Coexisting structural disorder and robust spin-polarization in half-metallic FeMnVAl

TL;DR

This study synthesizes and characterizes a novel FeMnVAl Heusler alloy, demonstrating its robust half-metallic ferromagnetic properties and resilience of spin polarization despite structural disorder, with implications for spintronic applications.

Contribution

It reports the first synthesis and detailed analysis of FeMnVAl, revealing its stable half-metallic ferromagnetic state and the robustness of spin polarization against atomic disorder.

Findings

Identified the optimal ordered structure through energy minimization.

Confirmed half-metallic ferromagnetic ground state via band structure calculations.

Demonstrated spin polarization remains high (~90%) despite site disorder.

Abstract

Half-metallic ferromagnets (HMF) are on one of the most promising materials in the field of spintronics due to their unique band structure consisting of one spin sub-band having metallic characteristics along with another sub-band with semiconductor-like behavior. In this work, we report the synthesis of a novel quaternary Heusler alloy FeMnVAl and have studied the structural, magnetic, transport, and electronic properties complemented with first-principles calculations. Among different possible structurally ordered arrangements, the optimal structure is identified by theoretical energy minimization. The corresponding spin-polarized band structure calculations indicates the presence of a half-metallic ferromagnetic ground state. A detailed and careful investigation of the x-ray diffraction data, M\"{o}ssbauer and nuclear magnetic resonance spectra suggest the presence of site-disorder between the Fe and Mn atoms in the stable ordered structure of the system. The magnetic susceptibility measurement clearly establishes a ferromagnetic-like transition below $\sim$213 K. The ${^{57}}$Fe M\"{o}ssbauer spectrometry measurements suggest only the Mn-spins could be responsible for the magnetic order, which is consistent with our theoretical calculation. Surprisingly, the density-functional-theory calculations reveal that the spin-polarization value is almost immunized (92.4\% ${\rightarrow}$ 90.4\%) from the Mn-Fe structural disorder, even when nonmagnetic Fe and moment carrying Mn sites are entangled inseparably. Robustness of spin polarization and half metallicity in the studied FeMnVAl compound comprising structural disorder is thus quite interesting and could provide a new direction to investigate and understand the exact role of disorders on spin polarization in these class of materials, over the available knowledge.