Octahedral Rotation Induced, Antiferroelectric-like Double Hysteresis in Strained Perovskites

TL;DR

This paper explores how octahedral rotations in strained perovskites induce antiferroelectric-like double hysteresis loops, expanding the understanding of polarization behavior for energy storage applications.

Contribution

It demonstrates the role of octahedral rotation coupling in creating double hysteresis in perovskites using first-principles and Landau-Ginzburg-Devonshire theory.

Findings

Rotation coupling leads to double hysteresis behavior.

Epitaxial strain tunes polarization and rotation interactions.

Expanded material space for antiferroelectric-like properties.

Abstract

Antiferroelectrics, which host both polar and antipolar order parameters, are characterized by the double hysteresis loops which are advantageous for various applications such as high-density energy storage. In this study, we investigate the coupling between oxygen octahedral rotations and polarization in well-known perovskites, with a focus on SrTiO$_3$. Using first-principles calculations and symmetry-adapted Landau-Ginzburg-Devonshire theory, we construct an energy landscape to analyze how this coupling shapes polarization-voltage hysteresis behavior. We show that tuning the relative strength of polar and rotational instabilities by exploiting epitaxial strain and layering leads to nontrivial hysteresis behavior. Consequently, the rotation coupling with polarization leads to an expanded search space of materials exhibiting antiferroelectric-like double hysteresis.