Ferroelectricity in Pb1+δZrO3 Thin Films

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

Resultado de la investigación: Article

4 Citas (Scopus)

Resumen

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.

Idioma originalEnglish
Páginas (desde-hasta)6544-6551
Número de páginas8
PublicaciónChemistry of Materials
Volumen29
N.º15
DOI
EstadoPublished - 8 ago 2017

Huella dactilar

Ferroelectricity
Heterojunctions
Thin films
Ferroelectric materials
Antiferroelectricity
Defects
Metastable phases
Pulsed laser deposition
Hysteresis loops
X ray scattering
Epitaxial growth
Ground state
Lattice constants
Density functional theory
Cations
Materials properties
Stabilization
Diffraction
Positive ions
X rays

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

Citar esto

Gao, R., Reyes-Lillo, S. E., Xu, R., Dasgupta, A., Dong, Y., Dedon, L. R., ... Martin, L. W. (2017). Ferroelectricity in Pb1+δZrO3 Thin Films. Chemistry of Materials, 29(15), 6544-6551. https://doi.org/10.1021/acs.chemmater.7b02506
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. / Ferroelectricity in Pb1+δZrO3 Thin Films. En: Chemistry of Materials. 2017 ; Vol. 29, N.º 15. pp. 6544-6551.
@article{77ed104e7fd34793acd3147aaccbedbf,
title = "Ferroelectricity in Pb1+δZrO3 Thin Films",
abstract = "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.",
author = "Ran Gao and Reyes-Lillo, {Sebastian E.} and Ruijuan Xu and Arvind Dasgupta and Yongqi Dong and Dedon, {Liv R.} and Jieun Kim and Sahar Saremi and Zuhuang Chen and Serrao, {Claudy R.} and Hua Zhou and Neaton, {Jeffrey B.} and Martin, {Lane W.}",
year = "2017",
month = "8",
day = "8",
doi = "10.1021/acs.chemmater.7b02506",
language = "English",
volume = "29",
pages = "6544--6551",
journal = "Chemistry of Materials",
issn = "0897-4756",
publisher = "American Chemical Society",
number = "15",

}

Gao, R, Reyes-Lillo, SE, Xu, R, Dasgupta, A, Dong, Y, Dedon, LR, Kim, J, Saremi, S, Chen, Z, Serrao, CR, Zhou, H, Neaton, JB & Martin, LW 2017, 'Ferroelectricity in Pb1+δZrO3 Thin Films', Chemistry of Materials, vol. 29, n.º 15, pp. 6544-6551. https://doi.org/10.1021/acs.chemmater.7b02506

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.

En: Chemistry of Materials, Vol. 29, N.º 15, 08.08.2017, p. 6544-6551.

Resultado de la investigación: Article

TY - JOUR

T1 - Ferroelectricity in Pb1+δZrO3 Thin Films

AU - Gao, Ran

AU - Reyes-Lillo, Sebastian E.

AU - Xu, Ruijuan

AU - Dasgupta, Arvind

AU - Dong, Yongqi

AU - Dedon, Liv R.

AU - Kim, Jieun

AU - Saremi, Sahar

AU - Chen, Zuhuang

AU - Serrao, Claudy R.

AU - Zhou, Hua

AU - Neaton, Jeffrey B.

AU - Martin, Lane W.

PY - 2017/8/8

Y1 - 2017/8/8

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=85027379132&partnerID=8YFLogxK

U2 - 10.1021/acs.chemmater.7b02506

DO - 10.1021/acs.chemmater.7b02506

M3 - Article

VL - 29

SP - 6544

EP - 6551

JO - Chemistry of Materials

JF - Chemistry of Materials

SN - 0897-4756

IS - 15

ER -

Gao R, Reyes-Lillo SE, Xu R, Dasgupta A, Dong Y, Dedon LR y otros. Ferroelectricity in Pb1+δZrO3 Thin Films. Chemistry of Materials. 2017 ago 8;29(15):6544-6551. https://doi.org/10.1021/acs.chemmater.7b02506