The invention relates to a process for obtaining crystals of intermetallic compounds, in particular isolated monocrystals, by cooling alloys in the molten state. The process involves using an alloy in the molten state which has a composition such that the first phase to crystallize during its solidification corresponds to the compound to be isolated, cooling it slowly by subjecting it to cyclic stirring and thermal cycling without attaining the temperature at which another solid phase appears then abruptly expelling the residual liquid. The process is used for obtaining large monophase primary crystals of compounds which melt congruently or incongruently, in particular compounds having symmetry of order 5 known as "quasi-crystals".
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