rh-doped U(Ru,Rh)2Si2, but not for CeRu2Si2, is consistent with a stronger super-exchange in the case of the U 5-f system, with irreversible processes at the transition revealing a strong coupling of the 5f orbitals to the lattice, most suggestive of orbital or electric quadrupolar order.
Actinide elements produce a plethora of interesting physical behaviors due to the 5f states. This review compiles and analyzes progress in understanding of the electronic and magnetic structure of the 5f states in actinide metals. Particular interest is given to electron energy-loss spectroscopy and many-electron atomic spectral calculations, since there is now an appreciable library of core d -> valence f transitions for Th, U, Np, Pu, Am, and Cm. These results are interwoven and discussed against published experimental data, such as x-ray photoemission and absorption spectroscopy, transport measurements, and electron, x-ray, and neutron diffraction, as well as theoretical results, such as density-functional theory and dynamical mean-field theory.
We present a theoretical model of the electronic structure of delta-Pu that is consistent with many of the electronic structure related properties of this complex metal. In particular we show that the theory is capable of reproducing the valence band photoelectron spectrum of delta-Pu. We report new experimental photoelectron spectra at several photon energies and present evidence that the electronic structure of delta-Pu is unique among the elements, involving a 5f shell with four 5f electrons in a localized multiplet, hybridizing with valence states, and approximately one 5f electron forming a completely delocalized band state.
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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