Gabriel Kotliar

Electronic structure calculations with dynamical mean-field theory

We present a review of the basic ideas and techniques of the spectral density functional theory which are currently used in electronic structure calculations of strongly{correlated materials where the one{electron description breaks down. We illustrate the method with several examples where interactions play a dominant role: systems near metal{insulator transition, systems near volume collapse transition, and systems with local moments.

Peierls distortion as a route to high thermoelectric performance in In4Se3―δ crystals

Thermoelectric energy harvesting—the transformation of waste heat into useful electricity—is of great interest for energy sustainability. The main obstacle is the low thermoelectric efficiency of materials for converting heat to electricity, quantified by the thermoelectric figure of merit, ZT. The best available n-type materials for use in mid-temperature (500–900 K) thermoelectric generators have a relatively low ZT of 1 or less, and so there is much interest in finding avenues for increasing this figure of merit. Here we report a binary crystalline n-type material, In4Se3-δ, which achieves the ZT value of 1.48 at 705 K—very high for a bulk material. Using high-resolution transmission electron microscopy, electron diffraction, and first-principles calculations, we demonstrate that this material supports a charge density wave instability which is responsible for the large anisotropy observed in the electric and thermal transport. The high ZT value is the result of the high Seebeck coefficient and the low thermal conductivity in the plane of the charge density wave. Our results suggest a new direction in the search for high-performance thermoelectric materials, exploiting intrinsic nanostructural bulk properties induced by charge density waves.

Strongly Correlated Materials: Insights From Dynamical Mean-Field Theory

Materials with correlated electrons exhibit some of the most intriguing phenomena in condensed matter physics. A new theoretical framework is now allowing theorists to calculate the electronic structure of these materials, which can exist in a rich variety of phases.

Correlated electrons in δ-plutonium within a dynamical mean-field picture

Given the practical importance of metallic plutonium, there is considerable interest in understanding its fundamental properties. Plutonium undergoes a 25 per cent increase in volume when transformed from its α-phase (which is stable below 400 K) to the δ-phase (stable at around 600 K), an effect that is crucial for issues of long-term storage and disposal. It has long been suspected that this unique property is a consequence of the special location of plutonium in the periodic table, on the border between the light and heavy actinides—here, electron wave–particle duality (or itinerant versus localized behaviour) is important. This situation has resisted previous theoretical treatment. Here we report an electronic structure method, based on dynamical mean-field theory, that enables interpolation between the band-like and atomic-like behaviour of the electron. Our approach enables us to study the phase diagram of plutonium, by providing access to the energetics and one-electron spectra of strongly correlated systems. We explain the origin of the volume expansion between the α- and δ-phases, predict the existence of a strong quasiparticle peak near the Fermi level and give a new viewpoint on the physics of plutonium, in which the α- and δ-phases are on opposite sides of the interaction-driven localization–delocalization transition.

Correlated Electronic Structure of LaO1 xFxFeAs

We compute the electronic structure, momentum resolved spectral function and optical conductivity of the new superconductor LaO1-xFxFeAs within the combination of the density functional theory and dynamical mean field theory. We find that the compound in the normal state is a strongly correlated metal and the parent compound is a bad metal at the verge of the metal insulator transition. We argue that the superconductivity is not phonon mediated.

Correlated electronic structure of LaOFeAs

We compute the electronic structure, momentum resolved spectral function and optical conductivity of the new superconductor LaO1-xFxFeAs within the combination of the density functional theory and dynamical mean field theory. We find that the compound in the normal state is a strongly correlated metal and the parent compound is a bad metal at the verge of the metal insulator transition. We argue that the superconductivity is not phonon mediated.

Two energy scales and two distinct quasiparticle dynamics in the superconducting state of underdoped cuprates

The superconducting temperature Tc of hole-doped high-temperature superconductors has a dome-like shape as a function of hole concentration, with a maximum Tc at ‘optimal’ doping. On the underdoped side, the superconducting state is often described in terms of one energy scale, associated with the maximum of the d-wave gap (at the antinodes), which increases as the doping decreases. Here, we report electronic Raman scattering experiments that show a second energy scale in the gap function: the slope of the gap at the nodes, which decreases with decreasing doping. Our measurements also reveal two distinct quasiparticle dynamics; electronic coherence persists down to low doping levels at the nodes, whereas antinodal quasiparticles become incoherent. Using a sum-rule, we find that the low-frequency Raman response and the temperature dependence of the superfluid density, both controlled by nodal excitations, behave in a qualitatively similar manner with doping variation.

Frequency-dependent local interactions and low-energy effective models from electronic structure calculations

We propose a systematic procedure for constructing effective models of strongly correlated materials. The parameters, in particular the on-site screened Coulomb interaction

The Metal-Insulator Transition in Correlated Disordered Systems

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Fluctuating valence in a correlated solid and the anomalous properties of δ-plutonium

, are calculated from first principles, using the random-phase approximation. We derive an expression for the frequency-dependent