basically follow the phase diagram. In Fe-rich range, the phase-separated Au-core/Fe-shell particles were formed, because quenching induces an earlier solidification of the Fe-rich component as a result of cooling from the surrounding ethanol. If the particle size is small, the quenching rate becomes very rapid and particles were less phase-separated. For high Au contents exceeding 70% in weight, crystalline Au-rich alloys were formed without phase separation. Thus, this aggregation control is required to selectively form homogeneous or phase-separated larger submicrometre-sized particles by PLML.