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

Abstract

An implementation of full self-consistency over the electronic density in the DFT+DMFT framework on the basis of a plane wave-projector augmented wave (PAW) DFT code is presented. It allows for an accurate calculation of the total energy in DFT+DMFT within a plane wave approach. In contrast to frameworks based on the maximally localized Wannier function, the method is easily applied to f electron systems, such as cerium, cerium oxide (Ce2O3) and plutonium oxide (Pu2O3). In order to have a correct and physical calculation of the energy terms, we find that the calculation of the self-consistent density is mandatory. The formalism is general and does not depend on the method used to solve the impurity model. Calculations are carried out within the Hubbard I approximation, which is fast to solve, and gives a good description of strongly correlated insulators. We compare the DFT+DMFT and DFT+U solutions, and underline the qualitative differences of their converged densities. We emphasize that in contrast to DFT+U, DFT+DMFT does not break the spin and orbital symmetry. As a consequence, DFT+DMFT implies, on top of a better physical description of correlated metals and insulators, a reduced occurrence of unphysical metastable solutions in correlated insulators in comparison to DFT+U.

19 pages, 9 figures. This is an author-created, un-copyedited version of an article accepted for publication in Journal of Physics: Condensed Matter. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at doi: 10.1088/0953-8984/24/7/075604

References in corpus (21)

• Electronic Structure Calculations with Dynamical Mean-Field Theory: A Spectral Density Functional Approach
• Dynamical Mean-Field Theory within the Full-Potential Methods: Electronic structure of Ce-115 materials
• Dynamical Mean-Field Theory within an Augmented Plane-Wave Framework: Assessing Electronic Correlations in the Iron Pnictide LaFeAsO
• 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 f-electron challenge: localized and itinerant states in lanthanide oxides united by GW@LDA+U
• 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
• Electronic structure and ionicity of actinide oxides from first principles calculations
• Thermodynamic and spectral properties of compressed Ce calculated by the merger of the local density approximation and dynamical mean field theory
• Construction and solution of a Wannier-functions based Hamiltonian in the pseudopotential plane-wave framework for strongly correlated materials
• Multiple scattering formalism for correlated systems: A KKR+DMFT approach
• Electronic Correlation and Transport Properties of Nuclear Fuel Materials
• Correlation effects in total energy of transition metals and related properties
• General DFT++ method implemented with projector augmented waves: Electronic structure of SrVO${}_3$ and the Mott Transition in Ca${}_{2-x}$Sr${}_x$RuO${}_4$
• Combined local-density and dynamical mean field theory calculations for the compressed lanthanides Ce, Pr, and Nd
• Real-space electronic-structure calculations with full-potential all-electron precision for transition-metals
• Electronic structure and spectral properties of Am, Cm and Bk: Charge density self-consistent LDA+HIA calculations in FP-LAPW basis
• Multiplets Matter: The Electronic Structure of Rare-Earth Semiconductors and Semimetals
• Combining the Hybrid Functional Method with Dynamical Mean-Field Theory
• Dynamical mean field theory of correlated gap formation in Pu monochalcogenides

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