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.

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