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Register a new userPersistence of antiferromagnetic order upon La substitution in the $4d^4$ Mott insulator Ca$_2$RuO$_4$
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The chemical and magnetic structures of the series of compounds Ca$_{2-x}$La$_x$RuO$_4$ [$x = 0$, $0.05(1)$, $0.07(1)$, $0.12(1)$] have been investigated using neutron diffraction and resonant elastic x-ray scattering. Upon La doping, the low temperature S-Pbca space group of the parent compound is retained in all insulating samples [$xleq0.07(1)$], but with significant changes to the atomic positions within the unit cell. These changes can be characterised in terms of the local RuO$_6$ octahedral coordination: with increasing doping the structure, crudely speaking, evolves from an orthorhombic unit cell with compressed octahedra to a quasi-tetragonal unit cell with elongated ones. The magnetic structure on the other hand, is found to be robust, with the basic $k=(0,0,0)$, $b$-axis antiferromagnetic order of the parent compound preserved below the critical La doping concentration of $xapprox0.11$. The only effects of La doping on the magnetic structure are to suppress the A-centred mode, favouring the B mode instead, and to reduce the N{e}el temperature somewhat. Our results are discussed with reference to previous experimental reports on the effects of cation substitution on the $d^4$ Mott insulator Ca$_2$RuO$_4$, as well as with regard to theoretical studies on the evolution of its electronic and magnetic structure. In particular, our results rule out the presence of a proposed ferromagnetic phase, and suggest that the structural effects associated with La substitution play an important role in the physics of the system.
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The ground-state orbital occupancy of the Ru$^{4+}$ ion in Ca$_{2-x}$La$_x$RuO$_4$ [x=0, 0.05(1), 0.07(1) and 0.12(1)] was investigated by performing X-ray absorption spectroscopy (XAS) in the vicinity of the O K edge as a function of angle between the incident beam and the surface of the crystals. A minimal model of the hybridization between the O 2p states probed at the K edge and the Ru 4d orbitals was used to analyze the XAS data, allowing the ratio of hole occupancies $n_{xy}/n_{yz,zx}$ to be determined as a function of doping and temperature. For the samples displaying a low-temperature insulating ground-state ($xleq0.07$), $n_{xy}/n_{yz,zx}$ is found to increase significantly with increasing doping. For x=0.12, which has a metallic ground-state, the XAS spectra are found to be independent of temperature, and not to be describable by the minimal hybridization model. To understand the origin of the evolution of the electronic structure across the phase diagram, we have performed theoretical calculations based on a model Hamiltonian, comprising electron-electron correlations, crystal field ($Delta$) and spin-orbit coupling ($lambda$), of a Ru-O-Ru cluster. Our calculations of the Ru hole occupancy as a function of $Delta/lambda$ establish that the enhancement of $n_{xy}/n_{yz,zx}$ is driven by significant changes to the crystal field as the tetragonal distortion of the RuO$_6$ octahedral changes from compressive to tensile with La doping. It also shows that the hole occupancy of the O 2p and Ru 4d orbitals display the same trend as a function of $Delta/lambda$, thus validating the minimal hybridization model. In essence, our results suggest that the predominant mechanism driving the emergence of the low-temperature metallic phase in La doped Ca$_2$RuO$_4$ is the structurally induced redistribution of holes within the t2g orbitals, rather that the injection of free carriers.
A paradigmatic case of multi-band Mott physics including spin-orbit and Hunds coupling is realised 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 Hunds 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 stabilisation of the d$_{xy}$ orbital due to $c$-axis contraction is shown to be important in explaining the nature of the insulating state. It is thus a combination of multiband physics, Coulomb interaction and Hunds coupling that generates the Mott insulating state of Ca$_2$RuO$_4$. These results underscore the importance of Hunds coupling in the ruthenates and related multiband materials.
We present nonlinear conduction phenomena in the Mott insulator Ca2RuO4 investigated with a proper evaluation of self-heating effects. By utilizing a non-contact infrared thermometer, the sample temperature was accurately determined even in the presence of large Joule heating. We find that the resistivity continuously decreases with currents under an isothermal environment. The nonlinearity and the resulting negative differential resistance occurs at relatively low current range, incompatible with conventional mechanisms such as hot electron or impact ionization. We propose a possible current-induced gap suppression scenario, which is also discussed in non-equilibrium superconducting state or charge-ordered insulator.
We show that the pressure-temperature phase diagram of the Mott insulator Ca$_{2}$RuO$_{4}$ features a metal-insulator transition at 0.5GPa: at 300K from paramagnetic insulator to paramagnetic quasi-two-dimensional metal; at $T leq$ 12K from antiferromagnetic insulator to ferromagnetic, highly anisotropic, three-dimensional metal. % We compare the metallic state to that of the structurally related p-wave superconductor Sr$_{2}$RuO$_{4}$, and discuss the importance of structural distortions, which are expected to couple strongly to pressure.
Insulator-to-metal transition in Ca$_{2}$RuO$_{4}$ has drawn keen attention because of its sensitivity to various stimulation and its potential controllability. Here, we report a direct observation of Fermi surface, which emerges upon introducing excess oxygen into an insulating Ca$_{2}$RuO$_{4}$, by using angle-resolved photoemission spectroscopy. Comparison between energy distribution curves shows that the Mott insulating gap is closed by eV-scale spectral-weight transfer with excess oxygen. Momentum-space mapping exhibits two square-shaped sheets of the Fermi surface. One is a hole-like $alpha$ sheet around the corner of a tetragonal Brillouin zone, and the other is an electron-like $beta$ sheet around the $Gamma$ point. The electron occupancies of the $alpha$ and $beta$ bands are determined to be $n_{alpha}=1.6$ and $n_{beta}=0.6$, respectively. Our result indicates that the insulator-to-metal transition occurs selectively in $d_{xz}$ and $d_{yz}$ bands and not yet in $d_{xy}$ band. This orbital selectivity is most likely explained in terms of the energy level of $d_{xy}$, which is deeper for Ca$_{2}$RuO$_{4+delta}$ than for Ca$_{1.8}$Sr$_{0.2}$RuO$_{4}$. Consequently, we found substantial differences from the Fermi surface of other ruthenates, shedding light on a unique role of excess oxygen among the metallization methods of Ca$_{2}$RuO$_{4}$.
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