The gelation process of organic doped silica film fabricated by the sol-gel
technique was investigated by in-situ second harmonic generation (SHG) mea
surements. The SH signal came from the doped hemicyanine molecules which au
tomatically oriented in the film at or near the film-substrate interface. W
e found that film shrinkage during gelation resulted in disordering of the
doped hemicyanine molecules, so the SH intensity decreased during annealing
. Thus, the SHG measurement can be used as a semi-quantitative probe of the
gelation process in that particular region, which was hard to detect using
conventional methods. We found that the time for gelation depends sensitiv
ely on the annealing temperatures. The activation energy of the gelling pro
cess was obtained from the SHG relaxation measurement. In addition, aggrega
ted hemicyanine molecules dissociated with increasing annealing temperature
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