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We study the electronic thermal conductivity $\kappa_\textrm{el}$ and the thermal diffusion constant $D_\textrm{Q,el}$ in the square lattice Hubbard model using the finite-temperature Lanczos method. We exploit the Nernst-Einstein relation for thermal transport and interpret the strong non-monotonous temperature dependence of $\kappa_\textrm{el}$ in terms of that of $D_\textrm{Q,el}$ and the electronic specific heat $c_\textrm{el}$. We present also the results for the Heisenberg model on a square lattice and ladder geometries. We study the effects of doping and consider the doped case also with the dynamical mean-field theory. We show that $\kappa_\textrm{el}$ is below the corresponding Mott-Ioffe-Regel value in almost all calculated regimes, while the mean free path is typically above or close to lattice spacing. We discuss the opposite effect of quasi-particle renormalization on charge and heat diffusion constants. We calculate the Lorenz ratio and show that it differs from the Sommerfeld value. We discuss our results in relation to experiments on cuprates. Additionally, we calculate the thermal conductivity of overdoped cuprates within the anisotropic marginal Fermi liquid phenomenological approach., Comment: 8+5 figures

International audience; We consider non-Fermi liquids in which the inelastic scattering rate has an intrinsic particle-hole asymmetry and obeys ω/T scaling. We show that, in contrast to Fermi liquids, this asymmetry influences the low-temperature behavior of the thermopower even when the impurity scattering dominates. Implications for the unconventional sign and temperature dependence of the thermopower in cuprates in the strange metal (Planckian) regime are emphasized.

Mo$_8$O$_{23}$ is a low-dimensional chemically robust transition metal oxide coming from a prospective family of functional materials, MoO$_{3-x}$, ranging from a wide gap insulator $(x=0)$ to a metal $(x=1)$. The large number of stoichometric compounds with intermediate $x$ have widely different properties. In Mo$_8$O$_{23}$, an unusual charge density wave transition has been suggested to occur above room temperature, but its low temperature behaviour is particularly enigmatic. We present a comprehensive experimental study of the electronic structure associated with various ordering phenomena in this compound, complemented by theory. Density-functional theory (DFT) calculations reveal a cross-over from a semi-metal with vanishing band overlap to narrow-gap semiconductor behaviour with decreasing temperature. A buried Dirac crossing at the zone boundary is confirmed by angle-resolved photoemission spectroscopy (ARPES). Tunnelling spectroscopy (STS) reveals a gradual gap opening corresponding to a metal-to-insulator transition at 343 K in resistivity, consistent with CDW formation and DFT results, but with large non-thermal smearing of the spectra implying strong carrier scattering. At low temperatures, the CDW picture is negated by the observation of a metallic Hall contribution, a non-trivial gap structure in STS below $\sim 170$ K and ARPES spectra, that together represent evidence for the onset of the correlated state at $70$ K and the rapid increase of gap size below $\sim 30$ K. The intricate interplay between electronic correlations and the presence of multiple narrow bands near the Fermi level set the stage for metastability and suggest suitability for memristor applications., Comment: 13 pages, 6 figures, pre-print of an article published in Scientific Reports. The final authenticated version is available online at http://dx.doi.org/10.1038/s41598-019-52231-4

We investigate the nonequilibrium electronic structure and characteristic timescales in a candidate excitonic insulator, ${\mathrm{Ta}}_{2}\mathrm{Ni}{\mathrm{Se}}_{5}$, using time- and angle-resolved photoemission spectroscopy with a temporal resolution of 50 fs. Following a strong photoexcitation, the band gap closes transiently within 100 fs, i.e., on a timescale faster than the typical lattice vibrational period. Furthermore, we find that the characteristic time associated with the rise of the photoemission intensity above the Fermi energy decreases with increasing excitation strength, while the relaxation time of the electron population towards equilibrium shows an opposite behavior. We argue that these experimental observations can be consistently explained by an excitonic origin of the band gap in the material. The excitonic picture is supported by microscopic calculations based on the nonequilibrium Green's function formalism for an interacting two-band system. We interpret the speedup of the rise time with fluence in terms of an enhanced scattering probability between photoexcited electrons and excitons, leading to an initially faster decay of the order parameter. We show that the inclusion of electron-phonon coupling at a semiclassical level changes only the quantitative aspects of the proposed dynamics, while the qualitative features remain the same. The experimental observations and microscopic calculations allow us to develop a simple and intuitive phenomenological model that captures the main dynamics after photoexcitation in ${\mathrm{Ta}}_{2}\mathrm{Ni}{\mathrm{Se}}_{5}$.

We study the spin diffusion and spin conductivity in the square lattice Hubbard model by using the finite-temperature Lanczos method. We show that the spin diffusion behaves differently from the charge diffusion and has a nonmonotonic $T$ dependence. This is due to a progressive liberation of charges that contribute to spin transport and enhance it beyond that active at low temperature due to the Heisenberg exchange. We further show that going away from half filling and zero magnetization increases the spin diffusion, but that the increase is insufficient to reconcile the difference between the model calculations and the recent measurements on cold atoms.

We investigate the spin Seebeck coefficient $S_s$ in the square lattice Hubbard model at high temperatures of relevance to cold-atom measurements. We solve the model with the finite-temperature Lanczos and with the dynamical mean-field theory methods and find they give similar results in the considered regime. $S_s$ exceeds the atomic 'Heikes' estimates and the Kelvin entropic estimates drastically. We analyze the behavior in terms of a mapping onto the problem of a doped attractive model and derive an approximate expression that allows relating the enhancement of $S_s$ to distinct scattering of the spin-majority and the spin-minority excitations. Our analysis reveals the limitations of entropic interpretations of Seebeck coefficient even in the high-temperature regime. Large values of $S_s$ could be observed on optical lattices. We also calculate the full diffusion matrix. We quantify the spin-thermal diffusion, that is, the extent of the mixing between the spin and the thermal diffusion and discuss the results in the context of recent measurements of the spin-diffusion constant in cold atoms., Comment: 7 pages, 4 figures

We investigate the 5d transition metal oxide BaOsO$_3$ within a combination of density functional theory (DFT) and dynamical mean-field theory (DMFT), using a matrix-product-state impurity solver. BaOsO$_3$ has 4 electrons in the t$_{2g}$ shell akin to ruthenates but stronger spin-orbit coupling (SOC) and is thus expected to reveal an interplay of Hund's metal behavior with SOC. We explore the paramagnetic phase diagram as a function of SOC and Hubbard interaction strengths, identifying metallic, band (van-Vleck) insulating and Mott insulating regions. At the physical values of the two couplings we find that BaOsO$_3$ is still situated inside the metallic region and has a moderate quasiparticle renormalization $m^*/m \approx 2$; consistent with specific heat measurements. SOC plays an important role in suppressing electronic correlations (found in the vanishing SOC case) through the splitting of a van-Hove singularity (vHs) close to the Fermi energy, but is insufficient to push the material into an insulating van-Vleck regime. In spite of the strong effect of SOC, BaOsO$_3$ can be best pictured as a moderately correlated Hund's metal., 12 pages, 7 figures

High-temperature bad-metal transport has been recently studied both theoretically and in experiments as one of the key signatures of strong electronic correlations. Here we use the dynamical mean field theory (DMFT) and its cluster extensions, as well as the finite-temperature Lanczos method (FTLM) to explore the influence of lattice frustration on the thermodynamic and transport properties of the Hubbard model at high temperatures. We consider the triangular and the square lattice at half-filling and at 15\% hole-doping. We find that for $T \gtrsim 1.5t$ the self-energy becomes practically local, while the finite-size effects become small at lattice-size $4 \times 4$ for both lattice types and doping levels. The vertex corrections to optical conductivity, which are significant on the square lattice even at high temperatures, contribute less on the triangular lattice. We find approximately linear temperature dependence of dc resistivity in doped Mott insulator for both types of lattices., 11 pages

The transport properties of iron under Earth's inner core conditions are essential input for the geophysical modelling but are poorly constrained experimentally. Here we show that the thermal and electrical conductivity of iron at those conditions remains high even if the electron-electron-scattering (EES) is properly taken into account. This result is obtained by ab initio simulations taking into account consistently both thermal disorder and electronic correlations. Thermal disorder suppresses the non-Fermi-liquid behavior of the body-centered cubic iron phase, hence, reducing the EES; the total calculated thermal conductivity of this phase is 220 Wm$^{-1}$K$^{-1}$ with the EES reduction not exceeding 20%. The EES and electron-lattice scattering are intertwined resulting in breaking of the Matthiessen's rule with increasing EES. In the hexagonal close-packed iron the EES is also not increased by thermal disorder and remains weak. Our main finding thus holds for the both likely iron phases in the inner core., 8 pages, 4 figures, published main text. For supplementary material see https://www.nature.com/articles/s41467-020-18003-9

Perovskite rhodates are characterized by intermediate strengths of both electronic correlation as well as spin-orbit coupling (SOC) and usually behave as moderately correlated metals. A recent publication [Phys. Rev. B 95, 245121 (2017)] on epitaxial ${\mathrm{SrRhO}}_{3}$ thin films reported a bad-metallic behavior and suggested the occurrence of antiferromagnetism below 100 K. We have further studied this ${\mathrm{SrRhO}}_{3}$ thin film by hard x-ray photoemission spectroscopy and found a very small density of states (DOS) at the Fermi level (${E}_{F}$), which is consistent with the previously reported bad-metallic behavior. However, the absence of DOS persists up to room temperature, which contradicts the explanation of antiferromagnetic transition at $\ensuremath{\sim}100$ K. We also employed electronic structure calculations within the framework of density functional theory and dynamical mean-field theory. In contrast to the photoemission results, our calculations indicate metallic behaviors of both bulk ${\mathrm{SrRhO}}_{3}$ and the ${\mathrm{SrRhO}}_{3}$ thin film, and a stronger correlation effect was observed in the thin film than that in the bulk. The calculated uniform magnetic susceptibility is substantially larger in the thin film than that in the bulk. We also investigated the role of SOC and found only a moderate modulation of the band structure. Hence SOC is not expected to significantly affect the electronic correlation in ${\mathrm{SrRhO}}_{3}$. Extrinsic effects of finite-thickness effects beyond our calculations and localization effects may play important roles to induce the negligible spectral weight at ${E}_{F}$.

Even though no local order parameter in the sense of the Landau theory exists for topological quantum phase transitions in Chern insulators, the highly non-local Berry curvature exhibits critical behavior near a quantum critical point. We investigate the critical properties of its real space analog, the local Chern marker, in weakly disordered Chern insulators. Due to disorder, inhomogeneities appear in the spatial distribution of the local Chern marker. Their size exhibits power-law scaling with the critical exponent matching the one extracted from the Berry curvature of a clean system. We drive the system slowly through such a quantum phase transition. The characteristic size of inhomogeneities in the non-equilibrium post-quench state obeys the Kibble-Zurek scaling. In this setting, the local Chern marker thus does behave in a similar way as a local order parameter for a symmetry breaking second order phase transition. The Kibble-Zurek scaling also holds for the inhomogeneities in the spatial distribution of excitations and of the orbital polarization., Comment: Published version

Recent experiments on cold atoms in optical lattices allow for a quantitative comparison of the measurements to the conductivity calculations in the square lattice Hubbard model. However, the available calculations do not give consistent results and the question of the exact solution for the conductivity in the Hubbard model remained open. In this letter we employ several complementary state-of-the-art numerical methods to disentangle various contributions to conductivity, and identify the best available result to be compared to experiment. We find that at relevant (high) temperatures, the self-energy is practically local, yet the vertex corrections remain rather important, contrary to expectations. The finite-size effects are small even at the lattice size $4\times 4$ and the corresponding Lanczos diagonalization result is therefore close to the exact result in the thermodynamic limit., Comment: 6 pages, 3 figures + supp.mat. 7 pages, 6 figures

The Hall coefficient $R_H$ of Sr$_2$RuO$_4$ exhibits a non-monotonic temperature dependence with two sign reversals. We show that this puzzling behavior is the signature of two crossovers which are key to the physics of this material. The increase of $R_H$ and the first sign change upon cooling are associated with a crossover into a regime of coherent quasiparticles with strong orbital differentiation of the inelastic scattering rates. The eventual decrease and the second sign change at lower temperature is driven by the crossover from inelastic to impurity-dominated scattering. This qualitative picture is supported by quantitative calculations of $R_H(T)$ using Boltzmann transport theory in combination with dynamical mean-field theory, taking into account the effect of spin-orbit coupling. Our insights shed new light on the temperature dependence of the Hall coefficient in materials with strong orbital differentiation, as observed in Hund's metals., Comment: 20 pages, 4 figures

We investigate slow quenches in Chern insulators in ribbon geometry. We consider the Qi-Wu-Zhang model and slowly ramp the parameters (large time of the quench $\tau$) from a non-topological (Chern number = 0) to a topological regime (Chern number $\ne$ 0). In contrast to the Haldane model considered in [L. Privitera and G. E. Santoro, Phys. Rev. B 93, 241406(R) (2016)] earlier, the in-gap state degeneracy point is pinned to an inversion symmetric momentum, which changes the behavior drastically. The density of excitations in the in-gap states scales with the quench time as $\tau^{-1/2}$ as the ramp becomes slow, and the Kibble-Zurek mechanism applies. Despite the slower scaling of the density of in-gap excitations with $\tau$, the Hall conductance after the quench deviates from that of the ground state of the final Hamiltonian by an amount that drops as $\tau^{-1}$.

Monoclinic semimetallic ${\mathrm{Mo}}_{8}{\mathrm{O}}_{23}$ belongs to a multifunctional series of compounds showing multiple ordering phenomena that have not achieved much attention until now. Previous x-ray studies of this compound have revealed an incommensurate ordering transition at ${T}_{\mathrm{IC}}\ensuremath{\sim}350$ K, followed by a structural transition to commensurate order at ${T}_{\mathrm{IC}\ensuremath{-}\mathrm{C}}=285$ K. In addition, an enigmatic resistance maximum is observed at ${T}_{\mathrm{el}}\ensuremath{\sim}150$ K, whose origin has so far proved elusive. Aiming to disentangle these multiple orders we use the polarized transient optical spectroscopy supplemented by Raman spectroscopy to study the electronic relaxation dynamics and lattice vibrational modes in ${\mathrm{Mo}}_{8}{\mathrm{O}}_{23}$ single crystals. Remarkably, both the coherent vibrational mode response and single-particle response display extrema of damping/relaxation times close to ${T}_{\mathrm{el}}$ with the concurrent appearance of new coherent vibrational modes and a characteristic polarization asymmetry which saturates below ${T}_{\mathrm{el}}$. The single-particle relaxation data analysis shows the appearance of a temperature-independent gap in the electronic excitation spectrum below ${T}_{\mathrm{IC}}$ and additional temperature-dependent gap opening near ${T}_{\mathrm{el}}$. Concurrently, a low-frequency vibrational mode shows anomalous softening around ${T}_{\mathrm{m}}\ensuremath{\sim}200$ K, far below ${T}_{\mathrm{IC}\ensuremath{-}\mathrm{C}}$ and ${T}_{\mathrm{IC}}$. The observations are interpreted in terms of the appearance of a hidden gapped state below ${T}_{\mathrm{el}}$ that has so far eluded detection by structural analyses.

We investigate the influence of spin-orbit coupling $\ensuremath{\lambda}$ in strongly-correlated multiorbital systems that we describe by a three-orbital Hubbard-Kanamori model on a Bethe lattice. We solve the problem at all integer fillings $N$ with the dynamical mean-field theory using the continuous-time hybridization expansion Monte Carlo solver. We investigate how the quasiparticle renormalization $Z$ varies with the strength of spin-orbit coupling. The behavior can be understood for all fillings except $N=2$ in terms of the atomic Hamiltonian (the atomic charge gap) and the polarization in the $j$ basis due to spin-orbit induced changes of orbital degeneracies and the associated kinetic energy. At $N=2, \ensuremath{\lambda}$ increases $Z$ at small $U$ but suppresses it at large $U$, thus eliminating the characteristic Hund's metal tail in $Z(U)$. We also compare the effects of the spin-orbit coupling to the effects of a tetragonal crystal field. Although this crystal field also lifts the orbital degeneracy, its effects are different, which can be understood in terms of the different form of the interaction Hamiltonian expressed in the respective diagonal single-particle basis.

We present an implementation of the rotationally invariant slave boson technique as an impurity solver for density functional theory plus dynamical mean field theory (DFT+DMFT). Our approach provides explicit relations between quantities in the local correlated subspace treated with DMFT and the Bloch basis used to solve the DFT equations. In particular, we present an expression for the mass enhancement of the quasiparticle states in reciprocal space. We apply the method to the study of the electronic correlations in Sr2RuO4 under anisotropic strain. We find that the spin-orbit coupling plays a crucial role in the mass enhancement differentiation between the quasi-one-dimensional α and β bands, and on its momentum dependence over the Fermi surface. The mass enhancement, however, is only weakly affected by either uniaxial or biaxial strain, even across the Lifshitz transition induced by the strain. Fil: Facio, Jorge Ismael. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina. Leibniz-institut Für Festkörper- Und Werkstoffforschung Dresden; Alemania Fil: Mravlje, Jernej. Jozef Stefan Institute; Eslovenia Fil: Pourovskii, Leonid. Collège de France; Francia. Université Paris-Saclay; Francia Fil: Cornaglia de la Cruz, Pablo Sebastian. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina Fil: Vildosola, Veronica Laura. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica; Argentina

We investigate the interplay of spin-orbit coupling (SOC) and electronic correlations in ${\mathrm{Sr}}_{2}{\mathrm{RuO}}_{4}$ using dynamical mean-field theory. We find that SOC does not affect the correlation-induced renormalizations, which validates Hund's metal picture of ruthenates even in the presence of the sizable SOC relevant to these materials. Nonetheless, SOC is found to change significantly the electronic structure at $k$ points where a degeneracy applies in its absence. We explain why these two observations are consistent with one another and calculate the effects of SOC on the correlated electronic structure. The magnitude of these effects is found to depend on the energy of the quasiparticle state under consideration, leading us to introduce the notion of an energy-dependent quasiparticle spin-orbit coupling ${\ensuremath{\lambda}}^{*}(\ensuremath{\omega})$. This notion is generally applicable to all materials in which both the spin-orbit coupling and electronic correlations are sizable.

We investigate the interplay of spin-orbit coupling (SOC) and electronic correlations in Sr_{2}RuO_{4} using dynamical mean-field theory. We find that SOC does not affect the correlation-induced renormalizations, which validates Hund's metal picture of ruthenates even in the presence of the sizable SOC relevant to these materials. Nonetheless, SOC is found to change significantly the electronic structure at k points where a degeneracy applies in its absence. We explain why these two observations are consistent with one another and calculate the effects of SOC on the correlated electronic structure. The magnitude of these effects is found to depend on the energy of the quasiparticle state under consideration, leading us to introduce the notion of an energy-dependent quasiparticle spin-orbit coupling λ^{*}(ω). This notion is generally applicable to all materials in which both the spin-orbit coupling and electronic correlations are sizable.

We study the topological properties and transport in the Bernevig-Hughes-Zhang (BHZ) model undergoing a slow quench between different topological regimes. Due to the closing of the band gap during the quench, the system ends up in an excited state. For quenches governed by a Hamiltonian that preserves the symmetries present in the BHZ model (time-reversal, inversion, and conservation of spin projection), the $\mathbb{Z}_2$ invariant remains equal to the one evaluated in the initial state. The bulk spin Hall conductivity does change and its time average approaches that of the ground state of the final Hamiltonian. The deviations from the ground-state spin Hall conductivity as a function of the quench time follow the Kibble-Zurek scaling. We also consider the breaking of the time-reversal symmetry, which restores the correspondence between the bulk invariant and the transport properties after the quench., corrected version, references added, corresponding erratum submitted to PRB

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 $|\lambda| \lambda_c$, 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., Comment: 5 pages, 3 figures

Strong electronic correlations are often associated with the proximity of a Mott-insulating state. In recent years however, it has become increasingly clear that the Hund’s rule coupling (intra-atomic exchange) is responsible for strong correlations in multiorbital metallic materials that are not close to a Mott insulator. Hund’s coupling has two effects: It influences the energetics of the Mott gap and strongly suppresses the coherence scale for the formation of a Fermi liquid. A global picture has emerged recently, which emphasizes the importance of the average occupancy of the shell as a control parameter. The most dramatic effects occur away from half-filling or single occupancy. We review the theoretical understanding and physical properties of these Hund’s metals, together with the relevance of this concept to transition-metal oxides (TMOs) of the 3d, and especially 4d, series (such as ruthenates), as well as to the iron-based superconductors (iron pnictides and chalcogenides).

The electronic state and transport properties of hot dense iron are of the utmost importance for the understanding of Earths interior. Combining state-of-the-art density functional and dynamical mean field theories we study the impact of electron correlations on the electrical and thermal resistivity of hexagonal close-packed epsilon-Fe at Earths core conditions and show that the electron-electron scattering in epsilon-Fe exhibit a nearly perfect Fermi-liquid (FL) behavior. Accordingly, the quadratic dependence of the scattering rate, typical of FLs, leads to a modification of the Wiedemann-Franz law and suppresses the thermal conductivity with respect to the electrical one. The consequence is a significant increase of the electron-electron thermal resistivity, which is found to be of comparable magnitude to the electron-phonon one. Funding Agencies|European Research Council [ERC-319286 QMAC]; Slovenian Research Agency (ARRS) [P1-0044]; Swedish Research Council (VR) [2014-4750, 2015-04391]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009 00971]; Ministry of Education and Science of the Russian Federation [14.Y26.31.0005]

The existence of a quantum spin liquid (QSL) in which quantum fluctuations of spins are sufficiently strong to preclude spin ordering down to zero temperature was originally proposed theoretically more than 40 years ago, but its experimental realisation turned out to be very elusive. Here we report on an almost ideal spin liquid state that appears to be realized by atomic-cluster spins on the triangular lattice of a charge-density wave (CDW) state of 1T-TaS$_2$. In this system, the charge excitations have a well-defined gap of $\sim 0.3$ eV, while nuclear magnetic quadrupole resonance and muon spin relaxation experiments reveal that the spins show gapless quantum spin liquid dynamics and no long range magnetic order down to 70~mK. Canonical $T^{2}$ power-law temperature dependence of the spin relaxation dynamics characteristic of a QSL is observed from 200~K to $T_f= 55$ K. Below this temperature we observe a new gapless state with reduced density of spin excitations and high degree of local disorder signifying new quantum spin order emerging from the QSL., Comment: 15 pages, 4 figures, submitted for a publication

We discuss the low-energy physics of the three-orbital Anderson impurity model with the Coulomb interaction term of the Kanamori form which has orbital SO(3) and spin SU(2) symmetry and describes systems with partially occupied $t_{2g}$ shells. We focus on the case with two electrons in the impurity that is relevant to Hund's metals. Using the Schrieffer-Wolff transformation we derive an effective Kondo model with couplings between the bulk and impurity electrons expressed in terms of spin, orbital, and orbital quadrupole operators. The bare spin-spin Kondo interaction is much smaller than the orbit-orbit and spin-orbital couplings or is even ferromagnetic. Furthermore, the perturbative scaling equations indicate faster renormalization of the couplings related to orbital degrees of freedom compared to spin degrees of freedom. Both mechanisms lead to a slow screening of the local spin moment. The model thus behaves similarly to the related quantum impurity problem with a larger SU(3) orbital symmetry (Dworin-Narath interaction) where this was first observed. We find that the two problems actually describe the same low-energy physics since the SU(3) symmetry is dynamically established through the renormalization of the splittings of coupling constants to zero. The perturbative renormalization group results are corroborated with the numerical-renormalization group (NRG) calculations. The dependence of spin Kondo temperatures and orbital Kondo temperatures as a function of interaction parameters, the hybridization, and the impurity occupancy is calculated and discussed., Comment: 12 pages

We derive analytical expressions for the spectral moments of the dynamical response functions of the Hubbard model using the high-temperature series expansion. We consider generic dimension $d$ as well as the infinite-$d$ limit, arbitrary electron density $n$, and both finite and infinite repulsion $U$. We use moment-reconstruction methods to obtain the one-electron spectral function, the self-energy, and the optical conductivity. They are all smooth functions at high-temperature and, at large-$U$, they are featureless with characteristic widths of order the lattice hopping parameter $t$. In the infinite-$d$ limit we compare the series expansion results with accurate numerical renormalization group and interaction expansion quantum Monte-Carlo results. We find excellent agreement down to surprisingly low temperatures, throughout most of the bad-metal regime which applies for $T \gtrsim (1-n)D$, the Brinkman-Rice scale. The resistivity increases linearly in $T$ at high-temperature without saturation. This results from the $1/T$ behaviour of the compressibility or kinetic energy, which play the role of the effective carrier number. In contrast, the scattering time (or diffusion constant) saturate at high-$T$. We find that $\sigma(n,T) \approx (1-n)\sigma(n=0,T)$ to a very good approximation for all $n$, with $\sigma(n=0,T)\propto t/T$ at high temperatures. The saturation at small $n$ occurs due to a compensation between the density-dependence of the effective number of carriers and that of the scattering time. The $T$-dependence of the resistivity displays a knee-like feature which signals a cross-over to the intermediate-temperature regime where the diffusion constant (or scattering time) start increasing with decreasing $T$. At high-temperatures, the thermopower obeys the Heikes formula, while the Wiedemann-Franz law is violated with the Lorenz number vanishing as $1/T^2$., Comment: 38 pages, 16 figures

We calculate the in-plane Seebeck coefficient of Sr_{2}RuO_{4} within a framework combining electronic structure and dynamical mean-field theory. We show that its temperature dependence can be interpreted using entropic considerations based on the Kelvin formula and that it provides a meaningful probe of the crossover out of the Fermi liquid regime into an incoherent metal. This crossover proceeds in two stages: The entropy of spin degrees of freedom is released around room temperature, while orbital degrees of freedom remain quenched up to much higher temperatures. This is confirmed by a direct calculation of the corresponding susceptibilities and is a hallmark of "Hund's metals." We also calculate the c-axis thermopower and predict that it exceeds substantially the in-plane one at high temperature, a peculiar behavior which originates from an interlayer "hole-filtering" mechanism.

We present the TRIQS/DFTTools package, an application based on the TRIQS library that connects this toolbox to realistic materials calculations based on density functional theory (DFT). In particular, TRIQS/DFTTools together with TRIQS allows an efficient implementation of DFT plus dynamical mean-field theory (DMFT) calculations. It supplies tools and methods to construct Wannier functions and to perform the DMFT self-consistency cycle in this basis set. Post-processing tools, such as band-structure plotting or the calculation of transport properties are also implemented. The package comes with a fully charge self-consistent interface to the Wien2k band structure code, as well as a generic interface that allows to use TRIQS/DFTTools together with a large variety of DFT codes. It is distributed under the GNU General Public License (GPLv3)., Comment: 18 pages, 6 figures, Comp. Phys. Comm. accepted version

Spin-entanglement of two electrons occupying two spatial regions - domains - is expressed in a compact form in terms of spin-spin correlation functions. The power of the formalism is demonstrated on several examples ranging from generation of entanglement by scattering of two electrons to the entanglement of a pair of qubits represented by a double quantum dot coupled to leads. In the latter case the collapse of entanglement due to the Kondo effect is analyzed.

We consider electronic transport through break-junctions bridged by a single molecule in the Kondo regime. We describe the system by a two-channel Anderson model. We take the tunneling matrix elements to depend on the position of the molecule. It is shown, that if the modulation of the tunneling by displacement is large, the potential confining the molecule to the central position between the leads is softened and the position of the molecule is increasingly susceptible to external perturbations that break the inversion symmetry. In this regime, the molecule is attracted to one of the leads and as a consequence the conductance is small. We argue on semi-classical grounds why the softening occurs and corroborate our findings by numerical examples obtained by Wilson's numerical renormalization group and Schonhammer-Gunnarsson's variational method.

The electrons in atomic shells repel each other through the Coulomb force. When two electrons are placed in the same atomic orbital, the energetic cost of this repulsion is only partially compensated by the attraction of the electron towards the nucleus. The electronic configurations corresponding to the states where electrons are on average further apart are energetically favourable. The configurations found in the ground-state are those in which the electronic spins are maximally aligned. S...

Les couches electroniques des atomes se remplissent avec une grande regularite, qui se manifeste dans la classification periodique des elements. Non seulement le remplissage des couches externes se produit apres la saturation des couches les plus proches du noyau, mais les differentes orbitales de la derniere couche, partiellement remplie, se produisent encore de facon tres ordonnee. Ainsi, la double occupation (par un electron de chaque spin) ne se produit qu’apres l’occupation de toutes les...

Using a combination of spectroscopic ellipsometry and DC transport measurements, we determine the temperature dependence of the optical conductivity of NdNiO$_3$ and SmNiO$_{3}$ films. The optical spectra show the appearance of a characteristic two-peak structure in the near-infrared when the material passes from the metal to the insulator phase. Dynamical mean-field theory calculations confirm this two-peak structure, and allow to identify these spectral changes and the associated changes in the electronic structure. We demonstrate that the insulating phase in these compounds and the associated characteristic two-peak structure are due to the combined effect of bond-disproportionation and Mott physics associated with half of the disproportionated sites. We also provide insights into the structure of excited states above the gap., 12 pages, 13 figures

A comparative density functional plus dynamical mean field theory study of the pseudocubic ruthenate materials ${\text{CaRuO}}_{3}$ and ${\text{SrRuO}}_{3}$ is presented. Phase diagrams are determined for both materials as a function of Hubbard repulsion $U$ and Hund's rule coupling $J$. Metallic and insulating phases are found, as are ferromagnetic and paramagnetic states. The locations of the relevant phase boundaries are determined. Based on the computed phase diagrams, Mott dominated and Hund's dominated regimes of strong correlation are distinguished. Comparison of calculated properties to experiments indicates that the actual materials are in the Hund's coupling dominated region of the phase diagram so can be characterized as Hund's metals, in common with other members of the ruthenate family. Comparison of the phase diagrams for the two materials reveals the role played by rotational and tilt $({\text{GdFeO}}_{3}$-type) distortions of the ideal perovskite structure. The presence of magnetism in ${\text{SrRuO}}_{3}$ and its absence in ${\text{CaRuO}}_{3}$ despite the larger mass and larger tilt/rotational distortion amplitude of ${\text{CaRuO}}_{3}$ can be understood in terms of density of states effects in the presence of strong Hund's coupling. Comparison of the calculated low-$T$ properties of ${\text{CaRuO}}_{3}$ to those of ${\text{SrRuO}}_{3}$ provides insight into the effects of magnetic order on the properties of a Hund's metal. The study provides a simultaneous description of magnetism and correlations and explicates the roles played by band theory and Hubbard and Hund's interactions.

We calculate the in-plane Seebeck coefficient of Sr_{2}RuO_{4} within a framework combining electronic structure and dynamical mean-field theory. We show that its temperature dependence can be interpreted using entropic considerations based on the Kelvin formula and that it provides a meaningful probe of the crossover out of the Fermi liquid regime into an incoherent metal. This crossover proceeds in two stages: The entropy of spin degrees of freedom is released around room temperature, while orbital degrees of freedom remain quenched up to much higher temperatures. This is confirmed by a direct calculation of the corresponding susceptibilities and is a hallmark of "Hund's metals." We also calculate the c-axis thermopower and predict that it exceeds substantially the in-plane one at high temperature, a peculiar behavior which originates from an interlayer "hole-filtering" mechanism.

We theoretically investigate magnetic properties of Sr$_2$TcO$_4$, a 4d transition-metal layered perovskite of the K$_2$NiF$_4$-type with half-filled t$_{2g}$ states. The effect of local Coulomb repulsion between the t$_{2g}$ orbitals is included within the density-functional theory (DFT)+U and DFT+dynamical mean-field theory (DMFT) methods. The DFT+DMFT predicts paramagnetic Sr$_2$TcO$_4$ to be close to the Mott insulator-to-metal transition, similarly to the cubic compound SrTcO$_3$. The inter-site exchange interactions computed within the DFT+DMFT framework point to a strong antiferromagnetic coupling between the neighboring Tc sites within the layer. We then evaluate the N\'eel temperature $T_N$ within a classical Monte Carlo approach including dipolar interactions, which stabilize the magnetic order in the frustrated K$_2$NiF$_4$ lattice structure. Our approach is applied to a set of layered and cubic perovskites. The obtained $T_N$ are in fair agreement with experiment. Within the same approach we predict $T_N$ of Sr$_2$TcO$_4$ to be in the 500-600K range., Comment: 8 pages, 3 figures

Density functional plus dynamical mean field calculations are used to show that in transition metal oxides, rotational and tilting (GdFeO$_3$-type) distortions of the ideal cubic perovskite structure produce a multiplicity of low-energy optical transitions which affect the conductivity down to frequencies of the order of $1$ or $2$~mV (terahertz regime), mimicking non-Fermi-liquid effects even in systems with a strictly Fermi-liquid self-energy. For CaRuO$_3$, a material whose measured electromagnetic response in the terahertz frequency regime has been interpreted as evidence for non-Fermi-liquid physics, the combination of these band structure effects and a renormalized Fermi-liquid self-energy accounts for the low frequency optical response which had previously been regarded as a signature of exotic physics. Signatures of deviations from Fermi-liquid behavior at higher frequencies ($\sim 100$~meV) are discussed.

We investigate the electronic structure of a perovskite-type Pauli paramagnet ${\mathrm{SrMoO}}_{3}$ (${{t}_{2g}}^{2}$) thin film using hard x-ray photoemission spectroscopy and compare the results to realistic calculations that combine density functional theory within the local-density approximation (LDA) with dynamical mean-field theory (DMFT). Despite the clear signature of electron correlations in the electronic specific heat, the narrowing of the quasiparticle bands is not observed in the photoemission spectrum. This is explained in terms of the characteristic effect of Hund's rule coupling for partially filled ${t}_{2g}$ bands, which induces strong quasiparticle renormalization already for values of Hubbard interaction which are smaller than the bandwidth. This interpretation is supported by DMFT model calculations including Hund's rule coupling, which show a renormalization of low-energy quasiparticles without affecting the overall bandwidth. The photoemission spectra show additional spectral weight around $\ensuremath{-}2.5$ eV that is not present in the LDA+DMFT results, pointing to a source of correlations that is not present in our calculations that include only on-site interactions. We interpret this weight as a plasmon satellite, which is supported by the measured core-level spectra that all show satellites at this energy.

We have obtained the equilibrium volumes, bulk moduli, equations of state of the ferromagnetic cubic $\alpha$ and paramagnetic hexagonal $\epsilon$ phases of iron in close agreement with experiment using an ab initio dynamical mean-field theory approach. The local dynamical correlations are shown to be crucial for a successful description of the ground-state properties of paramagnetic $\epsilon$-Fe. Moreover, they enhance the effective mass of the quasiparticles and reduce their lifetimes across the $\alpha \to \epsilon$ transition leading to a step-wise increase of the resistivity, as observed in experiment. The calculated magnitude of the jump is significantly underestimated, which points to non-local correlations. The implications of our results for the superconductivity and non-Fermi-liquid behavior of $\epsilon$-Fe are discussed., Comment: 6 pages, 3 figures

We report optical measurements demonstrating that the low-energy relaxation rate (1/τ) of the conduction electrons in Sr(2)RuO(4) obeys scaling relations for its frequency (ω) and temperature (T) dependence in accordance with Fermi-liquid theory. In the thermal relaxation regime, 1/τ ∝ (ħω)(2)+(pπk(B)T)(2) with p = 2, and ω/T scaling applies. Many-body electronic structure calculations using dynamical mean-field theory confirm the low-energy Fermi-liquid scaling and provide quantitative understanding of the deviations from Fermi-liquid behavior at higher energy and temperature. The excess optical spectral weight in this regime provides evidence for strongly dispersing "resilient" quasiparticle excitations above the Fermi energy.

We have prepared high-quality epitaxial thin films of CaRuO$_3$ with residual resistivity ratios up to 55. Shubnikov-de Haas oscillations in the magnetoresistance and a $T^2$ temperature dependence in the electrical resistivity only below 1.5 K, whose coefficient is substantially suppressed in large magnetic fields, establish CaRuO$_3$ as a Fermi liquid (FL) with anomalously low coherence scale. Non-Fermi liquid (NFL) $T^{3/2}$ dependence is found between 2 and 25 K. The high sample quality allows access to the intrinsic electronic properties via THz spectroscopy. For frequencies below 0.6 THz, the conductivity is Drude-like and can be modeled by FL concepts, while for higher frequencies non-Drude behavior, inconsistent with FL predictions, is found. This establishes CaRuO$_3$ as a prime example of optical NFL behavior in the THz range.

We study the spin thermopower in the two-channel spin-1/2 Kondo model which exhibits the phenomenon of impurity spin overscreening and non-Fermi-liquid properties. While magnetic field lower than the Kondo temperature does not strongly polarize the impurity spin, we show that it nevertheless strongly affects the low-energy part of the spectral function. In turn, this leads to characteristic saturation of the spin Seebeck coefficient at the value of 0.388kB/|e| at T ~ T*, where T* ~ B^2/TK is the scale of the crossover between the intermediate-temperature non-Fermi-liquid regime and the low-temperature Fermi-liquid regime. We show that measuring the spin thermopower at low magnetic fields would provide a sensitive test for distinguishing regular Fermi liquid, singular Fermi liguid, and non-Fermi liquid behaviour in nanodevices., 15 pages, 5 figures

We investigate the frequency and temperature dependence of the low-energy electron dynamics in a Landau Fermi liquid with a local self-energy. We show that the frequency and temperature dependencies of the optical conductivity obey universal scaling forms, for which explicit analytical expressions are obtained. For the optical conductivity and the associated memory function, we obtain a number of surprising features that differ qualitatively from the Drude model and are universal characteristics of a Fermi liquid. Different physical regimes of scaling are identified, with marked non-Drude features in the regime where hbar omega ~ kB T. These analytical results for the optical conductivity are compared to numerical calculations for the doped Hubbard model within dynamical mean-field theory. For the "universal" low-energy electrodynamics, we obtain perfect agreement between numerical calculations and analytical scaling laws. Both results show that the optical conductivity displays a non-Drude "foot", which could be easily mistaken as a signature of breakdown of the Fermi liquid, while it actually is a striking signature of its applicability. The aforementioned scaling laws provide a quantitative tool for the experimental identification and analysis of the Fermi-liquid state using optical spectroscopy, and a powerful method for the identification of alternative states of matter, when applicable., Published version