Designing inverse-Heusler antiskyrmion hosts by chemically tailoring the effective magnetic Hamiltonian

Despite progress in the identification of mechanisms capable of stabilizing magnetic (anti)skyrmions, the number of bulk materials known to host these phases over a wide range of ambient temperatures remains small. Such thermal stability can be guaranteed by designing materials with C_nv, D_2d, or S₄ symmetry to have low magnetocrystalline anisotropy. An ideal platform for realizing this behavior are the tetragonal inverse Heusler alloys, where several proof-of-concept materials hosting thermally-robust antiskyrmions have been discovered. We report a systematic, first-principles exploration of potential antiskyrmion hosts in this family of materials, from known ordered compounds to hypothetical disordered alloys likely to maintain the tetragonal inverse Heusler structure. We construct a universal model relating mesoscale magnetic phase behavior to atomistic interactions and map out the magnetic behavior of a wide range of candidate chemistries to identify compositions yielding the precise magnetic Hamiltonian necessary for antiskyrmion formation. Our analysis reveals concrete chemical handles for controlling antiskyrmion formation and suggests new chemical spaces likely to host thermally-robust antiskyrmion phases.