Interplay between Local Moment and Itinerant Magnetism in the Layered Metallic Antiferromagnet TaFe_1.14Te₃

Two-dimensional antiferromagnets have garnered considerable interest for the next generation of functional spintronics. However, many bulk materials from which two-dimensional antiferromagnets are isolated are limited by their air sensitivity, low ordering temperatures, and insulating transport properties. TaFe₁₊Te₃ aims to address these challenges with increased air stability, metallic transport, and robust antiferromagnetism. Here, we synthesize TaFe₁₊Te₃ (y = 0.14), identify its structural, magnetic, and electronic properties, and elucidate the relationships between them. Axial-dependent high-field magnetization measurements on TaFe_1.14Te₃ reveal saturation magnetic fields ranging between 27 and 30 T with saturation magnetic moments of 2.05-2.12 μ_B. Magnetotransport measurements confirm that TaFe_1.14Te₃ is metallic with strong coupling between magnetic order and electronic transport. Angle-resolved photoemission spectroscopy measurements across the magnetic transition uncover a complex interplay between itinerant electrons and local magnetic moments that drives the magnetic transition. We demonstrate the ability to isolate few-layer sheets of TaFe_1.14Te₃, establishing TaFe_1.14Te₃ as a potential platform for two-dimensional spintronics.