Dynamical Mean-field Theory Study Research Articles

Single-site DFT+DMFT for vanadium dioxide using bond-centered orbitals

We present a combined density-functional theory and single-site dynamical mean-field theory (DMFT) study of vanadium dioxide (VO2) using an unconventional set of bond-centered orbitals as the basis of the correlated subspace. VO2 is a prototypical material undergoing a metal-insulator transition (MIT), hosting both intriguing physical phenomena and the potential for industrial applications. With our choice of correlated subspace basis, we investigate the interplay of structural dimerization and electronic correlations in VO2 in a computationally cheaper way compared to other state-of-the-art methods, such as cluster DMFT. Our approach allows us to treat the rutile and M1 monoclinic VO2 phases on an equal footing and to vary the dimerizing distortion continuously, exploring the energetics of the transition between the two phases. The choice of basis presented in this work hence offers a complementary view on the long-standing discussion of the MIT in VO2 and suggests possible future extensions to other similar materials hosting molecular-orbital-like states. Published by the American Physical Society 2024

Dynamical mean-field theory study of a ferromagnetic CrI3 monolayer

We have employed one of the well-known many-body techniques, density functional theory plus dynamical mean-field theory (DFT + DMFT), to investigate the electronic structure of ferromagnetic monolayer CrI3 as a function of temperature and hole-doping concentration. The computed magnetic susceptibility follows the Curie's law, indicating that the ferromagnetism of monolayer CrI3 originates from localized magnetic moments of Cr atoms rather than Stoner-type itinerant ones. The DFT + DMFT calculations show a different coherent temperature for each spin component, demonstrating apparent strong spin-dependent electronic correlation effects in monolayer CrI3. Furthermore, we have explored the doping-dependent electronic structure of monolayer CrI3 and found that its electronic and magnetic properties are easily tunable by the hole-doping.

Correlated electronic structure of a quintuple-layer nickelate

We present a comparative density-functional theory plus dynamical mean-field theory study of the two known superconducting members of the rare-earth $(R)$ layered nickelate family: hole-doped ${R\text{NiO}}_{2}$ $(n=\ensuremath{\infty})$ and ${R}_{6}{\mathrm{Ni}}_{5}{\mathrm{O}}_{12}$ $(n=5)$. At the same nominal carrier concentration, these two materials exhibit nearly identical electronic structures and many-body correlation effects: mass enhancements, self-energies, and occupations. However, the fermiology of the quintuple-layer nickelate is more two-dimensional-like than its infinite-layer counterpart, making this new superconducting quintuple-layer nickelate more cupratelike without the need for chemical doping.

Electronic structure of CeIr[formula omitted] superconductor: DMFT studies

We present the band structure of CeIr3 superconductor calculated within the dynamical mean field theory (DMFT). Standard GGA and GGA+U methods fail to reproduce the experimental electronic specific heat coefficient γexpt. due to the underestimated density of states at the Fermi level N(EF) followed by an overestimated strength of electron–phonon coupling (EPC) calculated as a renormalization of γexpt.. The DMFT study shows a strong hybridization of 4f states of Ce with 5d-states of Ir, which leads to the larger N(EF) giving the correct γexpt. with a moderate EPC in agreement with the experimental data.

Efficient Slave-Boson Approach for Multiorbital Two-Particle Response Functions and Superconductivity

We develop an efficient approach for computing two-particle response functions and interaction vertices for multiorbital strongly correlated systems based on fluctuation around rotationally-invariant slave-boson saddle-point. The method is applied to the degenerate three-orbital Hubbard-Kanamori model for investigating the origin of the s-wave orbital antisymmetric spin-triplet superconductivity in the Hund's metal regime, previously found in the dynamical mean-field theory studies. By computing the pairing interaction considering the particle-particle and the particle-hole scattering channels, we identify the mechanism leading to the pairing instability around Hund's metal crossover arises from the particle-particle channel, containing the local electron pair fluctuation between different particle-number sectors of the atomic Hilbert space. On the other hand, the particle-hole spin fluctuations induce the s-wave pairing instability before entering the Hund's regime. Our approach paves the way for investigating the pairing mechanism in realistic correlated materials.

Real-space dynamical mean field theory study of non-Hermitian skin effect for correlated systems: Analysis based on pseudospectrum

We analyze a correlated system in equilibrium with special emphasis on non-Hermitian topology inducing a skin effect. The pseudospectrum, computed by the real-space dynamical mean field theory, elucidates that additional pseudoeigenstates emerge for the open boundary condition in contrast to the dependence of the density of states on the boundary condition. We further discuss how the line-gap topology, another type of non-Hermitian topology, affects the pseudospectrum. Our numerical simulation clarifies that while the damping of the quasiparticles induces the nontrivial point-gap topology, it destroys the nontrivial line-gap topology. The above two effects are also reflected in the temperature dependence of the local pseudospectral weight.

Topological Mott transition in a Weyl-Hubbard model: Dynamical mean-field theory study

Weyl semimetals are three-dimensional, topologically protected, gapless phases which show exotic phenomena such as Fermi arc surface states or negative magnetoresistance. It is an open question whether interparticle interactions can turn the topological semimetal into a topologically nontrivial Mott insulating phase. We investigate an experimentally motivated model for Weyl physics of cold atoms in optical lattices, with the main focus on interaction effects and topological properties by means of dynamical mean-field theory (DMFT). We characterize topological phases by numerically evaluating the Chern number via the Ishsikawa-Matsuyama formula for interacting phases. Within our studies, we find that the Chern numbers become trivial when interactions lead to insulating behavior. For a deeper understanding of the Weyl-semimetal-to-Mott-insulator topological phase transition, we evaluate the topological properties of quasiparticle bands as well as so-called blind bands. Our study is complementary to recent studies of Weyl semimetals with DMFT.

Engineering Si doping in anatase and rutile TiO2 with oxygen vacancy for efficient optical application

In this paper, I demonstrate a density functional theory plus dynamical mean field theory study on the electronic properties of doped TiO2 rutile as well as another tetragonal phase anatase with oxygen vacancy. The density of states and optical properties have been obtained from the electronic structure applying screened hybrid exchange correlation density functionals. All the single-particle excitations are treated within the dynamical mean field theory for independent quasiparticles. For optical properties, excitations are considered by solving the Bethe-Salpeter equation for Coulomb correlated electron-hole duo. On this theoretical basis, band structure and optical spectra for the two structures of TiO2 are provided. Further, I compared the present results with earlier optical data of parent structure and established the increased optical efficiency in doped TiO2 with oxygen vacancy in both the structure.

Characterizing the Non-equilibrium Dynamics of Field-Driven Correlated Quantum Systems

Recent experimental advances in ultrafast phenomena have triggered renewed interest in the dynamics of correlated quantum systems away from equilibrium. We review nonequilibrium dynamical mean-field theory studies of both the transient and the steady states of a DC field-driven correlated quantum system. In particular, we focus on the nonequilibrium behavior and how it relates to the fluctuation-dissipation theorem. The fluctuation-dissipation theorem emerges as an indicator for how the system thermalizes and for how it reaches a steady state. When the system thermalizes in an infinite temperature steady state it can pass through a succession of quasi-thermal states that approximately obey the fluctuation-dissipation theorem. We also discuss the Wigner distribution and what its evolution tells us about the nonequilibrium many-body problem.

Loop currents in ladder cuprates: A dynamical mean field theory study

We investigate the possibility of spontaneous loop currents in the two-leg ladder cuprate Sr$_{14-x}$Ca$_x$Cu$_{24}$O$_{41}$ by applying cluster dynamical mean field theory (CDMFT) to a seven-band Hubbard model for that compound, with an exact diagonalization solver. We sample several values of the local interaction $U_d$ and of the Cu-O energy difference $E_{pd}$, by applying an external field that induces loop currents. We find no instance of spontaneous loop currents once the external field is brought to zero.

Robustness of the topological quantization of the Hall conductivity for correlated lattice electrons at finite temperatures

Electrons on a two-dimensional (2$d$) lattice which is exposed to a strong uniform magnetic field show intriguing physical phenomena. The spectrum of such systems exhibits a complex (multi-)band structure known as Hofstadter's butterfly. For fillings at which the system is a band insulator one observes a quantized integer-valued Hall conductivity $\sigma_{xy}$ corresponding to a topological invariant, the first Chern number $\mathcal{C}_1$. This is robust against many-body interactions as long as no changes in the gap structure occur. Strictly speaking, this stability holds only at zero temperatures $T$ while for $T>0$ correlation effects have to be taken into account. In this work, we address this question by presenting a dynamical mean field theory (DMFT) study of the Hubbard model in a uniform magnetic field. The inclusion of local correlations at finite temperature leads to (i) a shrinking of the integer plateaus of $\sigma_{xy}$ as a function of the chemical potential and (ii) eventually to a deviation from these integer values. We demonstrate that these effects can be related to a correlation-driven narrowing and filling of the band gap, respectively.

Dynamical effects on superconductivity in a BCS-BEC crossover: Dynamical mean field theory and numerical renormalization group study of the Holstein model in infinite dimensions

We investigate the dynamical effects of pairing interaction on superconductivity in BCS-BEC crossover by studying the Holstein model at half-filling where the electron-phonon coupling $g$ controls the crossover. The dynamical mean-field theory was employed in combination with the numerical renormalization group technique. The dynamical effects induce distinct features such as absenceof the dispersion back-bending of Bogoliubov quasi-particles, non-monotonous coupling dependence of the pairing gap, and the soft phonon spectrum due to the Goldstone mode of local pair phase fluctuations. Also interesting is the maximum critical temperature being at the normal state phase boundary. Some of these features have intriguing similarities with the recent observations in the FeSe$_{1-x}$S$_x$ and Fe$_{1+y}$Se$_x$Te$_{1-x}$ iron-chalcogenides in the BCS-BEC crossover.

Finite-temperature phase diagram of (111) nickelate bilayers

We report a density functional theory plus dynamical mean field theory (DFT+DMFT) study of an oxide heterostructure of LaNiO$_3$ (LNO) bilayers in [111] direction interleaved with four atomic monolayers of LaAlO$_3$. DFT+$U$ optimizations yield two stable solutions: a uniform structure with equivalent NiO$_6$ octahedra, as well as a bond-disproportionated (BD) structure featuring a breathing distortion. For both structures, we construct the low-energy models describing the Ni $e_g$ states by means of Wannier projections supplemented by the Kanamori interaction, and solve them by DMFT. Using the continuous-time quantum Monte Carlo algorithm in the hybridization expansion, we study the temperature range between 145 and 450 K. For the uniform and the BD structure, we find similar phase diagrams that comprise four phases: a ferromagnetic metal (FM), a paramagnetic metal (PM), an antiferro-orbitally-ordered insulator (AOI), as well as a paramagnetic insulator (PI). By calculating momentum-resolved spectral functions on a torus and a cylinder, we demonstrate that the FM phase is not a Dirac metal, while both insulating phases are topologically trivial. By a comparison with available experimental data and model DMFT studies for the two-orbital Hubbard model, we suggest that LNO bilayers are in the AOI phase at room temperature.

Magnetic exchange and susceptibilities in fcc iron: A supercell dynamical mean-field theory study

We study the momentum- and temperature dependencies of magnetic susceptibilities and magnetic exchange in paramagnetic fcc iron by a combination of density functional theory and supercell dynamical mean-field theory (DFT+DMFT). We find that in agreement with experimental results the antiferromagnetic correlations with the wave vector close to $(0,0,2\pi)$ dominate at low temperatures (as was also obtained previously theoretically), while the antiferromagnetic and ferromagnetic correlations closely compete at the temperatures $T\sim 1000$ K, where $\gamma$-iron exists in nature. Inverse staggered susceptibility has linear temperature dependence at low temperatures, with negative Weiss temperature $\theta_{\rm stagg} \approx -340$ K; the inverse local susceptibility is also linear at not too low temperatures, showing well formed local moments. Analysis of magnetic exchange shows that the dominant contribution comes from first two coordination spheres. In agreement with the analysis of the susceptibility, the nearest-neighbor exchange is found to be antiferromagnetic at low temperatures, while at temperature of the $\alpha$-$\gamma$ structural phase transition its absolute value becomes small, and the system appears on the boundary between the regimes with strongest antiferro- and ferromagnetic correlations.

Phase competition in a one-dimensional three-orbital Hubbard-Holstein model

We study the interplay between the electron-phonon (e-ph) and on-site electron-electron (e-e) interactions in a three-orbital Hubbard-Holstein model on an extended one-dimensional lattice using determinant quantum Monte Carlo. For weak e-e and e-ph interactions, we observe a competition between an orbital-selective Mott phase (OSMP) and a (multicomponent) charge-density-wave (CDW) insulating phase, with an intermediate metallic phase located between them. For large e-e and e-ph couplings, the OSMP and CDW phases persist, while the metallic phase develops short-range orbital correlations and becomes insulating when both the e-e and e-ph interactions are large but comparable. Many of our conclusions are in line with those drawn from a prior dynamical mean field theory study of the two-orbital Hubbard-Holstein model [Phys. Rev. B 95, 12112(R) (2017)] in infinite dimension, suggesting that the competition between the e-ph and e-e interactions in multiorbital Hubbard-Holstein models leads to rich physics, regardless of the dimension of the system.

Doublon-Holon Origin of the Subpeaks at the Hubbard Band Edges.

Dynamical mean-field theory (DMFT) studies frequently observe a fine structure in the local spectral function of the SU(2) Fermi-Hubbard model at half filling: In the metallic phase close to the Mott transition, subpeaks emerge at the inner edges of the Hubbard bands. Here we demonstrate that these subpeaks originate from the low-energy effective interaction of doublon-holon pairs, by investigating how the correlation functions of doublon and holon operators contribute to the subpeaks. A mean-field analysis of the low-energy effective Hamiltonian provides results consistent with our DMFT calculation using the numerical renormalization group as an impurity solver. In the SU(3) and SU(4) Hubbard models, the subpeaks become more pronounced due to the increased degeneracy of doublon-holon pair excitations.

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.

Spectral functions of a time-periodically driven Falicov-Kimball model: Real-space Floquet dynamical mean-field theory study

We present a systematic study of spectral functions of a time-periodically driven Falicov-Kimball Hamiltonian. In the high-frequency limit, this system can be effectively described as a Harper-Hofstadter-Falicov-Kimball model. Using real-space Floquet dynamical mean-field theory (DMFT), we take into account interaction effects and contributions from higher Floquet bands in a non-perturbative way. Our calculations show a high degree of similarity between the interacting driven system and its effective static counterpart with respect to spectral properties. However, as also illustrated by our results, one should bear in mind that Floquet DMFT describes a non-equilibrium steady state (NESS), while an effective static Hamiltonian describes an equilibrium state. We further demonstrate the possibility of using real-space Floquet DMFT to study edge states on a cylinder geometry.

Spin-orbit coupling in three-orbital Kanamori impurity model and its relevance for transition-metal oxides

We investigate the effects of the spin-orbit coupling (SOC) in a three-orbital impurity model with Kanamori interaction using the numerical renormalization group method. We focus on the impurity occupancy $N_d=2$ relevant to the dynamical mean-field theory studies of Hund's metals. Depending on the strength of SOC $\lambda$ we identify three regimes: usual Hund's impurity for $|\lambda|<\lambda_c$, van-Vleck non-magnetic impurity for $\lambda > \lambda_c$, and a $J=2$ impurity for $\lambda < -\lambda_c$. They all correspond to a Fermi liquid but with very different quasiparticle phase shifts and different physical properties. The crossover between these regimes is controlled by an emergent scale, the orbital Kondo temperature, $\lambda_c =T_K^\mathrm{orb}$ that drops with increasing interaction strength. This implies that oxides with strong electronic correlations are more prone to the effects of the spin-orbit coupling.

Selective orbital reconstruction in tetragonal FeS: A density functional dynamical mean-field theory study

Transport properties of tetragonal iron monosulfide, mackinawite, show a range of complex features. Semiconductive behavior and proximity to metallic states with nodal superconductivity mark this d-band system as unconventional quantum material. Here, we use the density functional dynamical mean-field theory (DFDMFT) scheme to comprehensively explain why tetragonal FeS shows both semiconducting and metallic responses in contrast to tetragonal FeSe which is a pseudogaped metal above the superconducting transition temperature. Within local-density-approximation plus dynamical mean-field theory (LDA+DMFT) we characterize its paramagnetic insulating and metallic phases, showing the proximity of mackinawite to selective Mott localization. We report the coexistence of pseudogaped and anisotropic Dirac-like electronic dispersion at the border of the Mott transition. These findings announce a new understanding of many-particle physics in quantum materials with coexisting Dirac-fermions and pseudogaped electronic states at low energies. Based on our results we propose that in electron-doped FeS substantial changes would be seen when the metallic regime was tuned towards an electronic state that hosts unconventional superconductivity.