Flash-annealing (FA) of metallic glasses (MGs) allows one to modulate their disordered structure. Here, we have flash-annealed a CuZr-based MG below the glass transition temperature at different cycles and generated MGs with various heterogeneous structures. We quantified the glassy structure via the relaxation enthalpy, ΔrelH, which did not significantly change for MGs flash-annealed at a low number of cycles. Their hardness monotonically reduced. However, when more than ten FA cycles were applied, ΔrelH, perceivably decreased, while corresponding hardness increased. High-energy x-ray diffraction analysis revealed that the medium-range ordering of the corresponding structure initially rose and then decreased with an increasing number of FA cycles. This structural change is accompanied by first a hardness decrease followed by an increase. Molecular dynamics simulations showed that throughout the shift from low to high cycles, the structural non-uniformity changed from being non-uniform to more uniform. Through a combination of experiments and simulations, we have shown the non-monotonic relationship between the structural heterogeneity of MGs and cyclic treatments, contributing to a better understanding of the relationship between structural control techniques, microstructure, and properties.
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