The spontaneous exchange bias (SEB) effect is a remarkable phenomenon recently observed in some reentrant spin-glass materials. Here we investigate the SEB in La(SrBa)CoMnO 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 raise of both the effective magnetic moment () and the antiferromagnetic (AFM) transition temperature that is observed below the ferromagnetic ordering. Such increases are likely related to the increased fraction of Co in the high spin configuration, leading to the enhancement of Co–O–Mn AFM phase and to the reduction in the uncompensation of the AFM coupling between Co and Mn. The combined effect of the increased and AFM phase plausible explains the changes in the SEB effect.

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