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 $α$ sheet around the corner of a tetragonal Brillouin zone, and the other is an electron-like $β$ sheet around the $Γ$ point. The electron occupancies of the $α$ and $β$ bands are determined to be $n_α=1.6$ and $n_β=0.6$, 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$_{4+δ}$ 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$_{4}$.
We investigated the optical properties of (Ca,Sr)RuO_3 films on the borderline of a metal-insulator (M-I) transition. Our results show all of the predicted characteristics for a metallic Mott-Hubbard system, including (i) a mass enhancement in dc-limit, (ii) an U/2 excitation, and (iii) an U excitation. Also, a self-consistency is found within the Gutzwiller-Brinkman-Rice picture for the Mott transition. Our finding displays that electron correlation should be important even in 4d materials.
We propose a new mechanism for the paramagnetic metal-insulator transition in the layered perovskite Ca$_{2-x}$Sr$_{x}$RuO$_{4}$ (0<x<0.2). The LDA+U approach including spin-orbit coupling is used to calculate the electronic structures. In Ca$_{2}$RuO$_{4}$, we show that the spin-orbit effect is strongly enhanced by the Coulomb repulsion, which leads to an insulating phase. When Ca is substituted by Sr, the effective spin-orbit splitting is reduced due to the increasing bandwidth of the degenerate $d_{xz}$ and $d_{yz}$ orbitals. For x=0.2, the compound is found to be metallic. We show that the…
The surprisingly low current density required for inducing the insulator to metal transition has made Ca$_2$RuO$_4$ 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 Ca$_2$RuO$_4$ 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…
Ambipolar doping-induced surface in-gap state on Mott-insulating Ca$_2$RuO$_4$
Institute for Solid State Physics, The University of Tokyo（东京大学固体物理研究所）；Roma Tre University（罗马第三大学）；CNR-SPIN（意大利国家研究委员会自旋电子学研究所）；Dipartimento di Fisica ”E.R. Caianiello”, Università di Salerno（萨莱诺大学E.R. Caianiello物理学系）；Physik-Institut, Universität Zürich（苏黎世大学物理研究所）
A paradigmatic case of multi-band Mott physics including spin-orbit and Hund's 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 Hund's coupling $J=0.4$ eV. …
Electrons in a simple correlated system behave either as itinerant charge carriers or as localized moments. However, there is growing evidence for the coexistence of itinerant electrons and local moments in transition metals with nearly degenerate $d$-orbitals. It demands one or more selective electron orbitals undergo the Mott transition while the others remain itinerant. Here we report the first observation of such an orbital selective Mott transition (OSMT) in Ca$_{1.8}$Sr$_{0.2}$RuO$_4$ by angle-resolved photoemission spectroscopy (ARPES). While we observed two sets of dispersing bands and…
We investigate the role of electron correlation in the electronic structure of honeycomb lattice Li$_2$RuO$_3$ using photoemission spectroscopy and band structure calculations. Monoclinic Li$_2$RuO$_3$ having Ru network as honeycomb lattice undergoes magneto-structural transition at T$_c$ $\sim$ 540 K from high temperature phase $C2/m$ to low temperature dimerized phase $P2_1/m$. Room temperature valence band photoemission spectra reveal an insulating ground state with no intensity at Fermi level ($E_F$). Ru 4$d$ band extracted from high and low photon energy valence band photoemission spectra…
The strongly correlated insulator Ca$_{2}$RuO$_4$ is 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 oxygen $K$-edge resonant inelastic X-ray scattering study of the antiferromagnetic Mott insulating state of Ca$_{2}$RuO$_4$. A set of low-energy ($\sim$80 and 400 meV) and high-energy ($\sim$1.3 and 2.2 eV) excitations are reported that show strong incident light polarization dependence. Our results strongly support a spin-orbit coupled …
The realistic description of correlated electron systems has taken an important step forward a few years ago as the combination of density functional methods and the dynamical mean-field theory was conceived. This framework allows access to both high and low energy physics and is capable of the description of the specific physics of strongly correlated materials, like the Mott metal-insulator transition. A very important step in the procedure is the interface between the band structure method and the dynamical mean-field theory and its impurity solver. We present a general interface between a …
We show that the pressure-temperature phase diagram of the Mott insulator Ca$_{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.
The electronic structures of the metallic and insulating phases of the alloy series Ca(2-x)Sr(x)RuO4 (0 <= x <= 2) are calculated using LDA, LDA+U and Dynamical Mean-Field Approximation methods. In the end members the groundstate respectively is an orbitally non-degenerate antiferromagnetic insulator (x=0) and a good metal (x=2). For x>0.5 the observed Curie-Weiss paramagnetic metallic state which possesses a local moment with the unexpected spin S=1/2, is explained by the coexistence of localized and itinerant Ru-4d-orbitals. For 0.2<x<0.5 we propose a state with partial orbital and spin orde…
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 [$x\leq0.07(1)$], 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 orthorhomb…
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-…
We report the synthesis of Ca$_2$RuO$_4$ thin films on NdCaAlO$_{4}$ (110), LaAlO$_3$ (100) and LaSrAlO$_4$ (001) substrates and show that epitaxial strain induces a transition from the Mott-insulating phase of bulk Ca$_2$RuO$_4$ into a metallic phase. Magnetometry and spin-polarized neutron reflectometry reveal a low-temperature, small-moment ferromagnetic state in metallic Ca$_2$RuO$_4$ films.
We report the evolution of the $k$-space electronic structure of lightly doped bulk Ca$_{2}$RuO$_{4}$ with uniaxial strain. Using ultrathin plate-like crystals, we achieve strain levels up to $-4.1\%$, sufficient to suppress the Mott phase and access the previously unexplored metallic state at low temperature. Angle-resolved photoemission experiments performed while tuning the uniaxial strain reveal that metallicity emerges from a marked redistribution of charge within the Ru $t_{2g}$ shell, accompanied by a sudden collapse of the spectral weight in the lower Hubbard band and the emergence of …
By means of polarized neutron diffraction in a magnetic field of 7.0 T at 1.6 K an anomalously large magnetization density is observed on the in-plane oxygen in Ca$_{1.5}$Sr$_{0.5}$RuO$_4$. Field-induced moments of different ions are determined by refinement on the flipping ratios, yielding $μ$$_{Ru}$ = 0.346(11) $μ$$_B$, $μ_{O1}$ = 0.076(6) $μ$$_B$ and $μ_{O2}$ = 0.009(6) $μ$$_B$. The moment on the oxygen arises from the strong hybridization between the Ru-4d and O-2p orbitals. %The maximum entropy method is used for the %reconstruction of the magnetization density and reveals a strongly anis…
The ground-state orbital occupancy of the Ru$^{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 …
Motivated by the earlier experimental results and \textit{ab initio} studies on the electronic structure of layered ruthenates (Sr$_2$RuO$_4$ and Ca$_2$RuO$_4$) we introduce and investigate the multiband $d-p$ charge transfer model describing a single RuO$_4$ layer, similar to the charge transfer model for a single CuO$_2$ plane including apical oxygen orbitals in high $T_c$ cuprates. The present model takes into account nearest-neighbor anisotropic ruthenium-oxygen $d-p$ and oxygen-oxygen $p-p$ hopping elements, crystal-field splittings and spin-orbit coupling. The intraorbital Coulomb repuls…
A comprehensive theory of superconductivity in Sr$_2$RuO$_4$ must explain experiments that suggest even parity superconducting order and others that suggest broken time reversal symmetry. Completeness further requires that the theory applies to Ca$_2$RuO$_4$, a Mott-Hubbard semiconductor that exhibits an unprecedented insulator-to-metal transition driven by very small electric field, and also by doping with very small concentration of electrons, leading to a metallic state proximate to ferromagnetism. A valence transition model, previously proposed for superconducting cuprates [Phys. Rev. B {\…
We show that spin-orbit coupling (SOC) plays Janus-faced roles on the orbitally-selective Mott transitions in a three-orbital Hubbard model with crystal field splitting at a specific filling of $2/3$, which is a minimal Hamiltonian for ruthenates. While the SOC favors metallic state due to enhancement of orbital hybridization at smaller on-site Coulomb repulsions, it stabilizes the Mott insulating state ascribed to lifting of orbital degeneracies and enhancement of band polarizations at larger electronic interaction. Moreover, an orbitally-selective non-Fermi liquid (OSnFL), where breakdown an…
We investigate the Mott transitions in two-band Hubbard models with different bandwidths. Applying dynamical mean field theory, we discuss the stability of itinerant quasi-particle states in each band. We demonstrate that separate Mott transitions occur at different Coulomb interaction strengths in general, which merge to a single transition only under special conditions. This kind of behavior may be relevant for the physics of the single-layer ruthenates, Ca$_{2-x}$Sr$_x$RuO$_4$.
Oxygen vacancies are a common source of excess electrons in complex oxides. In Mott insulators these additional electrons can induce a metal-insulator transition (MIT), fundamentally altering the electronic properties of the system. Here we study the effect of oxygen vacancies in LaTiO3, a prototypical Mott insulator close to the MIT. We show that the introduction of oxygen vacancies creates a vacancy-related band immediately below the partially filled Ti-t2g bands. We study the effect of this additional band on the Mott MIT using a combination of density functional theory and dynamical mean-f…
Strain engineering vanadium dioxide thin films is one way to alter this material's characteristic first order transition from semiconductor to metal. In this study we extend the exploitable strain regime by utilizing the very large lattice mismatch of 8.78 % occurring in the VO$_2$/RuO$_2$ system along the c axis of the rutile structure. We have grown VO$_2$ thin films on single domain RuO$_2$ islands of two distinct surface orientations by atomic oxygen-supported reactive MBE. These films were examined by spatially resolved photoelectron and x-ray absorption spectroscopy, confirming the corre…
We investigated optical spectra of quasi-two-dimensional multi-band Ca$% _{2-x} $Sr$_{x}$RuO$_{4}$ systems. The extended Drude model analysis on the ab-plane optical conductivity spectra indicates that the effective mass should be enhanced near $x=0.5$. Based on the sum rule argument, we showed that the orbital-selective Mott-gap opening for the $d_{yz/zx}$ bands, the widely investigated picture, could not be the origin of the mass enhancement. We exploited the multi-band effects in the extended Drude model analysis, and demonstrated that the intriguing heavy mass state near $x=0.5$ should com…
We report ARPES results of the Fermi surface of Ca_{1.5}Sr_{0.5}RuO$_{4}, which is at the boundary of magnetic/orbital instability in the phase diagram of the Ca-substituted Sr ruthenates. Three t_{2g} energy bands and the corresponding Fermi surface sheets are observed, which are also present in the Ca-free Sr_{2}RuO$_{4}. We find that while the Fermi surface topology of the alpha, beta (d_{yz, zx}) sheets remains almost the same in these two materials, the gamma (d_{xy}) sheet exhibits a hole-like Fermi surface in Ca_{1.5}Sr_{0.5}RuO_{4} in contrast to being electron-like in Sr_{2}RuO_{4}. O…
This Letter uses density functional, dynamical mean field, and Landau-theory methods to elucidate the interplay of electronic and structural energetics in the Mott metal-insulator transition. A Landau-theory free energy is presented that incorporates the electronic energetics, the coupling of the electronic state to local distortions and the coupling of local distortions to long-wavelength strains. The theory is applied to Ca$_2$RuO$_4$. The change in lattice energy across the metal-insulator transition is comparable to the change in electronic energy. Important consequences are a strongly fir…
In the present paper, we systematically studied the possible Orbital selective Mott transition (OSMT) in the $t_{2g}$ system, which has three orbital degeneracy. The slave Boson mean field theory is generalized to the three band systems with full Hund's rule coupling including spin flip and pair hopping terms. A new type of Mott transition which is driven by the crystal field splitting or the lattice distortion is found is this model. We argue that this new type of Mott transition may relate to the puzzling phase in $Sr_{x}Ca_{2-x}RuO_4$.
We perform nuclear magnetic resonance (NMR) measurements of the oxygen-17 Knight shifts for Sr$_2$RuO$_4$, while subjected to uniaxial stress applied along [100] direction. The resulting strain is associated with a strong variation of the temperature and magnetic field dependence of the inferred magnetic response. A quasi-particle description based on density-functional theory calculations, supplemented by many-body renormalizations, is found to reproduce our experimental results, and highlights the key role of a van-Hove singularity. The Fermi liquid coherence scale is shown to be tunable by …
By using a combination of detailed experimental studies and simple theoretical arguments, we identify a novel mechanism characterizing the hopping transport in the Mott insulating phase of Ca$_{2-x}$Sr$_x$RuO$_4$ near the metal-insulator transition. The hopping exponent $α$ shows a systematic evolution from a value of $α=1/2$ deeper in the insulator to the conventional Mott value $α=1/3$ closer to the transition. This behavior, which we argue to be a universal feature of disordered Mott systems close to the metal-insulator transition, is shown to reflect the gradual emergence of disorder-induc…
Quasi-particle spectra of the layer perovskite Sr$_2$RuO$_4$ are calculated within Dynamical Mean Field Theory for increasing values of the on-site Coulomb energy $U$. At small $U$ the planar geometry splits the $t_{2g}$ bands near $E_F$ into a wide, two-dimensional $d_{xy}$ band and two narrow, nearly one-dimensional $d_{xz,yz}$ bands. At larger $U$, however, the spectral distribution of these states exhibit similar correlation features, suggesting a common metal-insulator transition for all $t_{2g}$ bands at the same critical $U$.
While defects such as oxygen vacancies in correlated materials can modify their electronic properties dramatically, understanding the microscopic origin of electronic correlations in materials with defects has been elusive. Lanthanum nickelate with oxygen vacancies, LaNiO$_{3-x}$, exhibits the metal-to-insulator transition as the oxygen vacancy level $x$ increases from the stoichiometric LaNiO$_3$. In particular, LaNiO$_{2.5}$ exhibits a paramagnetic insulating phase, also stabilizing an antiferromagnetic state below $T_N\simeq152$K. Here, we study the electronic structure and energetics of La…
We study the magnetic order and excitations in strong spin-orbit coupled, Van Vleck-type, $d^4$ Mott insulators on a square lattice. Extending the previous work, we include the tetragonal crystal field splitting and explore its effects on magnetic phase diagram and magnon spectra. Two different ordered phases, with in-plane and out-of-plane orientation of the staggered moments, are found for the higher and lower values of the crystal field splitting, respectively. The magnetic excitation spectra for paramagnetic and magnetically ordered phases are calculated and discussed in the context of a c…
Strong electron correlations have long been recognized as driving the emergence of novel phases of matter. A well recognized example is high-temperature superconductivity which cannot be understood in terms of the standard weak-coupling theory. The exotic properties that accompany the formation of the two-channel Kondo effect including the emergence of an unconventional metallic state in the low-energy limit also originate from strong electron interactions. Despite its paradigmatic role for the formation of non-standard metal behavior, the stringent conditions required for its emergence have m…
The fate of a Mott insulator under strong low frequency optical driving conditions is a fundamental problem in quantum many-body dynamics. Using ultrafast broadband optical spectroscopy, we measured the transient electronic structure and charge dynamics of an off-resonantly pumped Mott insulator Ca$_2$RuO$_4$. We observe coherent bandwidth renormalization and nonlinear doublon-holon pair production occurring in rapid succession within a sub-100 femtosecond pump pulse duration. By sweeping the electric field amplitude, we demonstrate continuous bandwidth tuning and a Keldysh cross-over from a m…
We have investigated the in-plane uniaxial pressure effect on the antiferromagnetic Mott insulator Ca2RuO4 from resistivity and magnetization measurements. We succeeded in inducing the ferromagnetic metallic phase at lower critical pressure than by hydrostatic pressure, indicating that the flattening distortion of the RuO6 octahedra is more easily released under in-plane uniaxial pressure. We also found a striking in-plane anisotropy in the pressure responses of various magnetic phases: Although the magnetization increases monotonically with pressure diagonal to the orthorhombic principal axes…
The iso-electronic $d^{4}$ compounds of the $4d$ series show rich phase diagrams due to competing spin, charge and orbital degrees of freedom in presence of strong correlations and structural distortions. One such iso-electronic series, $Ca_{2-x}Sr_{x}RuO_{4}$, is studied within the GGA (and spin-orbit coupled GGA) plus DMFT formalism using the hybridization expansion of continuous time Quantum Monte Carlo solver. While the local dynamical correlations make $Sr_{2}RuO_{4}$ a Hund's metal, they drive $Ca_{2}RuO_{4}$ to a Mott insulating ground state. We study the dynamic and static single-parti…
The synthesis of stoichiometric Sr$_2$RuO$_4$ thin films has been a challenge because of the high volatility of ruthenium oxide precursors, which gives rise to ruthenium vacancies in the films. Ru vacancies greatly affect the transport properties and electronic phase behavior of Sr$_2$RuO$_4$, but their direct detection is difficult due to their atomic dimensions and low concentration. We applied polarized X-ray absorption spectroscopy at the oxygen K-edge and confocal Raman spectroscopy to Sr$_2$RuO$_4$ thin films synthesized under different conditions. The results show that these methods can…
Layered perovskite ruthenium oxides exhibit a striking series of metal-insulator and magnetic-nonmagnetic phase transitions easily tuned by temperature, pressure, epitaxy, and nonlinear drive. In this work, we combine results from two complementary state of the art many-body methods, Auxiliary Field Quantum Monte Carlo and Dynamical Mean Field Theory, to determine the low-temperature phase diagram of Ca$_2$RuO$_4$. Both methods predict a low temperature, pressure-driven metal-insulator transition accompanied by a ferromagnetic-antiferromagnetic transition. The properties of the ferromagnetic s…
We propose the concept of "hybridization-switching induced Mott transition" which is relevant to a broad class of ABO$_3$ perovskite materials including BiNiO$_3$ and PbCrO$_3$ which feature extended $6s$ orbitals on the A-site cation (Bi or Pb), and A-O covalency induced ligand holes. Using {\it ab initio} electronic structure and slave rotor theory calculations, we show that such systems exhibit a breathing phonon driven A-site to oxygen hybridization-wave instability which conspires with strong correlations on the B-site transition metal ion (Ni or Cr) to induce a Mott insulator. These Mott…
We reveal the crucial effect of strong spin-charge coupling on high-harmonic generation (HHG) in Mott insulators. In a system with antiferromagnetic correlations, the HHG signal is drastically enhanced with decreasing temperature, even though the gap increases and the production of charge carriers is suppressed. This anomalous behavior, which has also been observed in recent HHG experiments on Ca$_2$RuO$_4$, originates from a cooperative effect between the spin-charge coupling and the thermal ensemble, and the strongly temperature-dependent coherence between charge carriers. We argue that the …
Despite many efforts to rationalize the strongly correlated electronic ground states in doped Mott insulators, the nature of the doping induced insulator to metal transition is still a subject under intensive investigation. Here we probe the nanoscale electronic structure of the Mott insulator Sr$_2$IrO$_{4-δ}$ with low-temperature scanning tunneling microscopy and find enhanced local density of states (LDOS) inside the Mott gap at the location of individual apical oxygen site defects. We visualize paths of enhanced conductance arising from the overlapping of defect states which induces finite…
Cation displacements, oxygen octahedral tilts, and magnetism of epitaxial, ferrimagnetic, insulating GdTiO3 films sandwiched between cubic SrTiO3 layers are studied using scanning transmission electron microscopy and magnetization measurements. With decreasing GdTiO3 film thickness, structural (GdFeO3-type) distortions are reduced, concomitant with a reduction in the Curie temperature. Ferromagnetism persists to smaller deviations from the cubic perovskite structure than is the case for the bulk rare earth titanates. The results indicate that the FM ground state is controlled by the narrow ban…
The spectral properties of a one-dimensional (1D) single-chain Mott insulator Sr$_2$CuO$_{3}$ have been studied in angle-resolved photoemission and optical spectroscopy, at half filling and with small concentrations of extra charge doped into the chains via high oxygen pressure growth. The single- particle gap is reduced with oxygen doping, but the metallic state is not reached. The bandwidth of the charge-transfer band increases with doping, while the state becomes narrower, allowing unambiguous observation of separated spinon and holon branches in the doped system. The optical gap is not cha…
Accurate high-energy electron diffraction measurements of structure factors of NiO have been carried out to investigate how strong correlations in the Ni 3d shell affect electron charge density in the interior area of nickel ions and whether the new ab-initio approaches to the electronic structure of strongly correlated metal oxides are in accord with experimental observations. The generalized gradient approximation (GGA) and the local spin density approximation corrected by the Hubbard U term (LSDA+U) are found to provide the closest match to experimental measurements. The comparison of calcu…
Unusual metallic states involving breakdown of the standard Fermi-liquid picture of long-lived quasiparticles in well-defined band states emerge at low temperatures near correlation-driven Mott transitions. Prominent examples are ill-understood metallic states in $d$- and $f$-band compounds near Mott-like transitions. Finding of superconductivity in solid O$_{2}$ on the border of an insulator-metal transition at high pressures close to 96~GPa is thus truly remarkable. Neither the insulator-metal transition nor superconductivity are understood satisfactorily. Here, we undertake a first step in …
Stoichiometric Sr2IrO4 is a ferromagnetic Jeff = 1/2 Mott insulator driven by strong spin-orbit coupling. Introduction of very dilute oxygen vacancies into single-crystal Sr2IrO4-delta with delta < 0.04 leads to significant changes in lattice parameters and an insulator-to-metal transition at TMI = 105 K. The highly anisotropic electrical resistivity of the low-temperature metallic state for delta ~ 0.04 exhibits anomalous properties characterized by non-Ohmic behavior and an abrupt current-induced transition in the resistivity at T* = 52 K, which separates two regimes of resisitive switching …
The heat carriers responsible for the unexpectedly large thermal Hall conductivity of the cuprate Mott insulator La$_2$CuO$_4$ were recently shown to be phonons. However, the mechanism by which phonons in cuprates acquire chirality in a magnetic field is still unknown. Here, we report a similar thermal Hall conductivity in two cuprate Mott insulators with significantly different crystal structures and magnetic orders - Nd$_2$CuO$_4$ and Sr$_2$CuO$_2$Cl$_2$ - and show that two potential mechanisms can be excluded - the scattering of phonons by rare-earth impurities and by structural domains. Ou…
Transport and magnetic properties have been systematically investigated for SmMnAsO_{1-x} with controlled electron-doping. As the electron band-filling is increased with the increase of oxygen deficiency (x), the resistivity monotonically decreases and the transition from Mott-insulator to metal occurs between x=0.17 and 0.2. Seebeck coefficient at room temperature abruptly changes around the critical doping level from a large value (\sim -300 μV/K) to a small one (\sim -50 μV/K) both with negative sign. In the metallic compounds with x=0.2 and x=0.3, Mn spins order antiferromagnetically aroun…
Using an \textit{ab initio} approach based on the GW approximation which includes strong local \textbf{k}-space correlations, the Metal-Insulator Transition of M$_2$ vanadium dioxide is broken down into its component parts and investigated. Similarly to the M$_{1}$ structure, the Peierls pairing of the M$_{2}$ structure results in bonding-antibonding splitting which stabilizes states in which the majority of the charge density resides on the Peierls chain. This is insufficient to drop all of the bonding states into the lower Hubbard band however. An antiferroelectric distortion on the neighbor…
Late transition-metal oxides with small charge-transfer energy $Δ$ raise issues for state-of-the-art correlated electronic structure schemes such as the combination of density functional theory (DFT) with dynamical mean-field theory (DMFT). The accentuated role of the oxygen valence orbitals in these compounds asks for an enhanced description of ligand-based correlations. Utilizing the rocksalt-like NiO as an example, we present an advancement of charge self-consistent DFT+DMFT by including self-interaction correction (SIC) applied to oxygen. This introduces explicit onsite O correlations as w…
The $t_{2g}$ orbitals of an edge-shared transition-metal oxide with a honeycomb lattice structure form dispersionless electronic bands when only hopping mediated by the edge-sharing oxygens is accessible. This is due to the formation of isolated quasimolecular orbitals (QMOs) in each hexagon, introduced recently by Mazin et al. [Phys. Rev. Lett. 109, 197201 (2012)], which stabilizes a band insulating phase for $t_{2g}^5$ systems. However, with help of the exact diagonalization method to treat the electron kinetics and correlations on an equal footing, we find that the QMOs are fragile against …
