Controllable Synthesis Quadratic-Dependent Unsaturated Magnetoresistance of Two-Dimensional Nonlayered Fe₇S₈ with Robust Environmental Stability

Two-dimensional (2D) iron chalcogenides (FeX, X = S, Se, Te) are emerging as an appealing class of materials for a wide range of research topics, including electronics, spintronics, and catalysis. However, the controlled syntheses and intrinsic property explorations of such fascinating materials still remain daunting challenges, especially for 2D nonlayered Fe₇S₈ with mixed-valence states and high conductivity. Herein, we design a general and temperature-mediated chemical vapor deposition (CVD) approach to synthesize ultrathin and large-domain Fe₇S₈ nanosheets on mica substrates, with the thickness down to ∼4.4 nm (2 unit-cell). Significantly, we uncover a quadratic-dependent unsaturated magnetoresistance (MR) with out-of-plane anisotropy in 2D Fe₇S₈, thanks to its ultrahigh crystalline quality and high conductivity (∼2.7 × 10⁵ S m^-1 at room temperature and ∼1.7 × 10⁶ S m^-1 at 2 K). More interestingly, the CVD-synthesized 2D Fe₇S₈ nanosheets maintain robust environmental stability for more than 8 months. These results hereby lay solid foundations for synthesizing 2D nonlayered iron chalcogenides with mixed-valence states and exploring fascinating quantum phenomena.