LAUSR

Searching for 2D ferromagnetic materials with a high critical temperature, large spin polarization, and controllable magnetization direction is a key challenge for their broad applications in spintronics. Here, through a systematic study on a series of 2D ternary chalcogenides with first‐principles calculations, it is demonstrated that a family of experimentally available 2D CoGa2X4 (X = S, Se, or Te) are half‐metallic ferromagnets, and they exhibit high critical temperature, fully polarized spin state, and strain‐dependent magnetization direction simultaneously. Following the Goodenough–Kanamori rules, the half‐metallic ferromagnetism of CoGa2X4 family is caused by superexchange interaction mediated by CoXCo bonds. The half‐metal gaps are large enough (>0.5 eV) to ensure that the half‐metallicity is stable against the spin flipping at room temperature. Magnetocrystalline anisotropy energy calculations indicate that CoGa2X4 favor easy plane magnetization. Under achievable biaxial tensile strain (2–6%), the magnetization directions of CoGa2X4 can change from in‐plane to out‐of‐plane, providing a route to control the efficiency of spin injection/detection. Further, the critical temperatures Tc of ferromagnetic phase transition for CoGa2X4 are close to room temperature. Belonging to the big family of layered AB2X4 compounds, the proposed CoGa2X4 systems will enrich the available 2D candidates and their heterojunctions for various applications.