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Electronic structure origins of polarity-dependent high-TC ferromagnetism in oxide-diluted magnetic semiconductors

Nature Materials volume 5, pages 291–297 (2006)Cite this article

Abstract

Future spintronics technologies based on diluted magnetic semiconductors (DMSs) will rely heavily on a sound understanding of the microscopic origins of ferromagnetism in such materials. Discoveries of room-temperature ferromagnetism in wide-bandgap DMSs hold great promise, but this ferromagnetism remains poorly understood. Here we demonstrate a close link between the electronic structures and polarity-dependent high-TC ferromagnetism of TM2+:ZnO DMSs, where TM2+ denotes 3d transition metal ions. Trends in ferromagnetism across the 3d series of TM2+:ZnO DMSs predicted from the energies of donor- and acceptor-type excited states reproduce experimental trends well. These results provide a unified basis for understanding both n- and p-type ferromagnetic oxide DMSs.

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Figure 1: 300 K magnetization data for 0.2% Mn2+:ZnO and 3.5% Co2+:ZnO films prepared by direct chemical synthesis with or without addition of nitrogen.
Figure 2: Electronic absorption, photocurrent IQE, and MCD spectroscopic data for Co2+:ZnO and Mn2+:ZnO.
Figure 3: Schematic summary of the spectroscopic analysis for Co2+- and Mn2+-doped ZnO DMSs.
Figure 4: Schematic summary of dopant–donor/acceptor resonance thermodynamics determined from spectroscopic analysis and the binding energies of common shallow donors (Zni) or acceptors (NO2−) in ZnO.
Figure 5: Results of LVBMCT and MLCBCT analysis for the series of TM2+:ZnO DMSs.

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Acknowledgements

Financial support from the NSF (PECASE DMR-0239325 and ECS-0224138), the Research Corporation (Cottrell Scholar), the Dreyfus Foundation (Teacher/Scholar), and the NSF-IGERT program at U.W. (to W.K.L.) is gratefully acknowledged.

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  1. Department of Chemistry, University of Washington, Seattle, Washington, 98195-1700, USA

    Kevin R. Kittilstved, William K. Liu & Daniel R. Gamelin

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Correspondence to Daniel R. Gamelin.

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Supplementary tables S1, S2 and S3; supplementary figures S1 and S2 (PDF 245 kb)

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Kittilstved, K., Liu, W. & Gamelin, D. Electronic structure origins of polarity-dependent high-TC ferromagnetism in oxide-diluted magnetic semiconductors. Nature Mater 5, 291–297 (2006). https://doi.org/10.1038/nmat1616

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