The paper describes the syntheses of a NLO-tweezer, alpha,alpha’-bis[N-ethyl-N-{4’-stilbazolyl}-amino]-m-xylene (3), functionalized copolymers 4a [poly(2-bromoethyl methacrylate)/polystyrene], 4b [poly-(2-chloroethyl methacrylate)/polystyrene], and 4c [poly(3-chloropropyl methacrylate)/polystyrene], and NLO-phore 6,4’-(N-ethyl-N-hexylamino)stilbazole. Kinetic analyses were carried out for the cross-linking/quaternization reaction of the NLO-tweezer with copolymers 4a, 4b, and 4c. Energy of activation (E(a)) values of 15.3, 18.8, and 18.4 kcal/mol, respectively, were experimentally determined. Films containing 9.1 wt % of the NLO-tweezer and NLO-phore 6 were subjected to corona poling with heating (90-120 degrees C) for varying lengths of time. The materials displayed improved temporal stability for the second harmonic (SH) signal with an increasing degree of quaternization, and the best temporal stability (at 80 degrees C) for the SH signal was observed for the side-chain NLO polymer (i.e. from NLO-phore 6), which was not crosslinked. The NLO-tweezer, which did form a cross-linked material, showed an initial rapid loss of SH signal; however, the long term signal decay was similar to the side-chain analog.