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We reported spectroscopic investigations of high quality Mn-doped ZnO (ZnMnO) films grown by oxygen plasma-assisted molecular beam epitaxy. Raman scattering spectra revealed two local vibrational modes (LVMs) associated with Mn dopants at 523 and 712 cm−1. The LVMs and magnetic properties of ZnMnO films can be synchronously modulated by post annealing processing or by introducing tiny Co. The relative intensity of two LVMs clearly shows competitions arising from uncompensated acceptor and donor defects competition for ferromagnetic and nonmagnetic films. The experimental results indicated that LVM at 523 cm−1 is attributed to Mn—(Zinc-vacancy) complexes, while LVM at 712 cm−1 is attributed to Mn—(Oxygen-vacancy) complexes.

Local vibrational modes competitions in Mn-doped ZnO epitaxial films with tunable ferromagnetism