Termination-Dependent Surface States and Magnetic Fingerprints of Chiral Helimagnet Cr_1/3TaS₂

Chiral helimagnets based on intercalated transition-metal dichalcogenides, characterized by nanoscale spin ordering, provide a powerful route to engineer chiral spin textures (e.g., the topologically protected magnetic solitons) and explore emergent electronic functionalities associated with their surface and interface electronic structures. However, despite growing interest, direct experimental studies of termination-dependent surface electronic structures and their temperature-driven magnetic evolution remain largely unexplored, hindering a microscopic understanding of the electronic states that is crucial for the development of low-dimensional spintronic devices.

Here, taking Cr_1/3TaS₂ as a representative example, we systematically investigate the termination-dependent surface electronic states of the chiral helimagnets and uncover their distinct temperature evolution across the magnetic transition (<i>T</i>_<i>C</i> ∼ 142 K) by combining high-resolution angle-resolved photoemission spectroscopy with a microfocused beam and surface-state-resolved first-principles calculations.