Metastability effects in strained and stressed SrTiO3 films

TL;DR

This study uses first-principles calculations to explore how epitaxial strain and mechanical stress influence phase stability and metastability in SrTiO3 films, revealing complex phase sequences and metastable states.

Contribution

It provides a detailed analysis of phase sequences and metastable phases in SrTiO3 under different boundary conditions, highlighting the role of competing instabilities and octahedral rotations.

Findings

Phase sequences differ under fixed-strain and fixed-stress conditions.

Metastable phases increase under fixed-stress conditions due to competing instabilities.

Octahedral rotation patterns vary significantly in metastable phases.

Abstract

The sequence of ground states for SrTiO3 film subjected to epitaxial strain as well as to mechanical stress along the [001] and [110] axes is calculated from first principles within the density functional theory. Under the fixed-strain boundary conditions, an increase in the lattice parameter of a substrate results in the $I4cm \to I4/mcm \to Ima2 \to Cm \to Fmm2 \to Ima2$(II) sequence of ground states. Under the fixed-stress boundary conditions, the phase sequence is different and depends on how the stress is applied. It is revealed that the simultaneous presence of competing ferroelectric and antiferrodistortive instabilities in SrTiO3 gives rise to the appearance of metastable phases, whose number increases dramatically under the fixed-stress conditions. In the metastable phases, the octahedral rotation patterns are shown to differ substantially from those in the ground state. It is suggested that in systems with competing instabilities, each polar phase has its optimal octahedral rotation pattern which stabilizes this phase and creates a potential barrier preventing this phase to be transformed into other structures.