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Non-volatile electric-field control of inversion symmetry

Nature Materials volume 22, pages 207–215 (2023)Cite this article

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Abstract

Competition between ground states at phase boundaries can lead to significant changes in properties under stimuli, particularly when these ground states have different crystal symmetries. A key challenge is to stabilize and control the coexistence of symmetry-distinct phases. Using BiFeO3 layers confined between layers of dielectric TbScO3 as a model system, we stabilize the mixed-phase coexistence of centrosymmetric and non-centrosymmetric BiFeO3 phases at room temperature with antipolar, insulating and polar semiconducting behaviour, respectively. Application of orthogonal in-plane electric (polar) fields results in reversible non-volatile interconversion between the two phases, hence removing and introducing centrosymmetry. Counterintuitively, we find that an electric field ‘erases’ polarization, resulting from the anisotropy in octahedral tilts introduced by the interweaving TbScO3 layers. Consequently, this interconversion between centrosymmetric and non-centrosymmetric phases generates changes in the non-linear optical response of over three orders of magnitude, resistivity of over five orders of magnitude and control of microscopic polar order. Our work establishes a platform for cross-functional devices that take advantage of changes in optical, electrical and ferroic responses, and demonstrates octahedral tilts as an important order parameter in materials interface design.

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Fig. 1: Mixed-phase coexistence of polar and antipolar phases in the BFO/TSO superlattice.
Fig. 2: Piezoforce and non-linear optical response of mixed-phase coexistence.
Fig. 3: MIM and DFT band-structure calculations.
Fig. 4: Non-volatile electric-field manipulation of SHG intensity and resistivity.

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Data availability

Data presented in the main text are open access and can be found on Zenodo65 or as Source data accompanying this manuscript. Owing to the extent of data presented in the Supplementary Information, it is available upon request from the corresponding authors.

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Acknowledgements

R.R., L.W.M., D.A.M., L.-Q.C. and D.G.S. acknowledge support from the Army Research Office under the ETHOS MURI via cooperative agreement W911NF-21-2-0162. The MIM work (J.Y., D.L. and K.L.) was supported by the Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under contract no. DE-SC0019025. Computational resources were provided by ETH Zürich and the Swiss National Supercomputing Center (CSCS), project ID no. s889. Work at ETH was supported by ETH Zürich and the Körber Foundation. M.F. acknowledges support by the Swiss National Science Foundation project 200021_178825. Z.H. and X.G. were supported by the National Natural Science Foundation of China grant no. 92166104. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under contract no. DE-AC02-05CH11231. L.C. acknowledges financial support from the Ford Foundation and the University of California President’s Postdoctoral Fellowship Program. Y.-T.S. and D.A.M. acknowledge financial support from the Department of Defense, Air Force Office of Scientific Research under award FA9550-18-1-0480. The electron microscopy studies were performed at the Cornell Center for Materials Research, a National Science Foundation (NSF) Materials Research Science and Engineering Centers program (DMR-1719875, NSF-MRI-1429155). The microscopy work at Cornell was supported by the NSF PARADIM (DMR-2039380), with additional support from Cornell University, the Weill Institute and the Kavli Institute at Cornell. The authors acknowledge discussions regarding diffraction imaging with J.-M. Zuo as well as M. Thomas, J. G. Grazul, M. Silvestry Ramos and K. Spoth for technical support and careful maintenance of the instruments. We thank X. Huang, A. Fernandez and P. Meisenheimer for fruitful conversations and M. E. Holtz for preliminary electron microscopy studies. We also acknowledge I. Schulze-Jonack and M. S. Stypa for help with substrate crystal growth.

Author information

Author notes

  1. Lucas Caretta

    Present address: School of Engineering, Brown University, Providence, RI, USA

  2. Yu-Tsun Shao

    Present address: Mork Family Department of Chemical Engineering and Materials Science, University of Southern California, Los Angeles, CA, USA

  3. These authors contributed equally: Lucas Caretta, Yu-Tsun Shao.

Authors and Affiliations

  1. Department of Materials Science and Engineering, University of California, Berkeley, CA, USA

    Lucas Caretta, Piush Behera, Lane W. Martin & Ramamoorthy Ramesh

  2. School of Applied and Engineering Physics, Cornell University, Ithaca, NY, USA

    Yu-Tsun Shao, Harikrishnan K. P & David A. Muller

  3. Department of Physics, University of Texas, Austin, TX, USA

    Jia Yu, Daehun Lee & Keji Lai

  4. Department of Materials Science and Engineering, Cornell University, Ithaca, NY, USA

    Antonio B. Mei & Darrell G. Schlom

  5. Department of Materials, ETH Zurich, Zurich, Switzerland

    Bastien F. Grosso, Manfred Fiebig & Nicola A. Spaldin

  6. Department of Materials Science and Engineering, The Pennsylvania State University, University Park, PA, USA

    Cheng Dai, Fei Xue & Long-Qing Chen

  7. Department of Physics, University of California, Berkeley, CA, USA

    Margaret McCarter, Eric Parsonnet & Ramamoorthy Ramesh

  8. State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, China

    Xiangwei Guo & Zijian Hong

  9. Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou, China

    Xiangwei Guo

  10. Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Edward S. Barnard & Archana Raja

  11. Leibniz-Institut für Kristallzüchtung, Berlin, Germany

    Steffen Ganschow & Darrell G. Schlom

  12. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Lane W. Martin & Ramamoorthy Ramesh

  13. Kavli Institute at Cornell for Nanoscale Science, Ithaca, NY, USA

    David A. Muller & Darrell G. Schlom

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Contributions

R.R., D.G.S., L.C. and A.B.M. conceived the project and planned the experiments. Y.-T.S. and H.K.P. performed TEM, TEM sample preparation and atomically resolved polar and structural analysis under supervision of D.A.M. A.B.M. optimized synthesis of the superlattices and performed reciprocal space maps under supervision of D.G.S. L.C. and P.B. performed in-situ SHG measurements with help from A.R. and E.B, and M.F. L.C., P.B. and E.B. prepared the experimental SHG setup. P.B. performed PFM imaging under supervision from L.C. L.C. and P.B. performed electronic transport measurements. J.Y. and D.L. performed MIM and analysis with supervision from K.L. M.M. performed laboratory-based X-ray structural characterization and analysis. L.C. and E.P designed and microfabricated the electric-field devices. L.C. deposited metal layers. First-principles calculations were performed by B.F.G. under the supervision of N.A.S. Phase field calculations were performed by C.D. and F.X. under the supervision of L.-Q.C. and X.G. under the supervision of Z.H. SHG analysis was completed by L.C., P.B. and M.F. Scandate crystal substrates were grown by S.G. L.C., Y.-T.S., R.R., K.L. and L.W.M. wrote the manuscript.

Corresponding authors

Correspondence to Lucas Caretta or Ramamoorthy Ramesh.

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Competing interests

K.L. holds a patent on the MIM technology, which is licensed to PrimeNano, Inc., for commercial instruments. The terms of this arrangement have been reviewed and approved by the University of Texas at Austin in accordance with its policy on objectivity in research. The remaining authors declare no conflict of interest.

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Nature Materials thanks Charles Paillard, Paolo Radaelli and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–26, Table 1, Text 1–9 and refs. 1–10.

Source data

Source Data For Fig. 2

Source data for SHG data plotted in Fig. 2c–e.

Source Data For Fig. 4

Source data for DFT data plotted in Fig. 4e, SHG data plotted in Fig. 4i, resistivity data plotted in Fig. 4j and PFM data plotted in Fig. 4k.

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Caretta, L., Shao, YT., Yu, J. et al. Non-volatile electric-field control of inversion symmetry. Nat. Mater. 22, 207–215 (2023). https://doi.org/10.1038/s41563-022-01412-0

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