Improper Inversion Symmetry Breaking and Piezoelectricity through Oxygen Octahedral Rotations in Layered Perovskite Family, LiRTiO4 (R = Rare Earths)

Arnab Sen Gupta; Hirofumi Akamatsu; Megan E. Strayer; Shiming Lei; Toshihiro Kuge; Koji Fujita; Clarina dela Cruz; Atsushi Togo; Isao Tanaka; Katsuhisa Tanaka; Thomas E. Mallouk; Venkatraman Gopalan

doi:10.1002/aelm.201500196

Improper Inversion Symmetry Breaking and Piezoelectricity through Oxygen Octahedral Rotations in Layered Perovskite Family, LiRTiO₄ (R = Rare Earths)

Arnab Sen Gupta, Hirofumi Akamatsu, Megan E. Strayer, Shiming Lei, Toshihiro Kuge, Koji Fujita, Clarina dela Cruz, Atsushi Togo, Isao Tanaka, Katsuhisa Tanaka, Thomas E. Mallouk, Venkatraman Gopalan

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Abstract

An improper mechanism for breaking inversion symmetry is revealed and thus inducing piezoelectricity in the family of layered perovskites, LiRTiO₄ (R = rare earths), which are previously reported as centrosymmetric. Noncentrosymmetry in this family of compounds arises from TiO₆ octahedral rotation represented by a⁻b^oc^o/b^oa⁻c^o in the perovskite blocks between RO rock salt and LiO antifluorite layers. X-ray diffraction and optical second harmonic generation complemented by density functional theory predictions are crucial in determining the new structures. High transition temperature (T_ac) of up to 1200 K from noncentrosymmetric to centrosymmetric phase is observed. Piezoelectric coefficients (d₃₆) of up to −15 pC/N are predicted, and piezoelectric force microscopy experiments confirm a piezoelectric response. The demonstrated improper mechanism in this and other layered oxide families, with a wide range of available topologies and chemistries, could aid in the search for high temperature piezoelectrics.

Original language	English
Article number	1500196
Journal	Advanced Electronic Materials
Volume	2
Issue number	1
DOIs	https://doi.org/10.1002/aelm.201500196
State	Published - Jan 1 2016

Funding

This work was primarily supported by the National Science Foundation under MRSEC grant DMR-1420620. S. L. and V. G. were also partially supported by DMR-1210588. The authors thank Dr. James Rondinelli for helpful discussions about this project. The research conducted at ORNL's High Flux Isotope Reactor was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. H.A. would like to acknowledge support from Japan Society for the Promotion of Science for Research Abroad (No. 25-185). M.E.S. would like to acknowledge the National Science Foundation Graduate Fellowship grant DGE-1255832. K.F. would like to acknowledge Japan Synchrotron Radiation Research Institute (Proposal No. 2015A1151) for SXRD measurements and JSPS KAKENHI Grant-in-Aid for Scientific Research on Innovative Areas “Nano Informatics” (Grant No. 26106514).

Funders	Funder number
Japan Society for the Promotion of Science for Research Abroad	25-185, DGE-1255832
Japan Synchrotron Radiation Research Institute	2015A1151
Scientific User Facilities Division
National Science Foundation	1210588
U.S. Department of Energy
Basic Energy Sciences
Materials Research Science and Engineering Center, Harvard University	DMR-1210588, DMR-1420620
Japan Society for the Promotion of Science	26106514

Keywords

layered perovskite
octahedral rotation
piezoelectricity

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10.1002/aelm.201500196

Cite this

Gupta, A. S., Akamatsu, H., Strayer, M. E., Lei, S., Kuge, T., Fujita, K., dela Cruz, C., Togo, A., Tanaka, I., Tanaka, K., Mallouk, T. E., & Gopalan, V. (2016). Improper Inversion Symmetry Breaking and Piezoelectricity through Oxygen Octahedral Rotations in Layered Perovskite Family, LiRTiO₄ (R = Rare Earths). Advanced Electronic Materials, 2(1), Article 1500196. https://doi.org/10.1002/aelm.201500196

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abstract = "An improper mechanism for breaking inversion symmetry is revealed and thus inducing piezoelectricity in the family of layered perovskites, LiRTiO4 (R = rare earths), which are previously reported as centrosymmetric. Noncentrosymmetry in this family of compounds arises from TiO6 octahedral rotation represented by a−boco/boa−co in the perovskite blocks between RO rock salt and LiO antifluorite layers. X-ray diffraction and optical second harmonic generation complemented by density functional theory predictions are crucial in determining the new structures. High transition temperature (Tac) of up to 1200 K from noncentrosymmetric to centrosymmetric phase is observed. Piezoelectric coefficients (d36) of up to −15 pC/N are predicted, and piezoelectric force microscopy experiments confirm a piezoelectric response. The demonstrated improper mechanism in this and other layered oxide families, with a wide range of available topologies and chemistries, could aid in the search for high temperature piezoelectrics.",

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Gupta, AS, Akamatsu, H, Strayer, ME, Lei, S, Kuge, T, Fujita, K, dela Cruz, C, Togo, A, Tanaka, I, Tanaka, K, Mallouk, TE & Gopalan, V 2016, 'Improper Inversion Symmetry Breaking and Piezoelectricity through Oxygen Octahedral Rotations in Layered Perovskite Family, LiRTiO₄ (R = Rare Earths)', Advanced Electronic Materials, vol. 2, no. 1, 1500196. https://doi.org/10.1002/aelm.201500196

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AU - Kuge, Toshihiro

AU - Fujita, Koji

AU - dela Cruz, Clarina

AU - Togo, Atsushi

AU - Tanaka, Isao

AU - Tanaka, Katsuhisa

AU - Mallouk, Thomas E.

AU - Gopalan, Venkatraman

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N2 - An improper mechanism for breaking inversion symmetry is revealed and thus inducing piezoelectricity in the family of layered perovskites, LiRTiO4 (R = rare earths), which are previously reported as centrosymmetric. Noncentrosymmetry in this family of compounds arises from TiO6 octahedral rotation represented by a−boco/boa−co in the perovskite blocks between RO rock salt and LiO antifluorite layers. X-ray diffraction and optical second harmonic generation complemented by density functional theory predictions are crucial in determining the new structures. High transition temperature (Tac) of up to 1200 K from noncentrosymmetric to centrosymmetric phase is observed. Piezoelectric coefficients (d36) of up to −15 pC/N are predicted, and piezoelectric force microscopy experiments confirm a piezoelectric response. The demonstrated improper mechanism in this and other layered oxide families, with a wide range of available topologies and chemistries, could aid in the search for high temperature piezoelectrics.

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