Transition Metal‐Adsorbed Half‐Semimetal Ferromagnetic Covalent Triazine Framework with Topological Spin Structure

The covalent triazine framework (CTF‐1) has demonstrated significant potential in gas storage, catalysis, and photoelectric devices. However, its application in magnetism has rarely been investigated to date. Herein, a series of CTF‐1 by adsorbing transition metal atoms, using high‐throughput calculations, are systematically investigated. Among them, Hf‐adsorbed CTF‐1 (Hf‐CTF‐1) emerges as a promising candidate due to its exceptional structural stability and large magnetic exchange energy. Utilizing first‐principles density functional theory calculations, the geometric, electronic, and magnetic properties of Hf‐CTF‐1 are analyzed. The results reveal that Hf‐CTF‐1 is a XY‐type half‐semimetal ferromagnetic, and the Curie temperature ( T c ) is predicted to be about 166 K via Monte Carlo simulations. Further, compressive strain can modulate T c to ≈200 K, enhancing its potential for practical applications. Spin dynamics simulations suggest the presence of topological spin textures in Hf‐CTF‐1, consistent with the Berezinskii–Kosterlitz–Thouless theory. These findings position Hf‐CTF‐1 as a highly promising material for next‐generation 2D spintronic devices.