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A strong ferroelectric ferromagnet created by means of spin–lattice coupling

Nature volume 466, pages 954–958 (2010)Cite this article

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An Addendum to this article was published on 06 July 2011

Abstract

Ferroelectric ferromagnets are exceedingly rare, fundamentally interesting multiferroic materials that could give rise to new technologies in which the low power and high speed of field-effect electronics are combined with the permanence and routability of voltage-controlled ferromagnetism1,2. Furthermore, the properties of the few compounds that simultaneously exhibit these phenomena1,2,3,4,5 are insignificant in comparison with those of useful ferroelectrics or ferromagnets: their spontaneous polarizations or magnetizations are smaller by a factor of 1,000 or more. The same holds for magnetic- or electric-field-induced multiferroics6,7,8. Owing to the weak properties of single-phase multiferroics, composite and multilayer approaches involving strain-coupled piezoelectric and magnetostrictive components are the closest to application today1,2. Recently, however, a new route to ferroelectric ferromagnets was proposed9 by which magnetically ordered insulators that are neither ferroelectric nor ferromagnetic are transformed into ferroelectric ferromagnets using a single control parameter, strain. The system targeted, EuTiO3, was predicted to exhibit strong ferromagnetism (spontaneous magnetization, ∼7 Bohr magnetons per Eu) and strong ferroelectricity (spontaneous polarization, ∼10 µC cm−2) simultaneously under large biaxial compressive strain9. These values are orders of magnitude higher than those of any known ferroelectric ferromagnet and rival the best materials that are solely ferroelectric or ferromagnetic. Hindered by the absence of an appropriate substrate to provide the desired compression we turned to tensile strain. Here we show both experimentally and theoretically the emergence of a multiferroic state under biaxial tension with the unexpected benefit that even lower strains are required, thereby allowing thicker high-quality crystalline films. This realization of a strong ferromagnetic ferroelectric points the way to high-temperature manifestations of this spin–lattice coupling mechanism10. Our work demonstrates that a single experimental parameter, strain, simultaneously controls multiple order parameters and is a viable alternative tuning parameter to composition11 for creating multiferroics.

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Figure 1: Predicted effect of biaxial strain on EuTiO 3 and our approach to imparting such strain in EuTiO 3 films using epitaxy.
Figure 2: Structural characterization by X-ray diffraction and STEM of 22-nm-thick commensurate epitaxial EuTiO 3 films.
Figure 3: Commensurate EuTiO 3 strained in biaxial tension at +1.1% on DyScO 3 is ferroelectric below T c  ≈ 250 K.
Figure 4: Magnetization and capacitance measurements showing that EuTiO 3 on DyScO 3 is ferromagnetic below T C = 4.24 ± 0.02 K and that these two quantities are coupled.

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Acknowledgements

The authors acknowledge discussions and interactions with M. D. Biegalski, D. H. A. Blank, C. B. Eom, M. B. Holcomb, M. Ležaić, J. Mannhart, L. W. Martin, D. V. Pelekhov, R. Ramesh, K. Z. Rushchanskii, N. Samarth, A. Schmehl, D. A. Tenne, J.-M. Triscone, D. Viehland and L. Yan. In addition, the financial support of the National Science Foundation through grant DMR-0507146 and the MRSEC program (DMR-0520404, DMR-0820404 and DMR-0820414), and of the Czech Science Foundation (project no. 202/09/0682), is gratefully acknowledged. Use of the Advanced Photon Source was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357.

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Author notes

  1. Lei Fang, Eftihia Vlahos and Xianglin Ke: These authors contributed equally to this work.

Authors and Affiliations

  1. Department of Materials Science and Engineering, Cornell University, Ithaca, 14853-1501, New York, USA

    June Hyuk Lee, Tassilo Heeg & Darrell G. Schlom

  2. Department of Materials Science and Engineering, Pennsylvania State University, University Park, 16802-5005, Pennsylvania, USA

    June Hyuk Lee, Eftihia Vlahos & Venkatraman Gopalan

  3. Department of Physics, Ohio State University, Columbus, 43210-1117, Ohio, USA

    Lei Fang, Young Woo Jung, P. Chris Hammel & Ezekiel Johnston-Halperin

  4. Department of Physics and Materials Research Institute, Pennsylvania State University, University Park, 16802, Pennsylvania, USA

    Xianglin Ke & Peter Schiffer

  5. School of Applied and Engineering Physics, Cornell University, Ithaca, 14853, New York, USA

    Lena Fitting Kourkoutis, David A. Muller & Craig J. Fennie

  6. Advanced Photon Source, Argonne National Laboratory, Argonne, 60439, Illinois, USA

    Jong-Woo Kim, Philip J. Ryan & John W. Freeland

  7. Institute of Bio and Nanosystems, JARA-Fundamentals of Future Information Technologies, Research Centre Jülich, Jülich, D-52425, Germany

    Martin Roeckerath & Jürgen Schubert

  8. Institute of Physics ASCR, Na Slovance 2, 182 21 Prague 8, Czech Republic,

    Veronica Goian & Stanislav Kamba

  9. Leibniz Institute for Crystal Growth, Max-Born-Straße 2, D-12489 Berlin, Germany,

    Margitta Bernhagen & Reinhard Uecker

  10. Department of Physics and Astronomy, Rutgers University, Piscataway, 08854-8019, New Jersey, USA

    Karin M. Rabe

  11. Kavli Institute at Cornell for Nanoscale Science, Ithaca, 14853, New York, USA

    David A. Muller

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Contributions

The first-principles calculations were performed by C.J.F. and K.M.R. The thin films were synthesized by J.H.L. and D.G.S. on single-crystal substrates including DyScO3 grown by M.B. and R.U. The films were characterized using the MOKE by L.F., Y.W.J., P.C.H. and E.J.-H.; by SHG by E.V. and V. Gopalan; using a SQUID and by capacitance by X.K. and P.S.; by electron microscopy and spectroscopy by L.F.K. and D.A.M.; by X-ray diffraction by J.H.L., J.W.K. and P.J.R.; by X-ray absorption spectroscopy and X-ray magnetic circular dichroism by J.W.F.; by Rutherford backscattering spectrometry by T.H., M.R. and J.S.; and by far-infrared reflectance by V. Goian and S.K. D.G.S., C.J.F., J.W.F. and J.H.L. wrote the manuscript.

Corresponding author

Correspondence to Darrell G. Schlom.

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This file contains Supplementary Figures 1 - 16 with Legends, Supplementary Discussions 1- 8, Supplementary Equations 1 - 2, Supplementary Table 1 and References. (PDF 2535 kb)

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Lee, J., Fang, L., Vlahos, E. et al. A strong ferroelectric ferromagnet created by means of spin–lattice coupling. Nature 466, 954–958 (2010). https://doi.org/10.1038/nature09331

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