First-principles study of dielectric properties of ferroelectric perovskite oxides with on-site and inter-site Hubbard interactions

Abstract

We study the atomic and electronic structures of ferroelectric perovskite oxides, BaTiO${}_3$, LiNbO${}_3$, and PbTiO${}_3$ using ab initio extended Hubbard functionals in which the on-site and inter-site Hubbard interactions are determined self-consistently, adapted from the pseudohybrid density functional proposed by Agapito-Curtarolo-Buongiorno Nardelli. Band structures, ferroelectric distortions, polarization, Born effective charges, and switching barriers are calculated with extended Hubbard functionals, that are compared with those using local density approximation (LDA), generalized gradient approximation (GGA), and Hybrid (HSE06) functionals. The properties of all three compounds calculated by extended Hubbard functionals are in good agreement with experimental data. We find a substantial increase in band gaps due to the inter-site Coulomb interactions, which show better agreement with $GW$ results compared to those from LDA and GGA functionals. The crucial role of the inter-site Coulomb interactions in restoring the suppressed polar instability, which is computed when only the on-site Hubbard interactions are considered, is also highlighted. Overall, we find that the properties calculated using our extended Hubbard functionals exhibit trends similar to those obtained with the HSE06 functional, while reducing computational costs by over an order of magnitude. Thus, we propose that the current method is well-suited for high-throughput calculations for perovskite oxides, offering significantly improved accuracy in computing band gap and other related physical properties such as the shift current photovoltaic effect and band alignments in ferroelectric heterostructures.

arXiv comment13 pages, 5 figures

References in corpus (38)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Phonons and related properties of extended systems from density-functional perturbation theory
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Physics of thin-film ferroelectric oxides
• First-principles study of spontaneous polarization in multiferroic BiFeO${}_3$
• Weak ferromagnetism and magnetoelectric coupling in bismuth ferrite
• Quantum nonlinear Hall effect induced by Berry curvature dipole in time-reversal invariant materials
• Quasiparticle Self-Consistent GW Theory
• Frequency-dependent local interactions and low-energy effective models from electronic structure calculations
• First-principles theory of ferroelectric phase transitions for perovskites: The case of BaTiO3
• Observation of the nonlinear Hall effect under time reversal symmetric conditions
• Very large spontaneous electric polarization in BiFeO3 single crystals at room temperature and its evolution under cycling fields
• Origin of magnetoelectric behavior in BiFeO${}_3$
• Calculations of Hubbard U from first-principles
• A First-Principles Approach to Insulators in Finite Electric Fields
• Hybrid exchange-correlation functional for accurate prediction of the electronic and structural properties of ferroelectric oxides
• Hubbard parameters from density-functional perturbation theory
• Ab initio statistical mechanics of the ferroelectric phase transition in PbTiO3
• Berry-phase treatment of the homogeneous electric field perturbation in insulators
• Comparative first-principles studies of prototypical ferroelectric materials by LDA, GGA, and SCAN meta-GGA
• Self-consistent Hubbard parameters from density-functional perturbation theory in the ultrasoft and projector-augmented wave formulations
• Extended DFT+U+V method with on-site and inter-site electronic interactions
• Hybrid functional study of proper and improper multiferroics
• Post density functional theoretical studies of highly polar semiconductive Pb(Ti${}_{1-x}$Ni${}_x$)O${}_{3-x}$ solid solutions: The effects of cation arrangement on band gap
• Screening of Coulomb interactions in transition metals
• Efficacy of the DFT+U formalism for modeling hole polarons in perovskite oxides
• Machine Learning for Condensed Matter Physics
• Parameter-free hybrid functional based on an extended Hubbard model: DFT+U+V
• First-principles Calculation of Effective Onsite Coulomb Interaction of 3d Transition Metals: Constrained Local Density Functional Approach with Maximally Localized Wannier Function
• Efficient First-Principles Approach with a Pseudohybrid Density Functional for Extended Hubbard Interactions
• Accurate electronic properties and intercalation voltages of olivine-type Li-ion cathode materials from extended Hubbard functionals
• Electronic structure of pristine and Ni-substituted LaFeO${}_3$ from near edge x-ray absorption fine structure experiments and first-principles simulations
• Importance of intersite Hubbard interactions in $\beta$-MnO${}_2$: A first-principles DFT+$U$+$V$ study
• Understanding the role of Hubbard corrections in the rhombohedral phase of BaTiO${}_3$
• Intersite Coulomb Interactions in Charge Ordered Systems
• Effects of self-consistent extended Hubbard interactions and spin-orbit couplings on energy bands of semiconductors and topological insulators