Inter-orbital Coulomb Interactions Research Articles

Unconventional correlated metallic behavior due to interorbital Coulomb interaction

Unconventional correlated metallic behavior due to interorbital Coulomb interaction

Enhanced Spin–Orbit Coupling in a Correlated Metal

We investigate the correlation effects on spin-orbit coupling (SOC) in a two-orbital Hubbard model on a square lattice by applying the variational Monte Carlo method. We consider an effective SOC constant $\lambda_{\text{eff}}$ in the one-body part of the variational wave function and mainly discuss the cases of the electron number per site $n=1$, that is, quarter filling. We find that $\lambda_{\text{eff}}$ is proportional to the bare value $\lambda$ and depends on the electron-electron interactions through $(U'-J')$ in a relatively wide parameter range in the paramagnetic (PM) phase, where $U'$ is the interorbital Coulomb interaction and $J'$ is the pair hopping interaction. Increasing the electron-electron interactions in the PM phase leads to a transition to an effective one-band state, in which the upper band becomes empty due to the enhanced $\lambda_{\text{eff}}$. We also construct phase diagrams considering magnetic order. The carrier doping effect on $\lambda_{\text{eff}}$ is also investigated. We find that $\lambda_{\text{eff}}$ enhances in a strongly correlated region around the Mott transition point and it is necessary to include the correlation effects beyond the Hartree-Fock approximation to describe the enhanced SOC properly.

In-gap band in the one-dimensional two-orbital Kanamori-Hubbard model with interorbital Coulomb interaction

We study the electronic spectral properties at zero temperature of the one-dimensional (1D) version of the degenerate two-orbital Kanamori Hubbard model (KHM), one of the well established frameworks to study transition metal compounds, using state-of-the-art numerical techniques based on the Density Matrix Renormalization Group. While the system is Mott insulating for the half-filled case, as expected for an interacting 1D system, we find interesting and rich structures in the single-particle density of states (DOS) for the hole-doped system. In particular, we find the existence of in-gap states which are pulled down to lower energies from the upper Hubbard band (UHB) with increasing the inter-orbital Coulomb interaction $V$. We analyze the composition of the DOS by projecting it onto different local excitations and we observe that for large dopings these in-gap excitations are formed mainly by inter-orbital holon-doublon (HD) states and their energies follow approximately the HD states in the atomic limit. We observe that the Hund interaction $J$ increases the width of the in-gap band, as expected from the two-particle fluctuations in the Hamiltonian. The observation of a finite density of states within the gap between the Hubbard bands for this extended 1D model indicates that these systems present a rich excitation spectra which could help us understand the microscopic physics behind multi-orbital compounds.

Spectroscopic Determination of Key Energy Scales for the Base Hamiltonian of Chromium Trihalides

The van der Waals (vdW) chromium trihalides (CrX3) exhibit field-tunable, two-dimensional magnetic orders that vary with the halogen species and the number of layers. Their magnetic ground states with proximity in energies are sensitive to the degree of ligand-metal (p-d) hybridization and relevant modulations in the Cr d-orbital interactions. We use soft X-ray absorption (XAS) and resonant inelastic X-ray scattering (RIXS) spectroscopy at Cr L-edge along with the atomic multiplet simulations to determine the key energy scales such as the crystal field 10 Dq and interorbital Coulomb interactions under different ligand metal charge transfer (LMCT) in CrX3 (X= Cl, Br, and I). Through this systematic study, we show that our approach compared to the literature has yielded a set of more reliably determined parameters for establishing a base Hamiltonian for CrX3.

Subbands in the doped two-orbital Kanamori-Hubbard model

We calculate and resolve with unprecedented detail the local density of states (DOS) and momentum-dependent spectral functions at zero temperature of one of the key models for strongly correlated electron materials, the degenerate two-orbital Kanamori-Hubbard model, by means of a highly optimized Dynamical Mean Field Theory which uses the Density Matrix Renormalization Group as the impurity solver. When the system is hole doped, and in the presence of a finite interorbital Coulomb interaction we find the emergence of a novel holon-doublon in-gap subband which is split by the Hund's coupling. We also observe new interesting features in the DOS like the splitting of the lower Hubbard band into a coherent narrowly dispersing peak around the Fermi energy, and another subband which evolves with the chemical potential. We characterize the main transitions giving rise to each subband by calculating the response functions of specific projected operators and comparing with the energies in the atomic limit, obtaining excellent agreement. The detailed results for the spectral functions found in this work pave the way to study with great precision the microscopic quantum behavior in correlated materials.

Excitonic insulator phase and condensate dynamics in a topological one-dimensional model

We employ mean-field approximation to investigate the interplay between the nontrivial band topology and the formation of excitonic insulator (EI) in a one-dimensional chain of atomic $s-p$ orbitals in the presence of repulsive inter-orbital Coulomb interaction. We find that our model, in a non-interacting regime, admits topological and trivial insulator phases, whereas, in strong Coulomb interaction limit, the chiral symmetry is broken and the system undergoes a topological-excitonic insulator phase transition. The latter phase transition stems from an orbital pseudomagnetization and band inversion around $k=0$. Our findings show that contrary to the topological insulator phase, electron-hole bound states do not form exciton condensate in the trivial band insulator phase due to lack of band inversion. Interestingly, the EI phase in low $s-p$ hybridization limit hosts a Bardeen-Cooper-Schrieffer (BCS)/Bose-Einstein condensation (BEC) crossover. Irradiated by a pump pulse, our findings reveal that the oscillations of exciton states strongly depend on the frequency of the laser pulse. We further explore the signatures of dynamics of the exciton condensate in optical measurements.

Atomic-Scale Magnetic Toroidal Dipole under Odd-Parity Hybridization

Magnetic toroidal dipole (MTD) is one of a fundamental constituent to induce magneto-electric effects in the absence of both spatial inversion and time-reversal symmetries. We report on a microscopic investigation of the atomic-scale MTD in solids by taking into account the orbital degree of freedom with a different parity. We construct an effective two-orbital $d$-$f$ tight-binding model on a polar tetragonal system for describing the atomic-scale MTD, which are obtained by incorporating the atomic spin-orbit coupling and odd-parity hybridization. The effective model exhibits two types of the MTDs: in-plane $x, y$ components activated through spontaneous ferromagnetic ordering or external magnetic field and an out-of-plane $z$ component by a spontaneous odd-parity hybridization without spin moments. We show that the intra-orbital (inter-orbital) Coulomb interaction in multi-orbital systems plays an important role in stabilizing the in-plane (out-of-plane) MTD orderings. We also examine the magneto-electric effect under each MTD ordering by calculating a linear response tensor. We show that the odd-parity hybridization enhances the magneto-electric effect for the in-plane MTDs, while it suppresses that for the out-of-plane MTD.

Excitonic Order and Superconductivity in the Two-Orbital Hubbard Model: Variational Cluster Approach

Using the variational cluster approach based on the self-energy functional theory, we study the possible occurrence of excitonic order and superconductivity in the two-orbital Hubbard model with intra- and inter-orbital Coulomb interactions. It is known that an antiferromagnetic Mott insulator state appears in the regime of strong intra-orbital interaction, a band insulator state appears in the regime of strong inter-orbital interaction, and an excitonic insulator state appears between them. In addition to these states, we find that the $s^{\pm}$-wave superconducting state appears in the small-correlation regime, and the $d_{x^2 - y^2}$-wave superconducting state appears on the boundary of the antiferromagnetic Mott insulator state. We calculate the single-particle spectral function of the model and compare the band gap formation due to the superconducting and excitonic orders.

Photoinduced enhancement of excitonic order in the two-orbital Hubbard model

Photoinduced dynamics in an excitonic insulator is studied theoretically by using a two-orbital Hubbard model on the square lattice where the excitonic phase in the ground state is characterized by the BCS-BEC crossover as a function of the interorbital Coulomb interaction. We consider the case where the order has a wave vector $Q=(0,0)$ and photoexcitation is introduced by a dipole transition. Within the mean-field approximation, we show that the excitonic order can be enhanced by the photoexcitation when the system is initially in the BEC regime of the excitonic phase, whereas it is reduced if the system is initially in the BCS regime. The origin of this difference is discussed from behaviors of momentum distribution functions and momentum-dependent excitonic pair condensation. In particular, we show that the phases of the excitonic pair condensation have an important role in determining whether the excitonic order is enhanced or not.

Origin of Biquadratic Exchange Interactions in a Mott Insulator as a Driving Force of Spin Nematic Order

We consider a series of Mott insulators in unit of two orbitals each hosting spin-1/2 electron, and by pairing two spin-1/2 into spin-1 triplet, derive the effective exchange interaction between the adjacent units via fourth order perturbation theory. It turns out that the biquadratic exchange interaction between spin-1, which is one of the origins of the nematic order, arises only in processes where the four different electrons exchange cyclically along the twisted loop, which we call "twisted ring exchange" processes. We show that the term becomes the same order with the Heisenberg exchange interactions when the on-orbital Coulomb interaction is not too large. Whereas, the inter-orbital Coulomb interactions give rise to additional processes that cancel the twisted ring exchange, and strongly suppresses the biquadratic term. The Mott insulator with two electrons on degenerate two orbitals is thus not an ideal platform to study such nematic orders.

Zigzag and Checkerboard Magnetic Patterns in Orbitally Directional Double-Exchange Systems.

We analyze a t(2g) double-exchange system where the orbital directionality of the itinerant degrees of freedom is a key dynamical feature that self-adjusts in response to doping and leads to a phase diagram dominated by two classes of ground states with zigzag and checkerboard patterns. The prevalence of distinct orderings is tied to the formation of orbital molecules that in one-dimensional paths make insulating zigzag states kinetically more favorable than metallic stripes, thus allowing for a novel doping-induced metal-to-insulator transition. We find that the basic mechanism that controls the magnetic competition is the breaking of orbital directionality through structural distortions, and highlight the consequences of the interorbital Coulomb interaction.

Emergent topological mirror insulator int2g-orbital systems

Motivated by the itinerant band structure of high-${T}_{c}$ iron pnictides, which exhibit four Dirac cones in the bulk, we demonstrate the prospect of pnictides with transition elements to be topological insulators in two dimensions. In this report, we explore interaction-induced topological phases, in contrast to the spin-orbit-coupling interaction, as the crucial mechanism for tuning Dirac metals into ${Z}_{2}$-topological insulators protected by time reversal and mirror symmetries. We find spontaneous orbital currents generated through nearest-neighbor interorbital Coulomb interaction in the ${t}_{2g}$ manifold of the $d$ orbitals. When spin degrees of freedom are incorporated, spontaneous orbital currents lead to two stable topological phases of the ground state. The first topological insulator is an anomalous orbital Hall phase, characterized by an even Chern number, while the second topological insulator is realized by protected mirror symmetries with a ${Z}_{2}$ index.

Nematic phase transition in a multi-orbital Hubbard model

By using the reflection positivity method, we rigorously establish some exact properties of a multi-orbital Hubbard model, here adopted to describe a nematic orbital phase transition. We show that, when the on-site intra-orbital Coulomb interaction is equal to the on-site inter-orbital Coulomb interaction, this model supports a staggered nematic orbital order if repulsive or attractive on-site inter-orbital and intra-orbital interactions and off-site repulsive inter-orbital interaction are considered. Depending on the dimensions of the bipartite lattice where the model is defined, we find that, at half-filling, the order may or may not exist. In particular, we prove that the order may exist, in two and three dimensions, at sufficiently low temperatures if the hopping amplitude is small enough.

Spin-orbit density wave: a new phase of matter applicable to the hidden order state of URu2Si2

We provide a brief review and detailed analysis of the spin-orbit density wave (SODW) proposed as a possible explanation to the ‘hidden order’ phase of URuSi. Due to the interplay between inter-orbital Coulomb interaction and spin-orbit coupling (SOC) in this compound, the SODW is shown to arise from Fermi surface nesting instability between two spin-orbit split bands. An effective low-energy Hamiltonian including single-particle SOC and two-particle SODW is derived, while the numerical results are calculated using density-functional theory (DFT)-based band-structure input. Computed gapped quasiparticle spectrum, entropy loss and spin-excitation spectrum are in detailed agreement with experiments. Interestingly, despite the fact that SODW governs dynamical spin-excitations, the static magnetic moment is calculated to be zero, owing to the time-reversal invariance imposed by SOC. As a consequence, SODW can be destroyed by finite magnetic field even at zero temperature. Our estimation of the location of the quantum critical point is close to the experimental value of 35 T. Finally, we extend the idea of SODW to other SOC systems including iridium oxides (iridates) and two-dimensional electronic systems such as BiAg surface and LaAlO/SrTiO interface. We show hint of quasiparticle gapping, reduction of pre-existing magnetic moment, large magneto-resistance, etc. which can be explained consistently within the SODW theory.

Metal–Insulator Transition and Superconductivity in the Two-Orbital Hubbard–Holstein Model for Iron-Based Superconductors

We investigate a two-orbital model for iron-based superconductors to elucidate the effect of interplay between electron correlation and Jahn-Teller electron-phonon coupling by using the dynamical mean-field theory combined with the exact diagonalization method. When the intra- and inter-orbital Coulomb interactions, $U$ and $U'$, increase with $U=U'$, both the local spin and orbital susceptibilities, $\chi_{s}$ and $\chi_{o}$, increase with $\chi_{s}=\chi_{o}$ in the absence of the Hund's rule coupling $J$ and the electron-phonon coupling $g$. In the presence of $J$ and $g$, there are distinct two regimes: for $J \stackrel{>}{_\sim} 2g^2/\omega_0$ with the phonon frequency $\omega_0$, $\chi_{s}$ is enhanced relative to $\chi_{o}$ and shows a divergence at $J=J_c$ above which the system becomes Mott insulator, while for $J \stackrel{<}{_\sim} 2g^2/\omega_0$, $\chi_{o}$ is enhanced relative to $\chi_{s}$ and shows a divergence at $g=g_c$ above which the system becomes bipolaronic insulator. In the former regime, the superconductivity is mediated by antiferromagnetic fluctuations enhanced due to Fermi-surface nesting and is found to be largely dependent on carrier doping. On the other hand, in the latter regime, the superconductivity is mediated by ferro-orbital fluctuations and is observed for wide doping region including heavily doped case without the Fermi-surface nesting.

Excitonic insulator state in the two-orbital Hubbard model: Variational cluster approach

The variational cluster approximation is used to study the spontaneous symmetry breaking of the excitonic insulator (EI) state in the two-orbital Hubbard model defined on the two-dimensional square lattice. Evaluating the order parameter of the EI state, staggered magnetization, and number of particles on each orbital, we obtain the ground-state phase diagram of the model in a wide parameter space of the intra and interorbital Coulomb interactions. We also calculate the single-particle and anomalous Green's functions. We show that the normal metallic phase is unstable to the formation of the EI state and the EI phase appears in a wide parameter region between the band-insulator and Mott-insulator phases.

Onset and melting of local orbital order

The onset and melting of locally staggered charge/orbital correlations is investigated within a two-orbital correlated electron model with inter-orbital and inter-site Coulomb interactions. The CE-type orbital correlation exhibits a sharp onset close to the Curie temperature and rapid thermal melting thereafter, which provides quantitative understanding of the (π/2,π/2,0) feature observed in neutron scattering experiments on La0.7(CaySr1−y)0.3MnO3 single crystals. In the zig-zag AF state, the CE-type orbital correlations are found to be even more readily stabilized, but only within a narrow doping regime around x = 0.5.

An effective quantum parameter for strongly correlated metallic ferromagnets

The correlated motion of electrons in metallic ferromagnets is investigated in terms of a realistic interacting-electron model with N-fold orbital degeneracy and intra-orbital (U) and inter-orbital (J) Coulomb interactions. Correlation-induced self-energy and vertex corrections are incorporated systematically to provide a non-perturbative Goldstone-mode-preserving scheme. An effective quantum parameter is obtained which determines, in analogy with 1/S for quantum spin systems and 1/N for the N-orbital Hubbard model, the strength of correlation-induced quantum corrections to magnetic excitations. The rapid suppression of this quantum parameter with Hund’s coupling J, especially for large N, provides fundamental insight into the phenomenon of strong stabilization of metallic ferromagnetism by orbital degeneracy and Hund’s coupling. Correlation effects are investigated for spin stiffness, magnon dispersion, electronic spectral function, density of states, and finite-temperature spin dynamics using realistic bandwidth, interaction, and lattice parameters for iron.

An advanced multi-orbital impurity solver for dynamical mean field theory based on the equation of motion approach

We propose an improved fast multi-orbital impurity solver for the dynamical mean field theory based on equations of motion (EOM) for Green’s functions and a decoupling scheme. In this scheme the inter-orbital Coulomb interactions are treated fully self-consistently, and involve the inter-orbital fluctuations. As an example of the use of the derived multi-orbital impurity solver, the two-orbital Hubbard model is studied for various cases. Comparisons are made between numerical results obtained with our EOM scheme and those obtained with quantum Monte Carlo and numerical renormalization group methods. The comparison shows a good agreement, but also reveals a dissimilarity of the behaviors of the densities of states which is caused by inter-site inter-orbital hopping effects and on-site inter-orbital fluctuation effects, thus corroborating the assertion of the value of the EOM method for the study of multi-orbital strongly correlated systems.

Fast multi-orbital equation of motion impurity solver for dynamical mean field theory

We propose a fast multi-orbital impurity solver for dynamical mean field theory (DMFT). Our DMFT solver is based on the equations of motion (EOMs) for local Green’s functions and is constructed by generalizing from the single-orbital case to the multi-orbital case with the inclusion of the inter-orbital hybridizations and applying a mean field approximation to the inter-orbital Coulomb interactions. The two-orbital Hubbard model is studied using this impurity solver within a large range of parameters. The Mott metal–insulator transition and the quasiparticle peak are well described. A comparison of the EOM method with the quantum Monte Carlo method is made for the two-orbital Hubbard model and good agreement is obtained. The developed method hence holds promise as a fast DMFT impurity solver in studies of strongly correlated systems.