Orbital Hubbard Model Research Articles

Spin-orbital liquids and insulator-metal transitions on the pyrochlore lattice

The two orbital Hubbard model, with the electrons additionally coupled to a complex magnetic background, arises in the pyrochlore molybdates. The background involves local moments Hund's coupled to the electrons, driving double exchange ferromagnetism, and antiferromagnetic (AF) tendency arising from competing superexchange. The key scales include the Hubbard repulsion and the superexchange, both of which can be tuned in these materials. They control the phase transition from a ferromagnetic metal to a spin-glass metal and then to a spin-glass (Mott) insulator. We provide a comprehensive description of the ground state of this model using an unrestricted Hartree-Fock scheme implemented via a simulated annealing procedure and establish the metal-insulator transition line for varying Hubbard interaction and superexchange. The electrons see an effective disorder, due to orbital frustration, already in the ferromagnetic phase. The disorder is further enhanced by antiferromagnetic coupling and the resulting magnetic disorder. As a result, increasing AF coupling shifts the metal-insulator transition to lower Hubbard interaction and gives it an additional ``Anderson'' character. We provide detailed results on the magnetic and orbital correlations, the density of states, and the optical conductivity.

Correlation Renormalized and Induced Spin-Orbit Coupling

Interplay of spin-orbit coupling (SOC) and electron correlation generates a bunch of emergent quantum phases and transitions, especially topological insulators and topological transitions. We find that electron correlation will induce extra large SOC in multi-orbital systems under atomic SOC and change ground state topological properties. Using the Hartree–Fock mean field theory, phase diagrams of px /py orbital ionic Hubbard model on honeycomb lattice are well studied. In general, correction of strength of SOC δ λ ∝ (Uʹ–J). Due to breaking down of rotation symmetry, form of SOC on multi-orbital materials is also changed under correlation. If a non-interacting system is close to fermionic instability, spontaneous generalized SOC can also be found. Using renormalization group, SOC is leading instability close to quadratic band-crossing point. Mean fields at quadratic band-crossing point are also studied.

Correlation renormalized and induced spin-orbit coupling

Abstract Interplay of spin-orbit coupling (SOC) and electron correlation generates a bunch of emergent quantum phases and transitions, especially topological insulators (TI) and topological transitions. In this work, we find that electron correlation will induce extra large SOC in multi-orbital systems under atomic SOC and change ground state topological properties. Using Hartree-Fock mean field theory, phase diagrams of $p_{x}/p_{y}$ orbital ionic Hubbard model on honeycomb lattice are well studied. In general, correction of strength of SOC $\delta \lambda \propto (U'-J)$. Due to breaking down of rotation symmetry, form of SOC on multi-orbital materials are also changed under correlation. If non-interacting system is close to fermionic instability, spontaneous generalized SOC can also be found. Using renormalization group, SOC is leading instability close to quadratic band-crossing point. Mean fields at quadratic band-crossing point are also studied.

Orbital liquid in the eg orbital Hubbard model in d=∞ dimensions

We demonstrate that the three-dimensional $e_g$ orbital Hubbard model can be generalized to arbitrary dimension $d$, and that the form of the result is determined uniquely by the requirements that (i) the two-fold degeneracy of the $e_g$ orbital be retained, and (ii) the cubic lattice be turned into a hypercubic lattice. While the local Coulomb interaction $U$ is invariant for each basis of orthogonal orbitals, the form of the kinetic energy depends on the orbital basis and takes the most symmetric form for the so-called complex-orbital basis. Characteristically, with respect to this basis, the model has two hopping channels, one that is orbital-flavor conserving, and a second one that is orbital-flavor non-conserving. We show that the noninteracting electronic structure consists of two nondegenerate bands of plane-wave real-orbital single-particle states for which the orbital depends on the wave vector. Due to the latter feature each band is unpolarized at any filling, and has a non-Gaussian density of states at $d=\infty$. The \textit{orbital liquid} state is obtained by filling these two bands up to the same Fermi energy. We investigate the $e_g$ orbital Hubbard model in the limit $d\to\infty$, treating the on-site Coulomb interaction $U$ within the Gutzwiller approximation, thus determining the correlation energy of the orbital liquid and the (disordered) para-orbital states. (...) We show that the orbital liquid is the ground state everywhere in the $(n,U)$ phase diagram except close to half-filling at sufficiently large $U$, where ferro-orbital order with real orbitals occupied is favored. The latter feature is shown to be specific for $d=\infty$, being of mathematical nature due to the exponential tails in the density of states.

Precise ground state of multiorbital Mott systems via the variational discrete action theory

Determining the ground state of multi-orbital Hubbard models is critical for understanding strongly correlated electron materials, yet existing methods struggle to simultaneously reach zero temperature and infinite system size. The \textit{de facto} standard is to approximate a finite dimension multi-orbital Hubbard model with a $d=\infty$ version, which can then be formally solved via the dynamical mean-field theory (DMFT), though the DMFT solution is limited by the state of unbiased impurity solvers for zero temperature and multiple orbitals. The recently developed variational discrete action theory (VDAT) offers a new approach to solve the $d=\infty$ Hubbard model, with a variational ansatz that is controlled by an integer $\mathcal{N}$, and monotonically approaches the exact solution at an increasing computational cost. Here we propose a decoupled minimization algorithm to implement VDAT for the multi-orbital Hubbard model in $d=\infty$ and study $\mathcal{N}=2-4$ . At $\mathcal{N}=2$, VDAT rigorously recovers the multi-orbital Gutzwiller approximation, reproducing known results. At $\mathcal{N}=3$, VDAT precisely captures the competition between the Hubbard $U$, Hund $J$, and crystal field $\Delta$ in the two orbital Hubbard model over all parameter space, with a negligible computational cost. For sufficiently large $U/t$ and $J/U$, we show that $\Delta$ drives a first-order transition within the Mott insulating regime. In the large orbital polarization limit with finite $J/U$, we find that interactions have a nontrivial effect even for small $U/t$. VDAT will have far ranging implications for understanding multi-orbital model Hamiltonians and strongly correlated electron materials.

Polarization-dependent magnetic properties of periodically driven α−RuCl3

We study magnetic properties of a periodically driven Mott insulator with strong spin-orbit coupling and show some properties characteristic of linearly polarized light. We consider a $t_{2g}$-orbital Hubbard model driven by circularly or linearly polarized light with strong spin-orbit coupling and derive its effective Hamiltonian in the strong-interaction limit for a high-frequency case. We show that linearly polarized light can change not only the magnitudes and signs of the exchange interactions, but also their bond anisotropy even without the bond-anisotropic hopping integrals. Because of this property, the honeycomb-network spin system could be transformed into weakly coupled zigzag or step spin chains for the light field polarized along the $b$- or $a$-axis, respectively. Then, analyzing how the light fields affect several magnetic states in a mean-field approximation, we show that linearly polarized light can change the relative stability of the competing magnetic states, whereas such a change is absent for circularly polarized light. We also analyze the effects of both the bond anisotropy of nearest-neighbor hopping integrals and a third-neighbor hopping integral on the magnetic states and show that the results obtained in a simple model, in which the bond-averaged nearest-neighbor hopping integrals are considered, remain qualitatively unchanged except for the stability of zigzag states in the non-driven case and the degeneracy lifting of the zigzag or stripy states.

Efficient magnetic superstructure optimization with [formula omitted

Simulating the incommensurate spin density waves (ISDW) states is not a simple task within the standard ab initio methods. Moreover, in the context of new material discovery, there is a need for fast and reliable tool capable to scan and optimize the total energy as a function of the pitch vector, thus allowing to automatize the search for new materials. In this paper we show how the ISDW can be efficiently obtained within the recently released ΘΦ program. We illustrate this on an example of the single orbital Hubbard model and of γ-Fe, where the ISDW emerge within the mean-field approximation and by using the twisted boundary conditions. We show the excellent agreement of the ΘΦ with the previously published ones and discuss possible extensions. Finally, we generalize the previously given framework for spin quantization axis rotation to the most general case of spin-dependent hopping matrix elements.

Orbital Mott transition in two dimensional pyrochlore lattice

We study orbital Mott transition in two dimensional pyrochlore lattice, using a two orbital Hubbard model with only inter-orbital electronic hopping. We use a real space Monte Carlo based approach to study the model at finite temperature, and establish temperature-interaction phase diagram that highlights the Mott transition, orbital ordering, and spectral trends, and possible window of pseudogap. Due to only inter-orbital hopping, the Mott insulator ‘generates’ ferro exchange resulting in ferro-orbital ordering, with Tcorr/t peaked at ≈0.2 around U/t ≈ 6. The optical conductivity shows unusual two peak feature due to two dimensional pyrochlore lattice.

Anomalous magnetism in hydrogenated graphene

We revisit the problem of local moment formation in graphene due to chemisorption of individual atomic hydrogen or other analogous sp$^3$ covalent functionalizations. We describe graphene with the single orbital Hubbard model, so that the H chemisorption is equivalent to a vacancy in the honeycomb lattice. In order to circumvent artefacts related to periodic unit cells, we use either huge simulation cells of up to $8\times10^5$ sites, or an embedding scheme that allows the modelling of a single vacancy in an otherwise pristine infinite honeycomb lattice. We find three results that stress the anomalous nature of the magnetic moment ($m$) in this system. First, in the non-interacting ($U=0$), zero temperature ($T=0$) case, the $m(B)$ is a continuous smooth curve with divergent susceptibility, different from the step-wise constant function found for a single unpaired spins in a gapped system. Second, for $U=0$ and $T>0$, the linear susceptibility follows a power law $\propto{T}^{-\alpha}$ with an exponent of $\alpha=0.77$ different from conventional Curie's law. For $U>0$, in the mean field approximation, the integrated moment is smaller than $m=1\mu_B$, in contrast with results using periodic unit cells. These three results highlight that the magnetic response of the local moment induced by sp$^3$ functionalizations in graphene is different both from that of local moments in gaped systems, for which the magnetic moment is quantized and follows a Curie law, and from Pauli paramagnetism in conductors, for which a linear susceptibility can be defined at $T=0$.

J Freezing and Hund's Rules in Spin-Orbit-Coupled Multiorbital Hubbard Models.

We investigate the phase diagram of the spin-orbit-coupled three orbital Hubbard model at arbitrary filling by means of dynamical mean-field theory combined with the continuous-time quantum MonteCarlo method. We find that the spin-freezing crossover occurring in the metallic phase of the nonrelativistic multiorbital Hubbard model can be generalized to a J-freezing crossover, with J=L+S, in the spin-orbit-coupled case. In the J-frozen regime the correlated electrons exhibit a nontrivial flavor selectivity and energy dependence. Furthermore, in the regions near n=2 and n=4 the metallic states are qualitatively different from each other, which reflects the atomic Hund's third rule. Finally, we explore the appearance of magnetic order from exciton condensation at n=4 and discuss the relevance of our results for real materials.

Vector chirality for effective total momentum Jeff in a nonfrustrated Mott insulator: Effects of strong spin-orbit coupling and broken inversion symmetry

I propose the emergence of the spin-orbital-coupled vector chirality in a non-frustrated Mott insulator with the strong spin-orbit coupling due to $ab$-plane's inversion-symmetry (IS) breaking. I derive the superexchange interactions for a $t_{2g}$-orbital Hubbard model on a square lattice with the strong spin-orbit coupling and the IS-breaking-induced hopping integrals, and explain the microscopic origins of the Dzyaloshinsky-Moriya (DM) -type and the Kitaev-type interactions. Then, by adopting the mean-field approximation to a minimal model including only the Heisenberg-type and the DM-type nearest-neighbor interactions, I show that the IS breaking causes the spin-orbital-coupled chirality as a result of stabilizing the screw state. I also highlight the limit of the hard-pseudospin approximation in discussing the stability of the screw states in the presence of both the DM-type and the Kitaev-type interactions, and discuss its meaning. I finally discuss the effects of tetragonal crystal field and $J_{\textrm{eff}}=\frac{3}{2}$ states, and the application to the iridates near the $[001]$ surface of Sr$_{2}$IrO$_{4}$ and the interface between Sr$_{2}$IrO$_{4}$ and Sr$_{3}$Ir$_{2}$O$_{7}$.

A multi-orbital iterated perturbation theory for model Hamiltonians and real material-specific calculations of correlated systems

Perturbative schemes utilizing a spectral moment expansion are well known and extensively used for investigating the physics of model Hamiltonians and real material systems. The advantages they offer, in terms of being computationally inexpensive, with real frequency output at zero and finite temperatures, compensate for their deficiencies and offer a quick, qualitative analysis of the system behavior. In this work, we have developed a method, that can be classified as a multi-orbital iterative perturbation theory (MO-IPT) to study N-fold degenerate and non degenerate Anderson impurity models. As applications of the solver, we have combined the method with dynamical mean field theory to explore lattice models like the single orbital Hubbard model, covalent band insulator and the multi-orbital Hubbard model for density-density type interactions in different parameter regimes. The Hund's coupling effects in case of multiple orbitals is also studied. The limitations and quality of results are gauged through extensive comparison with data from the numerically exact continuous time quantum Monte Carlo method (hybridization expansion CTQMC). In general we observe that the agreement with CTQMC results gets better as we move away from particle-hole symmetry. We have integrated MO-IPT with density functional theory based electronic structure methods to study real material systems. As a test case, we have studied the classic, strongly correlated electronic material, SrVO$_3$. A comparison of density of states and photo emission spectrum (PES) with results obtained from different impurity solvers and experiments yields good agreement.

Microscopic theory on charge transports of a correlated multiorbital system

Current vertex correction (CVC), the back-flow-like correction to the current, comes from conservation laws, and the CVC due to electron correlation contains information about many-body effects. However, it has been little understood how the CVC due to electron correlation affects the charge transports of a correlated multiorbital system. To improve this situation, I studied the inplane resistivity, $\rho_{ab}$, and the Hall coefficient in the weak-field limit, $R_{\textrm{H}}$, in addition to the magnetic properties and the electronic structure, for a $t_{2g}$-orbital Hubbard model on a square lattice in a paramagnetic state away from or near an antiferromagnetic (AF) quantum-critical point (QCP) in the fluctuation-exchange (FLEX) approximation with the CVCs arising from the self-energy ($\Sigma$), the Maki-Thompson (MT) irreducible four-point vertex function, and the main terms of the Aslamasov-Larkin (AL) one. Then, I found three main results about the CVCs. First, the main terms of the AL CVC does not qualitatively change the results obtained in the FLEX approximation with the $\Sigma$ CVC and the MT CVC. Second, $\rho_{ab}$ and $R_{\textrm{H}}$ near the AF QCP have high-temperature region, governed mainly by the $\Sigma$ CVC, and low-temperature region, governed mainly by the $\Sigma$ CVC and the MT CVC. Third, in case away from the AF QCP, the MT CVC leads to a considerable effect on only $R_{\textrm{H}}$ at low temperatures, although $R_{\textrm{H}}$ at high temperatures and $\rho_{ab}$ at all temperatures considered are sufficiently described by including only the $\Sigma$ CVC. I also achieved the qualitative agreement with several experiments of Sr$_{2}$RuO$_{4}$ or Sr$_{2}$Ru$_{0.975}$Ti$_{0.025}$O$_{4}$. Moreover, I showed several better points of this theory than other theories.

Orbital selective directional conductor in the two-orbital Hubbard model

Employing a recently developed many-body technique that allows for the incorporation of thermal effects, the rich phase diagram of a two dimensional two orbital (degenerate $d_{xz}$ and $d_{yz}$) Hubbard model is presented varying temperature and the repulsion $U$. Our main result is the finding at intermediate $U$ of a novel antiferromagnetic orbital selective state where an effective dimensional reduction renders one direction insulating and the other metallic. Possible realizations of this state are discussed. In addition we also study nematicity above the N\'eel temperature. After a careful finite-size scaling analysis the nematicity temperature window appears to survive in the bulk limit although it is very narrow.

Charge fluctuations in the unconventional metallic state ofLi0.9Mo6O17

Charge fluctuations in the quasi-one-dimensional material Li0.9Mo6O17 are analyzed based on a multi orbital extended Hubbard model. A charge ordering transition induced by Coulomb repulsion is found with a charge ordering pattern different from a conventional charge density wave driven by Fermi surface nesting. The metallic state displays a characteristic charge collective mode which softens signalling the proximity to the transition. We argue that the strong scattering between electrons generated by these charge order fluctuations can lead to the unconventional metallic state observed above the superconducting transition temperature in Li0.9Mo6O17.

The two orbital Hubbard model in a square lattice: a DMFT + DMRG approach

We develop a precise and reliable numerical method for the calculation of electronic properties of the two orbital Hubbard model in a square lattice at half filling, based on the Dynamical Mean Field Theory (DMFT). We use the Density Matrix Renormalization Group (DMRG) as the impurity solver for the DMFT's selfconsistent equations to obtain accurate values for the Green's functions on the real axis. This way, reliable densities of states are obtained that do not need to resort to analytical continuation methods as those using quantum Monte Carlo techniques. Large system sizes can be achieved with increasing accuracy.

Orbital-cooperative spin fluctuation and orbital-dependent transport in ruthenates

Unusual transport properties deviating from the Fermi liquid are observed in ruthenates near a magnetic quantum-critical point (QCP). To understand the electronic properties of the ruthenates near and away from an antiferromagnetic (AF) QCP, I study the electronic structure and magnetic and transport properties for the $t_{2g}$-orbital Hubbard model on a square lattice in fluctuation-exchange approximation including Maki-Thompson (MT) current vertex correction (CVC). The results away from the AF QCP reproduce several experimental results of Sr$_{2}$RuO$_{4}$ qualitatively and provide new mechanisms about the enhancement of spin fluctuation at $Q_{\textrm{IC-AF}}\approx (0.66\pi,0.66\pi)$, larger mass enhancement of the $d_{xy}$ orbital than that of the $d_{xz/yz}$ orbital, and nonmonotonic temperature dependence of the Hall coefficient. Also, the results near the AF QCP explain the $T$-linear inplane resistivity in Sr$_{2}$Ru$_{0.075}$Ti$_{0.025}$O$_{4}$ and give an experimental test on the obtained temperature dependence of the Hall coefficient. I reveal spatial correlation including the self-energy of electrons beyond mean-field approximations is essential to determine the electronic properties of the ruthenates. I also show several ubiquitous transport properties near an AF QCP and characteristic transport properties of a multiorbital system by comparison with results of a single-orbital system near an AF QCP.

Hybridizing localized and itinerant electrons: A recipe for pseudogaps

In a system where selective Mott localization is realized, some electrons show a gap to charge excitations while others do not. A hybridization between these two kind of electrons will lead to a smoothening of this sharp difference and can even bring the system back to a complete delocalization. We show here that there is a large region of parameters at finite hybridization where the selective localization persists and the system shows a partial filling of the selective gap with incoherent states, giving rise to a pseudogap. This result is illustrated here in a two orbital Hubbard model with Hund's coupling, but is based on quite general assumptions and should hold for a larger class of systems, and possibly be a paradigm for the pseudogap mechanism in cuprates.

Comparative DMFT study of theeg-orbital Hubbard model in thin films

Heterostructures of transition-metal oxides have emerged as a new route to engineer electronic systems with desired functionalities. Motivated by these developments, we study a two-orbital Hubbard model in a thin-film geometry confined along the cubic [001] direction using the dynamical mean-field theory. We contrast the results of two approximate impurity solvers (exact diagonalization and one-crossing approximation) to the results of the numerically exact continuous-time quantum Monte Carlo solver. Consistent with earlier studies, we find that the one-crossing approximation performs well in the insulating regime, while the advantage of the exact-diagonalization-based solver is more pronounced in the metallic regime. We then investigate various aspects of strongly correlated ${e}_{g}$-orbital systems in thin-film geometries. In particular, we show how the interfacial orbital polarization dies off quickly a few layers from the interface and how the film thickness affects the location of the interaction-driven Mott transition. In addition, we explore the changes in the electronic structure with varying carrier concentration and identify large variations of the orbital polarization in the strongly correlated regime.

Orbital Nematic Instability in the Two-Orbital Hubbard Model: Renormalization-Group + Constrained RPA Analysis

Motivated by the nematic electronic fluid phase in Sr(3)Ru(2)O(7), we develop a combined scheme of the renormalization-group method and the random-phase-approximation-type method, and analyze orbital susceptibilities of the (d(xz), d(yz))-orbital Hubbard model with high accuracy. It is confirmed that the present model exhibits a ferro-orbital instability near the magnetic or superconducting quantum criticality, due to the Aslamazov-Larkin-type vertex corrections. This mechanism of orbital nematic order presents a natural explanation for the nematic order in Sr(3)Ru(2)O(7), and is expected to be realized in various multiorbital systems, such as Fe-based superconductors.