Extended Dynamical Mean-field Theory Research Articles

Correlated Electronic Structure of La_{3}Ni_{2}O_{7} under Pressure.

Recently, superconductivity with a T_{c} up to 78K has been reported in bulk samples of the bilayer nickelate La_{3}Ni_{2}O_{7} at pressures above 14GPa. Important theoretical tasks are the formulation of relevant low-energy models and the clarification of the normal state properties. Here, we study the correlated electronic structure of the high-pressure phase in a four-orbital low-energy subspace using different many-body approaches: GW, dynamical mean field theory (DMFT), extended DMFT (EDMFT) and GW+EDMFT, with realistic frequency-dependent interaction parameters. The nonlocal correlation and screening effects captured by GW+EDMFT result in an instability toward the formation of charge stripes, with the 3d_{z^{2}} as the main active orbital. We also comment on the potential relevance of the rare-earth self-doping pocket, since hole doping suppresses the ordering tendency.

First principles investigation of screened Coulomb interaction and electronic structure of low-temperature phase TaS2

By means of ab initio computation schemes, we examine the electronic screening, Coulomb interaction strength, and the electronic structure of a quantum spin liquid candidate monolayer TaS2 in its low-temperature commensurate charge-density-wave phase. Not only local () but non-local () correlations are estimated within random phase approximation based on two different screening models. Using GW+ EDMFT (GW plus extended dynamical mean-field theory) method, we investigate the detailed electronic structure by increasing the level of non-local approximation from DMFT () to EDMFT and GW+ EDMFT.

Generalized dynamical mean-field theory of two-sublattice systems with long-range interactions and its application to study charge and spin correlations in graphene

We investigate magnetic and charge correlations in graphene by using the formulation of extended dynamical mean-field theory (E-DMFT) for two-sublattice systems. First, we map the average non-local interaction onto the effective static interaction between different sublattices, which is treated together with the local interaction within an effective "two-orbital" local model. The remaining part of the non-local interaction is considered by introducing an effective retarded interaction within the E-DMFT approach. The non-local susceptibilities in charge and spin channel are further evaluated in the ladder approximation. We verify the applicability of the proposed method to describe the effect of uniformly screened long-range Coulomb potential $\propto 1/r$, as well as screened realistic long-range electron interaction [T. O. Wehling et al., Phys. Rev. Lett. 106, 236805 (2011)] in graphene. We show that the developed approach describes a competition of semimetal, spin density wave (SDW), and charge-density-wave (CDW) correlations. The obtained phase diagram is in a good agreement with recent results of functional renormalization group (fRG) for finite large graphene nanoflakes and scaling analysis of quantum Monte Carlo data on finite clusters. Similarly to the previously obtained results within the fRG approach, the realistic screening of Coulomb interaction by $\sigma$ bands causes moderate (strong) enhancement of critical long-range interaction strength, needed for the SDW (CDW) instability, compared to the results for the uniformly screened Coulomb potential.

Orbital Isotropy of Magnetic Fluctuations in Correlated Electron Materials Induced by Hund's Exchange Coupling.

Characterizing nonlocal magnetic fluctuations in materials with strong electronic Coulomb interactions remains one of the major outstanding challenges of modern condensed matter theory. In this Letter, we address the spatial symmetry and orbital structure of magnetic fluctuations in perovskite materials. To this aim, we develop a consistent multiorbital diagrammatic extension of dynamical mean-field theory, which we apply to an anisotropic three-orbital model of cubic t_{2g} symmetry. We find that the form of spatial spin fluctuations is governed by the local Hund's coupling. For small values of the coupling, magnetic fluctuations are anisotropic in orbital space, which reflects the symmetry of the considered t_{2g} model. Large Hund's coupling enhances collective spin excitations, which mixes orbital and spatial degrees of freedom, and magnetic fluctuations become orbitally isotropic. Remarkably, this effect can be seen only in two-particle quantities; single-particle observables remain anisotropic for any value of the Hund's coupling. Importantly, we find that the orbital isotropy can be induced both at half filling and for the case of four electrons per lattice site, where the magnetic instability is associated with different, antiferromagnetic and ferromagnetic, modes, respectively.

Improved treatment of fermion-boson vertices and Bethe-Salpeter equations in nonlocal extensions of dynamical mean field theory

We reconsider the procedure of calculation of fermion-boson vertices and numerical solution of Bethe-Salpeter equations, used in non-local extensions of dynamical mean-field theory. Because of the frequency dependence of vertices, finite frequency box for matrix inversions is typically used, which often requires some treatment of asymptotic behaviour of vertices. Recently [Phys. Rev. B 83, 085102 (2011); 97, 235140 (2018)] it was proposed to split the considered frequency box into smaller and larger one; in the smaller frequency box the numerically exact vertices are used, while beyond this box asymptotics of vertices are applied. Yet, this method requires numerical treatment of vertex asymptotics (including corresponding matrix manipulations) in the larger frequency box and/or knowing fermion-boson vertices, which may be not convenient for numerical calculations. In the present paper we derive the formulae which treat analytically contribution of vertices beyond chosen frequency box, such that only numerical operations with vertices in the chosen small frequency box are required. The method is tested on the Hubbard model and can be used in a broad range of applications of non-local extensions of dynamical mean-field theory.

The extended Hubbard model with attractive interactions

We discuss the phase diagram of the extended Hubbard model with both attractive and repulsive local and nonlocal interactions. The extended dynamical mean-field theory (EDMFT) and the dual boson method (DB) are compared. The latter contains additional nonlocal correlation effects that are not incorporated in EDMFT. We find that EDMFT and DB give almost identical results in the attractive V regime, where phase separation occurs. This is quite a difference with the previously studied repulsive V regime, where EDMFT and DB give very different phase boundaries for the checkerboard order phase, especially at small U.

Fermion-boson vertex within dynamical mean-field theory

In the study of strongly interacting systems, correlations on the two-particle level are receiving more and more attention. In this work, we study a particular two-particle correlation function: the fermion-boson vertex. It describes the response of the Green's function when an external field is applied and is an important ingredient of diagrammatic extensions of Dynamical Mean-Field Theory. We provide several perspectives on this object, using Ward identities, sum rules, perturbative analysis and asymptotic relations. We then use these tools to study the vertex across the doping-driven metal-insulator transition and find a divergence in the imaginary part.

Coupled charge and spin dynamics in a photoexcited doped Mott insulator

Using a nonequilibrium implementation of the extended dynamical mean field theory (EDMFT) we simulate the relaxation after photo excitation in a strongly correlated electron system with antiferromagnetic spin interactions. We consider the $t$-$J$ model and focus on the interplay between the charge- and spin-dynamics in different excitation and doping regimes. The appearance of string states after a weak photo excitation manifests itself in a nontrivial scaling of the relaxation time with the exchange coupling and leads to a correlated oscillatory evolution of the kinetic energy and spin-spin correlation function. A strong excitation of the system, on the other hand, suppresses the spin correlations and results in a relaxation that is controlled by hole scattering. We discuss the possibility of detecting string states in optical and cold atom experiments.

Collective charge excitations and the metal-insulator transition in the square lattice Hubbard-Coulomb model

In this article, we discuss the nontrivial collective charge excitations (plasmons) of the extended square lattice Hubbard model. Using a fully nonperturbative approach, we employ the hybrid Monte Carlo algorithm to simulate the system at half-filling. A modified Backus-Gilbert method is introduced to obtain the spectral functions via numerical analytic continuation. We directly compute the single-particle density of states which demonstrates the formation of Hubbard bands in the strongly correlated phase. The momentum-resolved charge susceptibility also is computed on the basis of the Euclidean charge-density-density correlator. In agreement with previous extended dynamical mean-field theory studies, we find that, at high strength of the electron-electron interaction, the plasmon dispersion develops two branches.

Conservation in two-particle self-consistent extensions of dynamical mean-field theory

Extensions of dynamical-mean-field-theory (DMFT) make use of quantum impurity models as non-perturbative and exactly solvable reference systems which are essential to treat the strong electronic correlations. Through the introduction of retarded interactions on the impurity, these approximations can be made two-particle self-consistent. This is of interest for the Hubbard model, because it allows to suppress the antiferromagnetic phase transition in two-dimensions in accordance with the Mermin-Wagner theorem, and to include the effects of bosonic fluctuations. For a physically sound description of the latter, the approximation should be conserving. In this paper we show that the mutual requirements of two-particle self-consistency and conservation lead to fundamental problems. For an approximation that is two-particle self-consistent in the charge- and longitudinal spin channel, the double occupancy of the lattice and the impurity are no longer consistent when computed from single-particle properties. For the case of self-consistency in the charge- and longitudinal as well as transversal spin channels, these requirements are even mutually exclusive so that no conserving approximation can exist. We illustrate these findings for a two-particle self-consistent and conserving DMFT approximation.

Diagrammatic Monte Carlo approach for diagrammatic extensions of dynamical mean-field theory: Convergence analysis of the dual fermion technique

The dual-fermion approach provides a formally exact prescription for calculating properties of a correlated electron system in terms of a diagrammatic expansion around dynamical mean-field theory (DMFT). Most practical implementations, however, neglect higher-order interaction vertices beyond two-particle scattering in the dual effective action and further truncate the diagrammatic expansion in the two-particle scattering vertex to a leading-order or ladder-type approximation. In this work we compute the dual-fermion expansion for the two-dimensional Hubbard model including all diagram topologies with two-particle interactions to high orders by means of a stochastic diagrammatic Monte Carlo algorithm. We benchmark the obtained self-energy against numerically exact Diagrammatic Determinant Monte Carlo simulations to systematically assess convergence of the dual-fermion series and the validity of these approximations. We observe that, from high temperatures down to the vicinity of the DMFT N\'eel transition, the dual-fermion series converges very quickly to the exact solution in the whole range of Hubbard interactions considered ($4 \leq U/t \leq 12$), implying that contributions from higher-order vertices are small. As the temperature is lowered further, we observe slower series convergence, convergence to incorrect solutions, and ultimately divergence. This happens in a regime where magnetic correlations become significant. We find however that the self-consistent particle-hole ladder approximation yields reasonable and often even highly accurate results in this regime.

From local to nonlocal correlations: The Dual Boson perspective

Extended dynamical mean-field theory (EDMFT) is insufficient to describe non-local effects in strongly correlated systems, since corrections to the mean-field solution are generally large. We present an efficient scheme for the construction of diagrammatic extensions of EDMFT that avoids usual double counting problem by using an exact change of variables (the dual boson formalism) to distinguish the correlations included in the mean-field solution and those beyond. With a computational efficiency comparable to EDMFT+GW approach, our scheme significantly improves on the charge order transition phase boundary in the extended Hubbard model.

Spin-density functional theories and their+Uand+Jextensions: A comparative study of transition metals and transition metal oxides

Previous work on the physical content of exchange correlation functionals that depend on both charge and spin densities is extended to elemental transition metals and a wider range of perovskite transition metal oxides. A comparison of spectra and magnetic moments calculated using exchange correlation functionals depending on charge density only or on both charge and spin densities, as well as the $+U$ and $+J$ extensions of these methods confirms previous conclusions that the spin-dependent part of the exchange correlation functional provides an effective Hund's interaction acting on the transition metal $d$ orbitals. For the local spin density approximation and spin-dependent Perdew-Burke-Ernzerhof generalized gradient approximation, the effective Hund's exchange is found to be larger than 1 eV. The results indicate that at least as far as applications to transition metals and their oxides are concerned, $+U$, $+J$ and +dynamical mean field theory extensions of density functional theory should be based on exchange-correlation functionals of charge density only.

Thermodynamic consistency of the charge response in dynamical mean-field based approaches

We consider the thermodynamic consistency of the charge response function in the (extended) Hubbard model. In dynamical mean-field theory (DMFT), thermodynamic consistency is preserved. We prove that the static, homogeneous DMFT susceptibility is consistent as long as vertex corrections obtained from the two-particle impurity correlation function are included. In the presence of a nonlocal interaction, the problem may be treated within extended DMFT (EDMFT), or its diagrammatic extension, the dual boson approach. We show that here maintaining thermodynamic consistency requires knowledge of three- and four-particle impurity correlation functions, which are typically neglected. Nevertheless, the dual boson approximation to the response is remarkably close to consistency. This holds even when two-particle vertex corrections are neglected. EDMFT is consistent only in the strongly correlated regime and near half-filling, where the physics is predominantly local.

Electronic structure ofLi2RuO3studied by LDA and LDA+DMFT calculations and soft x-ray spectroscopy

The electronic structure of ${\mathrm{Li}}_{2}{\mathrm{RuO}}_{3}$ was investigated using x-ray emission and absorption spectroscopy and by theoretical calculations employing two approaches: the local density approximation (LDA) and a combination of LDA with the cluster extension of dynamical mean-field theory (LDA+DMFT). The evolution of the spectral properties with the strength of electronic correlations is analyzed. We show that for moderate values of on-site Coulomb repulsion $U$ and intra-atomic Hund's rule exchange ${J}_{H},{\mathrm{Li}}_{2}{\mathrm{RuO}}_{3}$ is in an orbital-selective strongly correlated state in the sense that a part of the ${t}_{2g}$ manifold (i.e., $xz/yz)$ behaves as local atomic orbitals susceptible to Hubbard correlations, while the remaining $(xy)$ orbitals must be described as bond-centered molecular orbitals. Both theoretical approaches succeed in explaining the x-ray data, and a comparison of the theoretical and experimental spectra provides a reasonable estimate of the possible correlation strength $(U)$ and Hund's coupling $({J}_{H})$ in ${\mathrm{Li}}_{2}{\mathrm{RuO}}_{3}$.

Beyond extended dynamical mean-field theory: Dual boson approach to the two-dimensional extended Hubbard model

The dual boson approach [Ann. Phys. 327, 1320 (2012)] provides a means to construct a diagrammatic expansion around the extended dynamical mean-field theory (EDMFT). In this paper, we present the numerical implementation of the approach and apply it to the extended Hubbard model with nearest-neighbor interaction $V$. We calculate the EDMFT phase diagram and study the effect of diagrams beyond EDMFT on the transition to the charge-ordered phase. Including diagrammatic corrections to the EDMFT polarization shifts the EDMFT phase boundary to lower values of $V$. The approach interpolates between the random phase approximation in the weak coupling limit and EDMFT for strong coupling. Neglecting vertex corrections leads to results reminiscent of the EDMFT+$GW$ approximation. We however find significant deviations from the dual boson results already for small values of the interaction, emphasizing the crucial importance of fermion-boson vertex corrections.

Plasmons in strongly correlated systems: spectral weight transfer and renormalized dispersion.

We study the charge-density dynamics within the two-dimensional extended Hubbard model in the presence of long-range Coulomb interaction across the metal-insulator transition point. To take into account strong correlations we start from self-consistent extended dynamical mean-field theory and include nonlocal dynamical vertex corrections through a ladder approximation to the polarization operator. This is necessary to fulfill charge conservation and to describe plasmons in the correlated state. The calculated plasmon spectra are qualitatively different from those in the random-phase approximation: they exhibit a spectral density transfer and a renormalized dispersion with enhanced deviation from the canonical √q behavior. Both features are reminiscent of interaction induced changes found in single-electron spectra of strongly correlated systems.

Effects of non-local spin fluctuations in the orbital-selective Mott transition

Employing the extended dynamical mean field theory (EDMFT) and the quantum Monte Carlo (QMC) method, we investigate the effect of the spatial fluctuations in the two-band Hubbard model with anisotropic bandwidth in the vicinity of the Mott metal-insulator transition. At half filling, we demonstrate that while the inclusion of the non-local spin-spin interaction amounts to enhancing the correlation and suppressing the metallic character, the orbitally selective Mott transition (OSMT) remains stable for various strengths of the non-local correlation. The same is true when the system is doped away from half filling. The OSMT phase is evidenced at low dopant concentration and the simultaneous metallic phase emerges at overdoped regime. From the analysis of the self energy, it follows that the nature of the metallic phase upon doping violates the Fermi liquid character and persists at considerably large doping. Our theory also offers a new perspective for the investigation of the non-local fluctuation in the multi-orbital system within the single-site scheme.

Dynamical mean-field theory of indirect magnetic exchange

To analyze the physical properties arising from indirect magnetic exchange between several magnetic adatoms and between complex magnetic nanostructures on metallic surfaces, the real-space extension of dynamical mean-field theory (R-DMFT) appears attractive as it can be applied to systems of almost arbitrary geometry and complexity. While R-DMFT describes the Kondo effect of a single adatom exactly, indirect magnetic (RKKY) exchange is taken into account on an approximate level only. Here, we consider a simplified model system consisting of two magnetic Hubbard sites ("adatoms") hybridizing with a non-interacting tight-binding chain ("substrate surface"). This two-impurity Anderson model incorporates the competition between the Kondo effect and indirect exchange but is amenable to an exact numerical solution via the density-matrix renormalization group (DMRG). The particle-hole symmetric model at half-filling and zero temperature is used to benchmark R-DMFT results for the magnetic coupling between the two adatoms and for the magnetic properties induced in the substrate. In particular, the dependence of the local adatom and the nonlocal adatom-adatom static susceptibilities as well as the magnetic response of the substrate on the distance between the adatoms and on the strength of their coupling with the substrate is studied. We find both, excellent agreement with the DMRG data even on subtle details of the competition between RKKY exchange and the Kondo effect but also complete failure of the R-DMFT, depending on the parameter regime considered. R-DMFT calculations are performed using the Lanczos method as impurity solver. With the real-space extension of the two-site DMFT, we also benchmark a simplified R-DMFT variant.

Extension of dynamical mean-field theory by inclusion of nonlocal two-site correlations with variable distance

We present an approximation scheme for the treatment of strongly correlated electrons in arbitrary crystal lattices. The approach extends the well-known dynamical mean-field theory to include nonlocal two-site correlations of arbitrary spatial extent. We extract the nonlocal correlation functions from two-impurity Anderson models where the impurity-impurity distance defines the spatial extent of the correlations included. Translational invariance is fully respected by our approach since correlation functions of any two-impurity cluster are periodically embedded to $\underline{k}$ space via a Fourier transform. As a first application, we study the two-dimensional Hubbard model on a simple-cubic lattice. We demonstrate how pseudogap formation in the many-body resonance at the Fermi level results from the inclusion of nonlocal correlations. A comparison of the spectral function with the dynamical-cluster approximation shows qualitative agreement of high- as well as low-energy features.