Through the combination of the divergent and convergent approaches, coupled with the utilization of the powerful Sharpless "click-chemistry" reaction, two series of sulfonyl-based high-generation NLO dendrimers were conveniently prepared with high purity and in satisfactory yields. Thanks to the perfect three-dimensional (3D) spatial isolation from the highly branched structure and the isolation effect of the exterior benzene moieties and the interior triazole rings, these dendrimers exhibited large second harmonic generation coefficient (d33) values up to 181 pm V(-1), which, to the best of our knowledge, is the highest value so far for polymers containing sulfonyl-based chromophore moieties. Meanwhile, compared with the nitro-chromophore-based analogues, their optical transparency and NLO stability were improved in a large degree, due to the lower dipole moment (μ) and the special main-chain structure of sulfonyl-based chromophore in these dendrimers.
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