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

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.