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 (42)

• Maximally-localized generalized Wannier functions for composite energy bands
• Wannier90: A Tool for Obtaining Maximally-Localised Wannier Functions
• Maximally localized Wannier functions: Theory and applications
• Electronic Structure Calculations with Dynamical Mean-Field Theory: A Spectral Density Functional Approach
• Continuous-time Monte Carlo methods for quantum impurity models
• A continuous-time solver for quantum impurity models
• Dynamical singlets and correlation-assisted Peierls transition in VO2
• Quantum Monte Carlo Impurity Solver for Cluster DMFT and Electronic Structure Calculations in Adjustable Base
• Dynamical Mean-Field Theory within the Full-Potential Methods: Electronic structure of Ce-115 materials
• Calculations of Hubbard U from first-principles
• Hybridization expansion impurity solver: General formulation and application to Kondo lattice and two-orbital models
• Correlated metals and the LDA+U method
• Hubbard U and Hund's Exchange J in Transition Metal Oxides: Screening vs. Localization Trends from Constrained Random Phase Approximation
• Site-selective Mott transition in rare earth nickelates
• 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
• The Cerium volume collapse: Results from the LDA+DMFT approach
• Self-consistency over the charge-density in dynamical mean-field theory: a linear muffin-tin implementation and some physical implications
• The alpha-gamma transition of Cerium is entropy-driven
• Importance of electronic correlations for structural and magnetic properties of the iron pnictide superconductor LaFeAsO
• 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
• Electronic correlations at the alpha-gamma structural phase transition in paramagnetic iron
• Spectral Density Functionals for Electronic Structure Calculations
• Total energy calculations using DFT+DMFT: computing the pressure phase diagram of the rare earth nickelates
• 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
• Covalency in transition metal oxides within all-electron Dynamical Mean Field Theory
• Covalency, double-counting and the metal-insulator phase diagram in transition metal oxides
• 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
• A Self-consistent DFT+DMFT scheme in the Projector Augmented Wave : Applications to Cerium, Ce2O3 and Pu2O3 with the Hubbard I solver and comparison to DFT+U
• Orbital selective Fermi surface shifts and mechanism of high T${}_c$ superconductivity in correlated AFeAs (A=Li,Na)
• Computation of correlation-induced atomic displacements and structural transformations in paramagnetic KCuF3 and LaMnO3
• Evidence for mass renormalization in LaNiO$"" sub 3_: an in situ soft x-ray photoemission study of epitaxial films
• Thermodynamics of the α-γ transition in Cerium from first principles
• First-principles Calculation of Atomic Forces and Structural Distortions in Strongly Correlated Materials
• Density functional plus dynamical mean field theory of the metal-insulator transition in early transition metal oxides
• Covalency and the metal-insulator transition in titanate and vanadate perovskites
• High-frequency asymptotic behavior of self-energies in quantum impurity models
• Interpolative Approach for Solving the Anderson Impurity Model
• Stability of the Ni sites across the pressure-induced metallization in YNiO3

Cited by in corpus (70)

• Physics of ultrathin films and heterostructures of rare earth nickelates
• TRIQS/DFTTools: A TRIQS application for ab initio calculations of correlated materials
• Efficient Implementation of Ab Initio Quantum Embedding in Periodic Systems: Density Matrix Embedding Theory
• Free energy from stationary implementation of the DFT+DMFT functional
• Many-body Electronic Structure of NdNiO${}_2$ and CaCuO${}_2$
• A substantial hybridization between correlated Ni-d orbital and itinerant electrons in infinite-layer nickelates
• Thermal Energy Transport in Oxide Nuclear Fuel
• Applications of DFT+DMFT in Materials Science
• Efficient Formulation of Ab Initio Quantum Embedding in Periodic Systems: Dynamical Mean-Field Theory
• Metal-Insulator Transition and Lattice Instability of Paramagnetic V2O3
• Magnetic Collapse and the Behavior of Transition Metal Oxides at High Pressure
• Metal-insulator transition and local-moment collapse in FeO under pressure
• Rigorous wave function embedding with dynamical fluctuations
• Mott Transition and Magnetism in Rare Earth Nickelates and its Fingerprint on the X-ray Scattering
• Density Functional plus Dynamical Mean-Field Theory of the Spin-Crossover Molecule Fe(phen)${}_2$(NCS)${}_2$
• ComDMFT: a Massively Parallel Computer Package for the Electronic Structure of Correlated-Electron Systems
• Quantifying electronic correlation strength in a complex oxide: a combined DMFT and ARPES study of LaNiO${}_3$
• Correlated materials design: prospects and challenges
• Disentangling lattice and electronic contributions to the metal-insulator transition from bulk vs. layer confined RNiO${}_3$
• Energetics of the coupled electronic-structural transition in the rare-earth nickelates
• DMFTwDFT: An open-source code combining Dynamical Mean Field Theory with various Density Functional Theory packages
• Dependence of DFT+DMFT Results on the Construction of the Correlated Orbitals
• Charge self-consistency in density functional theory + dynamical mean field theory: k-space reoccupation and orbital order
• Energy-weighted density matrix embedding of open correlated chemical fragments
• High-density electron doping of SmNiO${}_3$ from first principles
• Emergence of quantum critical charge and spin-state fluctuations near the pressure-induced Mott transition in MnO, FeO, CoO, and NiO
• DFT+DMFT calculations of the complex band and tunneling behavior for the transition metal monoxides MnO, FeO, CoO and NiO
• Modeling many-body physics with Slave-Spin Mean-Field: Mott and Hund's physics in Fe-superconductors
• Effect of epitaxial strain on the electronic structure and magnetic correlations in infinite-layer (Nd,Sr)NiO${}_2$
• Effective model and electron correlations in trilayer nickelate superconductor La${}_4$Ni${}_3$O${}_{10}$
• Many-body renormalisation of forces in f-electron materials
• Oxygen vacancy induced site-selective mott transition in lanio3
• High photon energy spectroscopy of NiO: experiment and theory
• On the effect of charge self-consistency in DFT+DMFT calculations for complex transition metal oxides
• An electronic origin of charge order in infinite-layer nickelates
• LDA+DMFT approach to ordering phenomena and the structural stability of correlated materials
• DFT+DMFT study of spin-charge-lattice coupling in covalent LaCoO${}_3$
• Data-driven Approach to Parameterize SCAN+U for an Accurate Description of 3d Transition Metal Oxide Thermochemistry
• Compositional phase stability of correlated electron materials within DFT+DMFT
• Strong correlation effects in theoretical STM studies of magnetic adatoms
• Explicit demonstration of the equivalence between DFT+U and the Hartree-Fock limit of DFT+DMFT
• Importance of ligand on-site interactions for the description of Mott-insulators in DFT+DMFT
• Efficient computational screening of strongly correlated materials -- Multi-orbital phenomenology within the ghost Gutzwiller approximation
• Influence of quantum confinement and strain on orbital polarization of four-layer LaNiO${}_3$ superlattices: a DFT+DMFT study
• Magnetic ground state of SrRuO${}_3$ thin film and applicability of standard first-principles approximations to metallic magnetism
• Dynamical Mean-Field Theory of Strongly Correlated Electron Systems
• Compositional phase stability of strongly correlated electron materials within DFT+$U$
• Unusual Mott transition associated with charge-order melting in BiNiO${}_3$ under pressure
• Analytic continuation-free Green's function approach to correlated electronic structure calculations
• Pressure-induced spin-state transition of iron in magnesiowüstite (Fe,Mg)O
• Quantum embedding for molecules using auxiliary particles -- The ghost Gutzwiller Ansatz
• Electronic correlations in dense iron: from moderate pressure to Earth's core conditions
• First-principles study of magnetism and electric field effects in 2D systems
• Electronic correlation, magnetic structure and magnetotransport in few-layer CrI3
• Electronic correlations and long-range magnetic ordering in NiO tuned by pressure
• Valence skipping, internal doping and site-selective Mott transition in PbCoO${}_3$ under pressure
• The tilted-plane structure of the energy of finite quantum systems
• Exploring Metastable States in UO${}_2$ using Hybrid Functionals and Dynamical Mean Field Theory
• Conductivity of infinite-layer NdNiO${}_2$ as a probe of spectator bands
• Magnetic Compton profiles of Ni beyond the one-particle picture: numerically exact and perturbative solvers of dynamical mean-field theory
• Effect of Off-Diagonal Elements in Wannier Hamiltonian on DFT+DMFT for low-symmetry material: Study of Li${}_2$MnO${}_3$
• Delocalized polaron and Burstein-Moss shift induced by Li in $\alpha$-${\text{V}}_2{\text{O}}_5$: DFT+DMFT study
• Many-fermion wave functions: structure and examples
• Fundamental building blocks of strongly correlated wave functions
• Self-energy self-consistent density functional theory plus dynamical mean field theory
• Fundamental invariants of many-body Hilbert space
• Ghost Embedding Bridging Chemistry and One-Body Theories
• Stability and diffusion of oxygen vacancies in LaNiO${}_3$: a DMFT study
• Correlation-driven origin of shallow electron pocket in Co${}_{1/3}$TaS${}_2$ revealed by ARPES and cluster perturbation theory
• Interplay of electronic correlations and chemical bonding in FeN${}_2$ under pressure