Amorphous alloy films were formed by room temperature 200 keV xenon ion mixing of multilayers in a relatively broad composition range in the ZrTa system, which has a positive heat of formation of +4 kJ mol −1. A free energy diagram was constructed to include the free energy curves of the amorphous phase and the multilayers, to which the previously missing term of the excess interfacial free energy was calculated and added. It turned out that the interface plays a role in influencing the alloying behavior in such system and the calculated diagram provided a reasonable interpretation of the observed amorphization. Two new metastable crystalline phases of both fcc structures were obtained.
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