Hybrid exchange-correlation functional for accurate prediction of the electronic and structural properties of ferroelectric oxides

Abstract

Using a linear combination of atomic orbitals approach, we report a systematic comparison of various Density Functional Theory (DFT) and hybrid exchange-correlation functionals for the prediction of the electronic and structural properties of prototypical ferroelectric oxides. It is found that none of the available functionals is able to provide, at the same time, accurate electronic and structural properties of the cubic and tetragonal phases of BaTiO${}_3$ and PbTiO${}_3$. Some, although not all, usual DFT functionals predict the structure with acceptable accuracy, but always underestimate the electronic band gaps. Conversely, common hybrid functionals yield an improved description of the band gaps, but overestimate the volume and atomic distortions associated to ferroelectricity, giving rise to an unacceptably large $c/a$ ratio for the tetragonal phases of both compounds. This super-tetragonality is found to be induced mainly by the exchange energy corresponding to the Generalized Gradient Approximation (GGA) and, to a lesser extent, by the exact exchange term of the hybrid functional. We thus propose an alternative functional that mixes exact exchange with the recently proposed GGA of Wu and Cohen [Phys. Rev. B 73, 235116 (2006)] which, for solids, improves over the treatment of exchange of the most usual GGA's. The new functional renders an accurate description of both the structural and electronic properties of typical ferroelectric oxides.

13 pages, 4 figures, 7 tables

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• Phase transitions in BaTiO${}_3$ from first principles
• The physics of dynamical atomic charges: the case of ABO3 compounds
• Ab initio statistical mechanics of the ferroelectric phase transition in PbTiO3
• First Principles Investigation of Ferromagnetism and Ferroelectricity in Bismuth Manganite
• Density-Polarization Functional Theory of the response of a periodic insulating solid to an electric field.
• Systematic trends in the electronic structure parameters of 4d transition metal oxides SrMO_{3} (M = Zr, Mo, Ru, and Rh)
• Comparing the Weighted Density Approximation with the LDA and GGA for Ground State Properties of Ferroelectric Perovskites
• The long-wavelength behaviour of the exchange-correlation kernel in the Kohn-Sham theory of periodic systems
• First-principles calculation of the band offset at BaO/BaTiO${}_3$ and SrO/SrTiO${}_3$ interfaces
• Applications of the generalized gradient approximation to ferroelectric perovskites
• Strong-correlation effects in Born effective charges

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