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Materials with strongly correlated electrons often exhibit interesting physical properties. An example of these materials is the layered oxide perovskite Sr 2 RuO 4 , which has been intensively investigated due to its unusual properties. Whilst the debate on the symmetry of the superconducting state in Sr 2 RuO 4 is still ongoing, a deeper understanding of the Sr 2 RuO 4 normal state appears crucial as this is the background in which electron pairing occurs. Here, by using low-energy muon spin spectroscopy we discover the existence of surface magnetism in Sr 2 RuO 4 in its normal state. We detect static weak dipolar fields yet manifesting at an onset temperature higher than 50 K. We ascribe this unconventional magnetism to orbital loop currents forming at the reconstructed Sr 2 RuO 4 surface. Our observations set a reference for the discovery of the same magnetic phase in other materials and unveil an electronic ordering mechanism that can influence electron pairing with broken time reversal symmetry. Strontium Ruthenate, Sr 2 RuO 4 , displays a remarkable number of intriguing physical phenomena, from superconductivity, to strain-induced ferromagnetism. Here, using low-energy muon spectroscopy, Fittipaldi et al. demonstrate the existence of unconventional magnetism at the surface of Sr 2 RuO 4 in its normal state and without any applied strain.

A paradigmatic case of multi-band Mott physics including spin-orbit and Hund’s coupling is realized in Ca 2 RuO 4 . Progress in understanding the nature of this Mott insulating phase has been impeded by the lack of knowledge about the low-energy electronic structure. Here we provide—using angle-resolved photoemission electron spectroscopy—the band structure of the paramagnetic insulating phase of Ca 2 RuO 4 and show how it features several distinct energy scales. Comparison to a simple analysis of atomic multiplets provides a quantitative estimate of the Hund’s coupling J =0.4 eV. Furthermore, the experimental spectra are in good agreement with electronic structure calculations performed with Dynamical Mean-Field Theory. The crystal field stabilization of the d xy orbital due to c -axis contraction is shown to be essential to explain the insulating phase. These results underscore the importance of multi-band physics, Coulomb interaction and Hund’s coupling that together generate the Mott insulating state of Ca 2 RuO 4 . Detailed knowledge of the low-energy electronic structure is required to understand the Mott insulating phase of Ca 2 RuO 4 . Here, Sutter et al . provide directly the experimental band structure of the paramagnetic insulating phase of Ca 2 RuO 4 and unveil the electronic origin of its Mott phase.

A paradigmatic case of multi-band Mott physics including spin-orbit and Hund's coupling is realized in Ca RuO . Progress in understanding the nature of this Mott insulating phase has been impeded by the lack of knowledge about the low-energy electronic structure. Here we provide-using angle-resolved photoemission electron spectroscopy-the band structure of the paramagnetic insulating phase of Ca RuO and show how it features several distinct energy scales. Comparison to a simple analysis of atomic multiplets provides a quantitative estimate of the Hund's coupling J=0.4 eV. Furthermore, the experimental spectra are in good agreement with electronic structure calculations performed with Dynamical Mean-Field Theory. The crystal field stabilization of the d orbital due to c-axis contraction is shown to be essential to explain the insulating phase. These results underscore the importance of multi-band physics, Coulomb interaction and Hund's coupling that together generate the Mott insulating state of Ca RuO .

The single-layered ruthenate Sr2RuO4 is one of the most enigmatic unconventional superconductors. While for many years it was thought to be the best candidate for a chiral p-wave superconducting ground state, desirable for topological quantum computations, recent experiments suggest a singlet state, ruling out the original p-wave scenario. The superconductivity as well as the properties of the multi-layered compounds of the ruthenate perovskites are strongly influenced by a van Hove singularity in proximity of the Fermi energy. Tiny structural distortions move the van Hove singularity across the Fermi energy with dramatic consequences for the physical properties. Here, we determine the electronic structure of the van Hove singularity in the surface layer of Sr2RuO4 by quasi-particle interference imaging. We trace its dispersion and demonstrate from a model calculation accounting for the full vacuum overlap of the wave functions that its detection is facilitated through the octahedral rotations in the surface layer.

Abstract Understanding and controlling the transition between antiferromagnetic states having different symmetry content with respect to time-inversion and space-group operations are fundamental challenges for the design of magnetic phases with topologically nontrivial character. Here, we consider a paradigmatic antiferromagnetic oxide insulator, Ca $$_{2}$$ 2 RuO $$_{4}$$ 4 , with symmetrically distinct magnetic ground states and unveil a novel path to guide the transition between them. The magnetic changeover results from structural and orbital reconstruction at the transition metal site that in turn arise as a consequence of substitutional doping. By means of resonant X-ray diffraction we track the evolution of the structural, magnetic, and orbital degrees of freedom for Mn doped Ca $$_{2}$$ 2 RuO $$_{4}$$ 4 to demonstrate the mechanisms which drive the antiferromagnetic transition. While our analysis focuses on a specific case of substitution, we show that any perturbation that can impact in a similar way on the crystal structure, by reconstructing the induced spin–orbital exchange, is able to drive the antiferromagnetic reorganization.

Understanding and controlling the transition between antiferromagnetic states having different symmetry content with respect to time-inversion and space-group operations are fundamental challenges for the design of magnetic phases with topologically nontrivial character. Here, we consider a paradigmatic antiferromagnetic oxide insulator, Ca 2 RuO 4 , with symmetrically distinct magnetic ground states and unveil a novel path to guide the transition between them. The magnetic changeover results from structural and orbital reconstruction at the transition metal site that in turn arise as a consequence of substitutional doping. By means of resonant X-ray diffraction we track the evolution of the structural, magnetic, and orbital degrees of freedom for Mn doped Ca 2 RuO 4 to demonstrate the mechanisms which drive the antiferromagnetic transition. While our analysis focuses on a specific case of substitution, we show that any perturbation that can impact in a similar way on the crystal structure, by reconstructing the induced spin–orbital exchange, is able to drive the antiferromagnetic reorganization.

Understanding and controlling the transition between antiferromagnetic states having different symmetry content with respect to time-inversion and space-group operations are fundamental challenges for the design of magnetic phases with topologically nontrivial character. Here, we consider a paradigmatic antiferromagnetic oxide insulator, Ca$$_{2}$$2 RuO$$_{4}$$4 , with symmetrically distinct magnetic ground states and unveil a novel path to guide the transition between them. The magnetic changeover results from structural and orbital reconstruction at the transition metal site that in turn arise as a consequence of substitutional doping. By means of resonant X-ray diffraction we track the evolution of the structural, magnetic, and orbital degrees of freedom for Mn doped Ca$$_{2}$$2 RuO$$_{4}$$4 to demonstrate the mechanisms which drive the antiferromagnetic transition. While our analysis focuses on a specific case of substitution, we show that any perturbation that can impact in a similar way on the crystal structure, by reconstructing the induced spin–orbital exchange, is able to drive the antiferromagnetic reorganization.

The strongly correlated insulatorCa2RuO4is considered as a paradigmatic realization of both spin-orbital physics and a band-Mott insulating phase, characterized by orbitally selective coexistence of a band and a Mott gap. We present a high resolution oxygenK-edge resonant inelastic x-ray scattering study of the antiferromagnetic Mott insulating state ofCa2RuO4. A set of low-energy (about 80 and 400 meV) and high-energy (about 1.3 and 2.2 eV) excitations are reported, which show strong incident light polarization dependence. Our results strongly support a spin-orbit coupled band-Mott scenario and explore in detail the nature of its exotic excitations. Guided by theoretical modeling, we interpret the low-energy excitations as a result of composite spin-orbital excitations. Their nature unveils the intricate interplay of crystal-field splitting and spin-orbit coupling in the band-Mott scenario. The high-energy excitations correspond to intra-atomic singlet-triplet transitions at an energy scale set by Hund’s coupling. Our findings give a unifying picture of the spin and orbital excitations in the band-Mott insulatorCa2RuO4.

The surprisingly low current density required for inducing the insulator to metal transition has made Ca2RuO4 an attractive candidate material for developing Mott-based electronics devices. The mechanism driving the resistive switching, however, remains a controversial topic in the field of strongly correlated electron systems. Here we probe an uncovered region of phase space by studying high-purity Ca2RuO4 single crystals, using the sample size as principal tuning parameter. Upon reducing the crystal size, we find a four orders of magnitude increase in the current density required for driving Ca2RuO4 out of the insulating state into a non-equilibrium phase which is the precursor to the fully metallic phase. By integrating a microscopic platinum thermometer and performing thermal simulations, we gain insight into the local temperature during simultaneous application of current and establish that the size dependence is not a result of Joule heating. The findings suggest an inhomogeneous current distribution in the nominally homogeneous crystal. Our study calls for a reexamination of the interplay between sample size, charge current, and temperature in driving Ca2RuO4 towards the Mott insulator to metal transition.

Electronic band structures in solids stem from a periodic potential reflecting the structure of either the crystal lattice or electronic order. In the stoichiometric ruthenate Ca3Ru2O7, numerous Fermi surface-sensitive probes indicate a low-temperature electronic reconstruction. Yet, the causality and the reconstructed band structure remain unsolved. Here, we show by angle-resolved photoemission spectroscopy, how in Ca3Ru2O7 a C2-symmetric massive Dirac semimetal is realized through a Brillouin-zone preserving electronic reconstruction. This Dirac semimetal emerges in a two-stage transition upon cooling. The Dirac point and band velocities are consistent with constraints set by quantum oscillation, thermodynamic, and transport experiments, suggesting that the complete Fermi surface is resolved. The reconstructed structure—incompatible with translational-symmetry-breaking density waves—serves as an important test for band structure calculations of correlated electron systems.