Impact of H-bond with Oxygen and Zinc Vacancies on the Room Temperature
Ferromagnetic Behavior of ZnO Films
Preetam Singh1,2,*, Pankaj Srivastava2, and Santanu Ghosh2
1 Department of Physics, R.K. (P.G.) College, Shamli (U.P.), India-24776
2 Department of Physics, Indian Institute of Technology Bombay, Powai Mumbai-400076, India
Room temperature ferromagnetism in pure semiconductors can be used for spintronics and
optoelectronic applications in spin transistors, spin valves, and spin light emitting diodes. Magnetic
properties of H2-ambience annealed pure ZnO films have been reported. ZnO films prepared by
using DC magnetron sputtering show room temperature ferromagnetism (RT-FM) after annealing
in hydrogen atmosphere at two different temperatures (3500C and 400oC). Enhancement in O-H
concentration has been observed by analyzing core level spectra recorded using x-ray
photoelectron spectroscopy (XPS). The valence band spectra suggest the enhancement in carrier
concentration after annealing in H2-ambience. Enhancement in the vacancy type defects have been
observed by positron annihilation spectroscopy and tailoring of defects have been observed by
photoluminescence spectra. Electrical transport results also indicate rapid decrease in activation
energies corresponding to thermally activated band and nearest neighbor hopping (NNH)
conduction, i.e. increase in carrier concentration after annealing. Increase in saturation
magnetization and Zn vacancy (evident from M-H and PL data) along with the O-H concentration,
after annealing in H2-ambience, suggest that Zn vacancies along with O-H concentration play a
crucial role behind the ferromagnetic nature of the films. Surface morphology as examined by
atomic force microscopy (AFM) shows that there is no significant variation of grain size and
surface roughness of the films after annealing. The experimental results are further verified
theoretically by performing the density functional theory calculations. Based on both experimental
results and theoretical model, it has been explained that the enhancement of magnetic moment of
H2-ambience annealed ZnO is dominantly because of the increased carrier mediated exchange
interaction among the localized magnetic moment at VZn sites.