In contrast to conventional dilute magnetic semiconductors with concentrations of magnetic ions of just a few percent, here, we report the fabrication of epitaxial Cox Zn 1− xO single crystalline films with Co concentrations from x = 0.3 up to 0.45 by radio-frequency oxygen-plasma-assisted molecular beam epitaxy. The films retain their single crystalline wurtzite structure without any other crystallographic phase from precipitates, based on reflection high energy electron diffraction, X-ray diffraction, transmission electron microscopy, and Raman scattering. The results of X-ray diffraction, optical transmission spectroscopy, and in-situ X-ray photoelectron spectroscopy confirm the incorporation of Co2+ cations into the wurtzite lattice. The films exhibit robust ferromagnetism and the magneto-optical Kerr effect at room temperature. The saturation magnetization reaches 265 emu/cm3 at x = 0.45, which corresponds to the average magnetic moment of 1.5 μB per Co atom.
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