3 years ago

Ferroelectricity in Pb1+δZrO3 Thin Films

Ferroelectricity in Pb1+δZrO3 Thin Films
Yongqi Dong, Ruijuan Xu, Zuhuang Chen, Jieun Kim, Ran Gao, Lane W. Martin, Liv R. Dedon, Hua Zhou, Arvind Dasgupta, Sebastian E. Reyes-Lillo, Jeffrey B. Neaton, Claudy R. Serrao, Sahar Saremi
Antiferroelectric PbZrO3 is being considered for a wide range of applications where the competition between centrosymmetric and noncentrosymmetric phases is important to the response. Here, we focus on the epitaxial growth of PbZrO3 thin films and understanding the chemistry–structure coupling in Pb1+δZrO3 (δ = 0, 0.1, 0.2). High-quality, single-phase Pb1+δZrO3 films are synthesized via pulsed-laser deposition. Although no significant lattice parameter change is observed in X-ray studies, electrical characterization reveals that while the PbZrO3 and Pb1.1ZrO3 heterostructures remain intrinsically antiferroelectric, the Pb1.2ZrO3 heterostructures exhibit a hysteresis loop indicative of ferroelectric response. Further X-ray scattering studies reveal strong quarter-order diffraction peaks in PbZrO3 and Pb1.1ZrO3 heterostructures indicative of antiferroelectricity, while no such peaks are observed for Pb1.2ZrO3 heterostructures. Density functional theory calculations suggest the large cation nonstoichiometry is accommodated by incorporation of antisite PbZr defects, which drive the Pb1.2ZrO3 heterostructures to a ferroelectric phase with R3c symmetry. In the end, stabilization of metastable phases in materials via chemical nonstoichiometry and defect engineering enables a novel route to manipulate the energy of the ground state of materials and the corresponding material properties.

Publisher URL: http://dx.doi.org/10.1021/acs.chemmater.7b02506

DOI: 10.1021/acs.chemmater.7b02506

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