Ferroelectricity in Pb1+δZrO3 Thin Films

Gao, Ran; Reyes-Lillo, Sebastian E.; Xu, Ruijuan; Dasgupta, Arvind; Dong, Yongqi; Dedon, Liv R.; Kim, Jieun; Saremi, Sahar; Chen, Zuhuang; Serrao, Claudy R.; Zhou, Hua; Neaton, Jeffrey B.; Martin, Lane W.

doi:10.1021/acs.chemmater.7b02506

Title: Ferroelectricity in Pb_1+δZrO₃ Thin Films

Journal Article · Sun Jul 16 00:00:00 EDT 2017 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.7b02506· OSTI ID:1394834

Gao, Ran ^[1]; Reyes-Lillo, Sebastian E. ^[2]; Xu, Ruijuan ^[1]; Dasgupta, Arvind ^[1]; Dong, Yongqi ^[3]; Dedon, Liv R. ^[1]; Kim, Jieun ^[1]; Saremi, Sahar ^[1];

^[1]; Serrao, Claudy R. ^[4]; Zhou, Hua ^[5]; Neaton, Jeffrey B. ^[6];

^[7]

Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry, Materials Sciences Division
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source; Univ. of Science and Technology, Hefei (China). National Sychrotron Radiation Lab., CAS Key Lab. of Materials for Energy Conversion
Univ. of California, Berkeley, CA (United States). Dept. of Electrical Engineering
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source
Kavli Energy NanoSciences Inst., Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry, Materials Sciences Division
Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division

© 2017 American Chemical Society. Antiferroelectric PbZrO 3 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 PbZrO 3 thin films and understanding the chemistry-structure coupling in Pb 1+δ ZrO 3 (δ = 0, 0.1, 0.2). High-quality, single-phase Pb 1+δ ZrO 3 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 PbZrO 3 and Pb 1.1 ZrO 3 heterostructures remain intrinsically antiferroelectric, the Pb 1.2 ZrO 3 heterostructures exhibit a hysteresis loop indicative of ferroelectric response. Further X-ray scattering studies reveal strong quarter-order diffraction peaks in PbZrO 3 and Pb 1.1 ZrO 3 heterostructures indicative of antiferroelectricity, while no such peaks are observed for Pb 1.2 ZrO 3 heterostructures. Density functional theory calculations suggest the large cation nonstoichiometry is accommodated by incorporation of antisite Pb Zr defects, which drive the Pb 1.2 ZrO 3 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.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); US Army Research Office (ARO)

Grant/Contract Number:: AC02-06CH11357; AC02-05CH11231

OSTI ID:: 1394834

Alternate ID(s):: OSTI ID: 1436637

Journal Information:: Chemistry of Materials, Vol. 29, Issue 15; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 25 works

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