The correlated Kondo insulator state of the plutonium monochalcogenides is investigated using the dynamical mean field theory (DMFT) and the local density approximation +U (LDA+U). The DMFT-dynamical fluctuations lead to a correlated insulator state at elevated temperature, in sharp contrast to the static LDA+U approach that fails to reproduce both the insulating behavior and anomalous lattice constant. The DMFT conversely predicts the experimentally observed anomalous increase of the gap with pressure and explains the lattice constant very well.
We present results of an ab-initio study of the electronic structure of 140 rare earth compounds. Specifically we predict an electronic phase diagram of the entire range of rare earth monopnictides and monochalcogenides, composed of metallic, semiconducting and heavy fermion-like regions, and exhibiting valency transitions brought about by a complex interplay between ligand chemistry and lanthanide contraction. The calculations exploit the combined effect of a first-principles methodology, which can adequately describe the dual character of electrons, itinerant vs. localized, and high throughp…
Pressure induced isostructural insulator to metal transition for SmS is characterised by the presence of an intermediate valence state at higher pressure which cannot be captured by the density functional theory. As a direct outcome of including the charge and spin fluctuations incorporated in dynamical mean field theory, we see the emergence of insulating and metallic phases with increasing pressure as a function of changing valence. This is accompanied by significantly improved predictions of the equilibrium lattice constants and bulk moduli for all Sm-monochalcogenides verifying experiments…
A new approach for calculating spectral density functions of strongly correlated electron systems is proposed within the exact diagonalization method of dynamical mean-field theory (DMFT). This approach is based on the analytic continuation of spectral density function obtained by conventional exact diagonalization method of DMFT and its results are more reasonable in shape. As an example of its application, the Mott transition in a strongly correlated electron system is investigated using this new approach.
We propose a cellular version of dynamical-mean field theory which gives a natural generalization of its original single-site construction and is formulated in different sets of variables. We show how non-orthogonality of the tight-binding basis sets enters the problem and prove that the resulting equations lead to manifestly causal self energies.
The consequences of dynamical screening of Coulomb interaction among correlated electrons in realistic materials have not been widely considered before. In this letter we try to incorporate a frequency dependent Coulomb interaction into the state-of-the-art ab initio electronic structure computing framework of local density approximation plus dynamical mean-field theory, and then choose SrVO3 as a prototype material to demonstrate the importance of dynamical screening effect. It is shown to renormalise the spectral weight near the Fermi level, to increase the effective mass, and to suppress th…
We find an unconventional nucleation of low temperature paramagnetic metal (PMM) phase with monoclinic structure from the matrix of high-temperature antiferromagnetic insulator (AFI) phase with tetragonal structure in strongly correlated electronic system $BaCo_{0.9}Ni_{0.1}S_{1.97}$. Such unconventional nucleation leads to a decease in resistivity by several orders with relaxation at a fixed temperature without external perturbation. The novel dynamical process could arise from the competition of strain fields, Coulomb interactions, magnetic correlations and disorders. Such competition may fr…
Dynamical screening of the Coulomb interactions in correlated electron systems results in a low-energy effective problem with a dynamical Hubbard interaction U(omega). We propose a Green's function ansatz for the Anderson impurity problem with retarded interactions, in which the Green's function factorizes into a contribution stemming from an effective static-U problem and a bosonic high-energy part introducing collective plasmon excitations. Our approach relies on the scale separation of the low-energy properties, related to the instantaneous static U, from the intermediate to high energy fea…
We recently introduced the dynamical cluster approximation(DCA), a new technique that includes short-ranged dynamical correlations in addition to the local dynamics of the dynamical mean field approximation while preserving causality. The technique is based on an iterative self-consistency scheme on a finite size periodic cluster. The dynamical mean field approximation (exact result) is obtained by taking the cluster to a single site (the thermodynamic limit). Here, we provide details of our method, explicitly show that it is causal, systematic, $Φ$-derivable, and that it becomes conserving as…
Dynamical Coherent-Potential Approximation (CPA) to correlated electrons has been extended to a system with realistic Hamiltonian which consists of the first-principles tight-binding Linear Muffintin Orbital (LMTO) bands and intraatomic Coulomb interactions. Thermodynamic potential and self-consistent equations for Green function are obtained on the basis of the functional integral method and the harmonic approximation which neglects the mode-mode couplings between the dynamical potentials with different frequency. Numerical calculations have been performed for Fe and Ni within the 2nd-order d…
We present results of ab initio theoretical investigations of the excitation spectra of correlated electrons in metals (Al, K, and Li) and their interplay with inelastic scattering experiments. We resolve various anomalies contained in the data, which were originally viewed as signatures of strong dynamical electronic correlations; we show that, instead, the anomalies are due to band-structure effects. The underlying theoretical framework in our density-response calculations is time-dependent density-functional theory; with this scheme we discuss the lifetime of the K plasmon, and the dynamica…
The description of realistic strongly correlated systems has recently advanced through the combination of density functional theory in the local density approximation (LDA) and dynamical mean field theory (DMFT). This LDA+DMFT method is able to treat both strongly correlated insulators and metals. Several interfaces between LDA and DMFT have been used, such as (N-th order) Linear Muffin Tin Orbitals or Maximally localized Wannier Functions. Such schemes are however either complex in use or additional simplifications are often performed (i.e., the atomic sphere approximation). We present an alt…
We investigate the potential of a quantum Boltzmann equation without momentum conservation for description of strongly correlated electron systems out of equilibrium. In a spirit similar to dynamical mean field theory (DMFT), the momentum conservation of the electron-electron scattering is neglected, which yields a time-dependent occupation function for the equilibrium spectral function, even in cases where well-defined quasiparticles do not exist. The main assumption of this method is that the spectral function remains sufficiently rigid under the non-equilibrium evolution. We compare the res…
A versatile method for combining density functional theory (DFT) in the local density approximation (LDA) with dynamical mean-field theory (DMFT) is presented. Starting from a general basis-independent formulation, we use Wannier functions as an interface between the two theories. These functions are used for the physical purpose of identifying the correlated orbitals in a specific material, and also for the more technical purpose of interfacing DMFT with different kinds of band-structure methods (with three different techniques being used in the present work). We explore and compare two disti…
We present a new method to compute the electronic structure of correlated materials combining the hybrid functional method with the dynamical mean-field theory. As a test example of the method we study cerium sesquioxide, a strongly correlated Mott-band insulator. The hybrid functional part improves the magnitude of the pd-band gap which is underestimated in the standard approximations to density functional theory while the dynamical mean-field theory part splits the 4f-electron spectra into a lower and an upper Hubbard band.
Ab-initio relativistic dynamical mean-field theory is applied to resolve the long-standing controversy between theory and experiment in the "simple" face-centered cubic phase of plutonium called delta-Pu. In agreement with experiment, neither static nor dynamical magnetic moments are predicted. In addition, the quasiparticle density of states reproduces not only the peak close to the Fermi level, which explains the large coefficient of electronic specific heat, but also main 5f features observed in photoelectron spectroscopy.
Unified treatment of local dynamical interactions in correlated metals using Eliashberg theory
University of Bremen（不来梅大学）；Université catholique de Louvain（鲁汶天主教大学）；WEL Research Institute（WEL研究院）；École Polytechnique Fédérale de Lausanne（洛桑联邦理工学院）；University of Cambridge（剑桥大学）；California Institute of Technology（加州理工学院）
The dynamical-mean-field method is applied to investigate the transport properties of heterostructures consisting of a strongly-correlated electron system connected to metallic leads. The spectral function inside the correlated region is sensitive to the change of the interaction strength and bias voltage. Because of this sensitivity, current vs voltage characteristics of such heterostructures are rather nonlinear regardless of the detail of the potential profile inside the correlated region. The electronic properties such as the double occupancy are also changed by the bias voltage.
Dynamical Hubbard approach to correlated materials: the case of transition-metal monoxides
École Polytechnique Fédérale de Lausanne（洛桑联邦理工学院）；California Institute of Technology（加州理工学院）；Colleege Champittet（尚皮泰学院）；PSI Center for Scientific Computing, Theory and Data（瑞士保罗谢勒研究所科学计算、理论与数据中心）
Recent progress in treating the dynamically screened nature of the Coulomb interaction in strongly correlated lattice models and materials is reviewed with a focus on computational schemes based on the dynamical mean field approximation. We discuss approximate and exact methods for the solution of impurity models with retarded interactions, and explain how these models appear as auxiliary problems in various extensions of the dynamical mean field formalism. The current state of the field is illustrated with results from recent applications of these schemes to U-V Hubbard models and correlated …
Fermi surface is at the heart of our understanding of metals and strongly correlated many-body systems. An abrupt change in the Fermi surface topology, also called Lifshitz transition, can lead to the emergence of fascinating phenomena like colossal magnetoresistance and superconductivity. While Lifshitz transitions have been demonstrated for a broad range of materials by equilibrium tuning of macroscopic parameters such as strain, doping, pressure and temperature, a non-equilibrium dynamical route toward ultrafast modification of the Fermi surface topology has not been experimentally demonstr…
We formulate real-space dynamical mean-field theory within scattering theory. Thereby the Friedel sum rule is derived for interacting lattice fermions at zero temperature.
The use of effective local Coulomb interactions that are dynamical, that is, frequency-dependent, is an efficient tool to describe the effect of long-range Coulomb interactions and screening thereof in solids. The dynamical character of the interaction introduces the coupling to screening degrees of freedom such as plasmons or particle-hole excitations into the many-body description. We summarize recent progress using these concepts, putting emphasis on dynamical mean field theory (DMFT) calculations with dynamical interactions ("doubly dynamical mean field theory"). We discuss the relation to…
We introduce an approach to treat localized correlated electronic states in the otherwise weakly correlated host medium. Here, the environment is dynamically downfolded on the correlated subspace. It is captured via renormalization of one and two quasiparticle interaction terms which are evaluated using many-body perturbation theory. We outline the strategy on how to take the dynamical effects into account by going beyond the static limit approximation. Further, we introduce an efficient stochastic implementation that enables treating the host environment with a large number of electrons at a …
Low-temperature transport in high-conductivity correlated metals: a density-functional plus dynamical mean-field study of cubic perovskites
Center for Computational Quantum Physics, Flatiron Institute（平顿研究所计算量子物理中心）；Department of Physics and Astronomy, Stony Brook University（石溪大学物理与天文学系）；Institute for Theoretical Physics, University of Cologne（科隆大学理论物理研究所）；Department of Physics, Massachusetts Institute of Technology（麻省理工学院物理系）；Center for Computational Mathematics, Flatiron Institute（平顿研究所计算数学中心）；Collège de France（法兰西公学院）
Within the ionic Hubbard model, electron correlations transmute the single-particle gap of a band insulator into a Mott gap in the strong correlation limit. However understanding the nature of possible phases in between these two extreme insulating phases remains an outstanding challenge. We find two strongly correlated insulating phases in between the above extremes: (i) The insulating phase just before the Mott phase can be viewed as gapping a non-Fermi liquid state of spinons through staggered ionic potential. The quasi-particles of underlying spinons are orthogonal to physical electrons an…
The self-energy-functional approach (SFA) is discussed in the context of different variational principles for strongly correlated electron systems. Formal analogies between static and dynamical variational approaches, different types of approximation strategies and the relations to density-functional and dynamical mean-field theory are emphasized. The discussion elucidates the strengths of the SFA in the construction of new non-perturbative approximations but also the limitations of the approach and thereby opens up future perspectives.
We use non-equilibrium dynamical mean-field theory to demonstrate the existence of a critical interaction in the real-time dynamics of the Hubbard model after an interaction quench. The critical point is characterized by fast thermalization and separates weak-coupling and strong-coupling regimes in which the relaxation is delayed due to prethermalization on intermediate timescales. This dynamical phase transition should be observable in experiments on trapped fermionic atoms.
We investigate the properties of the frustrated underdoped Hubbard model on the square lattice using two complementary approaches, the dynamical cluster extension of dynamical mean field theory, and variational Monte Carlo simulations of Gutzwiller-Jastrow wavefunctions with backflow corrections. We compare and discuss data for the energy and the double occupancies, as obtained from both approaches. At small dopings, we observe a rapid crossover from a weakly correlated metal at low interaction strength U to a non-Fermi liquid correlated state with strong local spin correlations. Furthermore, …
We present an embedding approach based on localized basis functions which permits an efficient application of the dynamical mean field theory (DMFT) to inhomogeneous correlated materials, such as semi-infinite surfaces and heterostructures. In this scheme, the semi-infinite substrate leads connected to both sides of the central region of interest are represented via complex, energy-dependent embedding potentials that incorporate one-electron as well as many-body effects within the substrates. As a result, the number of layers which must be treated explicitly in the layer-coupled DMFT equation …
The dynamical mean-field method is used to formulate a computationally tractable theory of electron-phonon interactions in systems with arbitrary local electron-electron interactions in the physically relevant adiabatic limit of phonon frequency small compared to electron bandwidth or interaction scale. As applications, the phonon contribution to the effective mass of a carrier in a lightly doped Mott insulator is determined and the phase separation boundary is discussed.
The most intriguing properties of emergent materials are typically consequences of highly correlated quantum states of their electronic degrees of freedom. Describing those materials from first principles remains a challenge for modern condensed matter theory. Here, we review, apply and discuss novel approaches to spectral properties of correlated electron materials, assessing current day predictive capabilities of electronic structure calculations. In particular, we focus on the recent Screened Exchange Dynamical Mean-Field Theory scheme and its relation to generalized Kohn-Sham theory. These…
The periodized cluster dynamical mean-field theory (PCDMFT) combined with exact diagonalization as impurity solver has been applied to the half-filled standard Hubbard model on the honeycomb lattice. A correlated Dirac semimetal is found for weak interactions and it transforms into an antiferromagnetic insulating phase for strong interactions via a first-order quantum phase transition, not intervened by a spin liquid phase in between. In this application, the PCDMFT introduces the partial translation symmetry, but cures well the problem due to the translation symmetry breaking in the cluster d…
We use a recently developed formalism (combining an adiabatic expansion and dynamical mean-field theory) to obtain expressions for isotope effects on electronic properties in correlated systems. As an example we calculate the isotope effect on electron effective mass for the Holstein model as a function of electron-phonon interaction strength and doping. Our systematic expansion generates diagrams neglected in previous studies, which turn out to give the dominant contributions. The isotope effect is small unless the system is near a lattice instability. We compare this to experiment.
A formalism is presented for treating strongly-correlated graphene quantum Hall states in terms of an SO(8) fermion dynamical symmetry that includes pairing as well as particle--hole generators. The graphene SO(8) algebra is isomorphic to an SO(8) algebra that has found broad application in nuclear physics, albeit with physically very different generators, and exhibits a strong formal similarity to SU(4) symmetries that have been proposed to describe high-temperature superconductors. The well-known SU(4) symmetry of quantum Hall ferromagnetism for single-layer graphene is recovered as one subg…
A recently developed dynamical mean-field theory in the iterated perturbation theory approximation was used as a basis for construction of the "first principles" calculation scheme for investigating electronic structure of strongly correlated electron systems. This scheme is based on Local Density Approximation (LDA) in the framework of the Linearized Muffin-Tin-Orbitals (LMTO) method. The classical example of the doped Mott-insulator La_{1-x}Sr_xTiO_3 was studied by the new method and the results showed qualitative improvement in agreement with experimental photoemission spectra.
In order to investigate photoinduced insulator-metal transitions observed in correlated electron systems, we propose a new theoretical method, where we combine a Floquet-matrix method for AC-driven systems with the dynamical mean-field theory. The method can treat nonequilibrium steady states exactly beyond the linear-response regime. We have applied the method to the Falicov-Kimball model coupled to AC electric fields, and numerically obtained the spectral function, the nonequilibrium distribution function and the current-voltage characteristic. The results show that intense AC fields indeed …
We present a generalized dynamical mean-field approach for the nonequilibrium physics of a strongly correlated system in the presence of a time-dependent external field. The Keldysh Green's function formalism is used to study the nonequilibrium problem. We derive a closed set of self-consistency equations in the case of a driving field with frequency Omega and wave vector q. We present numerical results for the local frequency-dependent Green's function and the self-energy for different values of the field amplitude in the case of a uniform external field using the iterated perturbation theory…
The interplay of disorder and interactions is a subject of perennial interest. In this work, we have investigated the effect of disorder due to chemical substitution on the dynamics and transport properties of correlated Fermi liquids. A low frequency analysis in the concentrated and dilute limits shows that the dynamical local potentials arising through disorder averaging generate a linear (in frequency) term in the scattering rate. Such non-Fermi liquid behaviour (nFL) is investigated in detail for Kondo hole substitution in heavy fermions within dynamical mean field theory. We find closed f…
The role of non-local Coulomb correlations in the honeycomb lattice is investigated within cluster dynamical mean field theory combined with finite-temperature exact diagonalization. The paramagnetic semi-metal to insulator transition is found to be in excellent agreement with finite-size determinantal Quantum Monte Carlo simulations and with cluster dynamical mean field calculations based on the continuous-time Quantum Monte Carlo approach. As expected, the critical Coulomb energy is much lower than within a local or single-site formulation. Short-range correlations are shown to give rise to …
We develop, clarify and test various aspects of cluster methods dynamical mean field methods using a soluble toy model as a benchmark. We find that the Cellular Dynamical Mean Field Theory (C-DMFT) converges very rapidly and compare its convergence properties with those of the Dynamical Cluster Approximation (DCA). We propose and test improved estimators for the lattice self energy within C-DMFT.
We compute the spin susceptibility of the two-dimensional Hubbard model away from half-filling, and analyze the impact of frequency dependent vertex corrections as obtained from the dynamical mean field theory (DMFT). We find that the local dynamics captured by the DMFT vertex strongly affects non-local spin correlations, and thus the momentum dependence of the spin susceptibility. While the widely used random phase approximation yields commensurate Néel-type antiferromagnetism as the dominant instability over a wide doping range, the vertex corrections favor incommensurate ordering wave vecto…
We study theoretically the simultaneous, photo-induced two-particle excitations of strongly correlated systems on the basis of the Hubbard model. Under certain conditions specified in this work, the corre- sponding transition probability is related to the two-particle spectral function which we calculate using three different methods: the dynamical-mean field theory combined with quantum Monte Carlo (DMFT- QMC) technique, the first order perturbation theory and the ladder approximations. The results are analyzed and compared for systems at the verge of the metal-insulator transitions. The depe…
We present an efficient method for incorporating the dynamical effects of the screening of the Hubbard U by electronic degrees of freedom in the solid into the single site dynamical mean field approximation. The formalism is illustrated by model system calculations which capture the essential features of the frequency dependent interactions proposed for Gd, Ni, SrVO_3 and other compounds. Screening leads to shifts in the metal-insulator phase boundary, changes in the spectral function near the Mott-Hubbard gap edge and to a renormalization of the quasiparticle weight. Hubbard bands are generic…
These are introductory lectures to some aspects of the physics of strongly correlated electron systems. I first explain the main reasons for strong correlations in several classes of materials. The basic principles of dynamical mean-field theory (DMFT) are then briefly reviewed. I emphasize the formal analogies with classical mean-field theory and density functional theory, through the construction of free-energy functionals of a local observable. I review the application of DMFT to the Mott transition, and compare to recent spectroscopy and transport experiments. The key role of the quasipart…
Dynamical Mean-Field Theory (DMFT) has opened new perspectives for the investigation of strongly correlated electron systems and greatly improved our understanding of correlation effects in models and materials. In contrast to Hartree-Fock-type approximations the mean field of DMFT is dynamical, whereby local quantum fluctuations are fully taken into account. DMFT becomes exact in the limit of high spatial dimensions or coordination number. Using DMFT the dynamics of correlated electron systems can be investigated non-perturbatively at all interaction strengths, electron densities and temperat…
We study the Hubbard model using the Cellular Dynamical Mean-Field Theory (CDMFT) with quantum Monte Carlo (QMC) simulations. We present the algorithmic details of CDMFT with the Hirsch-Fye QMC method for the solution of the self-consistently embedded quantum cluster problem. We use the one- and two-dimensional half-filled Hubbard model to gauge the performance of CDMFT+QMC particularly for small clusters by comparing with the exact results and also with other quantum cluster methods. We calculate single-particle Green's functions and self-energies on small clusters to study their size depende…
Single-band Hubbard model at criticality of the metal-insulator transition is studied using approximations derived from parquet theory. It is argued that only the electron-hole and interaction two-particle channels in the parquet algebra are relevant. A scheme is proposed how to reduce the parquet equations to a manageable form the complexity of which is comparable with single-channel approximations such as the renormalized RPA. The newly derived approximation, however, contains dynamical vertex corrections, remains self-consistent at the two-particle level and allows only for integrable singu…
We have designed a new multi-scale approach for Strongly Correlated Systems by combining the Dynamical Cluster Approximation (DCA) and the recently introduced dual-fermion formalism. This approach employs an exact mapping from a real lattice to a DCA cluster of linear size Lc embedded in a dual fermion lattice. Short-length-scale physics is addressed by the DCA cluster calculation, while longer-length-scale physics is addressed diagrammatically using dual fermions. The bare and dressed dual Fermionic Green functions scale as O(1/Lc) so perturbation theory on the dual lattice converges very qui…
Dynamical mean field theory is employed to calculate the properties of multilayered inhomogeneous devices composed of semi-infinite metallic lead layers coupled via barrier planes that are made from a strongly correlated material (and can be tuned through the metal-insulator Mott transition). We find that the Friedel oscillations in the metallic leads are immediately frozen in and don't change as the thickness of the barrier increases from one to eighty planes. We also identify a generalization of the Thouless energy that describes the crossover from tunneling to incoherent Ohmic transport in …
In this article we study the thermal response functions for two one-dimensional models, namely the Hubbard and spin-less fermion $t$-$V$ models. By exactly diagonalizing finite sized systems we calculate dynamical electrical, thermoelectrical, and thermal conductivities via the Kubo formalism. The thermopower (Seebeck coefficient), Lorenz number, and dimensionless figure of merit are then constructed which are quantities of great interest to the physics community both theoretically and experimentally. We also geometrically frustrate these systems and destroy integrability by the inclusion of a…
We present a quantum embedding methodology to resolve the Anderson impurity model in the context of dynamical mean-field theory, based on an extended exact diagonalization method. Our method provides a maximally localized quantum impurity model, where the non-local components of the correlation potential remain minimal. This method comes at a large benefit, as the environment used in the quantum embedding approach is described by propagating correlated electrons and hence offers a polynomial increase $O(N^4)$ of the number of degrees of freedom for the embedding mapping without adding bath sit…
We study Friedel oscillations and screening effects of the impurity potential in the Hubbard model. Electronic correlations are accounted for by solving the real-space dynamical mean-field theory equations using the continuous time quantum Monte-Carlo simulations at finite temperatures and using a homogeneous self-energy approximation with the numerical renormalization group at zero temperature. We find that in the Fermi liquid phase both the amplitudes of Friedel oscillations and the screening charge decrease with increasing the interaction and follow the behavior of the Fermi liquid renormal…
We address the steady-state behavior of a system consisting of several correlated monoatomic layers sandwiched between two metallic leads under the influence of a bias voltage. In particular, we investigate the effect of the local Hubbard and of the long-range Coulomb interactions on the charge redistribution at the interface. We provide a detailed study of the importance of the various system parameters, like Hubbard $U$, lead-correlated region coupling strength, and the applied voltage on the charge distribution in the correlated region and in the adjacent parts of the leads. Our results are…
A general approach for the description of correlated hopping in infinite dimensions, which is based on an expansion over electron hopping around the atomic limit, is developed. Such an approach keeps the dynamical mean-field theory local ideology and allows one to calculate the thermodynamical functions. A grand-canonical potential functional and a $Φ$-derivatible theory that does not introduce the self-energy is proposed. As limiting cases the Falicov--Kimball model with correlated hopping and the model with broken bonds ("diluted" conductor) are investigated, and the connection with the Blac…
We present a fully self-consistent combined GW and dynamical mean field (GW+DMFT) study of the spectral properties of the extended two-dimensional Hubbard model. The inclusion of the local dynamical vertex stemming from the DMFT self-energy and polarization is shown to cure the problems of self-consistent GW in the description of spectral properties. We calculate the momentum-resolved spectral functions, the two-particle polarization and electron loss spectra, and show that the inclusion of GW in extended DMFT leads to a narrowing of the quasi-particle width and more pronounced Hubbard bands i…
