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We synthesized two novel organic nonlinear optical chromophores - chiral S(+)-N-[p-(4-nitrostyryl) phenyl] prolinol and non-chiral [p-(4-nitrostyryl) phenyl] piperdine - as potential laser-active dyes for photonic applications. Both materials show good optical transmittance in the telecommunication frequency region, desirable solubility in acrylic polymer optical fiber matrices, and attractive fluorescence properties that are advantageous for laser-gain materials and devices. Subsequently, these two chromophores were incorporated into poly(methyl methacrylate) and poly(ethyl methacrylate) and drawn into polymer optical fibers. The relevant properties of these organic dye-doped fibers have been studied, revealing essential attributes of laser-active characteristics.