Extended x-ray absorption fine structure (EXAFS) spectroscopy is used
to study the size-dependent structural evolution of free clusters. K-e
dge EXAFS data are obtained for Ar clusters in beams having mean clust
er size ranging from 17 to 2900 atoms per cluster. EXAFS analysis yiel
ds size-dependent features which indicate the presence of an fee struc
ture at (N) greater than or equal to 200. It has been proposed in the
literature that small rare-gas clusters have an icosahedral structure.
The transition of this structure to the experimentally observed fee l
attice of rare-gas solids has been of long-standing interest and debat
e. The implications of our results are discussed in this light.