The magnetic properties of 1 nm thick in-plane anisotropic Co ultrathin film on ZnO(0001) were investigated through successive 500 eV nitrogen-ion sputtering. Magneto-optical Faraday effects were used to observe the evolution of the ion-irradiated sample in longitudinal and perpendicular magnetic fields. The ferromagnetic phase of the initial in-plane anisotropic fcc β-Co phase transformation to β-Co(N) phase was terminated at paramagnetic CoNx phase. In-plane anisotropy with weak out-of-plane anisotropy of the Co/ZnO sample was initially observed in the as-grown condition. In the sputtering process, the N+ ions induced simultaneous sputtering and doping. An abrupt spin reorientation behavior from in-plane to out-of-plane was found under prolonged sputtering condition. The existence of perpendicular anisotropy measured from the out-of-plane Faraday effect may be attributed to the co-existence of residual β-Co and Co4N exchange bonding force by the gradual depletion of Co-N thickness.
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