Epitaxially grown C60 films on CaF2(111) substrates have been studied
by reflection high-energy electron diffraction at deposition temperatu
res of 30-300-degrees-C and average thicknesses of 1-50 nm. At these t
emperatures and thicknesses, C60 forms an incommensurate overgrowth of
fcc-stacked hexagonal layers with a characteristic nearest-neighbor s
pacing of 0.99 nm. Deposition temperatures below 150-degrees-C result
in unidirectional growth in accordance with the crystallographic direc
tions of the substrate. Higher deposition temperatures, however, resul
t in two equivalent, rotated domain orientations characterized by a si
gnificantly lower degree of lattice mismatch (3% versus 16% for the un
idirectional arrangement). The C60 films grown at high temperature pro
duce brilliant reflection patterns indicating a high degree of long-ra
nge order, uniformity and flatness.