Antiferromagnetic spin glass-like behavior in sintered multiferroic Aurivillius Bim+1Ti3Fem−3O3m+3 compounds

The structure, hyperfine interactions and magnetic properties of the series of multiferroic Bim+1Ti3Fem−3O3m+3 Aurivillius compounds with m=4-8 were studied using X-ray diffraction, 57Fe Mössbauer spectroscopy and vibrating sample magnetometry. Samples were prepared by the conventional solid-state sintering method. Bulk magnetic measurements showed that for m=4 the compound is paramagnetic down to 2 K while in the compound with m=5 the antiferromagnetic type transition was observed at 11 K. In the case of compounds with m=6-8 much more complex magnetic behavior was found. For these compounds a gradual spin freezing and antiferromagnetic spin glass-like ordering were observed on decreasing temperature. The temperature of spin glass freezing was determined as 260, 280 and 350 K for m=6, 7 and 8, respectively. Room-temperature Mössbauer spectra of all the compounds studied confirm their paramagnetic state. However, liquid nitrogen and liquid helium temperature measurements reveal magnetic ordering with a residual paramagnetic phase contribution for the compounds with m=5-8.