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Ferromagnetism above room temperature in bulk and transparent thin films of Mn-doped ZnO

Abstract

The search for ferromagnetism above room temperature in dilute magnetic semiconductors has been intense in recent years. We report the first observations of ferromagnetism above room temperature for dilute (<4 at.%) Mn-doped ZnO. The Mn is found to carry an average magnetic moment of 0.16 μB per ion. Our ab initio calculations find a valance state of Mn2+ and that the magnetic moments are ordered ferromagnetically, consistent with the experimental findings. We have obtained room-temperature ferromagnetic ordering in bulk pellets, in transparent films 2–3 μm thick, and in the powder form of the same material. The unique feature of our sample preparation was the low-temperature processing. When standard high-temperature (T > 700 °C) methods were used, samples were found to exhibit clustering and were not ferromagnetic at room temperature. This capability to fabricate ferromagnetic Mn-doped ZnO semiconductors promises new spintronic devices as well as magneto-optic components.

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Figure 1
Figure 2: Magnetization at 300 K for Zn0.978Mn0.022O pulsed-laser-deposited thin film on fused quartz.
Figure 3: HRTEM image and EELS spectra for a Zn(1−x)MnxO (x = 2.2 at.%) thin film.
Figure 4: Ferro- and paramagnetic resonance spectra for a nominal 2 at.% Mn-doped ZnO pellet.
Figure 5: Calculated density of states (DOS) for Zn0.958Mn0.042O, Fermi level is set at zero.

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Acknowledgements

R.A., J.G. and B.J. acknowledge the support from the ATOMICS and EXCITING programmes by the Swedish Strategic Foundation and the EU network. Some of the theoretical calculations were carried out at the National Supercomputer Centre at Linköping, Sweden. P.S., A.G. and K.V.R. acknowledge partial support for this research from the Swedish Agency VINNOVA. G.G. would like to acknowledge a visiting fellowship from the Swedish foundation STINT, and the hospitality during her stay at the Department of Materials Science of the Royal Institute of Technology. The use of the Center for High Resolution Electron Microscopy (CHREM) is gratefully acknowledged. Finally, we wish to thank very much the excellent and fruitful exchanges we have had with the reviewers of this manuscript. It has been the most enjoyable part of the scientific work.

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Correspondence to K. V. Rao.

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Sharma, P., Gupta, A., Rao, K. et al. Ferromagnetism above room temperature in bulk and transparent thin films of Mn-doped ZnO. Nature Mater 2, 673–677 (2003). https://doi.org/10.1038/nmat984

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