Atomistic Origin and Strain Control of the Finite-Temperature Dielectric Response in BaTiO3

RESUMO

Soft-mode theory specifies a frequency, not what a local polar unit does. What real-space motion underlies the dielectric response of BaTiO3 therefore remains unclear. Using electric-field-induced molecular dynamics with a machine-learning force field, we show that the permittivity tracks the field-induced angular redistribution of local Ti-O off-centering, not its magnitude. Temperature and biaxial strain modify the local structure through different microscopic routes, yet both dielectric responses collapse onto a common relation with the same orientational descriptor, providing a real-space counterpart to soft-mode behavior.