We argue for the existence of a liquid ground state in a class of square lattice models of orbitally degenerate insulators. Starting with the SU(4) symmetric Kugel-Khomskii model, we utilize a Majorana Fermion representation of spin-orbital operators to access novel phases. Variational wavefunctions of candidate liquid phases are thus obtained, whose properties are evaluated using Variational Monte Carlo. These states are disordered, and are found to have excellent energetics and ground state overlap ($>40%$) when compared with exact diagonalization on 16 site clusters. We conclude that these are spin-orbital liquid ground states with emergent nodal fermions and Z$_2$ gauge fields. Connections to spin 3/2 cold atom systems and properties in the absence of SU(4) symmetry are briefly discussed.
The Kugel-Khomskii model, the simplest model for orbital degenerate magnetic insulators, exhibits a zero temperature degeneracy in the classical limit which could cause genuine quantum disorder. Khaliullin and Oudovenko [Phys. Rev. B 56, R14 243 (1997)] suggested recently that instead a particular classical state could be stabilized by quantum fluctuations. Here we compare their approach with standard random phase approximation and show that it strongly underestimates the strength of the quantum fluctuations, shedding doubts on the survival of any classical state.
The Kugel-Khomskii Hamiltonian for cubic titanates describes spin and orbital superexchange interactions between $d^1$ ions having three-fold degenerate $t_{2g}$ orbitals. Since orbitals do not couple along "inactive" axes, perpendicular to the orbital planes, the total number of electrons in $|α>$ orbitals in any such plane and the corresponding total spin are both conserved. A Mermin-Wagner construction shows that there is no long-range spin ordering at nonzero temperatures. Inclusion of spin-orbit coupling allows such ordering, but even then the excitation spectrum is gapless due to a conti…
We study the effective spin-orbital model for honeycomb-layered transition metal compounds, applying the second-order perturbation theory to the three-orbital Hubbard model with the anisotropic hoppings. This model is reduced to the Kitaev model in the strong spin-orbit coupling limit. Combining the cluster mean-field approximations with the exact diagonalization, we treat the Kugel-Khomskii type superexchange interaction and spin-orbit coupling on an equal footing to discuss ground-state properties. We find that a zigzag ordered state is realized in the model within nearest-neighbor interacti…
We discuss spin and orbital ordering in the twofold orbital degenerate superexchange model in three dimensions relevant to perovskite transition metal oxides. We focus on the particular point on the classical phase diagram where orbital degeneracy is lifted by quantum effects exclusively. Dispersion and damping of the spin and orbital excitations are calculated at this point taking into account their mutual interaction. Interaction corrections to the mean-field order parameters are found to be small. We conclude that quasi-one-dimensional Neel spin order accompanied by the uniform d_{3z^2-r^2}…
We show that the $t_{2g}^2$ perovskite LaVO$_3$, in its orthorhombic phase, is a rare case of a system hosting an orbital-ordering Kugel-Khomskii phase transition, rather than being controlled by the Coulomb-enhanced crystal-field splitting. We find that, as a consequence of this, the magnetic transition is close to (and even above) the super-exchange driven orbital-ordering transition, whereas typically magnetism arises at much lower temperatures than orbital ordering. Our results support the experimental scenario of orbital-ordering and G-type spin correlations just above the monoclinic-to-o…
The Kugel--Khomskii model with entangled spin and orbital degrees of freedom is a good testing ground for many important features in quantum information processing, such as robust gaps in the entanglement spectra. Here, we demonstrate that the entanglement can be also robust under effect of temperature within a wide range of parameters. It is shown, in particular, that the temperature dependence of entanglement often exhibits a nonmonotonic behavior. Namely, there turn out to be ranges of the model parameters, where entanglement is absent at zero temperature, but then, with an increase in temp…
We investigate the zero-temperature phase diagrams of the bilayer square-lattice Kugel-Khomskii ($d^9$) model involving entangled and singlet phases using mean-field cluster approach. This diagram includes interlayer singlet phase observed in fluoride K$_3$Cu$_2$F$_7$ and exotic entangled spin-orbital phases. For a monolayer case, realized in K$_2$CuF$_4$, we perform similar calculations in finite temperature and show that the alternating-orbital ferromagnet decays first to an entangled uniform ferromagnet and then to a paramagnetic phase. Published in: J. Phys.: Conf. Series 391, 012085 (2012…
Using the exact diagonalization technique, we determine the energy spectrum and wave functions for finite chains described by the two-spin (Kugel--Khomskii) model with different types of intersubsystem exchange terms. The found solutions provide a possibility to address the problem of quantum entanglement inherent to this class of models. We put the main emphasis on the calculations of the concurrence treated as an adequate numerical measure of the entanglement. We also analyze the behavior of two-site correlation functions considered as a local indicator of entanglement. We construct the phas…
We study the quantum entanglement of the spin and orbital degrees of freedom in the one- dimensional Kugel-Khomskii model, which includes both gapless and gapped phases, using analytical techniques and exact diagonalization with up to 16 sites. We compute the entanglement entropy, and the entanglement spectra using a variety of partitions or "cuts" of the Hilbert space, including two distinct real-space cuts and a momentum-space cut. Our results show the Kugel-Khomski model possesses a number of new features not previously encountered in studies of the entanglement spectra. Notably, we find ro…
We derive the Kugel-Khomskii spin-orbital (SO) model for a bilayer and investigate its phase diagram depending on Hund's exchange $J_H$ and the $e_g$ orbital splitting $E_z$. In the (classical) mean-field approach with on-site spin $<S_i^z>$ and orbital $<τ_i^z>$ order parameters and factorized spin-and-orbital degrees of freedom, we demonstrate a competition between the phases with either $G$-type or $A$-type antiferromagnetic (AF) or ferromagnetic long-range order. Next we develop a Bethe-Peierls-Weiss method with a Lanczos exact diagonalization of a cube coupled to its neighbors in $ab$ pla…
We study zero temperature phase diagram of the three-dimensional Kugel-Khomskii model on a cubic lattice using the cluster mean field theory and different perturbative expansions in the orbital sector. The phase diagram is rich, goes beyond the single-site mean field theory due to spin-orbital entanglement. In addition to the antiferromagnetic (AF) and ferromagnetic (FM) phases, one finds also a plaquette valence-bond phase with singlets ordered either on horizontal or vertical bonds. More importantly, for increasing Hund's exchange we identify three phases with exotic magnetic order stabilize…
The Kugel-Khomskii (KK) Hamiltonian for the titanates describes spin and orbital superexchange interactions between $d^1$ ions in an ideal perovskite structure in which the three $t_{2g}$ orbitals are degenerate in energy and electron hopping is constrained by cubic site symmetry. In this paper we implement a variational approach to mean-field theory in which each site, $i$, has its own $n \times n$ single-site density matrix $\rhov(i)$, where $n$, the number of allowed single-particle states, is 6 (3 orbital times 2 spin states). The variational free energy from this 35 parameter density matr…
A possible mechanism for the removal of the orbital degeneracy in RTiO3 (where R=La, Y, ...) is considered. The calculation is based on the Kugel-Khomskii Hamiltonian for electrons residing in the t2g orbitals of the Ti ions, and uses a self-consistent pe rturbation expansion in the interaction between the orbital and the spin degrees of freedom. The latter are assumed to be ordered in a Neel state, brought about by delicate interactions that are not included in the Kugel-Khomskii Hamiltonian. Within our model calculations, each of the t2g bands is found to acquire a finite, temperature-depend…
The most elementary of all physical spin-orbital models is the Kugel-Khomskii model describing a S=1/2, $e_g$ degenerate Mott-insulator. Recent theoretical work is reviewed revealing that the classical limit is characterized by a point of perfect dynamical frustration. It is suggested that this might give rise to a quantum disordered ground state.
We investigate the phase diagrams of the spin-orbital $d^9$ Kugel-Khomskii model for a bilayer and a monolayer square lattice using Bethe-Peierls-Weiss method. For a bilayer we obtain valence bond phases with interlayer singlets, with alternating planar singlets, and two entangled spin-orbital (ESO) phases, in addition to the antiferromagnetic and ferromagnetic order. Possibility of such entangled phases in a monolayer is under investigation at present.
We analyze the possible types of ordering in a boson--fermion model. The Hamiltonian is inherently related to the Bose--Hubbard model for vector two-species bosons in optical lattices. We show that such model can be reduced to the Kugel--Khomskii type spin--pseudospin model, but in contrast to the usual version of the latter model, we are dealing here with the case of spin $S=1$ and pseudospin $1/2$. We show that the interplay of spin and pseudospin degrees of freedom leads to a rather nontrivial magnetic phase diagram including the spin-nematic configurations. Tuning the spin-channel interact…
We study the interplay of spin, orbital and lattice degrees of freedom in a one-dimensional Kugel-Khomskii model coupled to phonons. In the vicinity of the dimer point we analyze the excitation spectrum, mapping the spin and orbital degrees of freedom to bond operators. In particular we study the renormalization of the phonon propagator due to coupling to the orbital and magnetic excitations. Considering both, ferro- and antiferro-orbital ordering we will show that the appearance of orbiton shake-up processes in the phonon spectrum is sensitive to the type of Jahn-Teller distortion. The releva…
In addition to low-energy spin fluctuations, which distinguish them from band insulators, Mott insulators often possess orbital degrees of freedom when crystal-field levels are partially filled. While in most situations spins and orbitals develop long-range order, the possibility for the ground state to be a quantum liquid opens new perspectives. In this paper, we provide clear evidence that the SU(4) symmetric Kugel-Khomskii model on the honeycomb lattice is a quantum spin-orbital liquid. The absence of any form of symmetry breaking - lattice or SU(N) - is supported by a combination of semicl…
We examine magnon and orbiton behavior in localized O$_2$ anti-bonding molecular $π^*$ orbitals using an effective Kugel-Khomskii Hamiltonian derived from a two band Hubbard model with hopping parameters taken from {\em ab initio} density functional calculations. The considerable difference between intraband and interband hoppings leads to a strong coupling between the spin wave dispersion and the orbital ground state, providing a straightforward way of experimentally determining the orbital ground state from the measured magnon dispersion. The near degeneracy of different orbital ordered stat…
The interactions between charge and orbitally ordered $d$-electrons are important in many transition metal oxides. We propose an effective energy model for such interactions, parameterized with DFT+U calculations, so that energy contributions of both electronic and lattice origin can be simultaneously accounted for. The model is applied to the low-temperature phase of magnetite, for which we propose a new ground state structure. The effective interactions on the B-lattice of Fe$_3$O$_4$ can be interpreted in terms of electrostatics and short-range Kugel-Khomskii exchange coupling. The frustrat…
The rich phenomenology engendered by the coupling between the spin and orbital degrees of freedom has become appreciated as a key feature of many strongly-correlated electron systems. The resulting emergent physics is particularly prominent in a number of materials, from Fe-based unconventional superconductors to transition metal oxides, including manganites and vanadates. Here, we investigate the electronic ground states of $α$-Sr$_2$CrO$_4$, a compound that is a rare embodiment of the spin-1 Kugel-Khomskii model on the square lattice -- a paradigmatic platform to capture the physics of coupl…
We investigate the ground-state properties of the one-dimensional two-band Hubbard model with different bandwidths. The density-matrix renormalization group method is applied to calculate the averaged electron occupancies $n$ as a function of the chemical potential $μ$. Both at quarter and half fillings, "charge plateaux" appear in the $n$-$μ$ plot, where $dμ/dn$ diverges and the Mott insulating states are realized. To see how the orbital polarization in the one-quarter charge plateau develops, we apply the second-order perturbation theory from the strong-coupling limit at quarter filling. The…
We investigate heavy fermion behaviors in the vanadium spinel LiV_2O_4. We start from a three-orbital Hubbard model on the pyrochlore lattice and derive its low-energy effective Hamiltonian by an approach of real-space renormalization group type. One important tetrahedron configuration in the rochlore lattice has a three-fold orbital degeneracy and spin S=1, and correspondingly, the effective Hamiltonian has spin and orbital exchange interactions of Kugel-Khomskii type as well as correlated electron hoppings. Analyzing the effective Hamiltonian, we find that ferromagnetic double exchange proce…
We provide an exact study of dynamical correlations for the quantum spin-orbital liquid phases of an SU(2)-symmetric Kitaev honeycomb lattice model. We show that the spin dynamics in this Kugel-Khomskii type model is exactly the density-density correlation function of S=1 fermionic magnons, which could be probed in resonant inelastic x-ray scattering experiments. We predict the characteristic signatures of spin-orbital fractionalization in inelastic scattering experiments and compare them to the ones of the spin-anisotropic Kitaev honeycomb spin liquid. In particular, the resonant inelastic x-…
We introduce a novel mean-field theory (MFT) around the exactly soluble two-leg ladder limit for the planar quantum compass model (QCM). In contrast to usual MFT, our construction respects the stringent constraints imposed by emergent, lower (here $d=1$) dimensional symmetries of the QCM. Specializing our construction to the QCM on a periodic four-leg ladder, we find that a first-order transition separates two mutually dual Ising nematic phases, in good accord with state-of-the-art numerics for the planar QCM. One pseudo-spin-flip excitation in the ordered phase turns out to be two (Jordan-Wig…
In this short review, which is based on the works published between 2011 and 2016, we discuss the problem of the propagation of a collective orbital excitation (orbiton) created in the Mott insulating and antiferromagnetic ground state. On the theoretical side, the problem is solved by mapping a Kugel-Khomskii spin-orbital model describing an orbiton moving in an antiferromagnet onto an effective t-J model with a 'single hole' moving in an antiferromagnet. The most important consequence of the existence of the above mapping is the fractionalisation of the electron's spin and orbital degree of …
Using maximally localized Wannier functions obtained from DFT calculations, we derive an effective Hubbard Hamiltonian for a bilayer of Sr$_3$Cr$_2$O$_7$, the $n=2$ member of the Ruddlesden-Popper Sr$_{n+1}$Cr$_n$O$_{3n+1}$ system. The model consists of effective $t_{2g}$ orbitals of Cr in two square lattices, one above the other. The model is further reduced at low energies and two electrons per site, to an effective Kugel-Khomskii Hamiltonian that describes interacting spins 1 and pseudospins 1/2 at each site describing spin and orbitals degrees of freedom respectively. We solve this Hamilto…
The simplest spin-orbital model can host a nematic spin-orbital liquid state on the triangular lattice. We provide clear evidence that the ground state of the SU(4) Kugel-Khomskii model on the triangular lattice can be well described by a "single" Gutzwiller projected wave function with an emergent parton Fermi surface, despite it exhibits strong finite-size effect in quasi-one-dimensional cylinders. The finite-size effect can be resolved by the fact that the parton Fermi surface consists of open orbits in the reciprocal space. Thereby, a stripy liquid state is expected in the two-dimensional …
We investigate the phase diagrams of the spin-orbital $d^9$ Kugel-Khomskii model for increasing system dimensionality: from the square lattice monolayer, via the bilayer to the cubic lattice. In each case we find strong competition between different types of spin and orbital order, with entangled spin-orbital phases at the crossover from antiferromagnetic to ferromagnetic correlations in the intermediate regime of Hund's exchange. These phases have various types of exotic spin order and are stabilized by effective interactions of longer range which follow from enhanced spin-orbital fluctuation…
Several realistic spin-orbital models for transition metal oxides go beyond the classical expectations and could be understood only by employing the quantum entanglement. Experiments on these materials confirm that spin-orbital entanglement has measurable consequences. Here, we capture the essential features of spin-orbital entanglement in complex quantum matter utilizing 1D spin-orbital model which accommodates SU(2)xSU(2) symmetric Kugel-Khomskii superexchange as well as the Ising on-site spin-orbit coupling. Building on the results obtained for full and effective models in the regime of str…
To reveal the origin of the "nematic electronic fluid phase" in Sr$_3$Ru$_2$O$_7$, we apply the self-consistent vertex correction analysis to the ($d_{xz},d_{yz}$)-orbital Hubbard model. It is found that the Aslamazov-Larkin type vertex correction causes the strong coupling between spin and orbital fluctuations, which corresponds to the Kugel-Khomskii spin-orbital coupling in the local picture. Due to this mechanism, orbital nematic order with $C_2$ symmetry is induced by the magnetic quantum criticality in multiorbital systems, while this mechanism is ignored in the random-phase-approximation…
Specific features of orbital and spin structure of transition metal compounds in the case of the face-sharing MO$_6$ octahedra are analyzed. In this geometry, we consider the form of the spin--orbital Hamiltonian for transition metal ions with double ($e_g^σ$) or triple ($t_{2g}$) orbital degeneracy. Trigonal distortions typical of the structures with face-sharing octahedra lead to splitting of $t_{2g}$ orbitals into an $a_{1g}$ singlet and $e_g^π$ doublet. For both doublets ($e_g^σ$ and $e_g^π$), in the case of one electron or hole per site, we arrive at a symmetric model with the orbital and…
A number of recent experiments exhibit electronic anisotropy in the iron pnictides, and there is a growing body of experimental evidence that its origin is related to orbital ordering in Fe d_{xz} and d_{yz} orbitals. We examine this problem in the parent compounds of the iron pnictides by a combination of ab initio band theory calculations, phenomenological Ginzburg-Landau theory of coupled orbital and magnetic order parameters, and a microscopic mean-field study of the Kugel-Khomskii model. We find that orbital ordering is sufficient to explain a number of key experimental observations, in p…
The alloy Ca$_{2-x}$Sr$_x$RuO$_4$ exhibits a complex phase diagram with peculiar magnetic metallic phases. In this paper some aspects of this alloy are discussed based on a mean field theory for an effective Kugel-Khomskii model of localized orbital and spin degrees of freedom. This model results from an orbital selective Mott transition which in the three-band system localized two orbitals while leaving the third one itinerant. Special attention is given to the region around a structure quantum phase transition at $ x \approx 0.5 $ where the crystal lattice changes from tetragonal to orthorho…
The recently discovered superconductivity in Nd$_{1-x}$Sr$_x$NiO$_2$ provides a new opportunity for studying strongly correlated unconventional superconductivity. The single-hole Ni$^+$ ($3d^9$) configuration in the parent compound NdNiO$_2$ is similar to that of Cu$^{2+}$ in cuprates. We suggest that after doping, the intra-orbital spin-singlet and inter-orbital spin-triplet double-hole (doublon) configurations of Ni$^{2+}$ are competing, and we construct a two-band Hubbard model by including both the $3d_{x^2-y^2}$ and $3d_{xy}$-orbitals. The effective spin-orbital super-exchange model in th…
Spin-orbital exchange as a route to intertwined dipole-quadrupole orbital order in MnV$_2$O$_4$ under strong trigonal crystal field
Graduate School of Arts and Sciences, University of Tokyo（东京大学大学院人文社会系研究科）；Department of Physics, University of Toronto（多伦多大学物理系）；Institute for Materials Research (IMR), Tohoku University（东北大学物质材料研究机构）
The superconducting (SC) state of iron-based compounds in both tetragonal and orthorhombic phases is studied on the basis of an effective Hamiltonian composed of the kinetic energy including the five Fe 3d-orbitals, the orthorhombic crystalline electric field (CEF) energy, and the two-orbital Kugel'-Khomskiĭ-type superexchange interaction. Our basic assumption is that the antiferromagnetic (AF) state in the parent compounds can be described by the $d_{xz}$ and $d_{yz}$ orbitals, and that the electrons in these orbitals have relatively strong electron correlation in the vicinity of the AF state…
Recently, a Verwey-type transition in the mixed-valence alkali sesquioxide Cs$_4$O$_6$ was deduced from the charge ordering of molecular peroxide O$_2^{2-}$ and superoxide O$_2^-$ anions accompanied by the structural transformation and a dramatic change in electronic conductivity [Adler et al, Sci. Adv 4, eaap7581 (2018)]. Here, we report that in the sister compound Rb$_4$O$_6$ a similar Verwey-type charge ordering transition is strongly linked to O$_2^-$ orbital and spin dynamics. On cooling, a powder neutron diffraction experiment reveals a charge ordering and a cubic-to-tetragonal transitio…
Motivated by recent experiments on the quantum-spin-liquid candidate material LiZn2Mo3O8, we study a single-band extended Hubbard model on an anisotropic Kagome lattice with the 1/6 electron filling. Due to the partial filling of the lattice, the inter-site repulsive interaction is necessary to generate Mott insulators, where electrons are localized in clusters, rather than at lattice sites. We provide examples of such cluster Mott insulators and study the phase transitions between metallic states and cluster Mott insulators on an anisotropic Kagome lattice. It is shown that these cluster Mott…
The concept of the entanglement between spin and orbital degrees of freedom plays a crucial role in understanding various phases and exotic ground states in a broad class of materials, including orbitally ordered materials and spin liquids. We investigate how the spin-orbital entanglement in a Mott insulator depends on the value of the spin-orbit coupling of the relativistic origin. To this end, we numerically diagonalize a 1D spin-orbital model with the 'Kugel-Khomskii' exchange interactions between spins and orbitals on different sites supplemented by the on-site spin-orbit coupling. In the …
Vereshchagin Institute of High Pressure Physics, Russian Academy of Sciences（俄罗斯科学院韦列夏金高压物理研究所）；Moscow Institute of Physics and Technology (National Research University)（莫斯科物理技术学院（国立研究型大学））；Institute for Theoretical and Applied Electrodynamics Russian Academy of Sciences（俄罗斯科学院理论与应用电动力学研究所）；National Research University Higher School of Economics（国立研究型高等经济大学）
Orbital and spin ordering phenomena in strongly correlated systems are commonly studied using the local-density approximation + dynamical mean-field theory approach. Typically, however, such simulations are restricted to simplified models (density-density Coulomb interactions, high symmetry couplings and few-band models). In this work we implement an efficient general hybridization-expansion continuous-time quantum Monte Carlo impurity solver (Krylov approach) which allows us to investigate orbital and spin ordering in a more realistic setting, including interactions that are often neglected (…
Motivated by the recent developments on cluster Mott insulating materials such as the cluster magnet LiZn$_2$Mo$_3$O$_8$, we consider the strong plaquette charge ordered regime of the extended Hubbard model on a breathing Kagome lattice and reveal the properties of the cluster Mottness. The plaquette charge order arises from the inter-site charge interaction and the collective motion of three localized electrons on the hexagon plaquettes. This model leads naturally to a reduction of the local moments by 2/3 as observed in LiZn$_2$Mo$_3$O$_8$. Furthermore, at low temperatures each hexagon plaqu…
