Half-metallic, Co-based quaternary Heuslers for spintronics: defect- and pressure-induced transitions and properties

TL;DR

This study uses density-functional theory to analyze how pressure and various types of disorder affect the electronic and magnetic properties of Co-based quaternary Heusler alloys, crucial for spintronic applications.

Contribution

It provides detailed insights into the effects of pressure and intrinsic disorder on the half-metallicity and magnetic properties of specific Co-based Heusler alloys, informing material control for spintronics.

Findings

CoMnCrAl becomes metallic under pressure.

CoFeCrGe retains half-metallicity within a limited pressure range.

Certain antisite disorders preserve half-metallicity despite energetic favorability.

Abstract

Heusler compounds offer potential as spintronic devices due to their spin-polarization and half-metallicity properties, where electron spin-majority (minority) manifold exhibits states (band gap) at the electronic chemical potential, yielding full spin-polarization in a single manifold. Yet, Heuslers often exhibit intrinsic disorder that degrades its half-metallicity and spin-polarization. Using density-functional theory, we analyze the electronic and magnetic properties of equiatomic Heusler ($L$2$_{1}$) CoMnCrAl and CoFeCrGe alloys for effects of hydrostatic pressure and intrinsic disorder (thermal antisites, binary swaps, and vacancies). Under pressure, CoMnCrAl undergoes a metallic transition, while half-metallicity in CoFeCrGe is retained for a limited range. Antisite disorder between Co-Al pairs in CoMnCrAl and Co-Ge pairs in CoFeCrGe is energetically the most favored, and retain half-metallic character in Co-excess samples. However, Co-deficient samples undergo a transition from half-metallic to metallic, with a discontinuity in the saturation magnetization. For binary swaps, configurations that compete with the ground state are identified and show no loss of half-metallicity; however, the minority-spin bandgap and magnetic moments vary depending on the atoms swapped. For single binary swaps, there is a significant energy cost in CoMnCrAl but with no loss of half metallicity. Although a few configurations in CoFeCrGe energetically compete with the ground statei, however the minority-spin bandgap and magnetic moments vary depending on the atoms swapped. These informations should help in controlling these potential spintronic materials.