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In this paper, based on the embedded atom method (EAM) potential, molecular dynamics simulations of the solidification process of Al–4 at.%Cu alloy is carried out. The Al–Cu alloy melt is placed at different temperatures for isothermal solidification, and each stage of the entire solidification process is tracked, including homogeneous nucleation, nucleus growth, grain coarsening and microstructure evolution. In the nucleation stage, the transition from high temperature to low temperature manifests a change from spontaneous nucleation mode to divergent nucleation mode. The critical nucleation temperature of the Al–Cu alloy is determined to be about 0.42 T m ( T m is the melting point of Al–4 at.%Cu) by calculating the nucleation rate and the crystal nucleus density. In the nucleus growth stage, two ways of growing up are observed, that is, a large crystal nucleus will absorb a smaller heterogeneous crystal nucleus, and two very close crystal nuclei will merge. In the microstructure evolution of the isothermally solidified Al–Cu alloy, it is emerged that the interior of all nanocrystalline grains are long-period stacking structure composed of face centred cubic (FCC) and hexagonal close-packed (HCP). These details provide important information for the production of Al–Cu binary alloy nano-polycrystalline products.

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