Atomic structures of bulk glass-forming Cu64.5Zr35.5 and the eutectic composition Cu61.8Zr38.2 metallic glasses (MGs) have been studied by a combination of state-of-the-art experimental techniques and computational methods. Three-dimensional atomic configuration of the Cu64.5Zr35.5 MG is established. It is found that icosahedronlike clusters are dominant in both MGs. However, icosahedronlike clusters centered by Cu atoms are slightly denser packing and less distorted in Cu64.5Zr35.5, which can enhance the glass forming ability (GFA) by suppressing atomic movements and increasing the structural incompatibility with competing crystalline phases. The atomic arrangements from short to medium-range order are envisaged and compared between both MGs.
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