RESUMO
Using inelastic X-ray scattering beyond the dipole limit and hard X-ray photoelectron spectroscopy we establish the dual nature of the U [Formula: see text] electrons in U[Formula: see text] (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 [Formula: see text] configuration with the [Formula: see text] and [Formula: see text] quasi-doublet symmetry. The amount of the U 5[Formula: see text] configuration, however, varies considerably across the U[Formula: see text] series, indicating an increase of U 5f 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 [Formula: see text] and [Formula: see text], the availability of orbital degrees of freedom needed for the hidden order in [Formula: see text] to occur, as well as the appearance of Pauli paramagnetism in [Formula: see text] A unified and systematic picture of the U[Formula: see text] compounds may now be drawn, thereby providing suggestions for additional experiments to induce hidden order and/or superconductivity in U compounds with the tetragonal body-centered [Formula: see text] structure.
RESUMO
The one-dimensional cobaltate Ca[Formula: see text]Co[Formula: see text]O[Formula: see text] is an intriguing material having an unconventional magnetic structure, displaying quantum tunneling phenomena in its magnetization. Using a newly developed experimental method, [Formula: see text]-core-level non-resonant inelastic x-ray scattering ([Formula: see text]-NIXS), we were able to image the atomic Co [Formula: see text] orbital that is responsible for the Ising magnetism in this system. We can directly observe that corrections to the commonly accepted ideal prismatic trigonal crystal field scheme occur in Ca[Formula: see text]Co[Formula: see text]O[Formula: see text], and it is the complex [Formula: see text] orbital occupied by the sixth electron at the high-spin Co[Formula: see text] ([Formula: see text]) sites that generates the Ising-like behavior. The ability to directly relate the orbital occupation with the local crystal structure is essential to model the magnetic properties of this system.