In contrast to the previous reports that the divalent perovskite SrCrO$_3$ was believed to be cubic structure and nonmagnetic metal, recent measurements suggest coexistence of majority tetragonally distorted weak antiferromagnetic phase and minority nonmagnetic cubic phase. Within the local (spin) density approximation (L(S)DA) our calculations confirm that a slightly tetragonally distorted phase indeed is energetically favored. Using the correlated band theory method (LDA+ Hubbard U) as seems to be justified by the unusual behavior observed in SrCrO$_3$, above the critical value $U_c$=4 eV only the distorted phase undergoes an orbital-ordering transition, resulting in $t_{2g}^2 --> d_{xy}^1$($d_{xz}d_{yz}$)$^1$ corresponding to the filling of the $d_{xy}$ orbital but leaving the other two degenerate. The Fermi surfaces of the cubic phase are simple with nesting features, although the nesting wavevectors do not correlate with known data. This is not uncommon in perovskites; the strongly directional d-d bonding often leads to boxlike Fermi surfaces, and either the nesting is not strong enough, or the matrix elements are not large enough, to promote instabilities. Fixed spin moment calculations indicate the cubic structure is just beyond a ferromagnetic Stoner instability (IN(0)~1.1) in L(S)DA, and that the energy is unusually weakly dependent on the moment out to 1.5$μ_B$/Cr (varying only by 11 meV/Cr), reflecting low energy long-wavelength magnetic fluctuations. We observe that this system shows strong magneto-phonon coupling (change in Cr local moment is ~7.3 $μ_B$/Å) for breathing phonon modes.
We have studied the interplay between orbital ordering, Jahn-Teller and GdFeO3-type lattice distortions in perovskite-type transition-metal oxides using model Hartree-Fock calculations. It has been found that the covalency between A-site cations and oxygens causes interaction between the Jahn-Teller and GdFeO3-type distortions. The present calculations explain why the d-type Jahn-Teller distortion and orbital ordering compatible with it are realized in LaMnO3, YVO3 and YTiO3
We develop the cluster self-consistent field method incorporating both electronic and lattice degrees of freedom to study the origin of ferromagnetism in Cs$_{2}$AgF$_{4}$. After self-consistently determining the harmonic and anharmonic Jahn-Teller distortions, we show that the anharmonic distortion stabilizes the staggered x$^{2}$-z$^{2}$/y$^{2}$-z$^{2}$ orbital and ferromagnetic ground state, rather than the antiferromagnetic one. The amplitudes of lattice distortions, Q$_{2}$ and Q$_{3}$, the magnetic coupling strengthes, J$_{x,y}$, and the magnetic moment, are in good agreement with the ex…
Theoretical investigations of the electronic, magnetic and structural properties of LaTiO3 and YTiO3 have been made. In the framework of GGA and GGA+U scheme we analyzed the effect of the local Coulomb interaction (U) value on the atomic forces acting in the experimental structure. The optimal parameters of the electron-electron on-site interactions as well as the orbital configurations and magnetic properties are determined.
The role of lattice distortion in the charge, orbital and spin ordering in half doped manganites has been investigated. For fixed magnetic ordering, we show that the cooperative lattice distortion stabilize the experimentally observed ordering even when the strong on-site electronic correlation is taken into account. Furthermore, without invoking the magnetic interactions, the cooperative lattice distortion alone may lead to the correct charge and orbital ordering including the charge stacking effect, and the magnetic ordering can be the consequence of such a charge and orbital ordering. We pr…
The charge order of CE phase in half-doped manganites is studied, based on an argument that the charge-ordering is caused by the Jahn-Teller distortions of MnO6 octahedra rather than Coulomb repulsion between electrons. The uantitative calculation on the ferromagnetic zigzag chain as the basic structure unit of CE phase within the framework of two-orbital double exchange model including Jahn-Teller effect is performed, and it is shown that the charge-disproportionation of Mn cations in the charge-ordered CE phase is less than 13%. In addition, we predict the negative charge-disproportionation …
We have investigated electronic structures of antiferromagnetic YBaCo_2O_5 using the local spin-density approximation (LSDA) + U method. The charge and orbital ordered insulating ground state is correctly obtained with the strong on-site Coulomb interaction. Co^{2+} and Co^{3+} ions are found to be in the high spin (HS) and intermediate spin (IS) state, respectively. It is considered that the tetragonal to orthorhombic structural transition is responsible for the ordering phenomena and the spin states of Co ions. The large contribution of the orbital moment to the total magnetic moment indicat…
Temperature dependences of a magnetic and an orbital Bragg reflection at the Mn L2 and L3 edges of La0.5Sr1.5MnO4 have been collected. The temperature evolution of the orbital reflection depend strongly on the x-ray energy and reflects the different order parameteres for orbitals and Jahn-Teller distortions. The gradual increase of the orbital order parameter indicates that the orbital order and not the Jahn-Teller distortion drives the metal-insulator transition. Correspondingly, the orbital-orbital (super) exchange interaction dominates over the Jahn-Teller strain-field interaction.
LaMnO$_3$ is considered as a prototypical Jahn-Teller perovskite compound, exhibiting a metal to insulator transition at $T_{JT} = 750K$ related to the joint appearance of an electronic orbital ordering and a large lattice Jahn-Teller distortion. From first-principles, we revisit the behavior of LaMnO$_3$ and show that it is not only prone to orbital ordering but also to charge ordering. Both charge and orbital orderings appear to be enabled by rotations of the oxygen octahedra and the subtle competition between them is monitored by a large tetragonal compressive strain, that is itself a Jahn-…
We study double-exchange models with itinerant t2g electrons in spinel and pyrochlore crystals. In both cases the localized spins form a network of corner-sharing tetrahedra. We show that the strong directional dependence of t2g orbitals leads to unusual Fermi surfaces that induce spin superstructures and noncoplanar orderings for a weak coupling between itinerant electrons and localized spins. Implications of our results to ZnV2O4 and Cd2Os2O7 are also discussed.
Vanadium Sesquioxide (V$_2$O$_3$) is an antiferromagnetic insulator below $T_{\mathrm N}\approx$ 155 K. The magnetic order is not of C- or G-type as one would infer from the bipartite character of the hexagonal basal plane in the high-temperature corundum structure. In fact, the Néel transition is accompanied by a monoclinic distortion that makes one bond of the honeycomb plane inequivalent from the other two, thus justifying a magnetic structure with one ferromagnetic bond and two antiferromagnetic ones. We show here that the magnetic ordering, the accompanying monoclinic structural distortio…
We investigate the origin of the orbital ordering in the paramagnetic phase of KCrF$_3$. All previous studies described structural parameters of the paramagnetic phase using a magnetic ordering in the compound. Our simulations of real paramagnetic KCrF$_3$ were performed within an approach combining density functional theory and dynamical mean field theory (DFT+DMFT). As a result, it was found that the experimentally observed cooperative Jahn-Teller effect is successfully described in a lattice relaxation calculation for structure without any long-range magnetic ordering. It is established tha…
We have performed local STM studies on potassium-doped C60 (KxC60) monolayers over a wide regime of the phase diagram. As K content increases from x = 3 to 5, KxC60 monolayers undergo metal-insulator-metal reentrant phase transitions and exhibit a variety of novel orientational orderings. The most striking new structure has a pinwheel-like 7-molecule unit cell in insulating K4+dC60. We propose that the driving mechanism for the orientational ordering in KxC60 is the lowering of electron kinetic energy through maximization of the overlap of neighboring molecular orbitals over the entire doping …
I study the structural and magnetic instabilities in LaNiO$_3$ using density functional theory calculations. From the non-spin-polarized structural relaxations, I find that several structures with different Glazer tilts lie close in energy. The $Pnma$ structure is marginally favored compared to the $R\overline{3}c$ structure in my calculations, suggesting the presence of finite-temperature structural fluctuations and a possible proximity to a structural quantum critical point. In the spin-polarized relaxations, both structures exhibit the $\uparrow\!\!0\!\!\downarrow\!\!0$ antiferromagnetic or…
We demonstrate with LSDA+U calculations that x-ray scattering at the K edge of Mn is sensitive to orbital ordering in one energy range and Jahn-Teller distortion in another. Contrary to what is suggested by atomic or cluster models used to date we show that band structure effects rather than local Coulomb interactions dominate the polarization dependence of the K edge scattering and therefore it is sensitive to nearest neighbour bond length distortions and next nearest neighbour orbital occupation. Based on this we propose a new mechanism for K edge x-ray scattering in the manganates which we …
We investigated the origin of the energy splitting observed in the resonant x-ray scattering (RXS) in manganites. Using thin film samples with controlled lattice parameters and orbital states at a fixed orbital filling, we estimated that the contribution of the interatomic Coulomb interaction relative to the Jahn-Teller mechanism is insignificant and at most 0.27. This indicates that RXS probes mainly Jahn-Teller distortion in manganites.
Combined effects of electron correlations and lattice distortions are investigated on the charge ordering in θ-(BEDT-TTF)2RbZn(SCN)4 theoretically in a two-dimensional 3/4-filled extended Hubbard model with electron-lattice couplings. It is known that this material undergoes a phase transition from a high-symmetry metallic state to a low-symmetry insulating state with a horizontal-stripe charge order (CO) by lowering temperature. By means of the exact-diagonalization method, we show that electron-phonon interactions are crucial to stabilize the horizontal-stripe CO and to realize the low-symme…
Density functional theory calculations within the generalized gradient approximation are employed to study the ground state of Co2FeAl. Various magnetic configurations are considered to find out its most stable phase. The ferromagnetic ground state of the Co2FeAl is energetically observed with an optimized lattice constant of 5.70 Å. Thereafter, the system was subjected under uniform and non-uniform strains to see their effects on spin polarization (P) and half-metallicity. The effect of spin orbit coupling is considered in the present study. Half-metallicity (and 100 % P) is only retained und…
Synchrotron x-ray diffraction and resonant magnetic scattering experiments on single crystal DyMnO3 have been carried out between 4 and 40 K. Below TN(Dy) = 5K, the Dy magnetic moments order in a commensurate structure with propagation vector 0.5 b*. Simultaneous with the Dy magnetic ordering, an incommensurate lattice modulation with propagation vector 0.905 b* evolves while the original Mn induced modulation is suppressed and shifts from 0.78 b* to 0.81 b*. This points to a strong interference of Mn and Dy induced structural distortions in DyMnO3 besides a magnetic coupling between the Mn an…
We present a theoretical study on the relation between the size of the rare earth ions, often known as chemical pressure, and the stability of the coherent Jahn-Teller distortions in undoped perovskite manganites. Using a Keating model expressed in terms of atomic scale symmetry modes, we show that there exists a coupling between the uniform shear distortion and the staggered buckling distortion within the Jahn-Teller energy term. It is found that this coupling provides a mechanism by which the coherent Jahn-Teller distortion is more stabilized by smaller rare earth ions. We analyze the appear…
We present a systematic investigation of the antiferromagnetic ordering and structural distortion for the series of Ba(Fe{1-x}Ru{x})2As2 compounds (0 <= x <= 0.246). Neutron and x-ray diffraction measurements demonstrate that, unlike for the electron-doped compounds, the structural and magnetic transitions remain coincident in temperature. Both the magnetic and structural transitions are gradually suppressed with increased Ru concentration and coexist with superconductivity. For samples that are superconducting, we find strong competition between superconductivity, the antiferromagnetic orderi…
The orbital, lattice, and spin ordering phenomena in KCuF3 are investigated by means of LDA+U calculations, based on ab-initio pseudopotentials.We examine the Cu-3d orbital ordering and the associated Jahn-Teller distortion in several different spin-ordered structures of KCuF3. The ground state is correctly predicted to be an A-type antiferromagnetic structure, and the calculated Jahn-Teller distortion agrees also well with experiment. Concerning the orbital ordering, we find that even for a highly ionic compound such as KCuF3, the orbital-order parameter is significantly reduced with respect …
Possible order parameters of the phase IV in CexLa1-xB6 are discussed with special attention to the lattice distortion recently observed. A Γ_{5u}-type octupole order with finite wave number is proposed as the origin of the distortion along the [111] direction. The Γ_8 crystalline electric field (CEF) level splits into three levels by a mean field with the Γ_{5u} symmetry. The ground and highest singlets have the same quadrupole moment, while the intermediate doublet has an opposite sign. It is shown that any collinear order of Γ_{5u}-type octupole moment accompanies the Γ_{5g}-type ferro-quad…
We present powder and single crystal X-ray diffraction data as evidence for a monoclinic distortion in the low spin (S=0) and intermediate spin state (S=1) of LaCoO3. The alternation of short and long bonds in the ab plane indicates the presence of eg orbital ordering induced by a cooperative Jahn-Teller distortion. We observe an increase of the Jahn-Teller distortion with temperature in agreement with a thermally activated behavior of the Co3+ ions from a low-spin ground state to an intermediate-spin excited state.
Keeping in mind the experimental results that indicate local lattice distortions, charge and spin orderings, we have developed a phenomenological approach which allows us to describe the electronic phase diagram of cuprates and related systems in terms of few parameters.In the present work we consider a third-order parameter theory which characterize charge, spin and superconductivity orderings. We are thus led to a theory of three scalar fields. By coupling these scalars to gauge fields we are naturally led to string-like solutions, which we interpret as stripes. This ties nicely with our qua…
With the use of the density function calculations we show that the actual crystal structure of Cs$_2$CuCl$_2$Br$_2$ should contain elongated in the $ab-$plane CuCl$_4$Br$_2$ octahedra, in contrast to the experimentally observed compression in $c-$direction. We also predict that the spins on Cu$^{2+}$ ions should be ferromagnetically ordered in $ab-$plane, while the exchange interaction along $c-$direction is small and its sign is uncertain.
We use neutron scattering to study the lattice and magnetic structure of the layered half-doped manganite Pr$_{0.5}$Ca$_{1.5}$MnO$_4$. On cooling from high temperature, the system first becomes charge- and orbital- ordered (CO/OO) near $T_{CO}=300$ K and then develops checkerboard-like antiferromagnetic (AF) order below $T_{N}=130$ K. At temperatures above $T_{N}$ but below $T_{CO}$ ($T_N<T<T_{CO}$), the appearance of short-range AF spin correlations suppresses the CO/OO induced orthorhombic strain, contrasting with other half-doped manganites, where AF order has no observable effect on the la…
DyB4 has a two-dimensional Shastry-Sutherland (Sh-S) lattice with strong Ising character of the Dy ions. Despite the intrinsic frustrations, surprisingly, it undergoes two successive transitions: a magnetic ordering at TN = 20K, and a quadrupole ordering at TQ=12.5 K. From high-resolution neutron and synchrotron X-ray powder diffraction studies, we have obtained full structural information on this material in all phases, and demonstrate that structural modifications occurring at quadrupolar transition lead to the lifting of frustrations inherent in the Sh-S model. Our study thus provides a com…
We demonstrate that an A-type antiferromagnetic (AFM) state of Pr{0.5}Sr{0.5}MnO{3} exhibits a novel charge ordering which governs the transport property. This charge ordering is stripe-like, being characterized by a wave vector q ~ (0,0,0.3) with very anisotropic correlation parallel and perpendicular to the stripe direction. This charge ordering is specific to the manganites with relatively wide one-electron band width (W) which often exhibit a metallic A-type AFM state, and should be strictly distinguished from the CE-type checkerboard-like charge ordering which is commonly observed in mang…
Impurity effects on the stability of a ferromagnetic metallic state in a bicritical-state manganite, (La0.7Pr0.3)0.65Ca0.35MnO3, on the verge of metal-insulator transition have been investigated by substituting a variety of transition-metal atoms for Mn ones. Among them, Fe doping exhibits the exceptional ability to dramatically decrease the ferromagnetic transition temperature. Systematic studies on the magnetotransport properties and x-ray diffraction for the Fe-doped crystals have revealed that charge-orbital ordering evolves down to low temperatures, which strongly suppresses the ferromagn…
Neutron and x-ray diffraction studies of Ba(Fe{1-x}Mn{x})2As2 for low doping concentrations (x <= 0.176) reveal that at a critical concentration, 0.102 < x < 0.118, the tetragonal-to-orthorhombic transition abruptly disappears whereas magnetic ordering with a propagation vector of (1/2 1/2 1) persists. Among all of the iron arsenides this observation is unique to Mn-doping, and unexpected because all models for "stripe-like" antiferromagnetic order anticipate an attendant orthorhombic distortion due to magnetoelastic effects. We discuss these observations and their consequences in terms of pre…
We theoretically investigate effects of lattice distortions on the spin ordering of classical Heisenberg antiferromagnets on the breathing pyrochlore lattice. In the model, local lattice distortions originating from the site vibration are taken into account to yield effective spin interactions via the spin-lattice coupling (SLC). The breathing lattice-alternation is characterized by the ratio of the nearest-neighbor interaction for large tetrahedra to that for small ones, J'/J. It is found by Monte Carlo simulations that the system exhibits a first-order transition into four different types of…
First-principles calculations have been performed for different collinear magnetic orderings in orthorhombic manganites, such as HoMnO3, TbMnO3 and YMnO3, showing large GdFeO3-like distortions. Our results suggest that the AFM-E type ordering, experimentally observed in HoMnO3 and recently proposed from model hamiltonian studies as a potentially novel phase, is indeed the magnetic ground state. Its stability is strongly connected with octahedral distortions and points to the relevance of structural more than chemical effects. The calculated exchange constants, extracted from a Heisenberg model…
We employ a combination of density functional theory and dynamical mean-field theory to investigate the electronic structure of the recently synthesized insulator BaCrO$_3$. Our calculations show that Hund's coupling is responsible for strong correlation effects, which are however not sufficient to turn the system insulating. A finite Jahn-Teller distortion lifting the orbital degeneracy is necessary to stabilize an insulating state with orbital ordering and consequent magnetic ordering.
We have analyzed the experimental evidence of charge and orbital ordering in La0.5Sr1.5MnO4 using first principles band structure calculations. Our results suggest the presence of two types of Mn sites in the system. One of the Mn sites behaves like an Mn(3+) ion, favoring a Jahn-Teller distortion of the surrounding oxygen atoms, while the distortion around the other is not a simple breathing mode kind. Band structure effects are found to dominate the experimental spectrum for orbital and charge ordering, providing an alternate explanation for the experimentally observed results.
Interesting emergent behavior in quantum materials arises when the interaction of electrons with the lattice leads to partial localization and ordering of charge at low temperatures. The triangular lattice of some transition metal dichalcogenides additionally presents an interesting case, where spin order is frustrated, leading to an additional complex interplay of interactions involving spin, charge and lattice degrees of freedom. Here we present a study of local symmetry breaking of the lattice structure in the layered dichalcogenide material 1T-TaS$_{2}$ using x-ray pair-distribution functi…
We found, using density-functional theory calculations within the generalized gradient approximation, that Cs$_2$AgF$_4$ is stabilized in the insulating orthorhombic phase rather than in the metallic tetragonal phase. The lattice distortion present in the orthorhombic phase corresponds to the $x^2-z^2$/$y^2-z^2$ hole-orbital ordering of the Ag$^{2+}$ $4d^9$ ions, and this orbital ordering leads to the observed ferromagnetism, as confirmed by the present total-energy calculations. This picture holds in the presence of moderate 4d-electron correlation. The results are compared with the picture o…
The generalized gradient approximation (GGA) scheme in the first-principles calculations are used to study the effect of L21 and XA ordering on the phase stability, half-metallicity and magnetism of Co2FeAl (CFA) Heusler alloy. Various possible hypothetical structures: L21-I, L21-II, XA-I, and XA-II were prepared under the conventional L21 and inverse XA phases by altering the atomic occupancies at their Wyckoff sites. It is found that the XA-II phase of CFA is the most stable phase energetically among all the structures. The electronic structure calculations without U show the presence of hal…
The crystal structure and the magnetism of BaMn$_2$O$_3$ have been studied by thermodynamic and by diffraction techniques using large single crystals and powders. BaMn$_2$O$_3$ is a realization of a $S = 5/2$ spin ladder as the magnetic interaction is dominant along 180$^\circ$ Mn-O-Mn bonds forming the legs and the rungs of a ladder. The temperature dependence of the magnetic susceptibility exhibits well-defined maxima for all directions proving the low-dimensional magnetic character in BaMn$_2$O$_3$. The susceptibility and powder neutron diffraction data, however, show that BaMn$_2$O$_3$ exh…
We explore the magnetic phases in a Kondo lattice model on the geometrically frustrated Shastry-Sutherland lattice at metallic electron densities, searching for noncollinear and noncoplanar spin textures. Motivated by experimental observations in many rare-earth-based frustrated metallic magnets, we treat the local moments as classical spins and set the coupling between the itinerant electrons and local moments as the largest energy scale in the problem. Our results show that a noncollinear flux state is stabilized over an extended range of Hamiltonian parameters. These spin states can be quen…
We investigate the emergence of anti-ferromagnetic ordering and its effect on the helical edge states in a quantum spin Hall insulator, in the presence of strong Coulomb interaction. Using dynamical mean-field theory, we show that the breakdown of lattice translational symmetry favours the formation of magnetic ordering with non-trivial spatial modulation. The onset of a non-uniform magnetization enables the coexistence of spin-ordered and topologically non-trivial states. An unambiguous signature of the persistence of the topological bulk property is the survival of bona fide edge states. We …
We analyzed the possible magnetic and orbital orderings of double perovskites, using a simple extension of the double exchange model well suited for these compounds. Orbital ordering is favored by the on site repulsion at the Fe ions. We obtain a rich phase diagram, including ferri- and antiferromagnetic phases, which can, in turn, be metallic or insulating, depending on the existence of orbital order.
Using first principle band structure calculations, we critically examine results of resonant x-ray scattering experiments which is believed to directly probe charge and orbital ordering. Considering the specific case of La0.5Sr1.5MnO4, we show that this technique actually probes most directly and sensitively small structural distortions in the system. Such distortions, often difficult to detect with more conventional techniques, invariably accompany and usually cause the orbital and charge orderings. In this sense, this technique is only an indirect probe of such types of ordering. Our results…
To understand the orbital ordering of $LaMnO_3$ in the ground state, we study it in the A-type spin antiferromagnetic state. We calculate the two-dimensional response functions associated with the Jahn-Teller $Q_2$ and $Q_3$ distortions and find that they diverge at the wavevector $π$,$π$). Furthermore, the $Q_2$ response function diverges faster which indicates that perhaps the ordering of the orbitals at low temperatures is dominated by the $Q_2$ distortion. We calculate the ground state energy for the cases when only one of the $Q_2$ and $Q_3$ modes is excited cooperatively and find that th…
How particular bonds form in quantum materials has been a long-standing puzzle. Two key concepts dealing with charge degrees of freedom are dimerization (forming metal-metal bonds) and charge ordering (CO). Since the 1930s, these two concepts have been frequently invoked to explain numerous exciting quantum materials, typically insulators. Here we report dimerization and CO within the dimers coexisting in metallic NaRu$_2$O$_4$. By combining high-resolution x-ray diffraction studies and theoretical calculations, we demonstrate that this unique phenomenon occurs through a new type of bonding, w…
An electronic effect on a macroscopic domain structure is found in a strongly correlated half-doped manganite film Nd$_{0.5}$Sr$_{0.5}$MnO3 grown on a (011) surface of SrTiO3. The sample has a high-temperature (HT) phase free from distortion above 180K and two low-temperature (LT) phases with a large shear-mode strain and a concomitant twin structure. One LT phase has a large itinerancy (A-type), and the other has a small itinerancy (CE-type), while the lattice distortions they cause are almost equal. Our x ray diffraction measurement shows that the domain size of the LT phase made by the HT-C…
Motivated by recent experiments on the observation of room temperature skyrmions in a layered heterostructure and subsequent demonstration of topological Hall effect in the same system, we have studied a minimal model of itinerant electrons coupled to local moments with competing interactions in an external magnetic field. Working in the limit of strong magneto-electric coupling where the fast dynamics of the electrons can be decoupled from the slow dynamics of the local moments (treated as classical spins), we analyze the multiple field induced magnetic phases and the associated electronic tr…
We have performed powder neutron diffraction on $^7$Li-enriched sample of LiMn$_2$O$_4$ at 300 K. The crystal structure determined by Rietveld analysis is a cubic spinel with space group of $Fd\bar{3}m$ in which all Mn atoms are crystallograghically equivalent, consistent with many preceding studies. However, the atomic pair distrubution function (PDF) of this compound can not be fitted by the cubic structure with space group of $Fd\bar{3}m$ satisfactorily, and it can be reproduced by the orthorhombic structure with $Fddd$. It corresponds with the structure of charge ordered phase below about …
Roles of orbital and lattice degrees of freedom in strongly correlated systems are investigated to understand electronic properties of perovskite Mn oxides such as La_{1-x}Sr_{x}MnO_{3}. An extended double-exchange model containing Coulomb interaction, doubly degenerate orbitals and Jahn-Teller coupling is derived under full polarization of spins with two-dimensional anisotropy. Quantum fluctuation effects of Coulomb interaction and orbital degrees of freedom are investigated by using the quantum Monte Carlo method. In undoped states, it is crucial to consider both the Coulomb interaction and …
A novel metallic and magnetic transition metal oxide Ag2NiO2 is studied by means of resistivity, magnetic susceptibility, specific heat and X-ray diffraction. The crystal structure is characterized by alternating stacking of a Ni3+O2 layer and a (Ag2)+ layer, the former realizing a spin-1/2 triangular lattice with eg orbital degeneracy and the latter providing itinerant electrons. It is found that the NiO2 layer exhibits orbital ordering at Ts = 260 K and antiferromagnetic spin ordering at TN = 56 K. Moreover, a moderately large mass enhancement is found for the itinerant electrons, suggesting…
The electronic, magnetic and orbital structures of KCrF_3 are determined in all its recently identified crystallographic phases (cubic, tetragonal, and monoclinic) with a set of {\it ab initio} LSDA and LSDA+U calculations. The high-temperature undistorted cubic phase is metallic within the LSDA, but at the LSDA+U level it is a Mott insulator with a gap of 1.72 eV. The tetragonal and monoclinic phases of KCrF_3 exhibit cooperative Jahn-Teller distortions concomitant with staggered 3x^2-r^2/3y^2-r^2 orbital order. We find that the energy gain due to the Jahn-Teller distortion is 82/104 meV per …
The Mott insulating perovskite KCuF3 is considered the archetype of an orbitally-ordered system. By using the LDA+dynamical mean-field theory (DMFT) method, we investigate the mechanism for orbital-ordering (OO) in this material. We show that the purely electronic Kugel-Khomskii super-exchange mechanism (KK) alone leads to a remarkably large transition temperature of T_KK about 350 K. However, orbital-order is experimentally believed to persist to at least 800 K. Thus Jahn-Teller distortions are essential for stabilizing orbital-order at such high temperatures.
The electronic structure and magnetism in the sodium nickelate NaNiO_2 in the low-temperature phase is studied from density-functional calculations using the linear muffin-tin orbitals method. An antiferromagnetic solution with a magnetic moment of 0.7 m_B per Ni ion is found. A ferrodistorsive orbital ordering is shown to occur due to the Jahn-Teller distortion around the Ni^{3+} ion in agreement with the orbital ordering inferred from neutron diffraction. While the intralayer exchange is ferromagnetic, the interlayer exchange is weakly antiferromagnetic, mediated by a long Ni-O-Na-O-Ni super…
The origin of the antiferromagnetic order and puzzling properties of LaTiO_3 as well as the magnetic phase diagram of the perovskite titanates are studied theoretically. We show that in LaTiO_3, the t_{2g} degeneracy is eventually lifted by the La cations in the GdFeO_3-type structure, which generates a crystal field with nearly trigonal symmetry. This allows the description of the low-energy structure of LaTiO_3 by a single-band Hubbard model as a good starting point. The lowest-orbital occupation in this crystal field stabilizes the AFM(G) state, and well explains the spin-wave spectrum of L…
The roles of crystal-field splitting and Jahn-Teller distortions on the orbital ordering transition are investigated in the single-layer manganites near half doping. Crystal-field splitting of energy levels favoring the $d_{3z^2-r^2}$ occupancy provides not only the correct Fermi surface topology for La$_{0.5}$Sr$_{1.5}$MnO$_4$ having a circular electron pocket around the $Γ$ point, but also enhances the flatness of the hole pocket around the M point thereby improving the nesting. In the presence of the circular electron pocket, Jahn-Teller distortions are found to be crucial for the transitio…
The effective Hamiltonian for perovskite titanates is derived by taking into account the three-fold degeneracy of $t_{2g}$ orbitals and the strong electron-electron interactions. The magnetic and orbital ordered phases are studied in the mean-field approximation applied to the effective Hamiltonian. A large degeneracy of the orbital states in the ferromagnetic phase is found in contrast to the case of the doubly degenerate $e_g$ orbitals. Lifting of this orbital degeneracy due to lattice distortions and spin-orbit coupling is examined. A general form for the scattering cross section of the res…
Combining infrared reflectivity, transport, susceptibility and several diffraction techniques, we find compelling evidence that CaCrO3 is a rare case of a metallic and antiferromagnetic transition-metal oxide with a three-dimensional electronic structure. LSDA calculations correctly describe the metallic behavior as well as the anisotropic magnetic ordering pattern of C type: The high Cr valence state induces via sizeable pd hybridization remarkably strong next-nearest neighbor interactions stabilizing this ordering. The subtle balance of magnetic interactions gives rise to magneto-elastic cou…
We study FeO, a Mott insulator in GGA and GGA+U approximations. In the GGA we find a multi-band metallic state with remarkable inter-band nesting between two $t_{2g}$ bands of Fermi surface, which signals possible instability towards an orbital ordered insulating phase. Such broken symmetry state, although has lower energy than the underlying homogeneous metallic state, but the gap magnitude is less than the experimentally observed optical gap. Therefore we incorporate the calculated value of on-site Coulomb repulsion U on orbital ordered state. We find that symmetry breaking and Coulomb corre…
