Tunability of the dielectric response of epitaxially strained SrTiO3 from first principles

TL;DR

This study uses first-principles calculations to explore how in-plane strain affects the nonlinear dielectric properties of SrTiO3 thin films, revealing strain-dependent tunability relevant for device applications.

Contribution

It provides a detailed first-principles analysis of strain effects on dielectric tunability in SrTiO3, including phonons and polarization under electric fields.

Findings

Dielectric tunability varies significantly with tensile and compressive strains.

Strain influences phonon frequencies and Born effective charges.

Results align with recent experimental observations.

Abstract

The effect of in-plane strain on the nonlinear dielectric properties of SrTiO3 epitaxial thin films is calculated using density-functional theory within the local-density approximation. Motivated by recent experiments, the structure, zone-center phonons, and dielectric properties with and without an external electric field are evaluated for several misfit strains within +-3% of the calculated cubic lattice parameter. In these calculations, the in-plane lattice parameters are fixed, and all remaining structural parameters are permitted to relax. The presence of an external bias is treated approximately by applying a force to each ion proportional to the electric field. After obtaining zero-field ground state structures for various strains, the zone-center phonon frequencies and Born effective charges are computed, yielding the zero-field dielectric response. The dielectric response at finite electric field bias is obtained by computing the field dependence of the structure and polarization using an approximate technique. The results are compared with recent experiments and a previous phenomenological theory. The tunability is found to be strongly dependent on the in-plane lattice parameter, showing markedly different behavior for tensile and compressive strains. Our results are expected to be of use for isolating the role of strain in the tunability of real ultrathin epitaxial films.