Effect of anti-site disorder on magnetism in La2NiMnO6

La₂NiMnO₆ has been reported to exhibit a paramagnetic to ferromagnetic transition with a transition temperature of ~ 260 K. However, most of its magnetic properties, such as the saturation magnetization and even the transition temperature, appear to vary considerably among different reports. This is possibly because the crystallographic structure as well as the extent of the anti-site disorder (ASD) at the Ni/Mn sites are strongly influenced by the choice of synthesis routes. There are diverse reports connecting the extent of ASD to the valencies of Ni and Mn ions, such as Ni²⁺-Mn⁴⁺ and Ni³⁺-Mn³⁺, including suggestions of thermally induced valence transitions. Consequently, these reports arrive at very different conclusions on the mechanism behind the magnetic properties of La₂NiMnO₆. To address the correlation between ASD and valency, we have carried out a comparative study of two monoclinic La₂NiMnO₆ polycrystals with different degrees of ASD. Using a combination of x-ray absorption spectroscopy, x-raymagnetic circular dichroism, andmagnetometry, we conclude that the valency of the transition metal ions, and the transition temperature, are insensitive to the extent of ASD. Furthermore, we find the magnetic moment decreases strongly with an increasing ASD. We attribute this effect to the introduction of antiferromagnetic interactions in the anti-site disordered regions.