Temperature-dependent properties of the antiferroelectric model PbZrO 3 : An effective Hamiltonian study

Kinnary Patel (1) , Bin Xu (2) , Sergey Prosandeev (1) , Romain Faye (3) , Brahim Dkhil (3) , Pierre-Eymeric Janolin (3) , Laurent Bellaiche (1)

1 Institute for nanosciences and engineering and physics departement [University of Arkansas]
2 Soochow University
3 SPMS - Laboratoire Structures, Propriétés et Modélisation des solides

A novel atomistic effective Hamiltonian scheme, incorporating an original and simple bilinear energetic coupling, is developed and used to investigate the temperature dependent physical properties of the prototype antiferroelectric PbZrO 3 (PZO) system. This scheme reproduces very well the known experimental hallmarks of the complex Pbam orthorhombic phase at low temperatures and the cubic paraelectric state of Pm 3m symmetry at high temperatures. Unexpectedly, it further predicts a novel intermediate state also of Pbam symmetry, but in which anti-phase oxygen octahedral tiltings have vanished with respect to the Pbam ground state. Interestingly, such new state exhibits a large dielectric response and thermal expansion that remarkably agree with previous experimental observations and the x-ray experiments we performed. We also conducted direct first-principles calculations at 0K which further support such low energy phase. Within this fresh framework, a re-examination of the properties of PZO is thus called for.

Domains: Materials Science [cond-mat.mtrl-sci]

Kinnary Patel, Bin Xu, Sergey Prosandeev, Romain Faye, Brahim Dkhil, et al.. Temperature-dependent properties of the antiferroelectric model PbZrO 3 : An effective Hamiltonian study. Physical Review B, 2022, 106 (21), pp.214108. ⟨10.1103/PhysRevB.106.214108⟩. ⟨hal-03909045⟩