arXiv subjects

Gabriel Kotliar

Publications and source records attributed to Gabriel Kotliar.

At least 55 records · Page 3Linked to original sources

arXiv2020

Accelerated impurity solver for DMFT and its diagrammatic extensions

We present ComCTQMC, a GPU accelerated quantum impurity solver. It uses the continuous-time quantum Monte Carlo (CTQMC) algorithm wherein the partition function is expanded in terms of the hybridisation function (CT-HYB). ComCTQMC supports both partition and worm-space measurements, and it uses improved estimators and the reduced density matrix to improve observable measurements whenever possible. ComCTQMC efficiently measures all one and two-particle Green's functions, all static observables which commute with the local Hamiltonian, and the occupation of each impurity orbital. ComCTQMC can solve complex-valued impurities with crystal fields that are hybridized to both fermionic and bosonic baths. Most importantly, ComCTQMC utilizes graphical processing units (GPUs), if available, to dramatically accelerate the CTQMC algorithm when the Hilbert space is sufficiently large. We demonstrate acceleration by a factor of over 600 (100) in a simulation of $δ$-Pu at 600 K with (without) crystal fields. In easier problems, the GPU offers less impressive acceleration or even decelerates the CTQMC. Here we describe the theory, algorithms, and structure used by ComCTQMC in order to achieve this set of features and level of acceleration.

cond-mat.str-el↗

arXiv2020

Vacancy defect control of colossal thermopower in FeSb2

Iron diantimonide is a material with the highest known thermoelectric power. By combining scanning transmission electron microscope study with electronic transport neutron, X-ray scattering and first principle calculation we identify atomic defects that control colossal thermopower magnitude and nanoprecipitate clusters with Sb vacancy ordering which induce additional phonon scattering and substantially reduce thermal conductivity. Defects are found to cause rather weak but important monoclinic distortion of the unit cell Pnnm to Pm. The absence of Sb along [010] for high defect concentration forms conducting path due to Fe d orbital overlap. The connection between atomic defect anisotropy and colossal thermopower in FeSb2 paves the way for the understanding and tailoring of giant thermopower in related materials.

cond-mat.mtrl-sci↗

arXiv2020

Extending the Gutzwiller approximation to intersite interactions

We develop an extension of the Gutzwiller Approximation (GA) formalism that includes the effects of Coulomb interactions of arbitrary range (including density density, exchange, pair hopping and Coulomb assisted hopping terms). This formalism reduces to the ordinary GA formalism for the multi-band Hubbard models in the presence of only local interactions. This is accomplished by combining the 1/z expansion -- where z is the coordination number and only the leading order terms contribute in the limit of infinite dimensions -- with a P^2-I expansion, where P is the Gutzwiller projector. The method is conveniently formulated in terms of a Gutzwiller Lagrange function. We apply our theory to the extended single band Hubbard model. Similarly to the usual Brinkman-Rice mechanism we find a Mott transition. A valence skipping transition is observed, where the occupation of the empty and doubly occupied states for the Gutzwiller wavefunction is enhanced with respect to the uncorrelated Slater determinant wavefunction.

cond-mat.str-el↗

arXiv2020

Fermi liquid theory and divergences of the two-particle irreducible vertex in the periodic Anderson lattice

Here we analyze the divergences of the irreducible vertex function in dynamical mean field theory, which may indicate either a non-physical breakdown of the perturbation theory or a response to some physical phenomenon. To investigate this question, we construct a quasiparticle vertex from the diverging irreducible vertex functions. This vertex describes the scattering between quasiparticles and quasiholes in a Fermi liquid. We show that the quasparticle vertex \textit{does not} diverge in the charge channel, wherein the irreducible vertex \textit{does} diverge; and we show that the quasiparticle vertex does diverge in the spin channel, wherein the irreducible vertex does not diverge. This divergence occurs at the Mott transition wherein the Fermi liquid theory breaks down. Both Hubbard and Anderson lattices are investigated. In general, our results support that the divergences of the irreducible vertex function do not indicate a non-physical failure of the perturbation theory. Instead, the divergences are the mathematical consequence of inverting a matrix (the local charge susceptibility) which accumulates increasingly negative diagonal elements as the Hubbard interaction suppresses charge fluctuations. Indeed, we find that the first symmetric divergences of the irreducible vertex in both Hubbard and Anderson lattices occurs near the maximum magnitude of the (negative) vertex-connected part of the charge susceptibility, which suppresses charge fluctuations.

cond-mat.str-el↗

arXiv2020

Orbital differentiation in Hund metals

Orbital differentiation is a common theme in multiorbital systems, yet a complete understanding of it is still missing. Here, we consider a minimal model for orbital differentiation in Hund metals with a highly accurate method: We use the numerical renormalization group as a real-frequency impurity solver for a dynamical mean-field study of three-orbital Hubbard models, where a crystal field shifts one orbital in energy. The individual phases are characterized with dynamic correlation functions and their relation to diverse Kondo temperatures. Upon approaching the orbital-selective Mott transition, we find a strongly suppressed spin coherence scale and uncover the emergence of a singular Fermi liquid and interband doublon-holon excitations. Our theory describes the diverse polarization-driven phenomena in the $t_{2g}$ bands of materials such as ruthenates and iron-based superconductors, and our methodological advances pave the way towards real-frequency analyses of strongly correlated materials.

cond-mat.str-el↗

arXiv2019

Low energy band structure and symmetries of UTe2 from angle resolved photoemission spectroscopy

The compound UTe2 has recently been shown to realize spin triplet superconductivity from a non-magnetic normal state. This has sparked intense research activity, including theoretical analyses that suggest the superconducting order parameter to be topologically nontrivial. However, the underlying electronic band structure is a critical factor for these analyses, and remains poorly understood. Here, we present high resolution angle resolved photoemission (ARPES) measurements covering multiple planes in the 3D Brillouin zone of UTe2, revealing distinct Fermi-level features from two orthogonal quasi-one dimensional light electron bands and one heavy band. The electronic symmetries are evaluated in comparison with numerical simulations, and the resulting picture is discussed as a platform for unconventional many-body order.

cond-mat.str-el↗

arXiv2019

Orbital-selective Kondo-lattice and enigmatic f-electrons emerging from inside the antiferromagnetic phase of a heavy fermion

Novel electronic phenomena frequently form in heavy fermions as a consequence of the mutual nature of localization and itineracy of f electrons. On the magnetically ordered side of the heavy fermion phase diagram, f moments are expected to be localized and decoupled from the Fermi surface. It remains ambiguous whether a Kondo lattice can develop inside the magnetically ordered phase. Using spectroscopic imaging with the scanning tunneling microscope, complemented by neutron scattering, x ray absorption spectroscopy, and dynamical mean field theory, we probe the electronic states in the antiferromagnetic USb2 as a function of temperature. We visualize a large gap in the antiferromagnetic phase at high temperatures, T lower than TN 200 K, within which Kondo hybridization gradually develops below Tcoh 80 K. Our dynamical mean field theory calculations indicate the antiferromagnetism and Kondo lattice to reside predominantly on different f orbitals, promoting orbital selectivity as a new conception into how these two phenomena coexist in heavy fermions. Finally, at Tstar 45 K we discover a novel 1st order like electronic transition through the abrupt emergence of non trivial 5f electronic states that may share some resemblance to the hidden order phase of URu2Si2.

cond-mat.str-el↗

arXiv2019

ComDMFT: a Massively Parallel Computer Package for the Electronic Structure of Correlated-Electron Systems

ComDMFT is a massively parallel computational package to study the electronic structure of correlated-electron systems (CES). Our approach is a parameter-free method based on ab initio linearized quasiparticle self-consistent GW (LQSGW) and dynamical mean field theory (DMFT). The non-local part of the electronic self-energy is treated within ab initio LQSGW and the local strong correlation is treated within DMFT. In addition to ab initio LQSGW+DMFT, charge self-consistent LDA+DMFT methodology is also implemented, enabling multiple methods in one open-source platform for the electronic structure of CES. This package can be extended for future developments to implement other methodologies to treat CES

cond-mat.str-el↗

arXiv2019

High temperature singlet-based magnetism from Hund's rule correlations

Uranium compounds can manifest a wide range of fascinating many-body phenomena, and are often thought to be poised at a crossover between localized and itinerant regimes for 5f electrons. The antiferromagnetic dipnictide USb2 has been of recent interest due to the discovery of rich proximate phase diagrams and unusual quantum coherence phenomena. Here, linear-dichroic X-ray absorption and elastic neutron scattering are used to characterize electronic symmetries on uranium in USb2 and isostructural UBi2. Of these two materials, only USb2 is found to enable strong Hund's rule alignment of local magnetic degrees of freedom, and to undergo distinctive changes in local atomic multiplet symmetry across the magnetic phase transition. Theoretical analysis reveals that these and other anomalous properties of the material may be understood by attributing it as the first known high temperature realization of a singlet ground state magnet, in which magnetism occurs through a process that resembles exciton condensation.

cond-mat.str-el↗

arXiv2019

Energy Scales of the Doped Anderson Lattice Model

This paper explores the energy scales of the doped Anderson lattice model using dynamical mean-field theory (DMFT), using a continuous-time Quantum Monte Carlo (CTQMC) impurity solver. We show that the low temperature properties of the lattice can not be scaled using the single ion local Kondo temperature $T_K$ but instead are governed by a doping-dependent coherence temperature $T*$ which can be used to scale the temperature dependence of the spectral function, transport properties, and entropy. At half filling $T*$ closely approximates the single ion $T_K$, but as the filling $n_c$ is reduced to zero, $T*$ also vanishes. The coherence temperature $T*$ is shown to play a role of effective impurity Kondo temperature in the lattice model, and physical observables show significant evolution at $T*$. In the DMFT framework, we showed that the hybridization strength of the effective impurity model is qualitatively affected by the doping level, and determines $T*$ in the lattice model.

cond-mat.str-el↗

arXiv2019

Correlated materials design: prospects and challenges

The design of correlated materials challenges researchers to combine the maturing, high throughput framework of DFT-based materials design with the rapidly-developing first-principles theory for correlated electron systems. We review the field of correlated materials, distinguishing two broad classes of correlation effects, static and dynamics, and describe methodologies to take them into account. We introduce a material design workflow, and illustrate it via examples in several materials classes, including superconductors, charge ordering materials and systems near an electronically driven metal to insulator transition, highlighting the interplay between theory and experiment with a view towards finding new materials. We review the statistical formulation of the errors of currently available methods to estimate formation energies. Correlation effects have to be considered in all the material design steps. These include bridging between structure and property, obtaining the correct structure and predicting material stability. We introduce a post-processing strategy to take them into account.

cond-mat.str-el↗

arXiv2019

Signatures of Mottness and Hundness in archetypal correlated metals

Physical properties of multi-orbital materials depend not only on the strength of the effective interactions among the valence electrons but also on their type. Strong correlations are caused by either Mott physics that captures the Coulomb repulsion among charges, or Hund physics that aligns the spins in different orbitals. We identify four energy scales marking the onset and the completion of screening in orbital and spin channels. The differences in these scales, which are manifest in the temperature dependence of the local spectrum and of the charge, spin and orbital susceptibilities, provide clear signatures distinguishing Mott and Hund physics. We illustrate these concepts with realistic studies of two archetypal strongly correlated materials, and corroborate the generality of our conclusions with a model Hamiltonian study.

cond-mat.str-el↗

arXiv2019

Material design of indium based compounds: possible candidates for charge, valence, and bond disproportionation and superconductivity

We design and investigate the physical properties of new indium compounds AInX$_{3}$ (A = alkali metals, X = F or Cl). We find nine new In based materials in their ground state and are thermodynamically stable but are not reported in ICSD (Inorganic Crystal Structure Database). We also discuss several metastable structures. This new series of materials display multiple valences, charge and bond disproportionation, and dimerization. The most common valence of In is 3+. We also find two rare alternatives, one has In$^{2+}$ with In-In dimerization and the other shows valence disproportionation to In$^{1+}$ and In$^{3+}$ with bond disproportionation. We study the possibility of superconductivity in these new In compounds and find that CsInF$_{3}$ has a transition temperature about 24 K with sufficient hole doping and pressure.

cond-mat.mtrl-sci↗

arXiv2018

Rotationally invariant slave-boson and density matrix embedding theory: A unified framework and a comparative study on the 1D and 2D Hubbard Model

We present detailed benchmark ground-state calculations of the one- and two-dimensional Hubbard model utilizing the cluster extensions of the rotationally invariant slave-boson (RISB) mean-field theory and the density matrix embedding theory (DMET). Our analysis shows that the overall accuracy and the performance of these two methods are very similar. Furthermore, we propose a unified computational framework that allows us to implement both of these techniques on the same footing. This provides us with a new line of interpretation and paves the ways for developing systematically new generalizations of these complementary approaches.

cond-mat.str-el↗

arXiv2018

Hundness versus Mottness in a three-band Hubbard-Hund model: On the origin of strong correlations in Hund metals

Hund metals are multi-orbital systems with moderate Coulomb interaction, $U$, and sizeable Hund's rule coupling, $J<U$, that aligns the spins in different orbitals. They show strong correlation effects, like very low Fermi-liquid coherence scales and intriguing incoherent transport regimes, resulting in bad metallic behavior. But to what extent are these strong correlations governed by Mottness, i.e. the blocking of charge fluctuations close to a Mott insulator transition (MIT) induced by $U$, or by Hundness, a new route towards strong correlations induced by $J$? To answer this question, we study the full phase diagram of a degenerate three-band Hubbard-Hund model on a Bethe lattice at zero temperature using single-site DMFT and the numerical renormalization group as efficient real-frequency multi-band impurity solver. Hund metal behavior occurs in this minimal model for a filling close to $n_d=2$, moderate $U$ and sizeable $J$, the "Hund-metal regime", with strong correlations manifest by a low quasiparticle weight, $Z$. We show that "spin-orbital separation" (SOS) is a generic $J$-induced feature in the whole metallic regime of the phase diagram for $1<n_d<3$ and sizeable $J$: orbital screening occurs at much higher energies than spin screening, below which Fermi-liquid behavior sets in. The low $Z$ can then be explained in terms of the $J$-reduced Fermi-liquid scale. We further show that, in the Hund-metal regime, far from any MIT, Hundness -- the localization of large spins -- is the key player to induce strong correlations. There, physical properties are governed by a broad incoherent energy regime of SOS with intriguing Hund metal physics: large, almost unscreened spins are coupled to screened orbital degrees of freedom.

cond-mat.str-el↗

arXiv2018

Significant change in the electronic behavior associated with structural distortions in the single crystalline SrAg4As2

We report a combined study of transport and thermodynamic measurements on the layered pnictide material SrAg4As2. Upon cooling, a drop in electrical and Hall resistivity, a jump in heat capacity and an increase in susceptibility and magnetoresistance (MR) are observed around 110 K. These observations suggest that non-magnetic phase transitions emerge at around 110 K, that are likely associated with structural distortions. In sharp contrast with the first-principles calculations based on the crystal structure at room temperature, quantum oscillations reveal small Fermi pockets with light effective masses, suggesting a significant change in the Fermi surface topology caused by the low temperature structural distortion. No superconductivity emerges in SrAg$_4$As$_2$ down to 2 K and under pressures up to 2.13 GPa; instead, the low temperature structural distortion increases linearly with temperature at a rate of ~13 K/GPa above 0.89 GPa.

cond-mat.str-el↗

arXiv2018

Pairing Mechanism in Hunds Metal Superconductors and the Universality of the Superconducting Gap to Critical Temperature Ratio

We analyze a simple model containing the physical ingredients of a Hund's metal, the local spin fluctuations with power-law correlators, $(Ω_0/|Ω|)^γ$, with $γ$ greater than one, interacting with electronic quasiparticles. While the critical temperature and the gap change significantly with varying parameters, the $2Δ_{max}/k_BT_c$ remains close to twice the BCS value in agreement with experimental observations in the iron-based superconductors (FeSC).

cond-mat.supr-con↗

arXiv2018

Renormalized dispersing multiplets in the spectrum of nearly Mott localized systems

The spectrum of the strongly correlated systems usually shows resonant peaks at finite energy, with examples in the 115 Ce family which are reproduced by the dynamical mean-field theory. A similar structure has been seen recently in the orbitally selective Mott (OSM) phase of two-band model, known as doublon-holon bound state, with implications on the fate of such phase in the zero Hund's coupling limit. We show that these features can be captured with the slave-particle methods once their Hilbert space is taken into account. We use slave-spin calculations, justifiable in the limit of large dimensions, to explicitly demonstrate this and compare the results with dynamical mean-field theory.

cond-mat.str-el↗