The spontaneous exchange bias (SEB) effect is a remarkable phenomenon recently observed in some reentrant spin-glass materials. Here, we investigate the SEB in La1.5(Sr0.5−xBax)CoMnO6 double-perovskites, a system with multifarious magnetic phases for which a notable increase in the exchange bias field is observed for intermediate Sr/Ba concentrations. The Ba to Sr substitution leads to the enhancement of the crystal lattice, which is accompanied by the increase in both the effective magnetic moment (μeff) and the antiferromagnetic (AFM) transition temperature that is observed below the ferromagnetic ordering. Such an increase is likely related to the increased fraction of Co3+ in the high spin configuration, leading to the enhancement of the Co3+–O–Mn4+ AFM phase and the reduction in the uncompensation of the AFM coupling between Co and Mn. The combined effect of the increased μeff and AFM phase plausibly explains the changes in the SEB effect.

La 1.5 Ba 0.5 CoMnO 6 is a re-entrant cluster glass material exhibiting a robust negative exchange bias (EB) effect even after being cooled from an unmagnetized state down to low temperature in zero magnetic field. Here we thoroughly investigate this phenomena by performing magnetization as a function of applied field [M(H )] measurements at several different temperatures and maximum applied magnetic fields (H m ). The spontaneous EB (SEB) effect is observed below 20 K, and shows a maximum value for H m = 75 kOe. The effect is greatly enhanced when the M(H ) curves are measured after the system is cooled in the presence of a magnetic field. The asymmetry of the M(H ) curves here investigated can be well described by a recently proposed model based on the unconventional relaxation of the SG-like moments during the hysteresis cycle.

La1.5Sr0.5CoMn0.5Fe0.5O6 (LSCMFO) compound was prepared by solid state reaction and its structural, electronic and magnetic properties were investigated. The material forms in rhombohedral R 3 ̄ c structure, and the presence of distinct magnetic interactions leads to the formation of a Griffiths phase above its FM transition temperature (150 K), possibly related to the nucleation of small short-ranged ferromagnetic clusters. At low temperatures, a spin glass-like phase emerges and the system exhibits both the conventional and the spontaneous exchange bias (EB) effects. These results resemble those reported for La1.5Sr0.5CoMnO6 but are discrepant to those found when Fe partially substitutes Co in La1.5Sr0.5(Co1−x Fe x )MnO6, for which the EB effect is observed in a much broader temperature range. The unidirectional anisotropy observed for LSCMFO is discussed and compared with those of resembling double-perovskite compounds, being plausibly explained in terms of its structural and electronic properties.

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