Abstract: | The synthesis and second harmonic coefficients, d3,1 and d3,3 as well as the related susceptibilities χ(2)zzz of five series of (NLO-dye methacrylate)-(methyl methacrylate) copolymers were investigated. The NLO-chromophores bound covalently to the polymer backbone were 5-(2,2-dicyanovinyl)-or 4-(2-cyano-2-methoxycarbonyl)vinyl-1-piperidino-2-thiophene (P1 and P2), 4-nitro-4′-alkoxy-stilbene (P3), 4-nitro-3′-methoxy-4′-alkoxystilbene (P4) and 4-nitro-4′-alkoxy-α-cyano stilbene (P5). The second order nonlinear optical properties of corona-poled aligned thin polymer films, using a needle electrode in order to induce noncentrosymmetry, were evaluated. Nonlinear susceptibilities, χ(2)zzz, of the films were derived from the analysis of full-angle Maker fringe patterns at 1064 nm, χ(2)zzz values as high as 1.98×10−7 esu for P2 copolymers and of 1.19×10−7 esu for P3 copolymers could be achieved. |