Ab-initio Gutzwiller method: first application to Plutonium

TL;DR

This paper introduces an ab-initio Gutzwiller method tailored for strongly correlated electron systems, demonstrated through its initial application to Plutonium, aiming to improve the accuracy of electronic structure calculations beyond standard DFT approaches.

Contribution

It presents a novel ab-initio Gutzwiller approach specifically designed for complex correlated materials, with the first application to Plutonium to address limitations of existing methods.

Findings

Successfully applied to Plutonium, capturing its complex electronic behavior.

Provides a more accurate description of localized $f$-electron systems.

Outperforms traditional DFT-LDA in strongly correlated regimes.

Abstract

Except for small molecules, it is impossible to solve many electrons systems without imposing severe approximations. If the configuration interaction approaches (CI) or Coupled Clusters techniques \cite{FuldeBook} are applicable for molecules, their generalization for solids is difficult. For materials with a kinetic energy greater than the Coulomb interaction, calculations based on the density functional theory (DFT), associated with the local density approximation (LDA) \cite{Hohenberg64, Kohn65} give satisfying qualitative and quantitative results to describe ground state properties. These solids have weakly correlated electrons presenting extended states, like $sp$ materials or covalent solids. The application of this approximation to systems where the wave functions are more localized ($d$ or $f$-states) as transition metals oxides, heavy fermions, rare earths or actinides is more questionable and can even lead to unphysical results : for example, insulating FeO and CoO are predicted to be metalic by the DFT-LDA...