The geometrical structures of Ni-46, Ni-47, and Ni-48 are investigated by t
he chemical probe method using molecular nitrogen as the probe molecule. Ni
trogen saturation levels are determined and found to be consistent with clu
ster structures derived from two geometries, one having face-centered-cubic
(fcc) packing and the other fcc/hcp (hexagonal-close-packed) layered packi
ng. The fcc-based structures provide the best overall agreement with the ex
perimental measurements. The saturation levels are inconsistent with icosah
edral or decahedral packing, a structure found for Ni-49 and larger cluster
s in earlier experiments. The change in cluster structure between Ni-48 and
Ni-49 (most likely from fcc to icosahedral packing) is clearly evident in
the nitrogen adsorption experiments at both low and high coverages, as well
as with other reagent molecules. (C) 2001 American Institute of Physics.