Abstract: The hyper Rayleigh scattering (HRS) method was applied to determine the absolute value of second-order hyperpolarizabilities ($VBAR$beta$VBAR@) of stilbazolium p-toluenesulfonates and related ionic species in methanol. In general, the $VBAR$beta$VBAR values of stilbazolium derivatives become large with increasing wavelength of absorption maximum and are 1.1 $MUL 10$+$MIN@28$/ $MIN 3.9 $MUL 10$+$MIN@28$/ esu, i.e., 3 - 10 times larger than $VBAR$beta$VBAR of p-nitroaniline. By way of exception, halogenated stilbazoliums showed rather larger $VBAR$beta$VBAR compared with the unsubstituted stilbazolium having almost the same absorption cutoff and maximum. The calculated d value of hydroxystilbazolium p-toluenesulfonate obtained using the present $VBAR$beta$VBAR and the known crystal structure agreed well with the experimental d value by the Maker fringe method. !21
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