Anisotropic Ferromagnetism in CrAu3Sb6.

The crystal structure and properties of CrAu3Sb6 are presented, determined by measurements on single crystal and polycrystalline samples and first-principles calculations. The trigonal structure (space group P3̅1m) comprises a CdI2-like sublattice of AuSb2 with Cr occupying octahedral holes in a fully ordered triangular array. It can be viewed as a variation of the interesting and well-known families of partially intercalated transition metal dichalcogenides, but with stronger interactions along the stacking direction evidenced by short Cr-Au distances. The compound is metallic and ferromagnetic with a Curie temperature of 164 K. A strong anomalous contribution to the Hall effect is seen in the ferromagnetic state, and quantum oscillations are observed in magnetization at 2 K. Magnetization measurements show that the ordered moments of 1.5 μB per Cr are oriented along the c-axis with relatively strong magnetocrystalline anisotropy. Electronic structure calculations confirm this uniaxial anisotropy and the important role of spin-orbit coupling in CrAu3Sb6 and reveal strongly favored ferromagnetic ground state consistent with the measured Curie temperature. Through combined experiment and theory, this work provides a detailed picture of the basic properties and behaviors of this uniquely structured, Cr-based, anisotropic ferromagnet.