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

Abstract: Manipulation of long-range order in two-dimensional (2D) van der Waals (vdW) magnetic materials (e.g., CrI$3$, CrSiTe$_3$ 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 which, in turn, affects the nanoelectronic/spintronic device performance. Counterintuitively, our 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 Cr$_2$Te$_3$ (T${C2}$ ~ 160 K) in the parent vdW magnetic semiconductor Cr$2$Ge$_2$Te$_6$ (T${C1}$ ~ 69 K). In addition, the magnetic anisotropy energy (MAE) enhances in the hybrid by an order from the weakly anisotropic pristine Cr$_2$Ge$_2$Te$_6$ crystal, increasing the stability of the FM ground state with time. Comparing with the freshly prepared Cr$_2$Ge$_2$Te$_6$, 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 magnetotransport 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 rather common poor environmental stability of the vdW magnets, our results open possibilities of finding air-stable novel materials having multiple magnetic phases.