A systematic study of oxygen vacancy mediated short range and long range magnetic ordering in BaTi1-xFexO3(x = 0.02)

Abstract

A systematic study on the magnetic properties of the BaTi1-xFexO3-δ (x = 0.02) system with decrease in grain sizes is presented. The combined study of long range and short range magnetic orderings together was carried out. The samples were prepared in single tetragonal phase. The grains of the pristine sample were refined from micron to nanometer range by mechanical milling. Oxygen vacancies in different charge states gave rise to ferromagnetic and antiferromagnetic orderings among the Fe3+ ions whereas oxygen atoms acted as the medium for antiferromagnetic superexchange among the Fe3+ ions. Magnetization was found to increase significantly as a result of milling and eventually the saturation magnetization became four-fold in the sample with grain size around 18 nm. The increase in magnetization is attributed to the increase in oxygen vacancies as a consequence of increase in milling time. Clear sextet patterns in the Mössbauer spectra were observed in the sample wherein 57Fe–enriched iron was used in place of natural iron. These sextets were attributed to the presence of FM and AFM orderings among Fe3+ ions. Along with the sextet patters, we also observed a doublet pattern in Mössbauer spectra because of quadrupolar interaction of the isolated Fe3+ ions arranged in non-cubic environment and lacking any kind of magnetic interactions among them. Mössbauer Spectroscopic (MS) study revealed that FM ordering increased while AFM ordering disappeared after milling. Drastic fall of coercivity in samples with grain sizes below around 40 nm indicated that they became single magnetic domain.