Abstract
The emergence of intrinsic two-dimensional (2D) magnetic materials has spurred exploration of exotic physical phenomena at the atomic limit, while also opening new avenues for the design of compact, ultra-low-power spintronic devices. In contrast to the widely studied layered magnets, the ternary nonlayered magnets with excellent stability remain relatively unexplored. A key challenge lies in the scalable fabrication of high-quality, large-area samples. Herein, we propose a dual-confined chemical vapor deposition strategy for the first-time synthesis of 2D nonlayered ferrimagnetic FeCr2Te4 nanosheets. The as-grown nanosheets exhibit lateral dimensions up to 400 μm and outstanding stability under high-temperature and harsh chemical conditions. The Curie temperature of the samples is independent of thickness. Notably, a temperature-tunable antiferromagnetic state emerges in thicker nanosheets, driven by weak interlayer exchange coupling. Furthermore, the nanosheets exhibit an extrinsic skew-scattering-dominated anomalous Hall effect, with a high carrier concentration of 1020 cm-3 and mobility exceeding 30 cm2 v-1 s-1. This work opens up new avenues for the synthesis of ternary nonlayered 2D magnetic materials and significantly expands the material platform for developing high-performance spintronic devices.

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