We calculate correlation functions of exactly-solvable one-dimensional flat-band models by utilizing the "molecular-orbital" representation. The models considered in this paper have a gapped ground state with flat-band being fully occupied, even in the presence of the interaction. In this class of models, the space spanned by the "molecular-orbitals" is the co-space of that spanned by the flat bands. Thanks to this property, the correlation functions are calculated by using the information of the molecular-orbitals rather than the explicit forms of the flat-band wave functions, which simplifies the calculations. As a demonstration, several one-dimensional models and their correlation functions are presented. We also calculate the entanglement entropy by using the correlation function.
Spin-orbital entanglement in the ground state of a one-dimensional SU(2)$\otimes$SU(2) spin-orbital model is analyzed using exact diagonalization of finite chains. For $S=1/2$ spins and $T=1/2$ pseudospins one finds that the quantum entanglement is similar at the SU(4) symmetry point and in the spin-orbital valence bond state. We also show that quantum transitions in spin-orbital models turn out to be continuous under certain circumstances, in constrast to the discontinuous transitions in spin models with SU(2) symmetry.
We point out that large composite spin-orbital fluctuations in Mott insulators with $t_{2g}$ orbital degeneracy are a manifestation of quantum entanglement of spin and orbital variables. This results in a dynamical nature of the spin superexchange interactions, which fluctuate over positive and negative values, and leads to an apparent violation of the Goodenough-Kanamori rules. [{\it Published in Phys. Rev. Lett. {\bf 96}, 147205 (2006).}]
Spin-orbital entanglement in quantum spin-orbital systems is quantified by a reduced von Neumann entropy, and is calculated for the ground state of a coupled spin-orbital chain with $SU(2)\times SU(2)$ symmetry. By analyzing the discontinuity and local extreme of the reduced entropy as functions of the model parameters, we deduce a rich phase diagram to describe the quantum phase transitions in the model. Our approach provides an efficient and powerful method to identify phase boundaries in a system with complex correlation between multiply degrees of freedom.
We utilize a 1d Hubbard model to show that the superconductivity in cuprate superconductors likely arises due to the orbital entanglement between holes in the copper oxide plane mediated by orbitally-selective charge hopping. The main role of doping required to achieve superconductivity in cuprates is to suppress the Mott correlations and orbital ordering. The proposed mechanism explains superconductivity in other unconventional superconductors, and provides guidance in the search for new high-temperature superconductors.
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 demonstrate the role played by the von Neumann entropy spectra in quantum phase transitions we investigate the one-dimensional anisotropic SU(2)$\otimes XXZ$ spin-orbital model with negative exchange parameter. In the case of classical Ising orbital interactions we discover an unexpected novel phase with Majumdar-Ghosh-like spin-singlet dimer correlations triggered by spin-orbital entanglement and having $k=π/2$ orbital correlations, while all the other phases are disentangled. For anisotropic $XXZ$ orbital interactions both spin-orbital entanglement and spin-dimer correlations extend to th…
We discuss a number of illuminating results for tight binding models supporting a band with variable Chern number, and illustrate them explicitly for a simple class of two-banded models. First, for models with a fixed number of bands, we show that the minimal hopping range needed to achieve a given Chern number $C$ is increasing with $C$, and that the band flattening requires an exponential tail of long-range processes. We further verify that the entanglement spectrum corresponding to a real-space partitioning contains $C$ chiral modes and thereby complies with the archetypal correspondence be…
We investigate the phase diagram and the spin-orbital entanglement of a one-dimensional SU(2)$\otimes XXZ$ model with SU(2) spin exchange and anisotropic $XXZ$ orbital exchange interactions and negative exchange coupling. As a unique feature, the spin-orbital entanglement entropy in the entangled ground states increases here linearly with system size. In the case of Ising orbital interactions we identify an emergent phase with long-range spin-singlet dimer correlations triggered by a quadrupling of correlations in the orbital sector. The peculiar translational invariant spin-singlet dimer phas…
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 …
We study the two-orbital Hubbard model in the limit of vanishing kinetic energy. The phase diagram in the $V-J$ plane, with $V$ and $J$ denoting the interorbital hybridization and exchange coupling respectively, at half filling is obtained. A singlet(dimer)-triplet transition is found for a critical value of the ratio $V/J.$ The entropy of formation, both in the mode and in the particle picture, presents a jump as the same critical line in conformity with the suggested relation between criticality and entanglement.
We present the entanglement properties of the spin-orbital coupling systems with multiple degrees of freedom. After constructing the maximally entangled spin-orbital basis of bipartite, we find that the quantum entanglement length in the noninteracting itinerant Fermion system with spin and orbit is considerably larger than that in the system with only spin. In the SU(2)$\otimes$SU(2) spin-orbital interacting system, the entanglement, expressed in terms of the spin-orbital correlation functions, clearly manifests the close relationship with the quantum phases in strongly correlated systems; an…
With progress towards more compact quantum computing architectures, fundamental questions regarding the entanglement of indistinguishable particles need to be addressed. In a solid state device, this quest is naturally connected to the quantum correlations of electrons. Here, we investigate the entanglement between electrons, focusing on the entanglement of modes, the entanglement of particles and the effect of particle-number superselection rules. We elucidate the formation of mode and particle entanglement in strongly correlated materials and show that both represent important resources in q…
We consider the spin--orbital model for a magnetic system with singly occupied but triply degenerate $t_{2g}$ orbitals coupled into a planar, triangular lattice, as would be exemplified by NaTiO$_2$. We investigate the ground states of the model for interactions which interpolate between the limits of pure superexchange and purely direct exchange interactions. By considering ordered and dimerized states at the mean--field level, and by interpreting the results from exact diagonalization calculations on selected finite systems, we demonstrate that orbital interactions are always frustrated, and…
The concept of spin-orbital entanglement on superexchange bonds in transition metal oxides is introduced and explained on several examples. It is shown that spin-orbital entanglement in superexchange models destabilizes the long-range (spin and orbital) order and may lead either to a disordered spin-liquid state or to novel phases at low temperature which arise from strongly frustrated interactions. Such novel ground states cannot be described within the conventionally used mean field theory which separates spin and orbital degrees of freedom. Even in cases where the ground states are disentan…
We review the consequences of intrinsic frustration of the orbital superexchange and of spin-orbital entanglement. While Heisenberg perturbing interactions remove frustration in the compass model, the lowest columnar excitations are robust in the nanoscopic compass clusters and might be used for quantum computations. Entangled spin-orbital states determine the ground states in some cases, while in others concern excited states and lead to measurable consequences, as in the $R$VO$_3$ perovskites. On-site entanglement for strong spin-orbit coupling generates the frustrated Kitaev-Heisenberg mode…
We report the existence of \emph{flat bands} in a p-wave superconducting Kitaev ladder. We identify two sets of parameters for which the Kitaev ladder sustains flat bands. These flat bands are accompanied by highly localized eigenstates known as compact localized states. Invoking a Bogoliubov transformation, the Kitaev ladder can be mapped into an interlinked cross-stitch lattice. The mapping helps to reveal the compactness of the eigenstates each of which covers only two unit cells of the interlinked cross-stitch lattice. The Kitaev Hamiltonian undergoes a topological-to-trivial phase transit…
We investigate the non-universal part of the orbital entanglement spectrum (OES) of the nu = 1/3 fractional quantum Hall effect (FQH) ground-state with Coulomb interactions. The non-universal part of the spectrum is the part that is missing in the Laughlin model state OES whose level counting is completely determined by its topological order. We find that the OES levels of the Coulomb interaction ground-state are organized in a hierarchical structure that mimic the excitation-energy structure of the model pseudopotential Hamiltonian which has a Laughlin ground state. These structures can be ac…
On the basis of the "molecular-orbital" representation which describes generic flat-band models, we propose a systematic way to construct a class of flat-band models with finite-range hoppings that have topological natures. In these models, the topological natures are encoded not into the flat band itself but into the dispersive bands touching the flat band. Such a band structure may become a source of exotic phenomena arising from the combination of flat bands, topology and correlations.
Wave functions based on electron-pair states provide inexpensive and reliable models to describe quantum many-body problems containing strongly-correlated electrons, given that broken-pair states have been appropriately accounted for by, for instance, a posteriori corrections. In this article, we analyse the performance of electron-pair methods in predicting orbital-based correlation spectra. We focus on the (orbital-optimized) pair-coupled cluster Doubles (pCCD) ansatz with a linearized coupled-cluster (LCC) correction. Specifically, we scrutinize how orbital-based entanglement and correlatio…
We develop a framework to describe a wide class of flat-band models, with and without a translational symmetry, by using "molecular orbitals" introduced in the prior work (HATSUGAI Y. and MARUYAMA I., \textit{EPL}, \textbf{95}, (2011) 20003). Using the molecular-orbital representation, we shed new light on the band-touching problem between flat and dispersive bands. We show that the band touching occurs as a result of collapse, or the linearly dependent nature, of molecular orbitals. Conversely, we can gap out the flat bands by modulating the molecular orbitals so that they do not collapse, wh…
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…
One of the most critical tasks at the very beginning of a quantum chemical investigation is the choice of either a multi- or single-configurational method. Naturally, many proposals exist to define a suitable diagnostic of the multi-configurational character for various types of wave functions in order to assist this crucial decision. Here, we present a new orbital-entanglement based multi-configurational diagnostic termed $Z_{s(1)}$. The correspondence of orbital entanglement and static (or nondynamic) electron correlation permits the definition of such a diagnostic. We chose our diagnostic t…
We expand the concept of frustration in Mott insulators and quantum spin liquids to metals with flat bands. We show that when inter-orbital hopping $t_2$ dominates over intra-orbital hopping $t_1$, in a multiband system with strong spin-orbit coupling $λ$, electronic states with a narrow bandwidth $W\sim t_2^2/λ$ are formed compared to a bandwidth of order $t_1$ for intra-orbital hopping. We demonstrate the evolution of the electronic structure, Berry phase distributions for time-reversal and inversion breaking cases, and their imprint on the optical absorption, in a tight binding model of $d$…
Using a combined analytical and numerical approach, we study the collective spin and orbital excitations in a spin-orbital chain under a crystal field. Irrespective of the crystal field strength, these excitations can be universally described by fractionalized fermions. The fractionalization phenomenon persists and contrasts strikingly with the case of a spin chain, where fractionalized spinons cannot be individually observed but confined to form magnons in a strong magnetic field. In the spin-orbital chain, each of the fractional quasiparticles carries both spin and orbital quantum numbers, a…
The accurate calculation of the (differential) correlation energy is central to the quantum chemical description of bond-formation and bond-dissociation processes. In order to estimate the quality of single- and multi-reference approaches for this purpose, various diagnostic tools have been developed. In this work, we elaborate on our previous observation [J. Phys. Chem. Lett. 3, 3129 (2012)] that one- and two-orbital-based entanglement measures provide quantitative means for the assessment and classification of electron correlation effects among molecular orbitals. The dissociation behavior o…
Li and Haldane conjectured and numerically substantiated that the entanglement spectrum of the reduced density matrix of ground-states of time-reversal breaking topological phases (fractional quantum Hall states) contains information about the counting of their edge modes when the ground-state is cut in two spatially distinct regions and one of the regions is traced out. We analytically substantiate this conjecture for a series of FQH states defined as unique zero modes of pseudopotential Hamiltonians by finding a one to one map between the thermodynamic limit counting of two different entangl…
The chemical bond is an important local concept to understand chemical compounds and processes. Unfortunately, like most local concepts, the chemical bond and the bond order do not correspond to any physical observable and thus cannot be determined as an expectation value of a quantum chemical operator. We recently demonstrated [Boguslawski et al., J. Chem. Theory Comput., 2013, 9, 2959--2973] that one- and two-orbital-based entanglement measures can be applied to interpret electronic wave functions in terms of orbital correlation. Orbital entanglement emerged to be a powerful tool to provide …
We present general design principles for engineering and discovering periodic systems with flat bands. Our paradigm exploits spin-orbit assisted orbital frustration on a lattice to produce band structures that contain multiplets of narrowly dispersing bands whose bandwidth is smaller than all other energy scales of the problem including the band gap surrounding the flat bands. We present a series of models in 1D and 2D on various lattices with different intracellular spin-orbit like potentials that hybridize the degrees of freedom in the unit cell. As an alternative to machine learning based e…
Layered kagome-lattice 3d transition metals are emerging as an exciting platform to explore the frustrated lattice geometry and quantum topology. However, the typical kagome electronic bands, characterized by sets of the Dirac-like band capped by a phase-destructive flat band, have not been clearly observed, and their orbital physics are even less well investigated. Here, we present close-to-textbook kagome bands with orbital differentiation physics in CoSn, which can be well described by a minimal tight-binding model with single-orbital hopping in Co kagome lattice. The capping flat bands wit…
Theoretical models of the spin-orbital liquid (SOL) FeSc$_2$S$_4$ have predicted it to be in close proximity to a quantum critical point separating a spin-orbital liquid phase from a long-range ordered magnetic phase. Here, we examine the magnetic excitations of FeSc$_2$S$_4$ through time-domain terahertz spectroscopy under an applied magnetic field. At low temperatures an excitation emerges that we attribute to a singlet-triplet excitation from the SOL ground state. A three-fold splitting of this excitation is observed as a function of applied magnetic field. As singlet-triplet excitations ar…
Electronic flat band systems are a fertile platform to host correlation-induced quantum phenomena such as unconventional superconductivity, magnetism and topological orders. While flat band has been established in geometrically frustrated structures, such as the kagome lattice, flat band-induced correlation effects especially in those multi-orbital bulk systems are rarely seen. Here we report negative magnetoresistance and signature of ferromagnetic fluctuations in a prototypical kagome metal CoSn, which features a flat band in proximity to the Fermi level. We find that the magnetoresistance i…
Motivated by the recent activities on the Ni-based diamond lattice antiferromagnet NiRh$_2$O$_4$, we theoretically explore on a general ground the unique spin and orbital physics for the Ni$^{2+}$ ions with a $3d^8$ electron configuration in the tetrahedral crystal field environment and on a diamond lattice Mott insulator. The superexchange interaction between the local moments usually favors magnetic orders. Due to the particular electron configuration of the Ni$^{2+}$ ion with a partially filled upper $t_{2g}$ level and a fully filled lower $e_g$ level, the atomic spin-orbit coupling becomes…
Entanglement is one of the most fascinating concepts of modern physics. In striking contrast to its abstract, mathematical foundation, its practical side is, however, remarkably underdeveloped. Even for systems of just two orbitals or sites no faithful entanglement measure is known yet. By exploiting the spin symmetries of realistic many-electron systems, we succeed in deriving a closed formula for the relative entropy of entanglement between electron orbitals. Its broad applicability in the quantum sciences is demonstrated: (i) in light of the second quantum revolution, it quantifies the true…
We report a thorough study of Y$_{0.7}$La$_{0.3}$VO$_3$ single crystals by measuring magnetic properties, specific heat, thermal conductivity, x-ray and neutron diffraction with the motivation of revealing the lattice response to the spin-orbital entanglement in \textit{R}VO$_3$. Upon cooling from room temperature, the orbitally disordered paramagnetic state changes around T*$\sim$220\,K to spin-orbital entangled state which is then followed by a transition at T$_N$=116\,K to C-type orbital ordered (OO) and G-type antiferromagnetic ordered (AF) ground state. In the temperature interval T$_N<T<…
We introduce a one-dimensional plaquette orbital model with a topology of a ladder and alternating interactions between $x$ and $z$ pseudospin components along both the ladder legs and on the rungs. We show that it is equivalent to an effective spin model in a magnetic field, with spin dimers that replace plaquettes and are coupled along the chain by three-spin interactions. Using perturbative treatment and mean field approaches with dimer correlations we study the ground state spin configuration and its defects in the lowest excited states. By the exact diagonalization approach we find that t…
Spin-orbital liquids are quantum disordered states in systems with entangled spin and orbital degrees of freedom. We study exactly solvable spin-orbital models in two dimensions with selected Heisenberg-, Kitaev-, and $Γ$-type interactions, as well as external magnetic fields. These models realize a variety of spin-orbital-liquid phases featuring dispersing Majorana fermions with Fermi surfaces, nodal Dirac or quadratic band touching points, or full gaps. In particular, we show that Zeeman magnetic fields can stabilize nontrivial flux patterns and induce metamagnetic transitions between states…
We present a theory for the metal-insulator transition (MIT) in the quantum-spin-liquid candidate material Na4Ir3O8. We consider an extended Hubbard model on the hyperkagome lattice, which incorporates atomic spin-orbit coupling (SOC) and multi-orbital interactions of iridium 5d electrons. This model is analyzed using the slave-rotor mean-field theory and thermodynamic properties across the MIT are studied. The ground state in the insulating side is a U(1) quantum spin liquid with spinon Fermi surfaces that consist of multiple particle-like and hole-like pockets. It is shown that the Wilson ra…
In heavy-fermion compounds, the dual character of $f$ electrons underlies their rich and often exotic properties like fragile heavy quasipartilces, variety of magnetic orders and unconventional superconductivity. 5$f$-electron actinide materials provide a rich setting to elucidate the larger and outstanding issue of the competition between magnetic order and Kondo entanglement and, more generally, the interplay among different channels of interactions in correlated electron systems. Here, by using angle-resolved photoemission spectroscopy, we present detailed electronic structure of USb$_2$ an…
In this work, we study a molecular graphene model on the top of a superconductor in the presence of pseudomagnetic fields induced by coplanar strain fields. With the pseudomagnetic fields and the attractive interaction induced from the substrate, a flat band superconductor can be achieved according to mean field analysis on the effective Hamiltonian. Based on a semiclassical approximation, we first show that the orbital limit is hugely enhanced by the pseudomagnetic fields. The physical reason is that the orbital angular momenta locking at $K$ and $K'$ valleys due to the pseudomagnetic fields …
Quantum-chemical multi-configurational methods are required for a proper description of static electron correlation, a phenomenon inherent to the electronic structure of molecules with multiple (near-)degenerate frontier orbitals. Here, we review how a property of these frontier orbitals, namely the entanglement entropy is related to static electron correlation. A subset of orbitals, the so-called active orbital space, is an essential ingredient for all multi-configurational methods. We proposed an automated selection of this active orbital space, that would otherwise be a tedious and error pr…
The possibility of realizing lattice analogs of fractional quantum Hall (FQH) states, so-called fractional Chern insulators (FCIs), in nearly flat topological (Chern) bands has attracted a lot of recent interest. Here, we make the connection between Abelian as well as non-Abelian FQH states and FCIs more precise. Using a gauge-fixed version of Qi's Wannier basis representation of a Chern band, we demonstrate that the interpolation between several FCI states, obtained by short-range lattice interactions in a spin-orbit-coupled kagome lattice model, and the corresponding continuum FQH states is …
Molecular-Orbital Degeneracy Lifting and Suppression of a Flat-Band Metal in a Tetrahedral Cluster System NbSeI
Institute for Solid State Physics, the University of Tokyo（东京大学固体物理研究所）；Graduate School of Environmental, Life, Natural Science and Technology, Okayama University（冈山大学环境生命自然科技研究科）；Department of Physics, Nagoya University（名古屋大学物理学系）；Department of Advanced Materials Science, the University of Tokyo（东京大学先进材料科学系）；Japan Synchrotron Radiation Research Institute (JASRI)（日本同步辐射研究所）
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…
Electron correlation effects are essential for an accurate ab initio description of molecules. A quantitative a priori knowledge of the single- or multi-reference nature of electronic structures as well as of the dominant contributions to the correlation energy can facilitate the decision regarding the optimum quantum chemical method of choice. We propose concepts from quantum information theory as orbital entanglement measures that allow us to evaluate the single- and multi-reference character of any molecular structure in a given orbital basis set. By studying these measures we can detect po…
