High entropy effect on double exchange interaction and charge ordering in half doped Nd0.5Sr0.5MnO3 manganite

Abstract

The entropy stabilized oxides i.e., the so-called high-entropy oxides are of great interest in recent time due to their intriguing physical properties. This new category of advanced materials is stabilized by the high configurational entropy of randomly mixed elements, where a specific lattice site is populated by five or more elements. The present study is devoted to explore the high entropy effect in well-known charge ordered manganite Nd0.5Sr0.5MnO3 where a delicate balance exists between the ferromagnetic double exchange and the antiferromagnetic superexchange interactions. Powder X-ray diffraction analyses confirm phase purity of the samples. FE-SEM imaging revealed the microstructure and elemental mapping confirmed the chemical homogeneity of the samples as well as nominal cationic composition. Bond valence sum (BVS) calculation using refinement parameters supports the expected cationic valence in all the samples. Replacement of Nd3+ by five trivalent cations as in (La0.1Pr0.1Nd0.1Gd0.1Bi0.1)Sr0.5MnO3 with larger average A-site ionic radius,<rA>and smaller size variance, σ2 compared with Nd0.5Sr0.5MnO3 dramatically suppressed the ferromagnetic double exchange interaction. This observation is in contrast with the expected variation in<rA>and σ2. In (La0.1Nd0.1Gd0.1Bi0.1Y0.1)Sr0.5MnO3 with smaller<rA> and marginally higher σ2 the ferromagnetic state ceases to exist. In both the multicationic compositions, a long-range antiferromagnetic state is evolved around 200 K with the retention of charge ordering. In the high entropy (La1/6Nd1/6Dy1/6Ca1/6Ba1/6Sr1/6)MnO3 composition with nominal<rA> and larger σ2 values the high temperature long-range ordering is completely suppressed and a new antiferromagnetic state is evolved at 45 K without manifestation of any charge ordering. This composition also avoids magnetic frustration unlike the dopant variant with larger σ2. The present investigation thus highlights the role of local lattice distortion or high entropy effect apart from the<rA>and σ2 in manganites.