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Highly mobile ferroelastic domain walls in compositionally graded ferroelectric thin films

Abstract

Domains and domain walls are critical in determining the response of ferroelectrics, and the ability to controllably create, annihilate, or move domains is essential to enable a range of next-generation devices. Whereas electric-field control has been demonstrated for ferroelectric 180° domain walls, similar control of ferroelastic domains has not been achieved. Here, using controlled composition and strain gradients, we demonstrate deterministic control of ferroelastic domains that are rendered highly mobile in a controlled and reversible manner. Through a combination of thin-film growth, transmission-electron-microscopy-based nanobeam diffraction and nanoscale band-excitation switching spectroscopy, we show that strain gradients in compositionally graded PbZr1−xTixO3 heterostructures stabilize needle-like ferroelastic domains that terminate inside the film. These needle-like domains are highly labile in the out-of-plane direction under applied electric fields, producing a locally enhanced piezoresponse. This work demonstrates the efficacy of novel modes of epitaxy in providing new modalities of domain engineering and potential for as-yet-unrealized nanoscale functional devices.

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Figure 1: Domain structures in PbZr1−xTixO3 heterostructures.
Figure 2: Cross-sectional transmission electron microscopy studies of compositionally graded heterostructures.
Figure 3: Understanding switching in PbZr0.2Ti0.8O3 heterostructures.
Figure 4: Understanding switching in compositionally graded heterostructures.
Figure 5: Breaking down the differences between homogeneous and compositionally graded heterostructures.

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Acknowledgements

J.C.A., G.A.V. and L.W.M. acknowledge support from the National Science Foundation under grant DMR-1451219. A.R.D. and S.P. acknowledge support from the Army Research Office under grant W911NF-14-1-0104. L.R.D. acknowledges support from the Department of Energy, Basic Energy Sciences under grant No. DE-SC0012375 for chemical studies of the materials. R.V.K.M. acknowledges support from the National Science Foundation under grant CMMI-1434147. R.K.V. and S.V.K. acknowledge support from the Division of Materials Sciences and Engineering, Basic Energy Sciences, Department of Energy. Portions of this research were conducted at the Center for Nanophase Materials Sciences, which is a Department of Energy, Office of Science User Facility sponsored at Oak Ridge National Laboratory by the Scientific User Facilities Division, Basic Energy Sciences, Department of Energy which also provided support for M.B.O., S.J. and N.B. J.K. and A.M.M. acknowledge support from the National Science Foundation CMMI/MoM Program under GOALI Grant 1235610. C.G. acknowledges support from the Austrian Science Fund (FWF):[J3397]. Portions of this work were carried out at the Molecular Foundry, Lawrence Berkeley National Laboratory, which is supported by the US Dept. of Energy under Contract No. DE-AC02-29705CH11231.

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J.C.A. and L.W.M. designed the experiments. J.C.A., R.V.K.M. and G.A.V. grew the films and conducted the macroscopic electrical and structural characterization. L.R.D. completed the Rutherford backscattering spectrometry studies. J.K., C.G. and A.M.M. prepared the samples for STEM and conducted the STEM imaging and nanobeam diffraction strain mapping. J.C.A., J.K., C.G., A.M.M. and L.W.M. analysed the STEM and nanobeam diffraction strain mapping data. M.B.O., S.J., N.B. and S.V.K. designed the custom band-excitation system. J.C.A., M.B.O. and R.K.V. conducted the band-excitation measurements. M.B.O., S.J., R.K.V. and S.V.K. designed the band-excitation fitting and piezoelectric loop fitting algorithm and software. J.C.A., M.B.O., R.K.V., S.J., N.B., S.V.K. and L.W.M. analysed the band-excitation results. J.C.A., A.R.D., S.P. and L.W.M. determined the switching mechanism. J.C.A. and L.W.M. co-wrote the paper.

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Correspondence to L. W. Martin.

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Agar, J., Damodaran, A., Okatan, M. et al. Highly mobile ferroelastic domain walls in compositionally graded ferroelectric thin films. Nature Mater 15, 549–556 (2016). https://doi.org/10.1038/nmat4567

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