Computing total energies in complex materials using charge self-consistent DFT+DMFT

Abstract

We have formulated and implemented a fully charge-self-consistent density functional theory plus dynamical mean field theory methodology which enables an efficient calculation of the total energy of realistic correlated electron systems. The density functional portion of the calculation uses a plane wave basis set within the projector augmented wave method enabling study of systems with large, complex unit cells. The dynamical mean field portion of the calculation is formulated using maximally localized Wannier functions, enabling a convenient implementation which is independent of the basis set used in the density functional portion of the calculation. The importance of using a correct double counting term is demonstrated. A generalized form of the standard double counting correction, which we refer to as the $U^{\prime }$ form, is described in detail and used. For comparison the density functional plus U method is implemented within the same framework including the generalized double counting. The formalism is validated via a calculation of the metal-insulator and structural phase diagrams of the rare-earth nickelate perovskites as functions of applied pressure and A-site rare-earth ions. The calculated density functional plus dynamical mean field results are found to be consistent with experiment. The density functional plus U method is shown to grossly overestimate the tendency for bond-disproportionation and insulating behavior.

19 pages, 13 figures

References in corpus (15)

• Continuous-time Monte Carlo methods for quantum impurity models
• Quantum Monte Carlo Impurity Solver for Cluster DMFT and Electronic Structure Calculations in Adjustable Base
• Calculations of Hubbard U from first-principles
• Hybridization expansion impurity solver: General formulation and application to Kondo lattice and two-orbital models
• Hubbard U and Hund's Exchange J in Transition Metal Oxides: Screening vs. Localization Trends from Constrained Random Phase Approximation
• Plane-wave based electronic structure calculations for correlated materials using dynamical mean-field theory and projected local orbitals
• Dynamical mean-field theory using Wannier functions: a flexible route to electronic structure calculations of strongly correlated materials
• Self-consistency over the charge-density in dynamical mean-field theory: a linear muffin-tin implementation and some physical implications
• Double Counting in LDA+DMFT - The Example of NiO
• Thermodynamic and spectral properties of compressed Ce calculated by the merger of the local density approximation and dynamical mean field theory
• Two-stage metal-insulator transition in the 2D Hubbard model: momentum selectivity in the 8-site dynamical cluster approximation
• Correlation effects in total energy of transition metals and related properties
• Approaching finite-temperature phase diagrams of strongly correlated materials: a case study for V2O3
• Structural relaxation due to electronic correlations in the paramagnetic insulator KCuF3
• Density functional plus dynamical mean field theory of the metal-insulator transition in early transition metal oxides

Cited by in corpus (7)

• Physics of ultrathin films and heterostructures of rare earth nickelates
• Metal-Insulator Transition and Lattice Instability of Paramagnetic V2O3
• Magnetic Collapse and the Behavior of Transition Metal Oxides at High Pressure
• Density Functional plus Dynamical Mean-Field Theory of the Spin-Crossover Molecule Fe(phen)${}_2$(NCS)${}_2$
• Compositional phase stability of strongly correlated electron materials within DFT+$U$
• Fundamental building blocks of strongly correlated wave functions
• Fundamental invariants of many-body Hilbert space