Comparative first-principles studies of prototypical ferroelectric materials by LDA, GGA, and SCAN meta-GGA

Abstract

Originating from a broken spatial inversion symmetry, ferroelectricity is a functionality of materials with an electric dipole that can be switched by external electric fields. Spontaneous polarization is a crucial ferroelectric property, and its amplitude is determined by the strength of polar structural distortions. Density functional theory (DFT) is one of the most widely used theoretical methods to study ferroelectric properties, yet it is limited by the levels of approximations in electron exchange-correlation. On the one hand, the local density approximation (LDA) is considered to be more accurate for the conventional perovskite ferroelectrics such as BaTiO3 and PbTiO3 than the generalized gradient approximation (GGA), which suffers from the so-called super-tetragonality error. On the other hand, GGA is more suitable for hydrogen-bonded ferroelectrics than LDA, which largely overestimates the strength of hydrogen bonding in general. We show here that the recently developed general-purpose strongly constrained and appropriately normed (SCAN) meta-GGA functional significantly improves over the traditional LDA/GGA for structural, electric, and energetic properties of diversely-bonded ferroelectric materials with a comparable computational effort, and thus enhances largely the predictive power of DFT in studies of ferroelectric materials. We also address the observed system-dependent performances of LDA and GGA for ferroelectrics from a chemical bonding point of view.

23 pages, 7 figures, 5 tables, 137 references

References in corpus (5)

• First-principles study of spontaneous polarization in multiferroic BiFeO${}_3$
• Weak ferromagnetism and magnetoelectric coupling in bismuth ferrite
• Very large spontaneous electric polarization in BiFeO3 single crystals at room temperature and its evolution under cycling fields
• Hybrid exchange-correlation functional for accurate prediction of the electronic and structural properties of ferroelectric oxides
• The Individual and Collective Effects of Exact Exchange and Dispersion Interactions on the Ab Initio Structure of Liquid Water

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