Abstract: Fe-based metallic glasses are promising functional materials for advanced magnetism and sensor fields. Tailoring magnetic performance in amorphous materials requires a thorough knowledge of the correlation between structural disorder and magnetic order, which remains ambiguous. Two practical difficulties remain: the first is directly observing subtle magnetic structural changes on multiple scales, and the second is precisely regulating the various amorphous states. Here we propose a novel approach to tailor the amorphous structure through the liquid-liquid phase transition. In-situ synchrotron diffraction has unraveled a medium-range ordering process dominated by edge-sharing cluster connectivity during the liquid-liquid phase transition. Moreover, nanodomains with topological order have been found to exist in composition with liquid-liquid phase transition, manifesting as hexagonal patterns in small-angle neutron scattering profiles. The liquid-liquid phase transition can induce the nanodomains to be more locally ordered, generating stronger exchange interactions due to the reduced Fe-Fe bond length and the enhanced structural order, leading to the increment of saturation magnetization. Furthermore, the increased local heterogeneity at the medium-range scale enhances the magnetic anisotropy, promoting the permeability response under applied stress and leading to a better stress-impedance effect. These experimental results pave the way to tailor the magnetic structure and performance through the liquid-liquid phase transition.

Key words: Fe-based metallic glass, Liquid-liquid phase transition, Medium-range ordering, Magnetic nanodomain