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On the origin of high-temperature ferromagnetism in the low-temperature-processed Mn–Zn–O system

Nature Materials volume 3, pages 709–714 (2004)Cite this article

Abstract

The recent discovery of ferromagnetism above room temperature in low-temperature-processed MnO2–ZnO has generated significant interest. Using suitably designed bulk and thin-film studies, we demonstrate that the ferromagnetism in this system originates in a metastable phase rather than by carrier-induced interaction between separated Mn atoms in ZnO. The ferromagnetism persists up to ∼980 K, and further heating transforms the metastable phase and kills the ferromagnetism. By studying the interface diffusion and reaction between thin-film bilayers of Mn and Zn oxides, we show that a uniform solution of Mn in ZnO does not form under low-temperature processing. Instead, a metastable ferromagnetic phase develops by Zn diffusion into the Mn oxide. Direct low-temperature film growth of Zn-incorporated Mn oxide by pulsed laser deposition shows ferromagnetism at low Zn concentration for an optimum oxygen growth pressure. Our results strongly suggest that the observed ferromagnetic phase is oxygen-vacancy-stabilized Mn2−xZnxO3−δ.

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Figure 1: Magnetization, TGA and XRD data for bulk compounds.
Figure 2: XRD patterns, RBS spectra and magnetization data for thin-film bilayer samples of the oxides of Zn and Mn.
Figure 3: XRD and magnetization (insets) data for Zn incorporated manganese oxide films grown by pulsed laser deposition.

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Acknowledgements

The authors gratefully acknowledge support under Defense Advanced Research Projects Agency grant number N000140210962 and National Science Foundation-MRSEC DMR-00-80008, including support under NSF-MRSEC for shared experimental facilities of PLD and RBS at the Center for Superconductivity Research, University of Maryland. The authors would like to thank Sang Wook Cheong, Sankar Das Sarma and Richard Greene for fruitful discussions.

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Authors and Affiliations

  1. Department of Physics, Center for Superconductivity Research, University of Maryland, College Park, 20742-4111, Maryland, USA

    Darshan C. Kundaliya, S. B. Ogale, S. Dhar, S. R. Shinde & T. Venkatesan

  2. Department of Materials Science, University of Maryland, College Park, 20742-4111, Maryland, USA

    S. B. Ogale, Z. Ma & L. Salamanca-Riba

  3. Department of Physics and Astronomy, Rowan University, Glassboro, 08028-1701, New Jersey, USA

    S. E. Lofland & C. J. Metting

  4. Department of Chemistry, University of Maryland, College Park, 20742, Maryland, USA

    B. Varughese

  5. Department of Chemistry and Biochemistry, Rowan University, Glassboro, 08028-1701, New Jersey, USA

    K.V. Ramanujachary

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  1. Darshan C. Kundaliya
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Correspondence to S. B. Ogale.

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Kundaliya, D., Ogale, S., Lofland, S. et al. On the origin of high-temperature ferromagnetism in the low-temperature-processed Mn–Zn–O system. Nature Mater 3, 709–714 (2004). https://doi.org/10.1038/nmat1221

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