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Formation mechanisms of self-organized core/shell (CS) and core/shell/corona (CSC) microstructures observed in liquid droplets of immiscible Cu–Fe-based alloys produced by gas atomization processing are investigated with computer simulations. The simulation method is based on a phase field approach that incorporates spinodal decomposition, subsequent coarsening, decomposition-induced fluid flow and Marangoni motion of second-phase droplets immersed in a major liquid-phase matrix. The roles played by each of these processes at different stages during the formation of CS and CSC structures are analyzed systematically as a function of droplet size. Other concurrent mechanisms responsible for the CS and CSC formation, such as coalescence and collisions, and attractive interactions between second-phase droplets, are identified. The differences in volume fraction and surface energies between the …