Dual nature of 5$f$ electrons in the isostructural UM${}_2$Si${}_2$ family: from antiferro- to Pauli paramagnetism via hidden order

Abstract

Using inelastic x-ray scattering beyond the dipole limit and hard x-ray photoelectron spectroscopy we establish the dual nature of the U $5f$ electrons in UM${}_2$Si${}_2$ (M = Pd, Ni, Ru, Fe), regardless of their degree of delocalization. We have observed that the compounds have in common a local atomic-like state that is well described by the U $5f^2$ configuration with the ${\Gamma }_1^{(1)}$ and ${\Gamma }_2$ quasi-doublet symmetry. The amount of the U 5$f^3$ configuration, however, varies considerably across the UM${}_2$Si${}_2$ series, indicating an increase of U5$f$ itineracy in going from M=Pd to Ni to Ru, and to the Fe compound. The identified electronic states explain the formation of the very large ordered magnetic moments in UPd${}_2$Si${}_2$ and UNi${}_2$Si${}_2$, the availability of orbital degrees of freedom needed for the hidden order in URu${}_2$Si${}_2$ to occur, as well as the appearance of Pauli paramagnetism in UFe${}_2$Si${}_2$. A unified and systematic picture of the U$M_2$Si${}_2$ compounds may now be drawn, thereby providing suggestions for new experiments to induce hidden order and/or superconductivity in U compounds with the tetragonal body-centered ThCr${}_2$Si${}_2$ structure.

References in corpus (29)

• Fermi-liquid instabilities at magnetic quantum phase transitions
• Colloquium: Hidden Order, Superconductivity, and Magnetism -- The Unsolved Case of URu2Si2
• Arrested Kondo effect and hidden order in URu_2Si_2
• Emergent Rank-5 'Nematic' Order in URu2Si2
• Fermi surface instability at the hidden-order transition of URu2Si2
• Chirality density wave of the 'hidden order' phase in URu${}_2$Si${}_2$
• Hidden Order Behaviour in URu2Si2 (A Critical Review of the Status of Hidden Order in 2014)
• Electronic structure theory of the hidden order material URu${}_2$Si${}_2$
• Parasitic small-moment-antiferromagnetism and non-linear coupling of hidden order and antiferromagnetism in URu2Si2 observed by Larmor diffraction
• Fermi surface and heavy masses for UPd${}_2$Al${}_3$
• Hidden order and beyond: an experimental-theoretical overview of the multifaceted behavior of URu${}_2$Si${}_2$
• The dual nature of 5f electrons and origin of heavy fermions in U compounds
• Photoemission Imaging of 3D Fermi Surface Pairing at the Hidden Order Transition in URu2Si2
• Superconductivity in Ce- and U-based "122" heavy-fermion compounds
• 5d-5f Electric-multipole Transitions in Uranium Dioxide Probed by Non-resonant Inelastic X-ray Scattering
• Electronic Structure of Heavy Fermion Uranium Compounds Studied by Core-Level Photoelectron Spectroscopy
• Complex Landau Ginzburg Theory of the Hidden Order in URu_2Si_2
• Spectroscopic determination of the atomic f-electron symmetry underlying hidden order in URu${}_2$Si${}_2$
• Field-induced spin-density wave beyond hidden order in URu2Si2
• Direct bulk sensitive probe of 5f symmetry in URu2Si2
• Dual model for magnetic excitations and superconductivity in UPd2Al3
• Quantum criticality in the two-dimensional periodic Anderson model
• Long-range interactions in the effective low energy Hamiltonian of Sr2IrO4: a core level resonant inelastic x-ray scattering study
• Direct imaging of orbitals in quantum materials
• Probing the $J_{eff}=0$ ground state and the Van Vleck paramagnetism of the Ir${}^{5+}$ ions in the layered Sr${}_2$Co${}_{0.5}$Ir${}_{0.5}$O${}_4$
• U 5$f$ crystal-field ground state of UO${}_2$ probed by directional dichroism in nonresonant inelastic x-ray scattering
• The dual nature of magnetism in a uranium heavy fermion system
• The quartet ground state in CeB${}_6$: an inelastic x-ray scattering study
• f-electron charge densities probed using core level non-resonant inelastic x-ray scattering

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• Metastable phase of UTe${}_2$ formed under high pressure above 5 GPa
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• Global perspectives of the bulk electronic structure of URu${}_2$Si${}_2$ from angle-resolved photoemission
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• Quantitative investigation of the 4$f$ occupation in the quasikagome Kondo lattice CeRh${}_{1-x}$Pd${}_x$Sn
• Polarized Neutron Diffraction Study on UPt${}_2$Si${}_2$
• UCd${}_{11}$: A strongly localized 5$f^3$ material
• Large Kohn anomaly and phonon collapse induced by charge density wave in UPt${}_2$Si${}_2$
• Pressure-enhanced $f$-electron orbital weighting in UTe2 mapped by quantum interferometry
• Multiple localized-itinerant dualities in magnetism of 5f electron systems. The case of UPt${}_2$Si${}_2$