Author: ["Zhixue Zhu","Christine J. Cardin","Yu Gan","Howard M. Colquhoun"]
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Abstract
Information storage and processing is carried out at the level of individual macromolecules in biological systems, but there is no reason, in principle, why synthetic copolymers should not be used for the same purpose. Previous work has suggested that monomer sequence information in chain-folding synthetic copolyimides can be recognized by tweezer-type molecules binding to adjacent triplet sequences, and we show here that different tweezer molecules can show different sequence selectivities. This work, based on 1H NMR spectroscopy in solution and on single-crystal X-ray analysis of tweezer–oligomer complexes in the solid state, provides the first clear-cut demonstration of polyimide chain-folding and adjacent-tweezer binding. It also reveals a new and entirely unexpected mechanism for sequence recognition, which, by analogy with a related process in biomolecular information processing, may be termed ‘frameshift-reading’. The ability of one particular tweezer molecule to detect, with exceptionally high sensitivity, long-range sequence information in chain-folding aromatic copolyimides is readily explained by this novel process. Monomer-sequence information in synthetic copolyimides can be recognized by tweezer-type molecules binding to adjacent triplet-sequences through complementary aromatic π–π-stacking, with different tweezer molecules showing different sequence-selectivities. Single-crystal X-ray analysis of tweezer–oligomer complexes confirms the tweezer-binding selectivity, and NMR spectroscopy reveals a new mechanism (‘frameshift-reading’) for tweezer-based sequence recognition in chain-folding copolyimides.Cite this article
Zhu, Z., Cardin, C., Gan, Y. et al. Sequence-selective assembly of tweezer molecules on linear templates enables frameshift-reading of sequence information. Nature Chem 2, 653–660 (2010). https://doi.org/10.1038/nchem.699 