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1.
Phys Rev Lett ; 132(4): 046401, 2024 Jan 26.
Artigo em Inglês | MEDLINE | ID: mdl-38335370

RESUMO

CeRh_{2}As_{2} is a new multiphase superconductor with strong suggestions for an additional itinerant multipolar ordered phase. The modeling of the low-temperature properties of this heavy-fermion compound requires a quartet Ce^{3+} crystal-field ground state. Here, we provide the evidence for the formation of such a quartet state using x-ray spectroscopy. Core-level photoelectron and x-ray absorption spectroscopy confirm the presence of Kondo hybridization in CeRh_{2}As_{2}. The temperature dependence of the linear dichroism unambiguously reveals the impact of Kondo physics for coupling the Kramer's doublets into an effective quasiquartet. Nonresonant inelastic x-ray scattering data find that the |Γ_{7}^{-}⟩ state with its lobes along the 110 direction of the tetragonal structure (xy orientation) contributes most to the multiorbital ground state of CeRh_{2}As_{2}.

2.
Proc Natl Acad Sci U S A ; 117(48): 30220-30227, 2020 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-33203673

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.

3.
Nat Commun ; 10(1): 5447, 2019 11 29.
Artigo em Inglês | MEDLINE | ID: mdl-31784516

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.

4.
Proc Natl Acad Sci U S A ; 113(49): 13989-13994, 2016 12 06.
Artigo em Inglês | MEDLINE | ID: mdl-27872287

RESUMO

The second-order phase transition into a hidden order phase in URu2Si2 goes along with an order parameter that is still a mystery, despite 30 years of research. However, it is understood that the symmetry of the order parameter must be related to the symmetry of the low-lying local electronic [Formula: see text]-states. Here, we present results of a spectroscopic technique, namely core-level nonresonant inelastic X-ray scattering (NIXS). This method allows for the measurement of local high-multipole excitations and is bulk-sensitive. The observed anisotropy of the scattering function unambiguously shows that the 5[Formula: see text] ground-state wave function is composed mainly of the [Formula: see text] with majority [Formula: see text] = [Formula: see text] + [Formula: see text] and/or [Formula: see text] singlet states. The incomplete dichroism indicates the possibility that quantum states of other irreducible representation are mixed into the ground state.

5.
Sci Rep ; 5: 17937, 2015 Dec 10.
Artigo em Inglês | MEDLINE | ID: mdl-26658647

RESUMO

Topological insulators form a novel state of matter that provides new opportunities to create unique quantum phenomena. While the materials used so far are based on semiconductors, recent theoretical studies predict that also strongly correlated systems can show non-trivial topological properties, thereby allowing even the emergence of surface phenomena that are not possible with topological band insulators. From a practical point of view, it is also expected that strong correlations will reduce the disturbing impact of defects or impurities, and at the same increase the Fermi velocities of the topological surface states. The challenge is now to discover such correlated materials. Here, using advanced x-ray spectroscopies in combination with band structure calculations, we infer that CeRu4Sn6 is a strongly correlated material with non-trivial topology.

6.
Proc Natl Acad Sci U S A ; 112(8): 2384-8, 2015 Feb 24.
Artigo em Inglês | MEDLINE | ID: mdl-25675488

RESUMO

The interplay of structural, orbital, charge, and spin degrees of freedom is at the heart of many emergent phenomena, including superconductivity. Unraveling the underlying forces of such novel phases is a great challenge because it not only requires understanding each of these degrees of freedom, it also involves accounting for the interplay between them. Cerium-based heavy fermion compounds are an ideal playground for investigating these interdependencies, and we present evidence for a correlation between orbital anisotropy and the ground states in a representative family of materials. We have measured the 4f crystal-electric field ground-state wave functions of the strongly correlated materials CeRh1-xIrxIn5 with great accuracy using linear polarization-dependent soft X-ray absorption spectroscopy. These measurements show that these wave functions correlate with the ground-state properties of the substitution series, which covers long-range antiferromagnetic order, unconventional superconductivity, and coexistence of these two states.

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