We have studied the thickness dependence of the crystal structure in v
anadyl phthalocyanine (VOPc) films epitaxially grown on KBr(100) surfa
ce. Optical second-harmonic generation observed in oblique incidence i
ncreases nearly quadratically with film thickness up to at least 64 nm
and saturates, indicating a structural change from an epitaxial polar
VO orientation to a nonpolar bulk crystal structure. The latter was a
ssigned to monoclinic structure based on X-ray diffraction. Optical ab
sorption spectra in visible and infrared regions and scanning electron
microscopy also show the structural difference between the films thic
ker and thinner than about 80 nm.