First principles constrained density functional theory scheme in Wannier functions formalism has been used to calculate Coulomb repulsion U and Hund's exchange J parameters for iron 3d electrons in LaFeAsO. Results strongly depend on the basis set used in calculations: when O-2p, As-4p, and Fe-3d orbitals and corresponding bands are included, computation results in U=3-4 eV, however, with the basis set restricted to Fe-3d orbitals and bands only, computation gives parameters corresponding to F^0=0.8 eV, J=0.5 eV. LDA+DMFT (the Local Density Approximation combined with the Dynamical Mean-Field Theory) calculation with this parameters results in weakly correlated electronic structure that is in agreement with X-ray experimental spectra.
LDA+DMFT (Local Density Approximation combined with Dynamical Mean-Field Theory) computation scheme has been used to calculate spectral properties of LaFeAsO -- the parent compound for new high-T$_c$ iron oxypnictides. Coulomb repulsion $U$ and Hund's exchange $J$ parameters for iron 3d electrons were calculated using \textit {first principles} constrained density functional theory scheme in Wannier functions formalism. Resulting values strongly depend on the number of states taken into account in calculations: when full set of O-$2p$, As-$4p$, and Fe-3d orbitals with corresponding bands are i…
To understand the recently established unique magnetic and superconducting phase diagram of LaFeAsO$_{1-x}$H$_x$, we analyze the realistic multiorbital tight-binding model for $x=0 \sim 0.4$ beyond the rigid band approximation. Both the spin and orbital susceptibilities are calculated in the presence of the Coulomb and charge quadrupole interactions. It is found that both orbital and spin fluctuations strongly develop at both $x \sim 0$ and 0.4, due to the strong violation of the rigid band picture in LaFeAsO$_{1-x}$H$_x$. Based on this result, we discuss the experimental phase diagram, especi…
Effective Hamiltonians for LaFeAsO and LaFePO are derived from the downfolding scheme based on first-principles calculations and provide insights for newly discovered superconductivity in the family of LnFeAsO$_{1-x}$F$_x$, Ln = La, Ce, Pr, Nd, Sm, and Gd. Extended Hubbard Hamiltonians for five maximally localized Wannier orbitals per Fe are constructed dominantly from five-fold degenerate iron-3$d$ bands. They contain parameters for effective Coulomb and exchange interactions screened by the polarization of other electrons away from the Fermi level. The onsite Coulomb interaction estimated as…
We investigate the evolution of magnetic properties as a function of hydrogen doping in iron based superconductor LaFeAsO$_{1-x}$H$_x$ using the dynamical mean-field theory combined with the density-functional theory. We find that two independent consequences of the doping, the increase of the electron occupation and the structural modification, have the opposite effects on the strength of electron correlation and magnetism, resulting in the minimum of the calculated magnetic moment around the intermediate doping level as a function of $x$. Our result provides a natural explanation for the puz…
We present an approach that combines the local density approximation (LDA) and the dynamical mean-field theory (DMFT) in the framework of the full-potential linear augmented plane waves (FLAPW) method. Wannier-like functions for the correlated shell are constructed by projecting local orbitals onto a set of Bloch eigenstates located within a certain energy window. The screened Coulomb interaction and Hund's coupling are calculated from a first-principle constrained RPA scheme. We apply this LDA+DMFT implementation, in conjunction with continuous-time quantum Monte-Carlo, to study the electroni…
The role of Coulomb correlations in the iron pnictide LaFeAsO is studied by generalizing exact diagonalization dynamical mean field theory to five orbitals. For rotationally invariant Hund's rule coupling a continuous transition from a paramagnetic Fermi-liquid phase to a non-Fermi-liquid metallic phase exhibiting frozen moments is found at moderate Coulomb energies. For Ising-like exchange, this transition is first order and occurs at a lower critical Coulomb energy. The correlation-induced scattering rate as a function of doping relative to half-filling, i.e., delta = n/5-1, where n=6 for th…
We estimate theoretically the strength of the local Coulomb interaction for the Fe 3d and Ce 4f shells in the REFeAsO compunds. In LaFeAsO and CeFeAsO we obtain values of the local Coulomb interaction parameter U for both Fe and Ce which are larger than those of elemental Fe and Ce metals. The Fe 3d bandwidth of REFeAsO is found to increase slightly as one moves along the RE-series. Using a combined local density approximation and dynamical mean-field theory (LDA+DMFT) approach, we study the behaviour of the localized 4f states along the rare-earth oxyarsenides REFeAsO series (RE=Ce,Pr,Nd). In…
Orbital polarization and electronic correlation are two essential aspects in understanding the normal state and superconducting properties of multiorbital FeAs-based superconductors. In this Letter, we present a systematical study on the orbital polarization of iron pnictides from weak to strong Coulomb correlations within the KRSB approach. The magnetic phase diagram of the two-orbital model for LaFeAsO clearly shows that the striped antiferromagnetic metallic phase with considerable orbital polarization exists over a wide doping range. The reversal of the orbital polarization occurs in the i…
LDA+DMFT (Local Density Approximation combined with Dynamical Mean-Field Theory) computation scheme has been used to calculate spectral properties of LaFeAsO -- the parent compound of the new high-T_c iron oxypnictides. The average Coulomb repulsion U=3-4 eV and Hund's exchange J=0.8 eV parameters for iron 3d electrons were calculated using the first principles constrained density functional theory scheme in the Wannier functions formalism. DMFT calculations using these parameters result in moderately correlated electronic structure with effective electron mass enhancement m^*~2 that is in agr…
Deviations of low-energy electronic structure of iron-based superconductors from density functional theory predictions have been parametrized in terms of band- and orbital-dependent mass renormalizations and energy shifts. The former have typically been described in terms of a local self-energy within the framework of dynamical mean field theory, while the latter appears to require non-local effects due to interband scattering. By calculating the renormalized bandstructure in both random phase approximation (RPA) and the two-particle self-consistent approximation (TPSC), we show that correlati…
We study optimally doped Bi$_{2}$Sr$_{2}$Ca$_{0.92}$Y$_{0.08}$Cu$_{2}$O$_{8+δ}$ (Bi2212) using angle-resolved two-photon photoemission spectroscopy. Three spectral features are resolved near 1.5, 2.7, and 3.6 eV above the Fermi level. By tuning the photon energy, we determine that the 2.7-eV feature arises predominantly from unoccupied states. The 1.5- and 3.6-eV features reflect unoccupied states whose spectral intensities are strongly modulated by the corresponding occupied states. These unoccupied states are consistent with the prediction from a cluster perturbation theory based on the sing…
To obtain an effective many-body model of graphene and related materials from first principles we calculate the partially screened frequency dependent Coulomb interaction. In graphene, the effective on-site (Hubbard) interaction is U_00 = 9.3 eV in close vicinity to the critical value separating conducting graphene from an insulating phase emphasizing the importance of non-local Coulomb terms. The nearest-neighbor Coulomb interaction strength is computed to U_01 = 5.5 eV. In the long wavelength limit, we find the effective background dielectric constant of graphite to be ε= 2.5 in very good ag…
The one-band extended Hubbard model in two dimensions near band-filling 1/2 is solved in the fluctuation exchange approximation, including the long-range (1/r) part of the Coulomb interaction, up to 4th neighbor distance. Our results suggest that d_(x^2 - y^2) pairing in the Hubbard model is robust against the inclusion of long-range Coulomb interactions with moderate 1st neighbor repulsion strength V_1. d_(x^2 - y^2) pairing is suppressed only at large V_1 (>~ 0.25U-0.4U), due to incipient charge density wave instabilities.
We study analytically and numerically dynamics and eigenstates of two electrons with Coulomb repulsion on a tight-binding lattice in one and two dimensions. The total energy and momentum of electrons are conserved and we show that for a certain momentum range the dynamics is exactly reduced to an evolution in an effective narrow energy band where the energy conservation forces the two electrons to propagate together through the whole system at moderate or even weak repulsion strength. We argue that such a mechanism of electron pair formation by the repulsive Coulomb interaction is rather gener…
The structural flexibility at three substitution sites in LaFeAsO enabled investigation of the relation between superconductivity and structural parameters over a wide range of crystal compositions. Substitutions of Nd for La, Sb or P for As, and F or H for O were performed. All these substitutions modify the local structural parameters, while the F/H-substitution also changes band filling. It was found that the superconducting transition temperature $T_{c}$ is strongly affected by the pnictogen height $h_{Pn}$ from the Fe-plane that controls the electron correlation strength and the size of t…
The ability to control the strength of interaction is essential for studying quantum phenomena emerging from a system of correlated fermions. For example, the isotope effect illustrates the effect of electron-phonon coupling on superconductivity, providing an important experimental support for the BCS theory. In this work, we report a new device geometry where the magic-angle twisted bilayer graphene (tBLG) is placed in close proximity to a Bernal bilayer graphene (BLG) separated by a 3 nm thick barrier. Using charge screening from the Bernal bilayer, the strength of electron-electron Coulomb …
We calculate the strength of the effective onsite Coulomb interaction (Hubbard $U$) in two-dimensional (2D) transition-metal (TM) dihalides MX$_2$ and trihalides MX$_3$ (M=Ti, V, Cr, Mn, Fe, Co, Ni; X=Cl, Br, I) from first principles using the constrained random-phase approximation. The correlated subspaces are formed from $t_{2g}$ or $e_g$ bands at the Fermi energy. Elimination of the efficient screening taking place in these narrow bands gives rise to sizable interaction parameters U between the localized $t_{2g}$ ($e_g$) electrons. Due to this large Coulomb interaction, we find $U/W >1$ (wi…
The effective on-site Coulomb interaction (Hubbard $U$) between localized electrons at crystal surfaces is expected to be enhanced due to the reduced coordination number and reduced subsequent screening. By means of first principles calculations employing the constrained random-phase approximation (cRPA) we show that this is indeed the case for simple metals and insulators but not necessarily for transition metals and insulators that exhibit pronounced surface states. In the latter case, the screening contribution from surface states as well as the influence of the band narrowing increases the…
We calculate the strength of the frequency-dependent on-site electronic interactions in the iron pnictides LaFeAsO, BaFe2As2, BaRu2As2, and LiFeAs and the chalcogenide FeSe from first principles within the constrained random phase approximation. We discuss the accuracy of an atomic-like parametrization of the two-index density-density interaction matrices based on the calculation of an optimal set of three independent Slater integrals, assuming that the angular part of the Fe-d localized orbitals can be described within spherical harmonics as for isolated Fe atoms. We show that its quality dep…
Self-Consistent Coulomb Interactions from Constrained Dynamical Mean-Field Theory
Department of Physics and Astronomy, West Virginia University（西弗吉尼亚大学物理与天文系）；Center for Materials Theory and Department of Physics and Astronomy, Rutgers University（罗格斯大学材料理论中心及物理与天文系）
Taking into account the interplay between the disorder and Coulomb interaction, the phase diagram of three-dimensional anisotropic Weyl semimetal is studied by renormalization group theory. Weak disorder is irrelevant in anisotropic Weyl semimetal, while the disorder becomes relevant and drives a quantum phase transition from semimetal to compressible diffusive metal phases if the disorder strength is larger than a critical value. The long-range Coulomb interaction is irrelevant in clean anisotropic Weyl semimetal. However, interestingly, we find that the long-range Coulomb interaction exerts …
We study the consequences of Coulomb interactions on a system undergoing a putative first order phase transition. In two dimensions (2D), near the critical density, the system is universally unstable to the formation of new intermediate phases, which we call ``electronic microemulsion phases,'' which consist of an intermediate scale mixture of regions of the two competing phases. A correlary is that there can be no direct transition as a function of density from a 2D Wigner crystal to a uniform electron liquid. In 3D, %we find that if the strength of the Coulomb interactions exceeds a critical…
We present first-principle calculation of the on-site and nearest neighbor Coulomb interaction strength of the Ni $d$ orbitals in bulk $LaNiO_{2}$, using the constrained Random Phase Approximation method. The nearest neighbor correlation within Ni-O plane turns out to be more significant when considering the frequency dependent $U(ω)$, which can be as strong as about 25\% of the on-site value at medium and high frequencies. The inter Ni-O plane nearest neighbor correlation is found to be the same strength as that within the Ni-O plane, indicating the material is non-locally correlated also bet…
We use a density-functional theoretical approach to set up a computationally simple self-consistent scheme to calculate the pair distribution functions and the effective interactions in quantum Coulomb liquids. We demonstrate the accuracy of the approach for different statistics and space dimensionalities by reporting results for a two-dimensional electron gas and for a three-dimensional boson plasma over physically relevant ranges of coupling strength, in comparison with Monte Carlo data.
The electronic properties of single-layer antimony are studied by a combination of first-principles and tight-binding methods. The band structure obtained from relativistic density functional theory is used to derive an analytic tight-binding model that offers an efficient and accurate description of single-particle electronic states in a wide spectral region up to the mid-UV. The strong ($λ=0.34$ eV) intra-atomic spin-orbit interaction plays a fundamental role in the band structure, leading to splitting of the valence band edge and to a significant reduction of the effective mass of the hole …
We apply a molecular dynamics scheme to analyze classically chaotic properties of a two-dimensional circular billiard system containing two Coulomb-interacting electrons. As such, the system resembles a prototype model for a semiconductor quantum dot. The interaction strength is varied from the noninteracting limit with zero potential energy up to the strongly interacting regime where the relative kinetic energy approaches zero. At weak interactions the bouncing maps show jumps between quasi-regular orbits. In the strong-interaction limit we find an analytic expression for the bouncing map. It…
The effective on-site Coulomb interaction (Hubbard $U$) between localized \textit{d} electrons in 3\textit{d}, 4\textit{d}, and 5\textit{d} transition metals is calculated employing a new parameter-free realization of the constrained random-phase approximation using Wannier functions within the full-potential linearized augmented-plane-wave method. The $U$ values lie between 1.5 and 5.7 eV and depend on the crystal structure, spin polarization, \textit{d} electron number, and \textit{d} orbital filling. On the basis of the calculated $U$ parameters, we discuss the strength of the electronic co…
Above the Kondo temperature, the Kohn-Sham zero-bias conductance of an Anderson junction has been shown to completely miss the Coulomb blockade. Within a standard model for the spectral function, we deduce a parameterization for both the onsite exchange-correlation potential and the bias drop as a function of the site occupation that applies for all correlation strengths. We use our results to sow doubt on the common interpretation of such corrections as arising from dynamical exchange-correlation contributions.
We present a systematic study clarifying an electronic correlation trend of electrides from first principles. By using the maximally localized Wannier function and the constrained random phase approximation, we calculated the electronic correlation strength $(U-U_{nn})/|t|$ of 19 inorganic electrides, where $U$, $U_{nn}$, and $t$ are the effective onsite Coulomb repulsion, nearest-neighbor Coulomb repulsion, and the nearest-neighbor transfer integrals, respectively. The electronic correlation was found to be highly correlated with the dimensionality of the Wannier-function network of anionic e…
We present results on spin and charge correlations in two-dimensional quantum dots as a function of increasing Coulomb strength (dielectric constant). We look specifically at the orbital occupation of both spin and charge. We find that charge and spin evolve separately, especially at low Coulomb strength. For the charge, we find that a hole develops in the core orbitals at strong Coulomb repulsion, invalidating the common segregation of confined electrons into an inert core and active valence electrons. For excitations, we find a total spin-projection $S_z = -1/2$ breaks apart into separate oc…
We study the interaction driven localization transition, which a recent experiment in Ga_{1-x}Mn_xAs As has shown to come along with multifractal behavior of the local density of states (LDoS) and the intriguing persistence of critical correlations close to the Fermi level. We show that the bulk of these phenomena can be understood within a Hartree-Fock treatment of disordered, Coulomb-interacting spinless fermions. A scaling analysis of the LDoS correlation demonstrates multifractality with correlation dimension d_2=1.57, which is significantly larger than at a non-interacting Anderson transi…
We present explicit expressions for the correlation functions of interacting fermions in one dimension which are valid for arbitrary system sizes and temperatures. The result applies to a number of very different strongly correlated systems, including mesoscopic quantum wires, quantum Hall edges, spin chains and quasi-one-dimensional metals. It is for example possible to calculate Coulomb blockade oscillations from our expression and determine their dependence on interaction strength and temperature. Numerical simulations show excellent agreement with the analytical results.
We address the interaction of graphene with 3d transition metal adatoms and the formation of localized magnetic moments by means of first-principles calculations. By comparing calculations within the generalized gradient approximation (GGA) to GGA+U we find that the electronic configuration and the adsorption geometries can be very sensitive to effects of local Coulomb interactions U in the transition metal d-orbitals. We find high-spin configurations being favorable for Cr and Mn adatoms independent of the functional. For Fe, Co and Ni different electronic configurations are realized dependin…
There is a close connection between various new phenomena in Weyl semimetals and the existence of linear band crossings in the single particle description. We show, by a full self-consistent mean-field calculation, how this picture is modified in the presence of long-range Coulomb interactions. The chiral symmetry breaking occurs at strong enough interactions and the internode interband excitonic pairing channel is found to be significant, which determines the gap-opened band profile varying with interaction strength. Remarkably, in the resultant interacting phase, finite band Chern number jum…
