First‐Principles Approach for Predicting Chiral Helimagnetism

Abstract Chiral helimagnets have attracted significant attention due to their unique spin textures, dynamics, and potential in next‐generation spintronic technologies. However, calculating helimagnetic properties accurately remains a challenge owing to the complexity of the helical spin configurations and the long‐range periodicity. Here, a universal approach is reported for modeling and predicting helimagnetic spin structures by extracting the total energy as a function of the spin rotation angle between successive layers of helimagnets using first‐principles calculations. Applying this approach to Cr‐intercalated transition metal dichalcogenides, Cr 1/3 MX 2 (where M = Nb, Ta; X = S, Se), their monoaxial magnetic helix parameters are successfully predicted, including helix wavevector, helix period, and critical magnetic field. This approach opens new avenues for the discovery of helimagnetic materials.