Spectroscopic ellipsometry and magneto-transport investigations of Mn-doped ZnO nanocrystalline films deposited by a non-vacuum sol–gel spin-coating method

Nanocrystalline Zn1−xMnxO films (x = 0, 0.05, 0.1, 0.15, and 0.2) were deposited onto corning glass substrates by a non-vacuum sol–gel spin coating method. All of the films were annealed at 450 °C for 2 h. The structural, optical and magneto-transport properties were investigated by X-ray diffraction, spectroscopic ellipsometry and a system for the measurement of the physical properties. X-ray diffraction analysis of the films reveals that the Mn-doped ZnO films crystallize in the form of a hexagonal wurtzite-type structure with a crystallite size decreases with an increase of the Mn concentration. It was also found that the microstrain increases with the increase of the Mn content. Evidence of nanocrystalline nature of the films was observed from the investigation of surface morphology using transmission, scanning electron microscopy and atomic force microscopy. The optical constants and film thicknesses of nanocrystalline Zn1−xMnxO films were obtained by fitting the spectroscopic ellipsometric data (ψ and Δ) using a three-layer model system in the wavelength range from 300 to 1200 nm. The refractive index was observed to increase with increasing Mn concentration. This increase in the refractive index with increasing Mn content may be attributed to the increase in the polarizability due to the large ionic radius of Mn2+ compared to the ionic radius of Zn2+. The optical band gap of the nanocrystalline Mn–ZnO films was determined by an analysis of the absorption coefficient. The direct transition of the series of films was observed to have energies increasing linearly from 3.17 eV (x = 0) to 3.55 eV (x = 0.2). Magnetoresistance (MR) was measured from 5 K to 300 K in a magnetic field of up to 6 T. Low-field positive MR and high-field negative MR were detected in Mn-doped ZnO at 5 K. Only negative MR was observed for temperatures above 200 K. The positive MR in Mn-doped ZnO films was observed to decrease drastically when the temperature increased from 5 K to 100 K. The isothermal MR of Zn1−xMnxO films with different Mn concentrations at 5 K reveals that the increase of the Mn content induces a giant positive MR above x = 0.05 and reaches up to 55% at an applied field of 30 kOe for x = 0.2.