A new class of organic/inorganic sol-gel second-order nonlinear optica
l (NLO) materials based on the prepolymer of hexakis(methoxymethyl)mel
amine (HMM) and an alkoxysilane dye (ASD) has been investigated. The N
LO-active alkoxysilane dye containing nitroazobenzene was incorporated
into the melamine matrixes with a weight ratio of 1:1. This organic-i
norganic composite (HMM/ASD) was formed via sol-gel reaction of the re
spective components. The optically clear (HMM/ASD) sample exhibits lar
ge second-order optical nonlinearity (d(33) = 40 pm/V) after poling an
d curing at 220 degrees C for 30 min. The poled/cured HMM/ASD sample h
as better temporal stability at 100 degrees C compared to that of the
poled/cured ASD, due to its higher cross-linking density. This is conf
irmed by dielectric relaxation results indicating that the molecular m
obility associated with the glass transition was suppressed remarkably
for the cured HMM/ASD sample. Furthermore, the second harmonic genera
tion (SHG) relaxations of these NLO-active sol-gel materials were stud
ied via biexponential function curve-fitting.