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Tilt-driven antiferroelectricity in PbZrO3

Konstantin Shapovalov1,* and Massimiliano Stengel2,1

  • 1Institut de Ciència de Materials de Barcelona (ICMAB-CSIC), Campus UAB, 08193 Bellaterra, Spain
  • 2ICREA—Institució Catalana de Recerca i Estudis Avançats, 08010 Barcelona, Spain

  • *Corresponding author: shapovalov.kos@gmail.com

Phys. Rev. Materials 7, L071401 – Published 12 July, 2023

DOI: https://doi.org/10.1103/PhysRevMaterials.7.L071401

Abstract

Antiferroelectricity is a state of matter that has so far eluded a clear-cut definition. Even in the best-known material realization, PbZrO3, the physical nature of the driving force towards an antipolar order has not been settled yet. Here, by building a Landau-like continuum Hamiltonian from first principles via an exact long-wave approach, we reconcile the existing theories in terms of a single physical mechanism. In particular, we find that a formerly overlooked trilinear coupling between tilts, tilt gradients, and polarization provides a surprisingly accurate description of the energetics and structure of the antiferroelectric ground state of PbZrO3. We discuss the relevance of our findings to other ferrielectric and incommensurate polar structures that were recently observed in perovskites.

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