Free energy from stationary implementation of the DFT+DMFT functional

Abstract

The stationary functional of the all-electron density functional plus dynamical mean field theory (DFT+DMFT) formalism to perform free energy calculations and structural relaxations is implemented for the first time. Here, the first order error in the density leads to a much smaller, second order error in the free energy. The method is applied to several well known correlated materials; metallic SrVO${}_3$, Mott insulating FeO, and elemental Cerium, to show that it predicts the lattice constants with very high accuracy. In Cerium, we show that our method predicts the iso-structural transition between the $\alpha$ and $\gamma$ phases, and resolve the long standing controversy in the driving mechanism of this transition.

References in corpus (13)

• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Continuous-time Monte Carlo methods for quantum impurity models
• Quantum Monte Carlo Impurity Solver for Cluster DMFT and Electronic Structure Calculations in Adjustable Base
• Exact double-counting in combining the Dynamical Mean Field Theory and the Density Functional Theory
• Self-consistency over the charge-density in dynamical mean-field theory: a linear muffin-tin implementation and some physical implications
• Thermodynamic and spectral properties of compressed Ce calculated by the merger of the local density approximation and dynamical mean field theory
• Computing total energies in complex materials using charge self-consistent DFT+DMFT
• 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
• Electronic properties and magnetism of iron at the Earth's inner core conditions
• Interplay of spin-orbit and entropic effects in Cerium

Cited by in corpus (68)

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• Thermal Energy Transport in Oxide Nuclear Fuel
• Forces for Structural Optimizations in Correlated Materials within DFT+Embedded DMFT Functional Approach
• Applications of DFT+DMFT in Materials Science
• Mott metal-insulator transitions in pressurized layered trichalcogenides
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• Magnetic Collapse and the Behavior of Transition Metal Oxides at High Pressure
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• ComDMFT: a Massively Parallel Computer Package for the Electronic Structure of Correlated-Electron Systems
• Correlated materials design: prospects and challenges
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• Reliability and applicability of magnetic force linear response theory: Numerical parameters, predictability, and orbital resolution
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• Nature of the 5$f$ electronic structure of plutonium
• Emergence of quantum critical charge and spin-state fluctuations near the pressure-induced Mott transition in MnO, FeO, CoO, and NiO
• The phonon softening due to melting of the ferromagnetic order in elemental iron
• Correlated Electronic Structure and Incipient Flat Bands of the Kagome Superconductor CsCr3Sb5
• Spectroscopic and first principle DFT+eDMFT study of complex structural, electronic, and vibrational properties of $M_2$Mo${}_3$O${}_8$ ($M$=Fe, Mn) polar magnets
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• Role of Entropy and Structural Parameters in the Spin State Transition of LaCoO${}_3$
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• LDA+DMFT approach to ordering phenomena and the structural stability of correlated materials
• Correlation-corrected band topology and topological surface states in iron-based superconductors
• Diatomic molecule as a testbed for combining DMFT with electronic structure methods such as $GW$ and DFT
• Charge self-consistent electronic structure calculations with dynamical mean-field theory using Quantum ESPRESSO, Wannier90 and TRIQS
• Compositional phase stability of correlated electron materials within DFT+DMFT
• Molecular Mott state in the deficient spinel GaV${}_4$S${}_8$
• Efficient computational screening of strongly correlated materials -- Multi-orbital phenomenology within the ghost Gutzwiller approximation
• Calculating DMFT forces in ab-initio ultrasoft pseudopotential formalism
• Correlation-Induced Octahedral Rotations in SrMoO${}_3$
• Topological Phase Transition in an Archetypal f-electron Correlated System: Ce
• Magnetic ground state of SrRuO${}_3$ thin film and applicability of standard first-principles approximations to metallic magnetism
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• Correlation Driven Phonon Anomalies in Bulk FeSe
• Heavy-fermions in frustrated Hund's metal with portions of incipient flat-bands
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• Analytic continuation-free Green's function approach to correlated electronic structure calculations
• Studying the occupied and unoccupied electronic structure of LaCoO${}_3$ by using DFT+embedded DMFT method with the calculated value of $\text{U}$
• Superconductivity of cerium under pressures up to 54GPa
• Experimental and computational approaches to study the high temperature thermoelectric properties of novel topological semimetal CoSi
• Dichotomy in Low- and High-energy Band Renormalizations in Trilayer Nickelate $L{a}_{4}N{i}_3{O}_{10}$: a Comparison with Cuprates
• Quantum embedding for molecules using auxiliary particles -- The ghost Gutzwiller Ansatz
• Electronic correlations in dense iron: from moderate pressure to Earth's core conditions
• Self-Consistent Determination of Single-Impurity Anderson Model Using Hybrid Quantum-Classical Approach on a Spin Quantum Simulator
• Entropy and electronic orders of the three-orbital Hubbard model with antiferromagnetic Hund coupling
• A "hidden" transition in heavy fermion compound CeB${}_6$ at $T\sim$ 20 K?
• Novel $J_{\mathrm{eff}}$=3/2 Metallic Phase and Unconventional Superconductivity in GaTa${}_4$Se${}_8$
• Boson Slave Solver (BoSS) v1.1
• Electronic Correlation Effects on Stabilizing a Perfect Kagome Lattice and Ferromagnetic Fluctuation in LaRu${}_3$Si${}_2$
• Anderson impurity solver integrating tensor network methods with quantum computing
• Impact of electronic correlations on the superconductivity of high-pressure CeH${}_9$
• Charge self-consistent density functional theory plus ghost rotationally-invariant slave-boson theory for correlated materials
• Impact of strong electronic correlations on altermagnets: the case of NiS2
• Correlated electronic structure of high-temperature superconductor Ba${}_2$CuO${}_{3+\delta }$
• Internal consistency of multi-tier $GW$+EDMFT
• Stability and diffusion of oxygen vacancies in LaNiO${}_3$: a DMFT study
• Ghost Embedding Bridging Chemistry and One-Body Theories
• Phase transitions of correlated systems from graph neural networks with quantum embedding techniques
• Correlation-driven phonon renormalisation and the equation of state of $\gamma$-cerium
• Symmetry-breaking-induced topology in FeSe
• Charge disproportionation as a possible mechanism towards polar antiferromagnetic metal in molecular orbital crystal
• Self-Consistent Coulomb Interactions from Constrained Dynamical Mean-Field Theory
• Relevance of long-range screening in Mott transition examined via a hydrogen lattice
• Many-body electronic structure, self-doped double-exchange, and Hund metallicity in 1T-CrTe2 bulk and monolayer