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A metastable {\epsilon}-Al60Sm11 phase appears during the initialdevitrification of as-quenched Al-10.2 at.% Sm glasses. The {\epsilon} phase isnonstoichiometric in nature since Al occupation is observed on the 16f Smlattice sites. Scanning transmission electron microscopic images revealprofound spatial correlation of Sm content on these sites, which cannot beexplained by the "average crystal" description from Rietveld analysis ofdiffraction data. Thermodynamically favorable configurations, established byMonte Carlo (MC) simulations based on a cluster-expansion model, also givequalitatively different correlation functions from experimental observations.On the other hand, molecular dynamics simulations of the growth of{\epsilon}-Al60Sm11 in undercooled liquid show that when the diffusion range ofSm is limited to ~ 4 {\AA}, the correlation function of the as-grown crystalstructure agrees well with that of the STEM images. Our results show thatkinetic effects, especially the limited diffusivity of Sm atoms plays thefundamental role in determining the nonstoichiometric site occupancies of the{\epsilon}-Al60Sm11 phase during the crystallization process.

Spatially-correlated Site Occupancy in the Nonstoichiometric Meta-stable {\epsilon}-Al60Sm11 Phase during Devitrification of Al-10.2 at.% Sm Glasses