Predicting polarization and nonlinear dielectric response of arbitrary perovskite superlattice sequences

TL;DR

This paper develops a first-principles modeling approach to predict the nonlinear dielectric response of arbitrary ferroelectric superlattices, enabling tailored design of materials with specific polarization properties.

Contribution

The authors introduce a method that uses layer-specific Wannier-based polarizations to accurately predict the nonlinear dielectric behavior of complex superlattice sequences.

Findings

Successfully applied to SrTiO₃, CaTiO₃, BaTiO₃ superlattices

Provides a predictive model for arbitrary superlattice sequences

Enhances understanding of ferroelectric multilayer responses

Abstract

We carry out first-principles calculations of the nonlinear dielectric response of short-period ferroelectric superlattices. We compute and store not only the total polarization, but also the Wannier-based polarizations of individual atomic layers, as a function of electric displacement field, and use this information to construct a model capable of predicting the nonlinear dielectric response of an arbitrary superlattice sequence. We demonstrate the successful application of our approach to superlattices composed of SrTiO$_3$, CaTiO$_3$, and BaTiO$_3$ layers.