In situ observation of second-harmonic generation (SHG) was made as a
function of film thickness of centrosymmetric copper phthalocyanine du
ring the evaporation process. In order to clarify the origin of the re
latively strong SHG, the experimental results were compared with calcu
lations based on the electric dipole, electric quadrupole and magnetic
dipole mechanisms. The comparison clearly ruled out dipolar origin an
d strongly indicates electric quadrupolar or, more preferably, magneti
c dipolar origin.