Orbital-engineered anomalous Hall conductivity in stable full Heusler compounds: a pathway to optimized spintronics

Abstract

This comprehensive study leverages high-throughput density functional theory (DFT) to systematically explore the electronic, magnetic, and transport properties of 2904 full Heusler compounds, focusing on anomalous Hall conductivity (AHC). The investigation unveils a pronounced influence of the crystallographic phase and valence electron count on material stability and AHC. We report that Heusler compounds, particularly within the L2₁ phase and with 20 to 30 valence electrons, exhibit superior stability and AHC. Notably, Rh₂MnGa and Co₂MnAl emerge as exemplary, with AHCs of 1847 S cm⁻¹ and 1646 S cm⁻¹, respectively, vastly outperforming traditional ferromagnets like Fe, Co, and Ni. The detailed electronic structure analysis of Co₂MnAl reveals a half-metallic character, crucial for high spin polarization and AHC, underscored by prominent Co–Co and Co–Mn hybridization. Furthermore, the study sheds light on the significant role of spin–orbit coupling in enhancing AHC through the modulation of band splitting and Berry curvature. The findings not only expand the understanding of Heusler compounds but also offer guidance in designing materials with tailored AHC for next-generation spintronic applications.