Precisely and continuously tunable, intrinsic, infinitely soluble alloy ferromagnetism in layered and quasi-layered CrVTe crystals

Summary Precise and continuous regulation of intrinsic two-dimensional (2D) ferromagnetism in van der Waals layered crystals is pivotal for the next generation of low-power electronic and spintronic devices. However, most van der Waals layered ferromagnetic crystals exhibit little adjustability of some ferromagnetic properties, such as saturation magnetization, coercivity, and easy axis of magnetization. Here, we report intrinsic, infinitely soluble alloy ferromagnetism in layered and quasi-layered CrVTe (CrxV1-3x/4Te2) crystals, which show intrinsic ferromagnetism with precise and continuous adjustability in a wide range, including Curie temperature (∼13.2–202.5 K), saturation magnetization (∼0.375–48.740 emu/g), coercivity (∼243.40–4930.33 Oe), magnetoresistance (approximately −0.14% to 32.39%), and anomalous Hall resistivity (∼0.1724–13.3148 μΩ·cm), and are different from most discovered van der Waals layered ferromagnetic crystals with highly limited concentrations of magnetic atoms. Our findings provide a highly tunable avenue for ferromagnetic 2D crystals and 2D spintronic devices.