A Self-Consistent Computational Framework for Displacive Ferroelectrics from the Condensed Ground State

Abstract

Quantitative description of finite-temperature properties of displacive ferroelectrics, and in particular the critical behavior, is of fundamental importance to both theory and device design, going beyond the Landau-Ginzburg approach, which requires known knowledge of critical behaviors and temperature-dependent parameter fitting. Here within quantum statistic description of polarization fluctuations, we develop a self-consistent, microscopically based computationalframework for finite-temperature thermodynamics and phase transitions in displacive ferroelectrics. It enables one to use only the ground-state properties to predict the finite-temperature properties and in particular, the criticality of phase transitions of various displacive ferroelectrics. Its applications to the classical ferroelectric PbTiO$_3$, quantum paraelectrics SrTiO$_3$ and KTaO$_3$, and recently fabricated ferroelectric strained SrTiO$_3$, demonstrate remarkable quantitative agreements with the experimentally measured dielectric/ferroelectric properties throughout the entire temperature ranges of the phases, including the critical behaviors of phase transitions. The proposed computational framework offers a tractable quantitative basis for bridging microscopic ground-state modeling and macroscopic device-level design in a broad range of ferroelectric systems under diverse thermodynamic and external conditions.