Dielectric, piezoelectric, and elastic properties of BaTiO$_3$/SrTiO$_3$ ferroelectric superlattices from first principles

TL;DR

This study uses first-principles calculations to explore how epitaxial strain influences the structural, dielectric, piezoelectric, and elastic properties of BaTiO3/SrTiO3 superlattices, revealing phase transitions and stability insights.

Contribution

It provides a detailed first-principles analysis of strain-induced phase transitions and property changes in BaTiO3/SrTiO3 superlattices, including stability comparisons with disordered solid solutions.

Findings

Phase transitions under strain from monoclinic to tetragonal and orthorhombic phases.

Critical divergence of dielectric, piezoelectric, and elastic tensor components at phase boundaries.

Superlattices are thermodynamically stable with tendencies for short-range ordering.

Abstract

The effect of epitaxial strain on the phonon spectra, crystal structure, spontaneous polarization, dielectric, piezoelectric, and elastic properties of (001)-oriented ferroelectric (BaTiO$_3$)$_m$/(SrTiO$_3$)$_n$ superlattices ($m = n = {}$1-4) was studied using the first-principles density-functional theory. The ground state of free-standing superlattices is the monoclinic $Cm$ polar phase. Under the in-plane biaxial compressive strain, it transforms to tetragonal $P4mm$ polar phase, and under the in-plane biaxial tensile strain, it transforms to orthorhombic $Amm2$ polar phase. When changing the in-plane lattice parameter, a softening of several optical and acoustic modes appears at the boundaries between the polar phases, and corresponding components of dielectric, piezoelectric, and elastic tensors diverge critically. The comparison of the mixing enthalpy of disordered Ba$_{0.5}$Sr$_{0.5}$TiO$_3$ solid solution modeled using two special quasirandom structures SQS-4 with the mixing enthalpy of the superlattices reveals a tendency of the BaTiO$_3$-SrTiO$_3$ system to short-range ordering and shows that these superlattices are thermodynamically quite stable.