A variable temperature EPR study of the manganites (La1/3Sm2/3)2/3SrxBa0.33−xMnO3 (x=0.0, 0.1, 0.2, 0.33): Small polaron hopping conductivity and Griffiths phase

Four manganite samples of the series, (La1/3Sm2/3)2/3SrxBa0.33−xMnO3, with x=0.0, 0.1, 0.2 and 0.33, were investigated by X-band (∼9.5 GHz) electron paramagnetic resonance (EPR) in the temperature range 4–300 K. The temperature dependences of EPR lines and linewidths of the samples with x=0.0, 0.1 and 0.2, containing Ba2+ ions, exhibit similar behavior, all characterized by the transition temperatures (TC) to ferromagnetic states in the 110–150 K range. However, the sample with x=0.33 (containing no Ba2+ ions) is characterized by a much higher TC=205 K. This is due to significant structural changes effected by the substitution of Ba2+ ions by Sr2+ ions. There is an evidence of exchange narrowing of EPR lines near Tmin, where the linewidth exhibits the minimum. Further, a correlation between the temperature dependence of the EPR linewidth and conductivity is observed in all samples, ascribed to the influence of small-polaron hopping conductivity in the paramagnetic state. The peak-to-peak EPR linewidth was fitted to ΔBpp(T)=ΔBpp,min+A/Texp(−Ea/kBT), with Ea=0.09 eV for x=0.0, 0.1 and 0.2 and Ea=0.25 eV for x=0.33. From the published resistivity data, fitted here to σ(T)∝1/T exp(−Eσ/kBT), the value of Eσ, the activation energy, was found to be Eσ=0.18 eV for samples with x=0.0, 0.1 and 0.2 and Eσ=0.25 eV for the sample with x=0.33. The differences in the values of Ea and Eσ in the samples with x= 0.0, 0.1and 0.2 and x=0.33 has been ascribed to the differences in the flip-flop and spin-hopping rates. The presence of Griffiths phase for the samples with x=0.1 and 0.2 is indicated; it is characterized by coexistence of ferromagnetic nanostructures (ferrons) and paramagnetic phase, attributed to electronic phase separation.