Ferroelectric, quantum paraelectric, or paraelectric? Calculating the evolution from <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mi>BaTiO</mml:mi><mml:mn>3</mml:mn></mml:msub></mml:math> to <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mi>SrTiO</mml:mi><mml:mn>3</mml:mn></mml:msub></mml:math> to <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mi>KTaO</mml:mi><mml:mn>3</mml:mn></mml:msub></mml:math> using a single-particle quantum mechanical description of the ions

Abstract

We present an inexpensive first-principles approach for describing quantum paraelectricity that combines density functional theory (DFT) treatment of the electronic subsystem with quantum mechanical treatment of the ions through solution of the single-particle Schr\"odinger equation with the DFT-calculated potential. Using ${\mathrm{BaTiO}}_{3}$, ${\mathrm{SrTiO}}_{3}$, and ${\mathrm{KTaO}}_{3}$ as model systems, we show that the approach can straightforwardly distinguish between ferroelectric, paraelectric, and quantum paraelectric materials, based on simple quantities extracted from standard density functional and density functional perturbation theories. We calculate the influence of isotope substitution and strain on quantum paraelectric behavior and find that, while complete replacement of oxygen-16 by oxygen-18 has a surprisingly small effect, experimentally accessible strains can induce large changes. Finally, we collect the various choices for the phonon mass that have been introduced in the literature. We identify those that are most physically meaningful by comparing them with our results that avoid such a choice through the use of mass-weighted coordinates.

Topics & Concepts