Thermodynamics and dielectric response of ${\text{BaTiO}}_3$ by data-driven modeling

Abstract

Modeling ferroelectric materials from first principles is one of the successes of density-functional theory, and the driver of much development effort, requiring an accurate description of the electronic processes and the thermodynamic equilibrium that drive the spontaneous symmetry breaking and the emergence of macroscopic polarization. We demonstrate the development and application of an integrated machine learning model that describes on the same footing structural, energetic and functional properties of barium titanate (${\text{BaTiO}}_3$), a prototypical ferroelectric. The model uses ab initio calculations as reference and achieves accurate yet inexpensive predictions of energy and polarization on time and length scales that are not accessible to direct ab initio modeling. These predictions allow us to assess the microscopic mechanism of the ferroelectric transition. The presence of an order-disorder transition for the Ti off-centered states is the main driver of the ferroelectric transition, even though the coupling between symmetry breaking and cell distortions determines the presence of intermediate, partly-ordered phases. Moreover, we thoroughly probe the static and dynamical behavior of ${\text{BaTiO}}_3$ across its phase diagram, without the need to introduce a coarse-grained description of the ferroelectric transition. Finally, we apply the polarization model to calculate dielectric response properties of the material in a fully ab initio manner, again reproducing the correct qualitative experimental behaviour.

26 pages, 14 figures

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Cited by in corpus (8)

• Ab initio structural optimization at finite temperatures based on anharmonic phonon theory: Application to the structural phase transitions of BaTiO${}_3$
• Adaptive energy reference for machine-learning models of the electronic density of states
• Real Space Visualization of Order-Disorder Transition in BaTiO3
• Graph-neural-network predictions of solid-state NMR parameters from spherical tensor decomposition
• Role of long-range dipolar interactions in the simulation of the properties of polar crystals using effective atomic potentials
• Ferroelectric Properties and Topological Polar Textures of PbTiO${}_3$ from a Second-Principles Open-Source Interatomic Potential
• Ultrafast polarization switching in BaTiO${}_3$ by photoactivation of its ferroelectric and central modes
• The thermodynamics of CaSiO3 in Earth's lower mantle