Structural, optical, magnetic and electrical properties of Zn_1−x Co _x O thin films

Despite a considerable effort aiming at elucidating the nature of ferromagnetism in ZnO-based magnetic semiconductor, its origin still remains debatable. Although the observation of above room temperature ferromagnetism has been reported frequently in the literature by magnetometry measurement, so far there has been no report on correlated ferromagnetism in magnetic, optical and electrical measurements. In this paper, we investigate systematically the structural, optical, magnetic and electrical properties of Zn_1−x Co _x O:Al thin films prepared by sputtering with x ranging from 0 to 0.33. We show that correlated ferromagnetism is present only in samples with x > 0.25. In contrast, samples with x < 0.2 exhibit weak ferromagnetism only in magnetometry measurement which is absent in optical and electrical measurements. We demonstrate, by systematic electrical transport studies that carrier localization indeed occurs below 20–50 K for samples with x < 0.2; however, this does not lead to the formation of ferromagnetic phase in these samples with an electron concentration in the range of 6 × 10¹⁹ cm⁻³ ∼1 × 10²⁰ cm⁻³. Detailed structural and optical transmission spectroscopy analyses revealed that the anomalous Hall effect observed in samples with x > 0.25 is due to the formation of secondary phases and Co clusters.