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The phase separation occurring in Fe-Ni thin films near the Invar compositionis studied by using high-resolution spectromicroscopy techniques and densityfunctional theory calculations. Annealed at temperatures around 300 C,Fe0.70Ni0.30 films on W(110) break into micron-sized bcc and fcc domains withcompositions in agreement with the bulk Fe-Ni phase diagram. Ni is found to bethe diffusing species in forming the chemical heterogeneity. The experimentallydetermined energy barrier of 1.59 +- 0.09 eV is identified as the vacancyformation energy via density functional theory calculations. Thus, theprincipal role of the surface in the phase separation process is attributed tovacancy creation without interstitials.

Vacancy-mediated fcc/bcc phase separation in Fe1-xNix ultrathin films