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Register a new userNature of the 5f states in actinide metals
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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.
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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.
In comparison to 3d or 4f metals, magnetism in actinides remains poorly understood due to experimental complications and the exotic behavior of the 5f states. In particular, plutonium metal is most especially vexing. Over the last five decades theories proposed the presence of either ordered or disordered local moments at low temperatures. However, experiments such as magnetic susceptibility, electrical resistivity, nuclear magnetic resonance, specific heat, and elastic and inelastic neutron scattering show no evidence for ordered or disordered magnetic moments in any of the six phases of plutonium. Beyond plutonium, the magnetic structure of other actinides is an active area of research given that temperature, pressure, and chemistry can quickly alter the magnetic structure of the 5f states. For instance, curium metal has an exceedingly large spin polarization that results in a total moment of about 8 Bohr magneton/atom, which influences the phase stability of the metal. Insight in the actinide ground state can be obtained from core-level x-ray absorption spectroscopy (XAS) and electron energy-loss spectroscopy (EELS). A sum rule relates the branching ratio of the core-level spectra measured by XAS or EELS to the expectation value of the angular part of the spin-orbit interaction.
We have carried out an analysis of magnetic data in 69 uranium, 7 neptunium and 4 plutonium ferromagnets with the spin fluctuation theory developed by Takahashi (Y. Takahashi, J. Phys. Soc. Jpn. 55, 3553 (1986)). The basic and spin fluctuation parameters of the actinide ferromagnets are determined and the applicability of the spin fluctuation theory to actinide 5f system has been discussed. Itinerant ferromagnets of the 3d transition metals and their intermetallics follow a generalized Rhodes-Wohlfarth relation between p_eff/p_s and T_C/T_0, viz., p_eff/p_s ~ (T_C/T_0)^(-3/2). Here, p_s, p_eff, T_C, and T_0 are the spontaneous and effective magnetic moments, the Curie temperature and the width of spin fluctuation spectrum in energy space, respectively. The same relation is satisfied for T_C/T_0 < 1.0 in the actinide ferromagnets. However, the relation is not satisfied in a few ferromagnets with T_C/T_0 ~1.0 that corresponds to local moment system in the spin fluctuation theory. The deviation from the theoretical relation may be due to several other effects not included in the spin fluctuation theory such as the crystalline electric field effect on the 5f electrons from ligand atoms. The value of the spontaneous magnetic moment p_s increases linearly as a function of T_C/T_0 in the uranium and neptunium ferromagnets below (T_C/T_0)_kink = 0.32 +- 0.02 where a kink structure appears in relation between the two quantities. p_s increases more weakly above (T_C/T_0)_kink. A possible interpretation with the T_C/T_0-dependence of p_s is given.
A dramatic temperature dependent enhancement of U 5f spectral weight at $E_F$ is observed in angle-resolved photoemission measurements of $URu_2Si_2$ at the center of an X-point hole-pocket. Comparison of this temperature dependent behavior for excitation both at and below the U $5d to 5f$ resonant threshold is presented.
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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