We have used the Stern-Gerlach deflection technique to study magnetism
in nickel clusters containing 5 to 740 atoms. These superparamagnetic
particles are highly magnetic, with magnetic moments per atom that de
crease toward the bulk value as their size increases. This approach to
ward the bulk is not monotonic; we observe magnetization minima for cl
usters with closed geometrical shells and maxima for relatively open c
lusters. This result is consistent with enhanced magnetization of the
cluster surface. We also observe a decrease in magnetization with incr
easing cluster vibrational temperature. The implications of various cl
uster geometries are discussed in conjunction with existing chemical p
robe studies and theoretical calculations.