Structural, electronic and magnetic properties of Sc3+doped CoCr2O4nanoparticles

The control over spin distribution to achieve magnetic properties in crystalline structures is crucial for materials design. A clear understanding of the relationship between structure and properties is essential for the development of magnetic materials. Herein, we investigate the effect of Sc-doping on the structural, electronic, and magnetic properties of Co1-xScxCr2O4(x= 0.0 and 0.05) nanoparticles synthesised by a solution combustion method and perform in-depth DFT calculations to clarify the spin distribution and magnetic states. The synthesized samples showed a single phase of the spinel cubic structure. Structural distortions associated with the creation of A-site vacancies originate from overall deformations of the tetrahedral [CoO4] and octahedral [CrO6] clusters. Aiming to understand the magnetic behavior of the sintered samples, temperature-dependent susceptibility and field-dependent magnetization studies were conducted, revealing two magnetic transitions defined as paramagnetic collinear ferrimagnetic (FIM) (T-C) and non-collinear spiral FIM (T-S) states. Further, upon Sc-doping of the [CoO4] cluster,T(C)andT(S)decreased because of structural defects acting directly on the exchange coupling constants. The modification resulted in an enhancement of A-B and B-B antiferromagnetic (AFM) interactions, deeply clarified by DFT calculations. Hence, our experimental and theoretical approach uncovers a Sc-doping mechanism able to control the CoCr(2)O(4)magnetic properties of the matrix using structural distortions and long-range spin ordering.