Restructuring disorder: transformation from the antiferromagnetic order in Fe2VSi to the ferromagnetic state in FeRuVSi by substitution of a non-magnetic element

Abstract

The delicate nature of the half-metallic ferromagnetic (HMF) properties in Heusler alloys is often compromised by inherent structural disorder within the systems. Fe₂VSi is a prime example, where such disorder prevents the realization of the theoretically proposed HMF state as the anti-site disorder leads to the formation of two anti-parallel magnetic lattices resulting in antiferromagnetic order. In this study, we propose an innovative and simple strategy to prevent this atomic disorder by replacing 50% of the magnetic element Fe by a large, isoelectronic, non-magnetic element: Ru. In this way, one of the magnetic sublattices of the antiferromagnetic lattice ceases to order while the ferromagnetic order is restored – an essential criterion for exhibiting HMF properties. Through various experimental measurements and theoretical calculations, we have shown that such partial replacement of Fe by Ru prevents the cross-site substitution of V/Si sites and the system regains its ferromagnetic order. Our theoretical calculations suggest that a perfect structural arrangement in Fe and Ru would have restored the HMF properties in FeRuVSi. However, the local atomic disorder of Fe and Ru was found to decrease the spin polarization value. The present work sheds light on the complex interplay between structural disorder and magnetic properties in Heusler alloys and provides insights for future design strategies in the pursuit of robust half-metallic ferromagnets.