Constructing Polymorphic Nanodomains in BaTiO3 Films via Epitaxial Symmetry Engineering

Constructing Polymorphic Nanodomains in BaTiO3 Films via Epitaxial Symmetry Engineering

Advanced Functional Materials

DOI: 10.1002/adfm.201910569

Wei Peng, Jacob A. Zorn, Junsik Mun, Muhammad Sheeraz, Chang Jae Roh, Jun Pan, Bo Wang, Kun Guo, Chang Won Ahn, Yaping Zhang, Kui Yao, Jong Seok Lee, Jin-Seok Chung, Tae Heon Kim, Long-Qing Chen, Miyoung Kim, Lingfei Wang, Tae Won Noh

oxide ferroelectrics, polymorphic nanodomains, epitaxial films, dielectric, piezoelectric

24 February 2020

Wei Peng, Jacob A. Zorn, Junsik Mun, Muhammad Sheeraz, Chang Jae Roh, Jun Pan, Bo Wang, Kun Guo, Chang Won Ahn, Yaping Zhang, Kui Yao, Jong Seok Lee, Jin-Seok Chung, Tae Heon Kim, Long-Qing Chen, Miyoung Kim, Lingfei Wang, and Tae Won Noh, “Constructing Polymorphic Nanodomains in BaTiO3 Films via Epitaxial Symmetry Engineering,” Advanced Functional Materials, Vol. 30, DOI: 10.1002/adfm.201910569, 1910569, 2020.

Ferroelectric materials owning a polymorphic nanodomain structure usually exhibit colossal susceptibilities to external mechanical, electrical, and thermal stimuli, thus holding huge potential for relevant applications. Despite the success of traditional strategies by means of complex composition design, alternative simple methods such as strain engineering have been intensively sought to achieve a polymorphic nanodomain state in lead-free, simple-composition ferroelectric oxides in recent years. Here, a nanodomain configuration with morphed structural phases is realized in an epitaxial BaTiO3 film grown on a (111)-oriented SrTiO3 substrate. Using a combination of experimental and theoretical approaches, it is revealed that a three-fold rotational symmetry element enforced by the epitaxial constraint along the [111] direction of BaTiO3 introduces considerable instability among intrinsic tetragonal, orthorhombic, and rhombohedral phases. Such a phase degeneracy induces ultrafine ferroelectric nanodomains (1-10 nanometers) with low-angle domain walls, which exhibit significantly enhanced dielectric and piezoelectric responses compared to the (001)-oriented BaTiO3 film with uniaxial ferroelectricity. Therefore, our finding highlights the important role of epitaxial symmetry in domain engineering of oxide ferroelectrics and facilitates the development of dielectric capacitors and piezoelectric devices.

J. A. Zorn and J. Mun contributed equally to this work. This work was supported by the Research Center Program of IBS (Institute for Basic Science) in Korea (IBS-R009-D1). STEM measurement was supported by the National Center for Inter-University Research Facilities (NCIRF) at Seoul National University in Korea. J.A.Z., B.W. and L.-Q.C. acknowledge and appreciate the support from NSF-MRSEC DMR-1420620 (B.W. and L.-Q.C), and a fellowship from 3M Incorporated. Computations for this research were performed on the Pennsylvania State University’s Institute for CyberScience Advanced CyberInfrastructure, and the Extreme Science and Engineering Discovery Environment (XSEDE) through NSF DMR170006. C.J.R. and J.S.L. acknowledge the support from Science Research Center and the Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT & Future Planning (2018R1A2B2005331). The authors from IMRE acknowledge the supports by National Research Foundation Competitive Research Programme of Singapore, NRF-CRP15-2015-04, (IMRE/16-9P1122).

This is the peer reviewed version of the following article: Wei Peng, Jacob A. Zorn, Junsik Mun, Muhammad Sheeraz, Chang Jae Roh, Jun Pan, Bo Wang, Kun Guo, Chang Won Ahn, Yaping Zhang, Kui Yao, Jong Seok Lee, Jin-Seok Chung, Tae Heon Kim, Long-Qing Chen, Miyoung Kim, Lingfei Wang, and Tae Won Noh, “Constructing Polymorphic Nanodomains in BaTiO3 Films via Epitaxial Symmetry Engineering,” Advanced Functional Materials, Vol. 30, DOI: 10.1002/adfm.201910569, 1910569, 2020., which has been published in final form at https://doi.org/10.1002/adfm.201910569. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions.

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Institute of Materials Research and Engineering