Emergence of a Non-Van der Waals Magnetic Phase in a Van der Waals Ferromagnet

Manipulation of long-range order in 2D van der Waals (vdW) magnetic materials (e.g., CrI₃, CrSiTe₃ ,etc.), exfoliated in few-atomic layer, can be achieved via application of electric field, mechanical-constraint, interface engineering, or even by chemical substitution/doping. Usually, active surface oxidation due to the exposure in the ambient condition and hydrolysis in the presence of water/moisture causes degradation in magnetic nanosheets that, in turn, affects the nanoelectronic /spintronic device performance. Counterintuitively, the current study reveals that exposure to the air at ambient atmosphere results in advent of a stable nonlayered secondary ferromagnetic phase in the form of Cr₂Te₃ (T_C2 ≈160 K) in the parent vdW magnetic semiconductor Cr₂Ge₂Te₆ (T_C1 ≈69 K). The coexistence of the two ferromagnetic phases in the time elapsed bulk crystal is confirmed through systematic investigation of crystal structure along with detailed dc/ac magnetic susceptibility, specific heat, and magneto-transport measurement. To capture the concurrence of the two ferromagnetic phases in a single material, Ginzburg-Landau theory with two independent order parameters (as magnetization) with a coupling term can be introduced. In contrast to the rather common poor environmental stability of the vdW magnets, the results open possibilities of finding air-stable novel materials having multiple magnetic phases.